Citation
Coal-tar colors used in food products

Material Information

Title:
Coal-tar colors used in food products
Series Title:
U.S. Dept. of agriculture. Bureau of chemistry. Bulletin
Creator:
Hesse, Bernhard Conrad
Place of Publication:
Washington
Publisher:
Govt. Print. Off.
Publication Date:
Language:
English
Physical Description:
228 p. : incl. tables, diagr. ; 23 cm.

Subjects

Subjects / Keywords:
Coal-tar colors ( lcsh )
Coloring matter in food ( lcsh )
Genre:
federal government publication ( marcgt )
non-fiction ( marcgt )

Notes

Statement of Responsibility:
By Bernhard C. Hesse ...

Record Information

Source Institution:
University of Florida
Rights Management:
This item is a work of the U.S. federal government and not subject to copyright pursuant to 17 U.S.C. §105.
Resource Identifier:
029774918 ( ALEPH )
09099650 ( OCLC )
agr12000256 ( LCCN )
Classification:
S585 .A1 no. 147 ( lcc )
668.7 H58 ( ddc )

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Issued February 10. 1912.
U. S. DEPARTMENT OF AGRICULTURE,
BUREAU OF CHEISTRY-BULLETIN No. 147.
H. W. WILEY, CHIEF OF BURxAU.





COAL-TAR COLORS USED IN

FOOD PRODUCTS.





BY


BERNHARD C. HESSE, PH. D.
Expert, Bureau Chemistry.


WASHINGTON:
GOVERNMENT PRINTING OFFICE.
1912.






ORGANIZATION OF BUREAU OF CHEMISTRY.
H. W. WILEY, Chemist and Chief of Bureau.
F. L. DUNLAP, Associate Chemist, and Acting Chief in absence of Chief.
W. D. BIGELOW, Assistant Chief of Bureau.
F. B. LINTON, Chief Clerk.
A. L. PIERCE, Editor.
A. E. DRAPER, Librarian.
Division of Foods, W. D. BIGELOW, Chief.
Food-Inspection Laboratory, L. M. TOLMAN, Chief.
Food Technology Laboratory, E. M. CHACE, Chief, and Assistant Chief of Division.
Oil, Fat, and Wax Laboratory, H. S. BAILEY, Chief.
Division of Drugs, L. F. KEBLER, Chief.
Drug-Inspection Laboratory, G. W. HOOVER, Chief.
Synthetic Products Laboratory, W. 0. EMERY, Chief.
Essential Oils Laboratory, under Chief of Division.
Pharmacological Laboratory, WM. SALANT, Chief.
Chief Food and Drug Inspector, W. G. CAMPBELL.
Miscellaneous Division, J. K. HAYWOOD, Chief.
Water Laboratory, W. W. SKINNER, Chief.
Cattle-Food and Grain Laboratory, G. L. BIDWELL, Acting.
Insecticide and Fungicide Laboratory, C. C. MCDONNELL, Chief.
Trade Wastes Laboratory, under Chief of Division.
Contracts Laboratory, P. H. WALKER, Chief.
Dairy Laboratory, G. E. PATRICK, Chief.
Food Research Laboratory, M. E. PENNINGTON, Chief.
Leather and Paper Laboratory, F. P. VEITCH, Chief.
Microchemical Laboratory, B. J. HOWARD, Chief.
Physical Chemistry Laboratory, C. S. HUDSON, Chief.
Sugar Laboratory, A. H. BRYAN, Chief.
Sections:
Animal Physiological Chemistry, F. C. WEBER, in Charge.
Bacteriological Chemistry, G. W. STILES, in Charge.
Enological Chemistry, W. B. ALWOOD, in Charge.
Nitrogen, T. C. TRESCOT, in Charge.
Plant Physiological Chemistry, J. A. LE CLERC, Chief.
Food and Drug Inspection Laboratories:
Boston, B. H. SMITH, Chief.
Buffalo, W. L. DUBOIS, Chief.
Chicago, A. L. WINTON, Chief.
Cincinnati, B. R. HART, Chief.
Denver, R. S. HILTNER, Chief.
Detroit, H. L. SCHULZ, Chief.
Galveston, T. F. PAPPE, Chief.
Honolulu, Hawaii, -
Kansas City, Mo., F. W. LIEPSNER, Chief.
Nashville, R. WV. BALCOM, Chief.
New Orleans, W. J. McGEE, Chief.
New York, R. E. DOOLITTrLE, Chief.
Omaha, S. H. Ross, Chief.
Philadelphia, C. S. BRINTON, ('Chief.
Pittsmburg, M. C. ALBRECH, Chief.
Portland, Oreg., A. L. KNISELY, Chief.
St. Louis, D. B. BISBEE, Chief.
St. Paul, A. S. MITCHELL, Chief.
Sain Francisco, R. A. GOULD, Chief.
San Juan, Porto Rico, A. E. TAYLOR, Acting.
Savannah, WN. C. BURNET, ('hief.
Seattle, H. M. LOOMIM, Chief.
2


















LETTER OF TRANSMITTAL


U. S. DEPARTMENT OF AGRICULTURE,
BUREAU OF CHEMISTRY,
"Washington, D. C., January 31, 1911.
SIR: I have the honor to transmit for your approval a report by
Bernhard C. Hesse, a color expert, containing both original chemical
work done in the bureau since the passage of the food law on anilin
dyes used for foods, and a valuable and extensive compilation of the
literature of the subject, especially with reference to the harmfulness
of coal-tar colors and their physiological effects. These data formed
the basis of the opinions stated in Food Inspection Decisions 76, 77,
and 106, and are presented in detail as of scientific and practical
interest to all those concerned in the use of coal-tar colors in foods,
whether as manufacturers, food officials, or consumers. I recommend
the publication of this report as Bulletin No. 147 of the Bureau of
Chemistry.
Respectfully, H. W. WILEY, C ief.

lion. JAMES WILSON,
Secretary of Agriculture.
















CONTENTS.

Page.
Introduction............................................................. 9
Purpose of the investigation........................................ 9
Number of colors permitted......................................... 11
Quality and efficiency of colors permitted........................... 12
I. Identity of coal-tar colors used in food products in the United States
in 1907....................................................... 15
Collection of samples............................................... 15
Classification of samples submitted............................... 17
Green Table numbers........................................ 17
Source...................................................... 18
Patents.................................................... 18
Shades of color................................................ 19
II. Purposes of food coloring............................................ .23
IM. Food color requirements............................................ 25
Adaptability for special purposes.............................. ... 25
Proportion of coal-tar color used.................................... 26
Suitability of shades of permitted colors and mixtures of same........ 28
IV. Conformity of food color market, 1907, to recommendations of the
National Confectioners' Association, 1899........................ 30
V. Some legal enactments relative to the use of coal-tar dyes ............... 35
List of thirteen foreign legal enactments........................... 35
Summary of colors permitted by.these legal enactments .............. 35
Colors said to be permitted under the German law of 18S7............. 37
Definiteness and detail necessary to effect quality control............ 40
State laws prohibiting the use of colors in certain foods, 1909 ........ 41
VI. Recommendations by associations and individuals as to use of coal-tar
dyes as food colors............................................. 42
Cazeneuve and L6pine............................................. 42
Society of Swiss Analytical C(hemi.sts ............................... -43
Tschirch.......................................................... 43
Kayser............................................................ 44
W eyl............................................................. 44
National 'Confectioners' Association................................. 45
Schacherl ......................................................... 45
Classification uf recommendations in the literature................... 46
Conclusions....................................................... 47
VII. Recommendations made by United States color industries and trades
to the Department of Agriculture................................... -47
Antagonistic to all added artificial ('duhr ........................... 48
Concerning restrictions and requirements ............................ 48
VIm. Investigations, other than on animals, bearing on the harmfulness of
coal-tar colors.................................................... 51
Pfeffer........:.................................................. 51
W inogradow..................................................... 52
Heidenhain..................................................... 52
Other authors...................................................... 54
5






5 CONTENTS.

Page.
IX. Compilation under the Green Table numbers of all information avail-
able as to the suitability of coal-tar colors for food.................. 56
General statements................................................. 56
Classification of opinions in literature and in legal enactments showing
condition of the market in 1907 .................................. 62
Classification according to chemical composition and suitability ...... 64
Physiological action of coal-tar dyes .............................. 67
Summary of symptoms...................................... 67
Experiments on dogs ..................................... 67
Experiments on human beings........................... 70
Experiments on small animals............................ 71
General statements.......................................... 71
Complete detailed statement of all combined data .................. 74
Abbreviations of authorities cited ............................. 74
Tabulation by Green Table numbers of physiological and other data 75
Alphabetical index of trade names of coal-tar colors ............. 148
X. Dosage and symptoms ............................................... 153
Confectioner's list as a basis for a rule ............................. 153
Lehmann's rules................................................. 158
Santori's work as a guide to a rule................................ 158
Young's rule.................................................... 159
XI. Oil-soluble or fat colors............................................ 159
XII. Rules and reasons for selecting the seven colors permitted by F. I. D. 76.. 161
Statement of rules............................................... 161
Analysis of three recommendations made to the Department of Agri-
culture ...................................................... 162
Process of elimination ............................................ 166
Reasons for adding Ponceau 3R.................................. 167
Quality, cleanliness, and efficiency ............................... 169
XIII. Lists of colors subsequently recommended by individuals and asso-
ciations....................................................... 169
Ernst ................. ...... .................................... 170
Muttelet's interpretation of the French law........................ 171
Second International White Cross Congress........................ 172
Beythien and lHempel ....... .................................. 173
Summary of three preceding recommendations ..................... 174
Unpublished recommendations of a manufacturer.................. 177
B6hal .......................................................... 177
Conclusions .......... .......................................... 178
XIV Chemical examination of the seven permitted colors, 1907 .............. 179
Need of chemical control........ ....................... ....... 179
First methods of analysis used.................................. 181
M oisture.................................................... 182
Chlorin as chlorids ........................................... 182
Sulphated ash............................................. 182
Total sulphur ............................................... 183
Gutzeit test.................................................. 183
Heavy metals............................................... 183
Total insolubles.............................................. 184
Ether extractive ..... ...................................... 184
Results of chemical examination, 1907.......................... 184
Detailed chemical data on each permitted color ................ 184
Recalculation of analytical data on basis of coloring matter pres-
ent ........................................................ 187
Market quality of the seven permitted colors................... 190






CONTENTS. 7
+
Page.
XV. Guides in determining degree of purity and cleanliness ............... 192
XVI. Analyses of certified lots of permitted colors, 1909-10 .................. 198
Tabulation of results............................................. 198
Comparison of analyses made in 1907 ............................... 201
Conformity of analytical data with theoretical composition .......... 202
Arsenic determinations on 86 batches............................... 204
Suggested requirements for certified colors ........................ 205
XVII. Methods of analysis used in testing colors for certification .............. 210
Introduction.................................................... 210
Naphthol Yellow S.............................................. 211
Ponceau 3R ..................................................... 215
Orange I........................................................ 217
Amaranth ....................................................... 220
Light Green S F Yellowish ...................................... 221
Erythrosin ............................................... 222
Indigo disulphoacid ............................................. 224
XVMi. Addenda......................................................... 225
Additional examination of coal-tar dyes ............................ 225
Supplementary list of trade names of coal-tar colors ................. 227
XIX. Index of authorities quoted ......................................... 227




ILLUSTRATION.

Page.
FIG. 1. Apparatus used in the determination of arsenic ...................... 213



















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COAL-TAR COLORS USED IN FOOD PRODUCTS.


INTRODUCTION.
PURPOSE OF THE INVESTIGATION.
For the purposes of the investigation reported in the following pages,
the legitimacy of the coloring of food and food products under certain
conditions is regarded as established; the ethical and dietetic aspects
of the question of food coloring are not here considered.
The means at hand for coloring food products may be conveniently
classified as vegetable, animal, mineral or inorganic, and synthetic
or so-called coal-tar colors or dyes. Representatives of each of these
have at one time or another all been used in the coloring of food, and
the laws of various European and American States have, from time
to time prohibited the use of certain specified members or all of each
or some of the foregoing classes. It is therefore obvious that even
for the legitimate purposes for which food can be colored, improper
means are at command, and some of these, if not all, have been
prohibited by law at some time or another.
It is the function of the present work to determine what members
of the synthetic or coal-car colors should be considered legitimate
for coloring foods. It is confidently believed flOat the material
collected in tlhe following pages points clearIly and solely to the
following conclusions:
1. Coal-tar dyes should not be used ilndiscrimfinately in foods.
2. Only specified coal-tar dyes should be used in foods.
3. Only tested and certified dyes should be used in foods.
The work here reported has furnished the basis for Food Inspection
Decisions Nos. 76, 77, and 1o0(, issued July 13, 1907, Sepltember 25,
1907, and March 25, 1909, respectively, and thie investigation itself
was practically terminated January 1, 1910.
The effect of these decisions lias been to restrict thle coal-tar colors
permitted for use in foods to seven spl)ecified and enumerated colors,
until such time as it shall be shown with reasonable conc'lusiveness
that other colors should be adldedl to suich list; and further, nil coal-tar
colors permitted for use in food are to be of a degree of purity and
cleanliness acceptable to the Department of Agriculture, and are to
be so certified.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


In order to avoid any uncertainty as to the chemical composition
of the enumerated colors, direct reference is made in Food Inspection
Decision No. 76 to a standard work in which such chemical composi-
tion is clearly and unequivocally set forth. The relevant parts of
Food Inspection Decision No. 76 are as follows:
The use of any dye, harmless or otherwise, to color or stain a food in a manner whereby
damage or inferiority is concealed is specifically prohibited by law. The use in food
for any purpose of any mineral dye or any coal-tar dye, except those coal-tar dyes
hereinafter listed, will be grounds for prosecution. Pending further investigations
now under way and the announcement thereof, the coal-tar dyes hereinafter named,
made specifically for use in foods, and which bear a guaranty from the manufacturer
that they are free from subsidiary products and represent the actual substance the
name of which they bear, may be used in foods. In every case a certificate that the
dye in question has been tested by competent experts and found to be free from
harmful constituents must be filed with the Secretary of Agriculture and approved
by him.
The following coal-tar dyes which may be used in this manner are given numbers,
the numbers preceding the names referring to the number of the dye in question as
listed in A. G. Green's edition of the Schultz-Julius Systematic Survey of the Or-
ganic Coloring Matters, published in 1904.
The list is as follows:
Red shades: 107. Amaranth. 56. Ponceau 3 R. 517. Erythrosin.
Orange shade: 85. Orange I.
Yellow shade: 4. Naphthol Yellow S.
Green shade: 435. Light Green S F Yellowish.
Blue shade: 692. Indigo disulfoacid.
Each of these colors shall be free from any coloring matter other than the one
specified and shall not contain any contamination due to imperfect or incomplete
manufacture.
The reasons, broadly considered, which led up to these food inspec-
tion decisions are given in concise fashion in this introduction.
Looking over the restrictions placed upon coal-tar colors by the
lawmakers of the various countries it will be found that certain
colors are in some instances specifically prohibited and in other
instances that certain specific colors, or classes of colors, and only
such, are permitted for the legitimate purposes of food coloring.
Private organizations, such as the Swiss Society of Analytical
Chemists and the National Confectioners' Association in the United
States, have also made recommendations permitting specific colors
only, and in addition specifically prohibiting others. Individual
authors have likewise made similar recommendations. The control
of the quality of the food colors practiced on the part of those Gov-
ernments which restrict tlhe use of coal-tar colors to certain individ-
uals, so far as any publications show, has not been very extensive.
The action taken against the use of coal-tar colors for food-coloring
purposes has ranged all the way from absolute prohibition of their
use for any purpose whatsoever to the practically unlimited use in
legitimate food coloring operations of all but two of such colors.


10





INTRODUCTION.


Intermediate between these two extremes we find the prohibition of
a greater number than two, or of all the members of this class except
certain specified colors, and even here with the restriction that they
shall be used only for certain legitimate food-coloring purposes.
It would be desirable to have a number of coal-tar colors of estab-
lished harmlessness specifically permitted, particularly if the number
be sufficient to meet all the legitimate demands arising in the food-
coloring art. To prohibit only specified coal-tar colors and, by
implication, to permit all the rest of this class, would allow tlhe
unrestricted use of newly discovered colors, and all other coal-tar
colors not examined as to their effect on health. A limited list of
permitted coal-tar colors which would make the use of all coal-tar
colors outside of the permitted list illegal would properly protect
the health and could work no substantial hardship upon those
engaged in food coloring. Any such hardship would be avoided by
providing that if it is shown that none of the colors of the permitted
list meets certain legitimate requirements and that coal-tar colors
outside the permitted list are capable of satisfying this need and are
in and of themselves harmless the permitted list can be expanded by
the proper authorities to meet additional needs or growing require-
ments without exposing the public health to any risk.
NUMBER OF COLORS PERMITTED.
It will be shown in the following pages that in thle summer of 1907
there were on the market of the United States SO different chemical
individuals, dr so-called coal-tar colors, offered for the coloring of
food. It has been known since 1888 that it is unsafe to attempt
to predict the harmfulness or the harmlessness of coal-tar colors by
inference or analogy; therefore an ideally perfect permitted list should
contain only such colors as have each been examined physiologic-ally,
separately, and specifically, and their harmlessness determined by
actual test. Out of the 80 colors referred to 30 had not been exam-
ined at all, so far as the literature shows, and therefore their harm-
lessness is certainly open to question; 26 had been examined physi-
ologically, and the published accounts with respect to their harm-
lessness or their harmfulness are in each case contradictory; oni 8
none but adverse reports were to be found in literature, leaving
only 16 out of 80 colors on the market which had been established
with more or less certainty as harmless-tlhat is, thle users of these S
colors were deliberately taking chances with thle public health, since
the harmful nature of those 8 had for a long time past been known to
those conversant with such subjects; the use of the 26 tldoulbtful
colors is more defensible than thle use of the S known to be harmful.
Out of the 30 of whose action nothing was known it can not lbe said






COAL-TAR COLORS USED IN FOOD PRODUCTS.


how many are or are not harmful, nor can the risk forced upon the
public health be satisfactorily measured.
This brief summary must suffice for the present as a justification
for the restrictions of the permitted colors to 7 in number. The full
reasons for each and every step will appear in their proper places in
the pages following.
QUALITY AND EFFICIENCY OF COLORS PERMITTED.
An examination of 30 specimens representative of the 7 selected
permitted colors on the United States market in the summer of
1907 disclosed such a condition of uncleanliness of product, or care-
less or improper manufacture, and the use of such utterly inferior
qualities of products for food coloring purposes, that control over
the quality of the seven permitted colors seemed necessary. The
results of the work in the making and maintaining of standardsof
quality for each of these seven colors also justify this control. That
there was in 1907, and for a year or more later, a considerable diver-
gence of opinion among chemists as to what should be the proper
quality requirements for these colors is shown by the fact that out
of 72 foundation certificates offered in accordance with Food Inspec-
tion Decisions Nos. 76 and 77, 57 were rejected on their face because
they did not comply with the standards of quality then in mind,
or then shown to be commercially attainable. Much objection has
been made by many of those whose certificates were rejected on the
ground that the standards then in mind were unreasonable, unjusti-
fiable, and nonattainable. The actual results, however, are that
with very few exceptions the standards in mind early in the work
have all been exceeded in practice; the 41,000 pounds (20.5 tons)
of certified colors now in existence made in 97 batches, or an average
of more than 420 pounds per batch, are, with the exception of perhaps
one or two first batches, far cleaner than was expected when the 57
certificates above referred to were rejected.
There has been no complaint against the permitted colors for want
of efficiency or for tlhe possession of unsuitable attributes, which has
been pressed or sustained with any such earnestness as would rea-
sonably be expected if the defects complained of were as great as
they were represented. Complaints have been made against the
yellow, when used in acidulated fruit sirups, on account of its pos-
sessing a bitter taste; the proof of this, so far as any has been offered,
was for a long time not of a convincing nature, and it was two years
after the first objection was raised before any concerted or positive
action was taken by those interested. The yellow has also been
criticized because it is not sufficiently fast to light; although it was
satisfactorily shown that another yellow was faster to light than the
permitted yellow, no one has maintained that the yellow desired


12





INTRODUCTION.


was actually preferable to the permitted yellow wholly and solely
because of its superior fastness to light.
The blue has been criticized because it is not of the proper shade
to permit of its use in the bluing of sugar, but the substitute offered
therefore has not been supported by its sponsors in a way to indicate
that a defect of serious magnitude exists. On the grounds of suffi-
ciency and of efficiency the list of permitted colors selected appears
to have been justified by the absence of any real or substantial com-
plaint against them, on either or both of these grounds, during a
period of more than three years.
None of the seven permitted colors is patented; their manufacture
and their purification are open to all, and none of the 80 colors on
the market in the summer of 1907, with perhaps one exception, had
been discovered since 1891; in other words, the advances in the coal-
tar industry from 1891 to 1907 had added nothing to the colors
serviceable to the art of food coloring.
The list of colors permitted in Food Inspection Decision No. 76
embraces, therefore, a sufficient number of colors for all legitimate
food-coloring purposes, the coloring of fats, oils, butter, etc., excepted,
for which no suitable color had been examined and reported in the
literature as being harmless and fit for use in foods; they can be made
by any one; no one can have a monopoly in any one of them by
virtue of patents; any competent maker can make all or any of
them and purify them to the required degree of cleanliness. The
standards growing out of the control exercised by the Department of
Agriculture are such as to insure that the colors used for food-coloring
purposes possess a proper degree of cleanliness and such a degree of
cleanliness is commercially feasible and is a commercial reality.
The policy adopted in this respect is therefore justified not only
from the viewpoint of the history of the attempts on the part of
various governments to control the quality of food colors, but also
by the results actually obtained by its adoption. This policy of
restricting food colors to certain chemical individuals and demand-
ing that those possess certain qualities is in complete harmony with
the following suggestion made to the commission on rules and regu-
lations under the food and drugs act, at its hearing in New York,
in September, 1906.
Any kind of a harmless color should be permitted, provided it is not a color., generally
known to be poisonous, or generally found to be poisonous, or one that may be almost
impossible to be produced without containing some poison within itself when finished
and ready for use. Coal-tar colors, as a class, should not be prohibited, but all those
coal-tar colors generally found to be poisonous, or which are hard to prtoduce without
containing some poisonous properties when ready for use, should be forbidden the
privilege of being used, or offered for sale for use in food.
Under the provisions of section 2, we have this to recommend to the commission,
that every person selling or using a coal-tar color in food or drink, should be required


13






COAL-TAR COLORS USED IN FOOD PRODUCTS.


to secure, either on his own account, or from the person from whom he buys such color,
a certificate to the effect that the identical color used has been tested for poisonous
ingredients, and is, to the knowledge of the chemist making the test, absolutely harm-
less. The chemist should be required to be a competent physiological chemist, and
must certify as above under oath. This would mean not that each package of color
would have to be tested, but that every batch would have to be tested, and the
certificate would then be held to relate to every batch. Such tests should be made
in the United States and the chemist certifying should reside in and be a citizen of
the United States.
It should not be deemed sufficient to have any particular brand of coal-tar color
tested once, and a blanket certificate given, covering the whole brand as long as it may
be sold, but every ounce of coal-tar color put out by a color manufacturer should be
shown by actual test to be harmless.
While the exact mode of reaching the end in view is somewhat dif-
ferent from the one suggested above, yet the fundamental object, that
each batch of color used in foods shall be specifically tested, and that
such colors shall be harmless, is attained with reasonable certainty;
and although there are colors other than these seven which are
undoubtedly equally as little objectionable, and while it is true that
the present policy contemplates the permitted use of but seven
specific colors, yet that policy, as before outlined, is sufficiently broad
and elastic to enable the addition of a color to the permitted list,
when it is shown that such color really fills a need, not properly satis-
fied by one of the colors already permitted or some combination of
these, and is in and of itself harmless. There can be no objection to
the expansion of the list to such an extent as to include every harmless
coal-tar color in existence; but the burden of proving such real need
and harmlessness is very properly placed upon those who are seek-
ing such expansion.
As far back as 1892 the following statement was made on page IV
of the Leffmann translation of Weyl's book on coal-tar colors, in con-
nection with the various European legislative enactments: "It is
certain that none of these plans is even approximately satisfactory
and the problem will be even more difficult of solution in the United
States; indeed, it seems to me to be unsolvable." In view of this
opinion the results of the food inspection decisions as herein shown
may properly be regarded as, at least, a step in the right direction
toward the solution of this problem.
Tllis opinion is further supported by C. A. Neufeld who, in review-
ing Food Inspection Decision No. 76, says: "The idea of permitting
only specific selected coloring matters for use in the production of
articles of food, and of excluding all other colors from such uses, must,
in tohe interest of control of articles of food, be regarded as an extra-
ordinarily happy one; a similar regulation is to be urgently recom-
mniended for our own country." (Zts. Nahr. Genussm., 1908, v. 15,
P. 434.)


14






IDENTITY OF COAL-TAR COLORS, 1907.


IDENTITY OF COAL-TAR COLORS USED IN FOOD PRODUCTS IN
THE UNITED STATES IN 1907.
COLLECTION OF SAMPLES.
The question "Which coal-tar colors shall be permitted for use in
coloring such food products as are to be consumed within the United
States?" can be answered, "All colors now in use, or to be used for
that purpose, provided they are harmless and necessary as defined on
page 14."
This involves the further questions:
1. Which coal-tar colors of the 695 different chemical individuals
now on the world's markets are actually used in the United States for
that purpose?
2. If restricted to such coal-tar colors as are now in use in the
United States for this purpose, would this be likely to hamper or inter-
fere with the invention of other coal-tar colors suitable for the
coloring of food ?
It would be physically impossible to go to every user of coal-tar
colors in food products in the United States and obtain specimens of
the coal-tar colors so employed; this would be impracticable not only
because of the large number of such users, and their wide geographical
distribution, but also because they often do not know what they arc
using, and further because of a reluctance, undoubtedly to be encoun-
tered among many, to disclose the nature of the products employed.
This is rendered more than likely by the attitude of some of the
makers of coal-tar colors, or their accredited agents, as will be shown
later.
However, the sources of coal-tar colors are limited in number. By
reference to pages IX and X of "A systematic survey of the organic
coloring matters," by Arthur G. Green, published in London and New
York by Macmillan & Co. (Ltd.), in 1904 (hereinafter referred to as
"Green Tables"), it will be seen that there are approximately 37
different concerns the world over engaged in the manufacture of (coal-
tar colors. Therefore a canvass of these sources for such coal-tar
colors as in their judgment, or in their business l)ractice, they regard
as proper for use in food products, is the best way of arriving at a fair
demarcation of tlhe field of coal-tar colors here in question.
Communication was therefore had with 13 actual manufacturers of
coal-tar colors, in an endeavor to obtain from them such coal-tar
colors as in their judgment or business practice are suitable for use, or
are used in food products.
A request was also made for information as to the chemical com-
position of the coal-tar color specimens submitted; in order to avoid
confusion, it was further asked that reference be made to tlie Green
Tables, in wlich each chemical individual or coal-tar color has its


15






16 COAL-TAR COLORS USED IN FOOD PRODUCTS.

own number, and if any of the contributed specimens was not so listed
that the chemical composition be stated in a manner analogous to
that used in the Green Tables. This procedure was necessary in
order to reduce the terminology to a common and nonequivocal basis.
Out of the 13 makers, or their accredited sole importers or selling
agents in the United States, who were consulted, 9 have supplied the
specimens requested; the remaining 4 promised to contribute, but
have not done so. In the following table is shown the amount and
character of the information obtained:

Tabulation of distribution of replies and character of information received.

Geographical distribution. Number Number
Number of of No
of samples samples composi-
Country. Coal-t Maker Ms Makers samples referred tion orabgu
Coal-tar asked not contri- to referred axnbigu-
Country. to ouis ter-
color to send sending sending buted. Green to ouster-
makers. samples. samples. sap1 Tables. Green minology.
Tables.

Germany ............. 16 6 ......... 6 181 106 1 74
England.............. 8 1 ....... .... 1 12 12 ....................
France............... 5 1 1 ............. .......................... . . ..........
Sw itzerland .......... 5 3 3 .......... .......... .......... ........ ..........
United States........ 1 2............ 2 61 35 21
Holland ................................................. ..... ......... ........ ..
Belgium............. 1 ...... ........ .................... ..... .........................
Total........... 7 13 4 9 254 153 6 95


In order to make provision for the 24 makers listed in the Green
Tables and not included in the 13 makers addressed requests for
samples were sent to two domestic houses which import coal-tar colors
from scources other than tlhe above, for use in food products; their
products must fairly represent any of the colors not covered by the
13 makers addressed. Of these two importers, one responded with
13 samples, and of each lie gave the number in the Green Tables
corresponding to each specimen; the other importer has not redeemed
his promise to contribute specimens.
A third importer volunteered the Green Table numbers of four out
of five coal-tar colors used in his business, but could not even approx-
imately say what the remaining color was chemically. lie did not
contribute any specimens, nor was that necessary at the time this
information was volunteered.
A fourth importer contributed specimens of five coal-tar colors
needed in his business, but was able to give Green Table numbers for
only three of them; lie ('ould not give even approximately the 'liem-
ical composition ()f Ilie remaining two.
Outof tlie 17 responsible concerns consulted 5, or 29 percent, have not
found it to their interest to contribute either specimens or information.






IDENTITY OF COAL-TAR COLORS, 1907. 17

CLASSIFICATION OF SAMPLES SUBMITTED.

GREEN TABLE NUMBERS.

Out of the 284 specimens contributed, or reported on, 172 (60.6
per cent) were identified as to their chemical composition, by refer-
ence to the Green Tables; 6 (2.1 per cent) were otherwise unequivo-
cally identified chemically, and for 106 (37.3 per cent) the makers,
or their responsible agents, declined to state the chemical composi-
tion, i. e., 62.8 per cent were unequivocally identified, and the remain-
ing 37.3 per cent were not so identified.
The specimens submitted are therefore divisible into the following
three classes:
Class I. Those for which numbers were given in the Green Tables,
numbering 172.
Class II. Those whose composition was given in chemical language,
numbering 6.
Class III. Those whose composition was not given in any lan-
guage capable of correct and certain translation into chemical terms,
numbering 106.
Consider Class I. The Green Tables, page VI, divide the coal-tar
colors into 21 groups, comprising 695 different chemical individual
coal-tar colors. The 172 members of Class I number in all 74 indi-
viduals, or 10.6 per cent of the Green Tables, and fall into 11 f the
21 groups of those Tables.
The following table classifies the samples according to the Green
Table groups:

Green Table groups and number of collected samplesfalling within thenim.

Collected samples I Collected samples
Number falling into the Number falling into the
Color groups of the of mem- several groups. Color groups of the of mem- several groups.
Green Tables. bers in _____G____ reen Tables. bers in _______
group. group.
Number. Percent. Number. Per cent.

Nitro .............. 6 1 16 Anthracene....... 37 ....................
Monoazo........... 126 30 24 Indophenol........ ....................
Disazo ............. 204 11 5 Azin ...............I 38 2 5
Trisazo. ....... .... .. 46................ .. Oxazin............ .i 32 .......... ..........
Tetrakisazo........ 11 .................. Thiazin............ i 9 2 12
Nitroso............ 5 1 20 Thiazol ............ ......... .........
Stllbene............ 18 .......... ........... Quinolin........... 4 1 2
Oxyketone......... 8 ...... .. ..... . Sulph id ............ 1 .......... .......
Dlphenylmethane.. 2 1 Indigo ............ 7 1 13
Triphenvlmethane. 1 6 15 23 : i ...
Xanthene.......... 35 9 26 (9> 74 iI.i.
Acridin ............ 1 6 .....................
972____91Bu._ I 147122___
972910-Bull. 147-12--2






18 COAL-TAR COLORS USED IN FOOD PRODUCTS.

SOURCE.

The distribution of the 74 different chemical individuals of Class I
among the 12 different sources from which they were obtained is as
follows:

Distribution of the 74 different samples of Class I among the 12 sources supplying same.

Number Number
of sources I of sources,
from from
Number. Percent. Number. Percent. which
each each
came. came.

35 417.3 1 1 1.35 7
20 27 2 1 1.35 8
4 5.4 3 0 .......... 9
4 5.4 4 1 1.35 10
5 8.1 5 11 .......... 11
3 2.7 0 ......... 12


It follows from this table that there is very little unanimity among
the different concerns furnishing coal-tar colors for use in food prod-
ucts as to which of their products are desirable, necessary, or suitable
for such use.
Inspection of this table shows that only three colors out of 74,
or 4 per cent, were wanted by more than half of all the sources; that
only 6, or 8.1 per cent, were wanted by half of the sources; and that
not one of the colors was wanted by all the sources. Tlis last state-
ment is true of manufacturers as well as importers, each group taken
by itself.
PATENTS.

This lack of unanimity is not due to the patent situation, because
not more than one of these 74 products is patented, and it is more
than likely that the United States patent on this product has long
since expired.
Moreover, only 6 of the 12 sources offered colors at one time
patented by themselves or others. The total number of such ex-
patented products is 45, and of these only 22 were offered by those
who had patented them; the remaining 23 were offered by sources
other than tihe ex-patentees, and were not offered by such
Px-I) Itentees.
i'aletlt I colors.
Total num- Total num-...
Totier of Ex.patented ber of Ex.patented
patenlcd] products patented products
pr'loaoffered by products offered by
'rol hwts i ^ product patentee.
ofTfere. patentee. offered. patentee.

4 '2
7 4 45 22


amom.







IDENTITY OF COAL-TAR COLORS, 1901.


19


It would, therefore, seem to be rather clear that others think more
favorably of such ex-patented products as food colors than do the
original patentees. In view of the fact that the latter would generally
be in a better position, and would have greater opportunity than any
one else to judge of the suitability of the patented products for use
in food products, it may well be inferred that such products are not
altogether free from disadvantages as food colors.
The second of the two questions propounded, namely, If restricted
to such coal-tar colors as are now in use in the United States for this
purpose, would this be likely to hamper or interfere with the invention
of further coal-tar colors suitable for the coloring of food products ?
can be answered "No" because none of the colors submitted was
discovered later than 1891; out of the 214 coal-tar colors since then
discovered not one was among those submitted for use in foods, and
out of the 481 discovered in 1891 and prior thereto, only 74 were so
submitted, or 2 out of every 13 of such colors. In the following
table these data are given year by year:

Coal-tar colors discovered from 1740 to 1891.


Num-
ber of
sub-
mitted
colors
discov-
ered.


Total
num-
ber of
coal-
tar
colors
discov-
ered.


Year
of dis-
covery.


Nu m-
ber of
sub-
mitted
colors
discov-
ered.


1 6 18S1 4
1 4 ISS2 5
6 12 1S'S3 9
5 9 1884 3
2 10 1 K5 2
12 26 1896 3
23'


Total
num-
ber of
coal-
tar
colors
discov-
ered.

11
20
25
16
21
32


'Year
of dis-
covery.




*1S87
1 SMq 7
S1S90
1891
Total.


Nurn- Total
ber of num-
s:ib- ber of
milledl coal-
molors tar
colors colors
disco- d6co I-
ered. ered.


1 29
1 36
1 46
3 33
74 378


SHADES OF COLOR.

The sufficiency of the 74 colors used for food-coloring purposes in
the United States, for any and all tinctorial ranges, no matter how
refined, appears from the following table:


Green Table numbers of the 74 submitted colors shiou iin shudcs u nd number of sources
su pp yIing ezc'h.


Shadea.


Number of sources out of a possilile 12 oIferiring each color.


1 i2 3 4 5 *; 7 9 o


104 i 5 ...... .... 106 103 107 . .. .
1 .. .... .... ..... ....... .
i11 5 i ii.......... ..... ....
240 4612


Toltal I
mninller
of dyes
ol'relt I
for each
shade.

12
S. .. ... .. .


Year
of dis-
covery.



1740
1856
1859
1861
1862
1863
1867


Nuum-
ber of
sub-
mitted
colors
discov-
ered.


1
1
1
2
1
1
1


Total
num-
ber of
coal-
tar
colors
discov-
ered.

1
3
1
3
5
3
3


Year
of dis-
covery.




1871
1S74
1 .75
1876
1.477
1878
1879


R ed ... . ............ ... ..







20 COAL-TAR COLORS USED IN FOOD PRODUCTS.

Green Table numbers of the 74 submitted colors showing shades and number of source
supplying each-Continued.


Shades.


Blue red......................



Yellowish red...............

Scarlet......................

Bluish scarlet................
Yellow......................


Reddish yellow..............
Orange yellow..............
Greenish yellow............
Orange.....................


Blue........................



Green blue.................
Violet......................
Blue violet.................
Grayish violet..............
Green......................

Blue green..................
Yellow green...............
Brown.....................


Reddish bjrown.............
Blue black..................
Blun to blu.ish red to vIlet,
according to brand .........
Oll-solublp colors .............
Total...................


Number of sources out of a possible 12 offering each color.


54
516
53
64
56
89
269
329
9


667
18
97

439
476
480
655
440
468
464
287
433
4.34




101
137
139


IRS

6001

160
4935
35'


2


502
518
520
523
512

55






84
14


17
85
95
650


425




692


452 ......


398

427






201





II


20


428


4


448










510


435








197


4 4


5


504
517









8


451


94




13


. . . . . . .

5 3


86


9 I10


1 .. ....


The six colors comprising Class II (those not listed in the Green
Tables but whloso composition was avowed or disclosed) are one
black, one yellow, and one orange among the water-soluble colors,
and three yellows among the water-insoluble colors. Therefore two-

thirds of the United States market as thus disclosed calls for a total


4


Total
number
of dyes
offered
for each
shade.

7



3

3


1
7


2
2
2
6


6
.... .. ..

1
3
1

1
4

1
1
3



2
1


. I.- I


4


74






IDENTITY OF COAL-TAR COLORS, 1907. 21

of 80 different chemical individuals, of which 73 are water-soluble and
7 are water-insoluble and are used as oil or fat colors. The remain-
ing third of the makers or dealers either do not possess the information
or are unwilling to give it. No attempt has yet been made to enter
systematically into this unknown region, but careful examination
warrants the belief that it can add nothing of material value to
the data already obtained which show a total of 23 shades for the
73 water-soluble coal-tar colors, summarized as follows:

Number of coal-tar colors.

5 red shades........................ 26 3 green shades6...................
4 yellow shades................. 14 2 brown shades..................... 5
1 orange shade...................... 7 1 blue-black shade................. 1
2 blue shades..................... 7 1 black shade..................... 1
3 violet shades..................... 5 1 blue to violukt .hade............... 1

The water-insoluble colors numbering 7 are not included, but will
be treated separately (p. 159).
This view of thle state of the United States market at or about the
middle of the year 1907 is without question a true reflection of that
market as far as it goes and the actual extent of the coal-tar color
market beyond those covered by this canvass of it is not likely to be
very great. In support of this view is the interchangeable treatment
of formerly patented products, the great lapse of time since a new food
color was discovered, and the fact that out of the 74 colors submitted
and contained in the Green Tables only 23 are now less than 25 yeaLrs
old, and none is less than 16 years old.
All the Green Table numbers and tlhe number of sources out of a
possible 12 offering them are given in tlhe following table:

Number of sources, out of a possible 12, ojfcring colors de.igpated in 1907.

G reen G green (;reen rcn
Table sources. 'Tl:)le Sources. Tihble Suurres. T.l1'il Suuurc'.s.
No. No. No. No.

1 4 1W 2*j1 1 4:1. i i
X 5 .49 24 i 19y 4 -A I
9 1 94 5 o*2 7 1 .H i ,'
I.1 2; IN 1N A 14
10 1 95 2 3.9 I 1- ;
11 2 97 1 3 -I 4
13 i 6 101 1 425 t3 :12 3
14 I 2 103 6 427 2 5 .. 1
4I? 3
17 "1 04 1 428 :3 J I
1. 1 Io5 1 433 1 5M 1
49 1 kli 5 4.14 1 '-1) 2
5 I liot 7 i 41 1 .r
1 11.S "J 4 .1!1 1 ., b4 1
55 '2 13:17 1 44fl i'l 1
b6 1 139 1 44h 4 ,.'14
1i0 1 144 2 451 .' i:.. 1
14 | 6 li9 1 4.72 ".' A.7 1
65 l 1 44iJ C 2*
84 2 197 4 46.4 1
85 2 I 21l 2 46W 1

Italicized figures Indickiite colors permitted by F. 1. 1). 76.






22 COAL-TAR COLORS USED IN FOOD PRODUCTS.

Nine manufacturers sent 261 specimens, an average of 29 each,
distributed as follows: 70; 38; 20; 20; 15; 43; 25; 18, and 12. Two
importers sent 5 specimens each, and one 13, a total of 23 specimens,
and an average of 8. These figures reflect a diversity of opinion as
to what is needful for food coloring, since each one of these 12 makers
or importers believed that for all practical food-coloring purposes
his selection was complete and sufficient.
Classifying the 284 specimens as red, yellow, brown, orange, blue,
green, violet, and black, the following table is obtained showing the
different requirements of each of the 12 makers or importers to
produce the necessary shades of the eight colors mentioned:

Total specimens submitted, grouped by makers and colors, showing number of shades
required by each.

Number
MedYcl- of Tot'hl
Maker's Red. l Brown. Orange. Blue. Green. Ve. Black. shades sped-
number. lw let. wanted mens.
by each.

1 ............ 25 18 14 4 2 5 2 ....... 7 70
2............ 10 6 2 1 3 1 2 ....... 7 25
3............ 7 5 ........ 2 1 1 1 1 7 18
4............ 11 10 10 5 2 2 3 ....... 7 43
5............ 6 2 ....... 3 4 2 2 1 7 20
6............. 4 3 2 1 3 1 1 ....... 7 15
7............. 6 2 1 2 1 ..... ............. 5 12
8........... 5 4 ........ 1 1 1 1 ....... 6 13
9........... ... 6 4 1 3 ....... 4 2 ....... 6 20
10............ 13 10 2 3 5 4 1 ....... 7 38
11 ........... 3 1 ........ I ..... .... ... ............. 3 5
12......... .. 3 1 ................ ....... .... .... .......3 5
Total.... 99 66 32 26 22 22 15 2 .......... 284
Percent..... 34.86 23.24 11.27 9.15 7.75 7.75 5.28 0.70 .......... 100
Maximum.... 25 18 14 5 5 5 3 1 .......... ........
Minimum.. 3 1 ........ .3 1........ ..... .. ..... .......... ...... ................
Average.... 8.25 5.50 2.75 2.17 1.83 1.83 1.25 0.17...... ........
Permitted.... 3 1 .............. 1 1.. ...... ..................


From this table it appears that not one of the 12 sources desired all
of the 8 shades into which tihe 284 specimens are classifiable to make
up a complete set of food colors; 7 out of the 12 sources wanted 7 of
the 8 shades; 2 sources wanted 6 out of the 8 shades; 1 source wanted
5 of the 8 shades, and 2 sources were content with 3 out of the 8
shades.
It will be noticed that the permitted list given in Food Inspection
Decision No. 76 Iprovides for 7 d(yes covering 5 out of the 8 shades of
the above classification. The 3 missing shades are brown, violet,
and black; the shades provided are red, yelloh)w, orange, and blue.
It will also be noticed that on the whole 6 out of the 8 shades were
not wanted by one or more of tlihe 12 sources. Tleio italicized shades
are the ones not provided for by the permitted list of Food Inspection
Decision No. 76.
Brown was not wanted by 5, nor orange by 1, blue by 3, green by 2,
violet by 3, nor black by 10.





PURPOSES OF FOOD COLORING.


The combinations not wanted were as follows: Five sources omitted
black only; 2, brown only; 1 blue and black; 1 brown and black; 1
green, violet, and black; and 1 brown, blue, green, violet, and black.
Not one of these 12 sources wanted only the three colors not found
on the permitted list, and 2 sources did not want any of the three
missing shades nor two of the permitted colors.
In view of this large difference of opinion among the 12 sources as
to the shades needed to make a complete set of food colors, the 5
shades selected for the permitted list of Food Inspection Decision
No. 76 seem reasonably close to any consensus of opinion derivable
from the tabulation of the collected facts.

II. PURPOSES OF FOOD COLORING.
The use of any color which conceals inferiority, or which gives an
article an appearance better than it properly possesses is, of course,
illegitimate, and such cases are not here considered. Among such
uses may be mentioned that of color in pastry to impart a yellow
color thereto, implying the presence of eggs, when they are either
wholly absent or are not present in sufficient quantities to produce a
shade of color which would indicate a superior quality. Such color-
ing is frequently resorted to in macaroni, spaghetti, noodles, and the
like, and it has also been stated in the literature that such coloring
has the additional function of concealing dirt actually present in tlhe
flour.
The addition of red coloring matter to meat products to give them
an appearance of freshness which they do not of themselves possess;
the addition of red coloring matter to strawberry, raspberry, and
similar jams, jellies, and preserves, to give them a color indicative of
exceptional quality, even though they may contain none of the fruit
whose presence is intimated by the label on the product; the injection
of red coloring matter into ordinary oranges to give them the appear-
ance of blood oranges; the sprinkling of lemons and oranges with
green coloring matter to give them tihe appearance of a particular
origin or of a particular state of ripeness wlien such origin or state of
ripeness is without foundation in fact; the injection (of redl coloring
matter into watermelons to give them the appearance of ripenlless,
which ripeness they dlo not possess, are practices nmet 1lore or less
frequently.
Among thlie purposes for wlicli food colors atire saili to be used 1 anid
the foods so colored, tlie following atire mentioned in tlie literal tire:
In European rountru's.
1. Macaroni is cnlord with Dinitnrocr ,1l (2 .Arch. Phaurm., .t sr., '.', p. fI2l
and Martius Yellow (3) ( Weyl, llandbuch).
2. Cordials and liiqueurs with l)init I ru rrt. i 12 (Arch. J'harmn .?id se'r., i !, t'i. : .


23






24


COAL-TAR COLORS USED IN FOOD PRODUCTS.


3. Oranges: Biebrich Scarlet (163) (Weyl, Handbuch).
4. Pastry: Dinitrocresol (2) (Weyl, Handbuch).
5. Butter: Dinitrocresol (2) (Weyl, Handbuch).
6. To whiten flour: Anilin blue (457) (Zts. Nahr. Genussm., 1906, v. I1, p. 298).
7. Noodles are colored to cover up cigar butts, burnt matches, mineral oil, etc.
(Zts. Nahr. Genussm., Vol. 11, p. 1018).

In the United States.

8. Jellies, fruit sirups, soda sirups, jams, ketchup, cheap cordials, lemon extract,
milk, butter, cheese, ice cream, confectionery, pastries, flavoring extracts, mustard,
cayenne pepper, sausage, noodles, wines, and liqueurs (Winton, Connecticut Agricul-
tural Experiment Station Report, 1901, pp. 179-182).
9. Cattle feed is colored yellow (Gudeman, J. Amer. Chem. Soc., 1908, v. 30, p. 1623).
10. "Egg color" (399); "Macaroni color" (94); "Tomato catsup color" (105);
"Raspberry color" (103); "Mustard color" and "Pie filling color" (4); "Orange
color" (87), and "Strawberry red color" (55) are corresponding United States com-
mercial food color names and their corresponding Green Table numbers (Meyer, J.
Amer. Chem. Soc., 1907, v. 29, p. 895).
Dr. E. Ludwig, of Vienna, stated, upon the authority of Dr.
Schacheri, at the International Congress of Medicine held in Budapest,
in August, 1909, as follows:
The rather widely distributed practice of coloring baker's goods yellow, such as
cakes and the like, further the yellow coloring of pastry, macaroni, noodles, and so
forth, has as its function the representation of a very large egg content in them; this
coloring has been made very convenient because there are in commerce colors intended
specifically for this purpose and designated "egg substitute" and which have nothing
whatever in common with egg yolk.
Marmalades such as apricot, raspberry, and currant marmalades are frequently found
in a colored condition in commerce; in this case the purpose of the coloring is frequently
to cover up adulteration; the adulteration may consist in an admixture of a cheap
fruit pulp, particularly apple pulp, or in an addition of glucose sirup. Since these
admixtures do not possess the color of the marmalades they are simply helped along
by the aid of color.
Old fruit sirups are toned up with color and then sold as fresh-sirup.
Red colored fermentation vinegar and red colored vinegar essence as well as vinegar
made from such essence are in commerce; such coloring has for its purpose to represent
the product as "genuine red wine vinegar," which in some countries is highly desired.
So-called "beer color," said to be an extract of roasted malt (malt caramel), is in fact
nothing but ordinary sugar caramel and is frequently from time to time publicly adver-
tised; breweries themselves do not use this preparation, but it has been frequently
shown that in small taverns by means of this color local beer was converted into
Bavarian beer.
The wholesale coloring of coffee beans serves the purpose of representing a better
quality than it actually is.
The coloring of cocoa and chocolate by the use of mineral additions and also of coal-
tar colors was often proven; in this case the coloring serves exclusively to cover up
poor quality. In the case of good products such coloring is not practiced.
Colored sausages, and in fact such with a colored meat body as well as such with a
colored casing, are frequently colored; coal-tar colors and cochineal serve this purpose,
the latter, however, only for the meat. This coloring is to preserve in old goods the
appearance of fresh goods.
The green canned goods of commerce are almost all colored with copper compounds.






FOOD-COLOR REQUIREMENTS.


Tomato pulp frequently comes into commerce colored with a coal-tar color; the pur-
pose of such coloring is to impart to the goods the appearance of having been prepared
with extraordinary care. In all these cases it is not at all a question of a harmless
change of the natural condition of the food product, but of improper manipulations
which are adapted to deceive the purchaser as to the real value of the goods; even,
indeed, to mask the danger to health.

III. FOOD-COLOR REQUIREMENTS.
ADAPTABILITY FOR SPECIAL PURPOSES.

Not all coal-tar colors are adapted for use in food products.
Colors are the more desirable for this purpose the higher their tinc-
torial power, and the greater the resistance they offer to the action
of the materials with which they are to be used, and under the con-
ditions existing. Obviously only such colors as of themselves have
their tinctorial properties fully developed can be used, and all such
colors as require a mordant to develop or bring out the color are not
fit for nor capable of use in food products.
Further, if the colored material is subjected to varying tempera-
tures in the process of manufacturing foods, it should be able to
withstand the effects of such temperatures, as, for example, in the
manufacture of candies. The colors should also withstand the action
of reducing agents, such as are generated in the course of fermenta-
tion and decomposition of the food product, or where a preservative
such as sulphur dioxid is added to thle food product to minimize the
effect of decomposition of the food upon the color. Such colors are
put on the European market, and perhaps, but not necessarily,
on the United States market with preservatives added to them.
Most of the coal-tar colors are susceptible to tlhe action of sulphur
dioxid, particularly %when the latter has been used in tlhe decolor-
izing of glucose, and Uranin (510) is one of the colors found to have
the greatest resistance to the sulphur dioxide which may remain
combined in candy.
For example, tlhe book entitled "IIenlcy's Twentieth Centulry
Book of Receipts, Formulas and Processes," published in 1907, on
page 359, says of sausage color:
It is absolutely necessary in using aniline .l, rs to, add a disiiif'taiit to the dye-
stuff uti, o the olbje(.t If which is. in case tlie satusave shitildid uiiilneeli 1' dectni-
pose, to prevent decomip(Psition of azi -dycstutff i y 1 ,tii disfiigat- d h-dr gt'n-. In ist;ad
of Ixoracic acid, forni.aline i, .ay be used as a lisinifeclailt.
J. Frienkel (Arbelt. Kaiserl. 6'sunll. 1902 r. 1S, .
abst. Zts. Na'air. (jenussm., 1902, v. 5, p. S'") reports as follows on
the composition of colors used in coloring sLusnlges, ImeItIs, and
preserves:
1. Blood color: Moisture, 15 per cent; cUnimuon salt, 6.6 per cent; loorax, 21 jwer
cent; and Punceau 2 R (G. T. 55).


25






COAL-TAR COLORS USED IN FOOD PRODUCTS.


2. Blood red for meat juices: Liquid of a specific gravity of 1.0163 not affected by
acids or alkalis and containing 27 per cent total solids; of these total solids 31 per cent
were salt, 12 per cent borax, and the remainder Ponceau 2 R (G. T. 55).
3. Casing red: This powder contained Orange II (G. T. 86).
4. Sausage red: A liquid containing Eosin.
5. Lobster color: A liquid of specific gravity 1.0064 containing 1.64 per cent of
solids, of which 10.9 per cent were salt and the remainder Ponceau R T (G. T. 44).
G. Possetto (Zts. Nahr. Hunters. Hygiene Waarenk. 1891, v. 5,
p. 105) cited the following 15 colors as being used for the coloring
of pastry:
G.T.No. G.T.No.
Martius Yellow ..................... 3 Tropseolin 00 ...................... 88
Victoria Yellow .................... 2 Tropweolin 000 No. 1 ................ 85
Naphthol Yellow S ............... 4 Tropseolin 000 No. 2................. 86
Aurantia Yellow .................... 6 17
Acid Yellow G .................... 8 Chrysoidin ......................... 18
Acid Yellow R ..................... 9 1 41
Citronin .............. ............ 91 Azoflavin.......................... 92
Tropseolin 0........................ 84
Algerian Saffron (a mixture of Nos. 4 and 86 and crocein).
Prussian Saffron (composition not given).
"Blood-red" on the American market is starch colored with red coal-tar colors
(Ibid., 1896, v. 10, p. 114).
"Butter yellow" is a clear saponifiable oil of reddish-yellow color, containing
3 per cent of anilin-azo-dimethylanilin (No. 16 of the Green Tables).
PROPORTION OF COAL-TAR COLOR USED.

The amount or proportion of coal-tar color used has been variously
stated. On page IV of the Leffmann translation of Weyl's book
entitled "The Sanitary Relations of the Coal-Tar Colors," it is
stated that 1 ounce of Auramin (G. T. 425) will color 2,000 pounds
of confectionery, which means 1 part of color in 32,000 parts of
colored product.
Frentzel (Zts. Nahr. Genussm., 1901, v. 4, pp. 968-974), on author-
ity not given, says that for sirups 1 part of color is used to from
4,000 to 5,000 parts of sirup; in colored sugars 1 part of coloring
matter to from 1,333 to 4,000 parts of sugar; and in flour 1 part of
coloring matter to from 666 to 1,000 parts of flour.
In pastry 1 to 100,000 parts (Zts. Nahr. Unters. IIygiene, Waarenk.
1893, v. 7, p. 34).
In chapter VII (p). 47), sections 15, 16, 17, and 18, are brought
together statements made before the commission on regulations for
tlhe Fedleral food and drugs act, as to the amount of color contained
in colored food products. Briefly these are as follows: Confec-
tionery, 1 part of color in 3,500 parts of product; beverages 1 part
of color in 128,000 parts, 256,000 parts, 1,024,000 parts; butter, 420
grains of color to 1,000 pounds of butter; or 1 part of color to
16,666 parts of butter.


26






FOOD-COLOR REQUIREMENTS.


One ounce of color to 30 pounds of "colored food;" the colored
food was not further defined; which means 1 part of color in 4SO
parts of colored product.
It has further been represented that 1 part of color is sufficient
to whiten 250,000 parts of yellow sugar.
From time to time others have presented information as to the
amount of color used in food products. All of these data available
have been tabulated, showing the number of parts of colored product
containing 1 part of coal-tar color, arranged in the order of the
amounts present:


Food ............. ......
Do 2..................
Flour ............... .........
Do......................
Sugar .......-...............
Confectionery ...............
Sirups......................
Sugar ............ ...........
Sirups......................
Confectionery...............
Butter......................
Confectionery...............


100
480
666
1,000
1,333
3,500
4,000
4,000
5,000
12,800
16,666
20, 000


Confectionery ...............
Do.....................
Do......................
Beverages ....................
Pastry .....................
Beverages....................
Do.....................
Confectionery ...............
Whitening sugar.............
Beverages ....................
Do......................


24,576
30. 000
32.000
SO. 000
100,000
120,000
12S,000
192,000
27)0. 000
256, 000
1,024,000


Grouped according to the kin
given are as follows:

Beverages...................... 80, 000;
120,000; 128,000;
256,000; 1,024,000
Butter......................... 16,666
Confectionery.................. 3,500;
12, 800; 20, 000;
24, 576; 30, 000;
32,000; 192,000
Flour .......................... 666;
1,000


d of material colored, tlhe ranges


'Food ..........................

Pastry .......................
Sugar .........................

Sirups.........................

WVhitening sugar...............


These statements have emanated from pirsons l)reslInmalbly ILc-
quainted with the facts of their own practice, and if tliat presilimptinii
is correct it appears tliat there are wide virizitiions ill practice not
only among individual users, but for individual colors. No at tenmpt
has been made to prove or disprove these statements by act iual deter-
mination of tihe amniount of color contained in cotinimercial 'colored
food products.
The 80 chemical individuals on tins market for food-c)oloring p)ur-
poses, it can be fairly assumed, have been tested an1d tried out us to
their utility, and in this respect further tests were regarded as super-
fluous and therefore have not been ,undertaken.

I Kind not defliiltely stated. Said to It,' for 'sre.rvi'd loniatocs.


'100;
41S
100,000
1,333;
4.000
4.000;
5l, 000
25(1, 000


27






COAL-TAR COLORS USED IN FOOD PRODUCTS.


SUITABILITY OF SHADES OF PERMITTED COLORS AND MIXTURES
OF SAME.
The shades produced by the seven permitted colors are, respec-
tively, yellow, orange, blue, green, red, bluish scarlet, and brilliant
cherry red. As statements are found in the literature against the
use of all of the chemical individuals producing a brown or a violet
shade, it will be necessary to produce these shades by a proper com-
bination of two or more of the permitted colors. So far no criti-
cism with regard to the shades produced by the seven colors them-
selves and by their appropriate mixture has been made that has been
substantiated.
Objection has been made to the violet producible from blue and
red, on the ground that when applied to a food product, such as
candy, the component parts do not evenly fix themselves upon the
material. This objection, however, has not been pressed and proba-
bly is not well taken, because of the fact, frequently reported, that
few, if any, coal-tar colors are used without admixture of one or more
other colors to shade or to tone the original color. This criticism,
therefore, of the use of mixed colors can be regarded as not a serious
objection.
One criticism urged with considerable persistency against the seven
permitted colors was that none of them would withstand the action
of the organic acids ordinarily found in beverages such as lemonade,
and it was suggested that no color was proper for use for such pur-
poses which would not withstand, unaltered, for a period of 12 hours
the action of a 10 per cent solution of citric acid. In urging this
objection substitutes were suggested for the permitted colors. The
substitutes so urged were Tartrazin (94), Azorubin (103), Orange
II (86), Ponceau 4 GB (13), and one other color designated as Scarlet
SR, of whose chemical composition no information whatever was
forthcoming. (The numbers in parentheses refer to the Green Tables.)
Of thle five colors suggested it can be said that concerning all but No.
103 adverse statements are found in the literature, and No. 86 is spe-
cifically regarded by every observer but one as being thoroughly
poisonous. The suggested substitute list is, therefore, objectionable
on the ground of injuriousness to lihealtlh.
To test thle valid(lity of the assertion that none of the permitted
colors could withstand the action of citric acid, solutions of the sug-
gested colors, as well as of tli permitted colors, each one in a thou-
sand, were submitted to the action of citric acid, added in such quan-
tity that it amoiinted to 10 per cent of the total bulk of solution.
This experiment slowed that Tartrazin is reddened by citric acid,
whereas Naphthol Yellow S loses in tinctorial power to a slight extent.
Thie shade produced by Ponceau 4GB can be closely imitated by a
mixture of Naphtlhol Yellow S, Orange I, and Amaranth, all per-


28






FOOD-COLOR REQUIREMENTS.


mitted colors. There is no choice whatever in the shade produced
by the desired Azorubin and the permitted Amaranth, nor is there
any difference in behavior toward citric acid. The difference in the
shade between the desired Orange II and the permitted Orange I is
so small that it requires a side-by-side comparison to distinguish
between them. Moreover, the desired Orange II produces a precipi-
tate when brought in contact with the citric acid, whereas the per-
mitted Orange I does not so precipitate. The permitted Erythrosin
is, of course, completely precipitated by the citric acid. The per-
mitted Light Green and Indigo disulphoacid are weakened in tinctorial
power by the addition of the citric acid. Of these colors the only
ones used to any extent in beverages, so far as either the suggested
or permitted list is concerned, are red, yellow, green, and orange.
As has been shown the permitted reds equal the desired reds and
the permitted orange is better than the desired orange. The tinc-
torial power of the permitted yellow is not so great as the tinctorial
power of the desired yellow, but this difference is so slight that the
objection urged against the list of permitted colors, namely that they
were so poor in quality that they had destroyed a profitable and
lucrative business in the coloring of beverages is untenable in view
of the fact that, assuming a price of $1 per pound for Tartrazin, and
40 cents for Naphthol Yellow S, and using them in the proportions
necessary to produce a lemonade color in a 10 per cent citric acid
solution, it would take 5,000 quarts of finished lemonade to cause
an increase of 1 cent in the cost of tlhe production of the colored
food product; that is, it. increases the price per quart by one
five-thousandth of a cent.
It has also been urged that the permitted green is not good enough
for cordials and liqueurs, and that it is impossible to bring about the
proper green by the use of the permitted yellow and blue. This criti-
cism, however, has not been persisted in; the fact is that mixtures of
the permitted yellow and blue can be made so as to obtain any desired
shade of green, having a yellow or blue cast, and great clarity and
brilliancy. How these mixed colors would look after a long period
of time has not been ascertained.
It has also been said that the permitted red, Amaranth, is not a
color suitable for the coloring of strawberry janms and it has be1en urged
that the same chemical individual under another commercial name
is better than the permitted red. This criticism has not been pressed,
probably for the reason that it can not be substantiated.
Again it was claimed that the deposits to be noticed in lbottledl
lemonades were duo to Naplhtliol Yellow S, but solutions of Nailithol
Yellow S in citric acid have remained without deposit for upward of
15 months; it is possible that such precipl)itation, if observed, may be
due to an admixture of the nonpermitted Oranitge 11 with Naphthol


29






COAL-TAR COLORS USED IN FOOD PRODUCTS.


Yellow S, and this difficulty can be obviated by the use of the per-
mitted Orange I, which does not precipitate in the citric acid, as
shown.
Naphthol Yellow S has been objected to on account of the bitter
taste it is said to impart to the beverages to which it is added, and
steps have finally been taken by those interested to have another
yellow placed on the permitted list.
It has also been objected that the permitted blue is not suitable for
the coloring of sugar, first, because it is soluble, and second, because
of the unsatisfactory shade. It may be sufficient, in answer to this
criticism, to state that there was no insoluble blue offered'on this
market, and there was no blue other than the one permitted offered
against which adverse statements did not exist in the literature, and
in view of this state of affairs the criticism may be said to be not well
taken.
As against all these specific criticisms it has been repeatedly stated
by those in a position to know that they have found no difficulty
whatever, by suitable mixtures of permitted colors, in reproducing
any desired shade of any desired quality, not even excepting browns
and violets.
Considering all of these criticisms, therefore, the conclusion seems
reasonable that there is no serious or permanent objection to be made
against the seven colors selected, either as to qualities for food-
coloring purposes or range of producible shades.

IV. CONFORMITY OF FOOD-COLOR MARKET, 1907, TO RECOM-
MENDATIONS OF THE NATIONAL CONFECTIONERS' ASSOCIA-
TION, 1899.1
Having thus shown that the food-color market of the United States
contains not less than 80 coal-tar colors which are distinct chemical
individuals, of which 74 are entered in the Green Tables and 6 are
not, the next question to be considered is whether all of these sub-
stances are harmless and fit for use in food products.
As a guide in determining this point the "Official circular from the
executive committee of the National Confectioners' Association of the
United States," pertaining to colors in confectionery, dated February 1,
1899, may well be considered.
The function of this circular is said to be "to throw light upon the
vexed question of what colors may be safely used in confectionery,"
evidently because "there may at times be a doubt in the mind of the
honest confectioner as to which colors, flavors, or ingredients he may
safely use and which ho may reject."
The circular also states that "but infinitesimal amounts of color
(coal-tar colors) need be or can be used to give the desired effects,"


I See also p. 45.


30






FOOD-COLOR REQUIREMENTS. 31

and in view of this statement as to quantity it must be self-evident
that a color harmful when used in the small quantities said to be used
in confectionery is certainly harmful when used in the large quantities
used in coloring other food products. This circular under the head-
ing, "Colors that are injurious and therefore to be rejected-Harm-
ful organic colors," enumerates 21 coal-tar colors. Of these 21 colors,
13, or 61.9 per cent, were among those submitted, and whose com-
position was stated by reference to Green Table numbers; the Green
Table numbers of these colorstogether with the number of sources
from which they were obtained, follow:
Green Number Green Number
Table of Table of
numbers, sources, numbers, sources.
11 ............................... 2 169 ............................... 1
17............................... 2 197 ............................... 4
18 ............................... 1 201 ............................... 2
84 ............................... 2 398 ............................... 2
86 ............................... 8 584 ............................... 1
95............. ................ 2 650............................... 2
106 ............................... 5

Out of these 13 colors 3 each came from one source; 7 each came
from two sources; 1 came from four sources; 1 came from five
sources, and 1 came from eight sources, out of a possible 12; that is,
one was wanted by more than half the sources.
It is further to be noted that of the trade names given to the sub-
mitted products of Class I the following appeared among the harmful
list of this circular and also were found in identical form and spelling
on the labels of the submitted products:
1. Bismarck Brown. 8. Orange A.
2. Chrysoidin R. 9. Orange A extra.
3. Chrysoidin Y. 10. Orange G.
4. Mandarin G extra. 11. Orange II.
5. Naphthol Green B. 12. Scarlet.
6. Napthol Yellow. 13. Vesuvin B.
7. New Coccine. 14. (C'rocein Scarlet 5 B.

The following parallel will serve to show the great resemblance
between the names given to the harmful colors of the circular and
those found on the samples submitted:

circular's s har nimfu I is. Labels of sunbmitt'd sam pl's.
Methylene Blue B B..................... Methylene Blue i.
Methylene Blue B B crystals ............ Methylene Blue ).
Methylene Blue B B G ................... Methylene Blue 0.
Methylene Blue D1) B B..................
New Coccine.......................... New ('occin 0 Z.
New Coccine Z.
Naphthol Green B....................... Naphthol Green.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


Circular's harmful list.

Orange II ...............................
Victoria Yellow..........................

Acid Yellow ............................
Bismarck Brown G.......................
Bismarck Brown T ......................






Chrysoin..............................



Cochineal Red A ........................
Crocein Scarlet 3 B ....................
Crocein Scarlet 7 B....................
Crocein Scarlet 8 B .....................
Fast Brown G.........................

Fast Yellow ............................



Imperial Scarlet, in powder, extra........
Safranin ..............................
Safranin A G extra.
Safranin AGT extra.
Safranin Cone.
Safranin extra G.
Safranin FF extra No. 0.
Safranin G extra GGS.
Safranin G 000.
Safran in T.


Labels of submitted samples.

Orange II Z.
Victoria Yellow Cone. Z.
Victoria Yellow Conc. T Z.
Acid Yellow G.
Bismarck Brown B.
Bismarck Brown B 216.
Bismarck Brown Dark.
Bismarck Brown R X.
Bismarck Brown T D.
Bismarck Brown Y Bril.
Bismarck Brown Y Dark.
Bismarck Brown 2 R X.
Chrysoin Brown G Z.
Chrysoin G E Z.
Chrysoin R E Z.
Chrysoin R Z.
Cochineal Red.
Crocein Scarlet 10 B.


Fast Brown N.
Fast Brown 0.
Fast Yellow G.
Fast Yellow 0 3 3.
Fast Yellow 0 3 4.
Fast Yellow Y.
Imperial Scarlet 3 B.
Safranin S P.


This comparison disclosed a considerable lack of conformity be-
tween the United States food-color trade in 1907 and the circular of
February, 1899, upon whose preparation for seven months prior to
its date "a great deal of thought and labor have been given to a
thorough investigation of the whole subject of 'colors in confec-
tionery,' in which the committee has been largely aided by the
researches of the association's chemist and by the results of his
analytical tests" and whose "classifications have been carefully
made, and are based upon the authority of the eminent chemists,
Prof. Koenig and Prof. Weyl, upon the resolutions of the Swiss
chemists and upon the French ordinances regarding the coloring of
food products," and which list was expected to be "of value to color


32






FOOD-COLOR MARKET, 1907.


dealers and chemists," and also was published to assist the confec-
tioner in obeying "the letter and the spirit" of the pure-candy laws.
Under the heading "Colors that have been shown to be harmless
as used in the confectioner's art, harmless organic colors," this cir-
cular enumerates 36 colors, for 4 of which there are no Green Table
numbers. Of the 32 colors having Green Table numbers, 20, or 62.5
per cent, were among those colors submitted. The Green Table num-


bers of these colors, together with
they were obtained, follow:

Green Number
Table of
numbers, sources.
4................................. 10
8 ................................. 5
9................................. 1
13................................. 6
55................................. 5
65................................. 2
85....... ........................ 2
103................................ 6
105................................ 1
107...............................--- 7


the number of sources from which


Green Number
Table of
numbers, sources.
240................................ 1
269............................. 1
287................................ 1
427................................ 2
448................................ 4
451................................ 5
462................................ 2
512................................ 3
517................................ 5
520 ............................... ..


Of these 20 colors 5 each came from 1 source; 5 each came from 2
sources; 1 came from 3 sources; 1 came from 4 sources; 4 each came
from 5 sources; 2 each came from 6 sources; 1 came from 7 sources,
and 1 came from 10 sources; that is, only 2 were wanted by more
than half the makers or importers, and only 4 by half the sources.
It will be noted that this circular provides for a total of only 57
different coal-tar colors; the number of avowed colors submitted
reached 80, or 23 in excess of this number, and further, that out of
the 57 colors referred to in this circular only 33 appeared among those
colors submitted whose composition was acknowledged, so that for
47, or 58.8 per cent of the avowed submitted colors, this circular is no
specific guide. From the data obtainable from this circular, the
following tabulation can b)e made:

Harni fi In ss of si bu, it td colors bascd on lUst in cirul ar.


I )l ii.


I Tultal on
Tnlirket.



*21


Disclosed
colors on
United
S11LIC$
lmarket'l.

Pe'rr cent.
HIi. .,
25. 4


Circular's
urre-
spilingllg
IL;sl.

I'er cent.
6Ii-. 5
62.5.


These figures disclose a (nsidnerailile and sellf-evident disregard of tlio
request, then eigt years old, as niade by the National ('onfectitiiers'
972910-Bull. 1-r- 12-3


33






34 COAL-TAR COLORS USED IN FOOD PRODUCTS.

Association of the United States, that coal-tar colors designated
by it as "colors that are injurious and therefore to be rejected,
harmful organic colors" be not used in confectionery, and by implica-
tion that they should not be used in other food products.
In view of this disregard with respect to 13 coal-tar colors out of
33 on the United States market in the summer of 1907, dealt with in
this confectioners' list, the conclusion seemed justified that the action
regarding other coal-tar colors on the United States market in the
summer of 1907 was equally heedless or indifferent, a conclusion
which is borne out by the material brought together under section IX.
The necessity of adhering to some unequivocal terminology, as has
been done in these pages by referring to the serial numbers in the
Green Tables, appears from the following:
Trade names are not definite with respect to the composition of
the article sold under a given name, although tinctorially the colors
may be substantially equivalent. In the Green Tables there are not
less than 29 instances where the same trade name is applied to two
or more different chemical individuals. In some cases these chemical
individuals are fairly closely related, in others they are only remotely
related. When the differences are greater than the presence or
absence of a sulpho group or the use of methyl for ethyl or the reverse,
the instances are given below:
1. Cotton Yellow........ 128 Primulin-azo-m-phenylene-diamin-disiilphonic acid.
191 Diphenylurea-disazo-bi-salicylic acid. W
2. Methyl Eosin .......... 513 Methylated tetrabromo-fluorescein.
375 Dinitro dibromo fluorescein.
3. New Yellow .......... 88 p-sulphanilic acid azo-diphenylamin.
91 Nitration product of diphenylamin yellow.
4. Orange III.........23 Meta-nitranilin azo-R salt.
87 p-sulphanilic acid azo-dimethylanilin.
5. Orange N ............. 43 Toluidin azo-Schaffer acid.
88 p-sulphanilic acid azo-diphenylamin.
6. Orange R ............. 97 o-toluidin-monosulphonic acid azo-hetanaphthol.
15 Anilin-azo-R salt.
99 Xylidin sulphoacid-azo-betanaphthol.
7. Toluylene Red....... 261 Dichloro-benzidin disazo R salt.
580 Dimethyl diamido toluphenazin.
The following quotation also bears on this point:
In attempts to group the aniline colors a kind of uncertainty appears even among
coirc (hernliMts. The same trade name does not always correspond to the same prepara-
tion. Many preparations are not chemical individuals, but mixtures of related colors.
Many preparations are "standardized" for the trade; for example, with dextrin. On
ac.omint of the patent laws, factory secrets surround the production of many coloring
matter, and frequently statements are met with which are directly intended for the
purpoHse (if misleading competition. (Hlueppe, Die Methoden der Bakterienforachung,
5th ed., 1891, p. 105.)






LEGAL ENACTMENTS.


V. SOME LEGAL ENACTMENTS RELATIVE TO THE USE OF
COAL-TAR DYES.
LIST OF THIRTEEN FOREIGN LEGAL ENACTMENTS.
The 13 foreign legal enactments compared are as follows:
1. The Austrian regulation of March 1, 1886, which forbids No.
483 of the Green Tables and all anilin colors.
2. The law of Austria of May 1, 1886, which forbids No. 1 of the
Green Tables and all anilin colors.
3. The Austrian regulation of September 19, 1895, in which cer-
tain colors only are permitted, and all others are forbidden. There
are 16 titles of permitted colors in this law, but these are in some
cases so elastic and so indefinite as to include 47 entries in the Green
Tables.
4. The Austrian law of January 22, 1896, in which there are 17
titles, but these are sufficiently elastic to allow of 22 entries in the
Green Tables being included in them.
5. The German law of July 5, 1887, which specifically prohibits
only Nos. 1 and 483 of the Green Tables. The interpretation which
seems to be generally placed upon this law is that all other Green
Table members are permitted in Germany for use in foods.
6. The Italian law of February 7, 1892, forbidding all colors except
9 different titles, which, however, were elastic enough to include 32
entries in the Green Tables.
7. The law of Italy of February 7, 1902, which prohibits 37 entries
in the Green Tables, and permits 11 specifically.
8. The Italian decree of June 29, 1893, in which there were 7
titles of permitted colors sufficiently elastic to include 34 different
individuals.
9. The Italian decree of March 24, 1895, forbidding four titles cov-
ering only four entries in the Green Tables.
10. The French police ordinance of May 21, 18.5, in which 4S9
entries in the Green Tables were p)rollibited.
11. The French police ordinance of December 31, 1890, in which
469 entries of thle Green Tables were l)rohibitel, and which also
permitted under 9 titles 23 entries in tlhe Green Tab)les.
12. The Belgian law o(f 1.S)1, which specifically forbids only four
entries in the Green Tables.
13. The law of the Canton of Tessin, dlated May IS, 1S97, whlcli
forbids only 4 specific entries in tihe Green Tables.
SUMMARY OF COLORS PERMITTED BY THESE LEGAL ENACTMENTS.
An examination of tlie 13 legal (ena.ctiients made in IEuroJpe with
respect to the use of coal-tar colors in foodl l)rodu(lcts dliscloses consid-
erable difference of opinion as to tim harminfulness or tlhe harlilessness
of even the same chemical individuals. To prepare an ap)proxiuate


35







36 COAL-TAR COLORS USED IN FOOD PRODUCTS.

and comprehensive summary of the effect of such legislation, the
following plan has been followed:
The provisions of a selected number of laws and regulations, 13 in
number and dating from 1883 to 1902, were read with respect to
permission or prohibition of the 695 chemical individuals listed in the
Green Tables. The effect of each law upon each separate entry in
the Green Table numbers was noted, either as permitted, forbidden,
or noncommittal when the law was silent upon such entry; the laws
were read with the understanding that what was not forbidden was
permitted, and what was neither forbidden nor permitted was non-
committal; if this were an incorrect or improper procedure the
number of permitted colors would be reduced but not augmented.
For the purposes of this first approximation, no attempt was made
to segregate those specifically permitted from those permitted by
blanket expressions or phrases.
For the purposes of a side-by-side comparison, the term "index
number" was coined; this "index number" gives in the first place the
number of legal enactments that permit the color; in the second place
the number of enactments that forbid it; and in the third place the
number of enactments that are silent or noncommittal. Thus: 283
as an index number would mean 2 enactments permit, 8 forbid,
and 3 are noncommittal; so that an index number with the
highest hundreds would have the greatest number of permissions,
and with the highest tens would have the highest number of pro-
hibitions. With this understanding of these terms, the following
table of so-called index or "P. F. N." numbers is offered:
Thirteen legal enactments classified by Green Table numbers and the "P. F. N. figure,"
or "''index number."

Total
number Index
of Green nuer. reen Table numbers.
Table n er
entries.

1 184 483.
1 274 534.
3 2,111,1 1-3.
217 3(&4 394-411, 415-426. 429-434, 4 35', 436-445, 484-492, 528-561, 564-583, 585-598,
600, 602-049, 651-691, 693-695.
1 373 103.
366; 3.s2 8,7,10,11,12,14,16,19-22,35-40,42, 43, 45-54, 58-6,4. 66-83, 89, 90, 93, 94, 96-
101, 104-106I, 109-113, 115-145, 1414, 151-156, 158, 159, 161, 162, 164-168,
172, 197, 19,9-243.245--393:, 412-414.493-511.524-527,650.
29 391 446,447,449,450,453,455.456,45.8-4til6, 463-476, 478,479,481,482.
3 454 428,563,599.
1 4t,3 69.
22 472 5. 8, 9.23-34, 84.i W-88,91,520,523.
7 481 95, 452,454,477,513,519,522.
2 544 562, 101.
2 51,2 515,516.
3 571 40, 514,521.
3 64:3 44,114,427.
11 (52 1.3,15,85,92, Ill. 14i,-1 4S. 150. 160,617.
fi (Ad 17.19, 41,169,512,51M.
2 t,70 451.46i2.
6 742 ,4. 55.5,. 57,102,244.
6 751 ti65, 107, lt13, 170, 198.448.
1 50 457.
2 931 157,171.
SItalicized figures Indicate colors permitted by F. I. D. 76.






LEGAL ENACTMENTS.


From the table it appears that there is no one Green Table number
that is permitted by each and all of these 13 legal enactments, nor
is there any one color that is prohibited by each and all of these 13
legal enactments; and as late as 1902 there was considerable con
fusion as to what should or should not be permitted or forbidden.
That the European enactments were not in reality consistent or
effective appears from the following:
1. In respect to the use of coal-tar colors, the views as to their harmfulness or harm-
lessness are very divergent, and this uncertainty is expressed in the various legislative
enactments. (v. Raumer, Zts. Nahr. Uniers. Hygiene & Waarenl'., 1895, v. 9, p. 207.)
2. After eating groats, which no doubt were free from ordinary poisons but had been
colored with Martius Yellow, a whole family became sick. Since this coloring matter
is not mentioned among those which, under the law of July 5, 1SS7, are forbidden
for the purpose of coloring articles of food, a complaint could not be lodged. Never-
theless, the use of Martins Yellow for the coloring of articles of fod would seem to be
dangerous, since this coloring matter exerts poisonous effects. It is a weakness in
the law that coal-tar colors, of which new members are continuously appearing on
the market, and whose physiological action is unknown, should be at all permitted
for the coloring of articles of food. (Dietrich, Th., Jahresicrhhte der landwirt1ischaj/?-
lichen Versuchsstation, Mfarburg, 1900-1901, p. 13; abst. Zts. Auihr. G ', ussm., 190P r. 5,
p. 364.)
On account of their large number and the great diversity of opinion
as to harmfulness of some coal-tar colors and the harmlessness of
others therein reflected, no attempt was made to collect all the
legal enactments and regulations made with respect to coal-tar
dyes. The foregoing are typical of the remainder.

COLORS SAID TO BE PERMITTED UNDER THE GERMAN LAW
OF 1887.

That some of the laws did not employ specific terms but used those
possessed of a great degree of elasticity appears from the following
taken from Weyl's "Sanitary relations of the coal-t ar colors,," page 3.
concerning the Chamber of Commerce and Trade of Sonneberg which
declared on December 4, 1SS7, that tlhe German law of July 5, 1SS7
allowed the unrestricted use of-
All blue and violet anilin (that is coal-tar) culurs, all ponceaus, all orange colors,
Methyl Green, Brilliant Green, Malachite Green, Chrysoidin, Naphthol Yellow, Mart iu
Yellow, Eosiii, Phloxin, Safranin, Erythro.in, Fijphsin, Phernyhlui Brown, and Anilin
Black.
This amounts to not less than 233 p)ernmitted(I colo(,rs, its will now be
shown.
Using thle Green Tables as a guide it will be found that under tlie
above ruling there are to-day no less than 107 blue coal-tar colors
which could be used for food coloring. They are arranged as follows.
showing the comments on same in the literature.


37






38 COAL-TAR COLORS USED IN FOOD PRODUCTS.

BLUE COLORS.

Unfavorable: 478, 479, 488, 490, 572, 602, 639. (Total, 7.)
Favorable: 477, 599, 600, 692. (Total, 4.)
Contradictory: 287, 457, 480, 563, 601, 650, 689. (Total, 7.)
.ot reported on: 36, 83, 119, 142, 175, 189, 209, 246, 247, 254, 257, 263, 266, 288, 290,
291, 292, 293, 294, 295, 301, 302, 310, 311, 314, 315, 316, 317, 318, 319, 323, 327, 345,
347, 348, 351, 352, 356, 359, 364, 430, 432, 439, 440, 442, 444, 456, 473, 476, 481, 482,
487, 492, 509, 542, 551, 556, 558, 559, 560, 562, 569, 595, 598, 608, 611, 612, 615, 618,
619, 621, 625, 627, 628, 634, 637, 638, 640, 641, 642, 643, 652, 655, 656, 657, 664, 682,
693, 694. (Total, 89.)
Similarly there would be 50 violets which are classified as follows:

VIOLET COLORS.

Unfavorable: 620, 649. (Total, 2.)
Favorable: 467, 593. (Total, 2.)
Contradictory: 450, 451. (Total, 2.)
Not reported on: 30, 34, 36, 118, 176, 179, 207, 244, 246, 248, 252, 256, 273, 320, 336,
338, 340, 342, 343, 444, 452, 454, 455, 463, 464, 465, 466, 468, 469, 470, 471, 472, 474, 486,
506, 507, 525, 552, 579, 581, 585, 592, 613, 625. (Total, 44.)
Similarly there would be 18 ponceaus which are classified as follows:

PONCEAUS.
Unfavorable: None.
Favorable: 169, 448. (Total, 2.)
Contradictory: 13, 15, 55, 160, 163. (Total, 5.)
Not reported on: 44, 56 ', 571, 108, 113, 114, 146, 147, 148, 150, 165. (Total, 11.)

Similarly there would be 35 Oranges which are classified as follows:

ORANGES.
Unfavorable: 2, 97. (Total, 2.)
Favorable: 85. (Total, 1.)
Contradictory: 14, 18, 43, 86, 87, 88, 95. (Total, 7.)
Not reported on: 10, 23, 47, 54, 99, 100, 136, 162, 196, 217, 218, 222, 225, 235, 236,
265, 275, 392, 406, 408, 409, 529, 531, 545, 547. (Total, 25.)
The remaining 23 colors named are classified as follows:

MISCELLANEOUS.

Unfavorable: Martius Yellow (3).2 (Total, 1.)
Favorable: Naphthol Yellow S. (4); Eosin (512, 517, 521); Phloxin (521); Erythrosin
(517). (Total, 6.)
Contradiicrtory: Brilliant Green (428); Malachite Green (127); Chrysoidin (17, 18, 41);
Safranin (584); Fuchsin (448); Phenylene Brown (197). (Total, 8.)
Not reported on: Methyl Green (460, 461); Eosin (514, 515); Phloxin (518); Safranin
(583, 585); ErythroHin (516); Anilin Black (577). (Total, 9.)
It will be noticed that namines such as Eosin, Erythrosin, and Phloxin
appear in more than one classification; thus some of each are favor-
ably reported on and the others are not reported on at all.

I Nos. 56 and 57 are included among the permitted colors of the Austrian law.
'The numbers In parentheses following the names are the Green Table numbers.





LEGAL ENACTMENTS.


The 233 colors said by the Sonneberg Chamber of Commerce and
Trade to be entitled to unrestricted use in food coloring under the
German law of 1887 referred to may also be classified as follows:
Summary of classification of colors permitted under the German law of 1887 according to
comments in the literature.

Comments in the literature.
Class. Total. vmr
class. Total. Unfa- Favor- Contra- Not re-
vorable. able. dictory. ported
I Oi ,
B lues............ ...................................... 107 7 4 7 89
Violets ................................................ 50 2 2 2 44
Ponceaus.............................................. 18 0 2 11
Oranges ................................................ 35 2 1 7 25
Miscellaneous........................................... 23 1 5 8 9
Total............................................ 233 12 14 29 178

Out of these 233 colors only 55, or about one-fourth, have been
reported on in the literature and the remaining three-fourths have
not been examined at all. To the 55 examined and reported on
there may be added 2, namely, Nos. 56 and 57, since they are included
among the colors once permitted by law in Austria, thus making a
total of 57 examined out of 232. Adding these two to the 14 favor-
ably reported on makes a total of 16. It finally appears that 41
out of 57 colors examined would in the light of present knowledge
be improper to be used in food and 12 at least should not be used for
such purposes at all.
The classification into unfavorable, favorable, contradictory, and
not reported on is based upon the tabulation on page 63; if that is
substantially correct the above conclusions are also true.
The foregoing side-by-side comparison of 13 legal enactments,
while it makes no claim to being absolutely and wholly accurate in
all the classifications or conclusions drawn, is no doubt a fair reflec-
tion of the condition of mind of those framinng the enactments, and
consequently of information upon which those enactments were based;
and the conclusion would therefore seem to be justified that the fact
that a color has been permitted or has been forbidden by any one or
the majority of these legal enactments ought not to constitute &
clean bill of health, nor an indictment, as the case may be.
This side-by-side comparison must not be pushed to extremes;
indeed the extent to which it can be employed is naturally very liin-
ited, and the purpose for which it was made was to reflect in a manner
easily and comprehensively grasped the confusion'and inconsistencies
which very persistently force themselves upon the mind of a person
reading those enactments and having in mind the chemical individ-
uals at which they are aimed.


39





COAL-TAR COLORS USED IN FOOD PRODUCTS.


The definite lesson to be learned from this side-by-side comparison
is that these enactments in many cases employed terms so vague and
indefinite as to permit the use of some bad colors as well as all good
ones, that is they were not sufficiently definite to exclude all that
were harmful.
DEFINITENESS AND DETAIL NECESSARY TO EFFECT QUALITY
CONTROL.
This apparent state of confusion in legal enactments that pre-
ceded the summer of 1907 was a very strong factor in the formation
of the conclusion that in order to be effective any law or regulation
dealing with coal-tar colors for use in foods must prohibit every coal-
tar color except certain definite specific ones.
The Austrian laws of September 19, 1895, and of January 22, 1896,
provided for quality control by public and other laboratories of the
coal-tar colors put upon the market for use in foods; the results of
such control, as reported in the Zeitschrift fuir Nahrungsmittel-
Untersuchung, Hygiene und Waarenkunde, 1896, v. 10, p. 335, are
as follows:
Coloring matters of commerce are mostly mixtures of various coloring matters, a
right which manufacturers will not part with; and further, while it is indeed possible
to test the coloring matter in substance, it is nevertheless impossible to test it in the
very small amounts which are used in the coloring of foodstuffs and to determine
with certainty the identity of the color as to whether it is or not one of the permitted
colors.
Of 21 samples of coloring matter examined, 14 were objectionable, partly
because of false labeling, or because they were mixtures, partly because they
contained poisonous metals, ora forbidden coloring matter. Thus, a so-called "Ever-
green" was Naphthol Green B, a poisonous nitroso color; Malachite Green contained
zinc; an Acid Magenta and a Rosalin contained traces of copper; Ponceau, Eosin,
Brown, and Roccellin contained traces of tin; Orange I and Waterblue contained
traces of tin and zinc. The last-named coloring matters were therefore not prepared
i'n proper state of purity.
The authorities in Vienna examined four and rejected two colors. (Ibid., 1898,
p. 107.)
The Swiss authorities exercised control over colors, after they
reached the market, with the result that the authorities in Basle
examined ten colors and rejected one. (Ibid., 1897, p. 292.)
These facts, together with the knowledge derived by even the most
superficial ocular examination of the 294 specimens received in the
summer of 1907, played a very great part in the formation of the con-
clusion that control of quality, in order to be even reasonably effec-
tive, must be thoroughgoing, and that colors must be excluded from
the market until they prove themselves to be clean, rather than
permitted promiscuously and then driven out of the market by the
authorities if unsuitable.
The effective quality control of food colors requires careful and
searching examination of a kind which can not usually be obtained


40






LEGAL ENACTMENTS.


by the general purchasing public. The quality of the food colors
offered in the summer of 1907 varied greatly, and the substances
contaminating them were of such indefinite and probably variable
composition (of whose physiological action nothing definite was
known and whose quick and certain detection in the colored food
product would be very complicated, if not impossible) that quality
control of greater efficiency than that exercised by those selling
food colors in the summer of 1907 seemed necessary on the part of
the authorities having charge of the enforcement of the food and
drugs act.
The points of original entry of food colors into the United States
food-color market are relatively few, whereas the points of distribu-
tion of food colors are very many, the former being less than 20 and
probably fewer than 10, while the latter may number up into the
hundreds; therefore, not only is the labor and the expense of quality
control of food colors reduced to its probable minimum by keeping
food colors off the market until they have shown their right to be
so used, but also the certainty and the efficiency of quality control
is increased to its probable maximum.
The quality control thus suggested is similar to that exercised by
the States of New York, Michigan, and Ohio over salt before it
enters the market for human consumption. The method of color
control here suggested differs only in degree, not in kind, from the
quality control exercised over salt by the States named. Experience
has shown such quality control of food colors to be not only practi-
cable but capable of realization without any hardship and but little,
if any, inconvenience to those concerned.
STATE LAWS PROHIBITING THE USE OF COLORS IN CERTAIN
FOODS, 1909.
The laws of the individual States of the United States have also
restricted the use of coal-tar coloring matters in foods. These
restrictions are directed principally against the use of color to con-
ceal inferiority, which restriction is found in almost all the States.
The sale of poisonous coloring matters for foods is prohibited in tlhe
State of New York, and in New York and North Carolina the addition
of injurious colors to foods is prohibited.
Minnesota and North Carolina prohibit coal-tar dyes in all foods.
Foods and beverages are considered adulterated in North Dakota
and Wyoming if they contain aniline dyes or other coal-tar dyes.
Artificial coloring is prohibited in sausages by Colorado and
Wisconsin.
Artificial coloring, including, of course, coal-tar colors, must not be
added to vinegar in the States of Arkansas, California, ('onnectieut,
Iowa, Minnesota, Missouri, New Jersey, New York, Pennsylvania,
Tennessee, Wisconsin, and Wyoming.


41






42 COAL-TAR COLORS USED IN FOOD PRODUCTS.

Distilled vinegar must not contain artificial color in Ohio and
Oklahoma, and must be free from harmful artificial coloring matter
in Utah.
In South Dakota oleomargarine must not be colored.
Artificial coloring is prohibited in milk by California, Oklahoma,
Pennsylvania, Utah, and Wisconsin and in cream by California
Connecticut, Pennsylvania, Utah, and Wisconsin.
Coal-tar dyes are inhibited in cakes, crackers, candy, ice cream,
and like products by Virginia. Ice cream is considered adulterated
in Michigan if it contains harmful colors.
Forty-six States prohibit the use of poisonous colors in candy.
They are as follows: Alabama, Arkansas, California, Colorado, Con-
necticut, Delaware, District of Columbia, Florida, Georgia, Idaho,
Illinois, Indiana, Iowa, Kansas, Kentucky, Louisiana, Maine,
Maryland, Michigan, Minnesota, Missouri, Montana, Nebraska,
Nevada, New Hampshire, New Jersey, New York, North Carolina,
North Dakota, Ohio, Oklahoma, Oregon, Pennsylvania, Philippine
Islands, Porto Rico, Rhode Island, South Carolina, South Dakota,
Tennessee, Texas, Utah, Vermont, Virginia, Washington, Wisconsin,
and Wyoming.
VI. RECOMMENDATIONS BY ASSOCIATIONS AND INDIVIDUALS
AS TO USE OF COAL-TAR DYES AS FOOD COLORS.
CAZENEUVE AND LAPINE.
Cazeneuve and Lepine (Bull. de l'acad. de medicine, April 27, 1886,
p. 643) says:
We have arrived at the following conclusions:
1. The nitro derivatives are especially poisonous (dinitronaphthol being comparable
with picric acid), but the sulphonated product is harmless.
2. Safranin and Methylene Blue are harmful, producing gastric intestinal dis-
turbances, being violent poisons.
3. The following coloring matters are tolerated by man, whether well or affected
with Bright's disease; similarly, too, animals (dogs, guinea pigs) without any noticeable
disturbances and a. rather high doses:
Probable Probable
U reen Table Green Table
Nos Nos.
1. Fast Yellow ............... 9 5. Ponceau R ................ 55
2. Roccellin ................ 102 6. Orange I .................. 85
3. Bordecaux B............... 65 7. Fuchsin S................ 462
4. Purple ................... 106 or 107
Among the nontoxic sulliphonatled colors we have been able to make out the following
list or ('la.Mificatiou, based upon their power of producing disturbances, proceeding
from the least inert to the most inert:
Probable Probable
Ureen Table Green Table
Nos. Nos.
1. Orange I .................. 85 5. Yellow NS.............. 4
2. Bordeaux B ............... 65 6. Fast Yellow............... 9
3. Ponceau R ................ 55 7. Purple .................. 106or 107
4. Roccellin ................ 102






RECOMMENDATIONS BY ASSOCIATIONS, ETC.


The results of our experiments have led us to the following conclusions:
1. The relative nonpoisonous nature of the azo colors used for coloring wines explains
why this artificial coloring has not caused any real epidemic.
2. This artificial coloring of wines by coal-tar colors is dangerous. It opens the door
to the employment of coloring matters of very variable and noxious properties. Thus
Martius Yellow, which is poisonous, has been used for 10 years past to color pastry
(3 grams per 100 kilograms) and it may be used to-morrow, perhaps, to color wines mixed
with a red or a blue.
3. A rigid law against the artificial coloring of wines ought to be promulgated,
particularly if this coloration covers detestable practices most prejudicial to the public
health. The addition of salicylic acid, glycerin, and tartaric acid, or the acidifying
by sulphuric acid, is cloaked by the use of the coloring matter.
Some sulphonated azo-coloring matters are sufficiently inert to enable their being
employed as artificial color in foods, bonbons, and liquors. These colors are manu-
factured according to simple processes which give theoretical yields and no metallic
salt, such as mercury, tin, or arsenic participates; sulphate of soda is the only impurity.
In view of the great extent of the use of these coloring. matter.-, it is better to regulate
their consumption by tolerating certain of these products; rather than to interpose an
illusory barrier to their use. Where you can not arrest a stream you can at least regu-
late its course.
It would be better definitely to classify these substances with respect to their noxious
properties, tolerate some and prohibit the others, rather than to be exposed to the
consequences of permitting manufacturers to introduce into food, without any scien-
tific control whatever, any products whatever.
These coloring matters should be sold in commerce under the names of harmless
colors as determined by analysis. By chemical analysis it would be recognized as to
whether we were dealing with one color or with a mixture of two or three colors.
The colors most used are made up of red, yellow, and blue, which apparently imitate
the appearance of the wines of the Midi. Thus we have recognized such coloring
matters in Roccellin, Naphthol Yellow, and Methylene Blue.
Sulphonated Fuchsin is very much used, combined with a yellow and a blue. This
mixture turns green with ammonia, like the coloring matter of wine. In fart, Acid
Fuchsin is decolorized by ammonia. The yellow and blue remain intact, and give a
green which suggests true wine color.
SOCIETY OF SWISS ANALYTICAL CHEMISTS.
In 1891 thle Society of Swiss Analytical Ch'lumists, recommended
that certain coloring matters which alre to be regar.l.l as harmful
to health should not be permitted to be u-sed in thie p)repatration of
articles of food intended for sale in which artificial coloring is at all
permitted.
The coal-tar colors thus prohibited are identified in tlie following
by their Green Table numbers, only one trade n111ame being given:
Picric Acid (1); Dinitrocresol (2); Martius Yellow (3); Aurantia (6);
Orange II (86); Metanil Yellow (95); Safranin (5S-l); Metlhylene
Blue (650). (Zts. Nahr. Unters. Hi/glenc. 18.91, v. 5, p. 293.)
TSCHIRCH.
In 1893 Tschirch recommended as follows:
1. The coal-tar colors, and in a narrow sense the aniline colors, are no longer harmful
on account of their arsenic content, since at the present tini, thi' gr ait majority 4f
them are prepared free from arsenic.
2. Some colors have shown themaelvcs ti, be hliarntiful I6 thte .\tt'.


43






COAL-TAR COLORS USED IN FOOD PRODUCTS.


3. Coal-tar colors in general should therefore be permitted for the coloring of foods,
but those that have been found to be harmful should be expressly and specifically
forbidden.
4. The amount of coloring matter which has been determined quantitatively in
bonbons and liqueurs is so small that even the ones regarded as poisonous would not
be able to develop their harmful effects. (Zts. Nahr. Unters. Hygiene Waarenk.,
1893, v. 7, p. 338.)
KAYSER.

In 1895 Kayser expressed himself as follows:
As to the poisonous nature of organic coloring, and in respect to their composition,
H. Erdmann (Pharm. Centralh, 1892, v. 33, p. 357) concludes that in general acid
dyestuffs can pass as nonpoisonous; whereas in the case of basic coloring matters it
is recommended to make a physiological examination before using them for the col-
oring of things in daily use, especially articles of food. Whether that portion of that
view which deals with acid dyestuffs will retain unexceptionable and positive validity
appears doubtful.
At the present time, speaking generally, interested manufacturers take the point
of view that all the coloring matters which are not forbidden in the food law are to be
regarded as permitted. Whether this point of view is free from legal objection can
not be discussed here; that, however, it can not be accepted from a hygienic point of
view under any circumstances whatever does not require any special proof for those
conversant with the facts. The hygienic requirements under all circumstances
can be summed up in the following rule:
Every coloring matter is to be regarded in every way as suspicious, so far as its
harmlessness is not proven by experience or by correct physiological experiments.
No one can say in advance that among the colors which are to-day manufactured
and used, which are as yet not called into question, there are none which possess
distinctly poisonous properties. Correct examination of artificial coloring matters in
this direction is, as iswell known, even to the present almost wholly lacking. (Forsch-
ungsberichte iiber Lebensmittel, etc., 1895, Vol. II, p. 181.)

WEYL.

In 1896 Weyl expressed himself as follows:
Since the number of the organic coloring matters already known is a very large one,
and since their number is increasing daily, and it seems to be unlikely that each
individual of these coloring matters will be examined as to its poisonous nature, there
are only two ways left in which to solve the question as to the use of coloring matters
in the manufacture of food and articles of daily use.
One of them, and at the same time the simplest, would be to prohibit the use of all
coloringg matters for the coloring of foods, etc. This rigorous point of view will hardly
ever be taken by legislators, because it would be tantamount to the removal of many
marks of differentiation which have become desirable and necessary.
The second way seems to be the much more practicable, and which Theodor Weyl
propnowjd sulie time ago.
It (n.-n:41tk in permitting the use of only a definite number of coloring matters, recog-
niztd as harmless, for the coloring of articles of fuod, etc. Which coloring matters
are to 6! -i permitted is to be determined by the authorities having jurisdiction.
The rsulme authorities are also to determine the maximum amount of each coloring
matter which can be used for any purpose. New coloring matters can be used only
for the above-mentioned purposes when they have been recognized as nonpoisonous
after official test. All permitted coloring matters must be also detectable, even in
small amounts. (11Handbuch devr Hygiene, 1896, Vol. Ill, p. 385.)


44






RECOMMENDATIONS BY ASSOCIATIONS, ETC.


NATIONAL CONFECTIONERS' ASSOCIATION.

In 1899 the National Confectioners' Association of the United
States issued an official circular, which has been previously discussed,1
designating certain colors as harmful, and certain others as harmless;
the members of each class are given in the following list, in which
only one trade name is given, the Green Table number appearing in
parentheses at the end of that name.
HARMFUL ORGANIC COLORS.
Red colors: Ponceau 3RB (163); Crocein Scarlet 3B (160); Cochineal Red A (106);
Orocein Scarlet 7B (169); Crocein Scarlet 0 extra (164); Safranin (5S4).
Yellow colors: Picric Acid (1); Martius Yellow (3); Acme Yellow (84); Victoria
Yellow (2); Orange II (86); Metanil Yellow (95); Sudan I (11); Orange IV (88).
Green colors: Naphthol Green B (398).
Blue colors: Methylene Blue BBG (650).
Brown colors: Bismarck Brown (197); Vesuvin B (201); Fast Brown G (I38); Chrys-
oidin (17, 18)
HARMLESS ORGANIC COLORS.
Red colors: Artificial Alizarin and Piirpurin (534); Eosin (512); Erythrosin (5171;
Rose Bengale (520); Phloxin (521); Ponceau 2R (551; Bordeaux B (65); P,>nceali 2(G
(15); Fuchsin S (462); Archil Substitute (28); Orange I (85); Congo Red (240); Azoru-
bin S (103); Fast Red D (107); Fast Red (105); Ponceau 4GB (13); Fuchsin (44q).
Yellow and Orange colors: Naphthol Yellow S (4); Brilliant Yellow (5); Fiast Yellow
(8); Fast Yellow R (9); Azarin S (70); Orange (43).
Green colors: Malachite Green (427); Dinitrosoresorcin (394).
Blue colors: Indigo (689); Gentian Blue (457); Couplers Blue (600).
Violet colors: Paris Violet (451); Wool Black (166); Azoblue (287); Mauvein (593).
Brown colors: Chrysamin R (269).
SCHACHERL.

SchacherI in 1903 made the following statement:

If coal-tar colors are to be permitted fur the coloring of food, then. in my piTi itn.
it is not right to limit the use of such to a few coloring matters, but groups (itf roluring
matters must be permitted which are without suspicion from a sanlitary statdlpiinit.
and which are characterized by definite reactions. Oilier gruiips, in th uilter limi1,,l
which contain harmful or merely suspicious colors, must hie :;.soluitly rixiiitld.
* * The selection would be easily made if sufflicint daita wervn at lhail with
respect to the physiological action. Unfortunately this is lackikig. a 'ircumsl.iiitm1
which need not be surprising in view of the very large number of syunthlet i, co ilrinu..
matters, Hincle the Schultz-Julius tables cninmerate (. ti sucli rdl,,rs. lif,'intunati-lv
the experiments of Th. Weyl, whieih wer. planned ill ; larirg sc'al', hlI\II o't l,,, el
completed, and apart frim isolated inve.stii-ations we are Ir limited iin li..,ing jIl .mtisiti
upon the most (if these colors to the proof that to diatt nothing will rrspri.t ti liarnful
action has lIw(.ome known. ('isin ( uti ily" it is still )i-1issilile that ione ir tli-
other coloring matter which may to-day be regarded as above suspiciiii, or a n.wly
discovered under all 'ircunistancts have the pl] wer to (xcliudr for ws. in fi,,ils :All s ..iiii i,,is
combinations, andi all su h coloring inatlit(rrs as are ,it <:sil v distiiiguii ,il. fri ,ii tl,,n .


I k.e also p. 30.


45







46 COAL-TAR COLORS USED IN FOOD PRODUCTS.

The final recommendations of Schacheri amount to permitting-
1. All the Azo colors, Nos. 7 to 393 of the Green Tables, except No. 86.
2. All the Triphenylmethane colors, Nos. 427 to 492 of the Green Tables, except
the hydroxyl derivatives, which would be Green Tables Nos. 483,484,485,486, and 491.
3. All Pyronins, Nos. 493 to 527 of the Green Tables.
4. All Oxyketones, Nos. 537 to 570 of the Green Tables.
5. All Indulins, Nos. 599, 601, and 603 of the Green Tables.
6. Naphthol Yellow S, G. T. No. 4.
7. Methylene Blue, G. T. No. 650.
The use of all other coal-tar colors would best be forbidden, partly from hygienic
and partly from practical considerations (rendering control more easy), until the
absolute harmlessness of the group in question is determined by physiological test.
* * It should be required of all permitted coloring matters that they shall not
contain substances which are harmful to health, or even suspicious, either in chemical
union or as contaminations. (Fifth Internationol Congress of Applied Chemnistry, Ber-
lin, 1903, Vol. IV, pp. 1041-1048.)
The exclusions recommended are all nitro-colors, except Naphthol
Yellow S; all acridin colors and all chinolin colors; Auramin, In-
dophenol and all nitro-colors, except Naphthol Yellow S, Schacheri
regards as not necessary; further, he has no knowledge of the physio-
logical action of any of the azoxy or the thiobenzenyl colors, and
aside from Methylene Blue, he has no knowledge of the physiological
action of the oxazins and thiazins.
CLASSIFICATION OF RECOMMENDATIONS IN THE LITERATURE.
The following table shows the groups of coal-tar colors of the
Green Table classification and the Green Table numbers of the
members of each of the groups, together with the favorable or unfa-
vorable recommendations found in the literature in regard to each
and a statement as to those regarding wliich no recommendations
are made:
Tabulation of recommendations found in the literature.
Number of Individuals Total number.
reported on-
Groupr Green
nuri- Table Name of color. Un- Favor- Con- Re- Not re-
ber. number. favor- ably. flict,- ported, ported.
ably. ingly.
(1) (2) (3) (4) (5)
1 ..... 1-6... N itro ...................................... 4 2 0 6 0
2..... 7- 132 M onoazo.............................. ..... ;1.3 10 19 32 94
S. -. 13;-:.f6. Disazo ...................................... 3 3 7 13 191
4..... 3.,7-A 3 2.. 'risazo ....................... ........... ................................ 46
.. 3Z.3;-{93. 'T trakisazo................ ................... ....... ................ 11
..... 3 4--:39.. Nitroso ..................................... 0 1 1 2 3
7... 399-4 6 l i libe .................................... 0 1 0 1 17
X. 417--12l1.. Oxvk toi ........................................ ........ .... 8
9 4 -25 121'A.. I)i ul e rivl n il j jan.ll .......................... 1 I 0 1 1
H ..... .127 l2.. T'riph rvlnei hai ne ......................... .5 .5 8 IS 48
1 I._ 49 1 27.. XialthhcrN................................... 2 5 1 8 27
1-.... Acridlin...................... ............... 2 0 0 2 4
13. ... .11 570.. A n hrnweni ....... ......................... I 0 0 1 1 36
14 ... 71 -574.. I ni opli.riiuL, ............................. .. 2 1 0 3 5
15..... 57 4 i 16. Azin ....................................... 2 3 2 7 31
.16 .... il7 ;4X.. Oxizln.s .................................... 2 0 0 2 30
17..... C5 ;:,7 ThiIlnsz..i.................................. 3 0 1 4 5
1H. 6. i -6i4;. l l'ioh nziri vI................................. 1 0 0 1 5
19 .... H6 -l4i,7.. (ilinulin... .............................. 1 0 0 1 3
0..... 6;W-lCiK. SHlphilds ................................ 2 0 0 2 19
21..... GK9-i95. Inhligos .................................... 0 1 1 2 5
"rotal .... . ... ..... ......... ....... 33 32 41 106 689






RECOMMENDATIONS BY COLOR INDUSTRIES.


CONCLUSIONS.

Applying the Schacheri rule, "Other groups which contain harmful
or merely suspicious colors must be absolutely excluded," to this
table and assuming that all entries in columns 1 and 3 shall be
regarded as rendering such colors as "harmful or merely suspicious,"
it will be found that only one group, namely the Stilbene group,
would be permitted under that rule; further, that this rule would
admit 17 colors, not one of which has been reported on in the litera-
ture as to its physiological action. This state of affairs tends to em-
phasize the difficulties in the way of any generalization which will be
safe so far as public health is concerned and fair to those who use
food colors for admittedly legitimate purposes and to make the
following recommendation appears to be the only satisfactory way
of solving the food-color problem:
Although it would be possible to draw quite reliable conclusions as to the advisa-
bility of employing certain colors for food products on the basis of their chemical
constituency, the mode of their manufacture and of the ingredients used in same,
nevertheless, I think that by far the safest way would be on the one side to force
the dealers of colors intended for food products to sell only such colors with which
exhaustive and careful physiological tests have been made by experienced and espe-
cially impartial and thoroughly reliable people, thereby establishing their harmless-
ness beyond a doubt. On the other hand, the manufacturers and canners of food
products of any description should be forced to purchase and use only those colors
which they're surehave been submitted to such careful tests as have been described
and by these tests found to be harmless. (Licber, The wuse of coal-tar colors in food
products, 1904, p. 150.)
This view is confirmed by Santori (Moleschott's Unternuchunycn,
1895, Vol. XV, p. 57), who says:
From all these experiments it follows that it is impossible, as some have desired to
do, to conclude simply from the chemical composition and constitution whether any
given coal-tar dye is poisonous or nonpoisonous. Thus Indulin belongs to the same
group as Printing Blue and Methyl Violet to the sameni group as does. Acid Violet;
therefore each individual coal-tar dye must be separately examined, and it is only
by this laborious method that the use of all really poisonous coal-tar dyes will be
prevented.

VII. RECOMMENDATIONS MADE BY UNITED STATES COLOR
INDUSTRIES AND TRADES TO THE DEPARTMENT OF AGRI-
CULTURE.

Prior to the issuance of any regulations, the commission on rules
and regulations for the food and drugs act, June 30, 1906, lhelid iieet-
ings in Now York City during September of that year. The steh'i-
graphic reports of those meetings, and the briefs filed, in so faLr Its t iC)

I Santori examined 15 ifrt blu and violet dyes on dogs by the mouth and hypodennicrnll. Of
these 15, R are poisonous b)y the mouth and 7 are nonposonous by the muthu, lie found Inlulin W b ipois-
onous and Printing Blue to be nonpoisonous: Acid Violet to be nonpoisonous anti Methlyl Violet to be
poisonous.


47






48


COAL-TAR COLORS USED IN FOOD PRODUCTS.


relate to colored food, colored food products, or material for coloring
foods or food products, have been condensed verbatim in the following
pages with the sole exception of omissions, as indicated; for obvious
reasons the names of those making the suggestions hereinafter quoted
are not given. This review of opinions expressed and recommenda-
tions given by the industries and trades most interested in the manu-
facture, use, and sale of food colors and colored food products is
believed to be fair and full with respect to each and every quotation.
The numbers in parentheses following each quotation refer to the
pages in the stenographic minutes of the hearing from which those
quotations are made.

ANTAGONISTIC TO ALL ADDED ARTIFICIAL COLOR.
1. Our position in the coloring question is thatwe are opposed to all artificial coloring
matter in food products. * (p. 109).
2. Secondly, speaking first of our own business, and I believe that my view would
hold as regards all food products, it is my opinion that all added artificial coloring
matter in food products should be prohibited. Mly experience in our line of business
demonstrates this to me beyond any question of doubt (p. 439).

CONCERNING RESTRICTIONS AND REQUIREMENTS.
WHAT CLASSES OF COLORS SHOULD BE PERMITTED TO BE USED.
1. All colors, irrespective of their class, whether animal, vegetable, or synthetic,
which have been physiologically and chemically examined, and which will neither
retard digestion nor have special physiological effects when consumed in quantities
corresponding to two grains per day per adult (p. 106).
2. On the use of colors we recommend that any kind of a harmless color should be
permitted provided it is not a color generally known to be poisonous, or generally
found to be poisonous, or one that may be almost impossible to be produced without
containing some poison within itself, when finished and ready for use (p. 119).
3. Only such colors as are guaranteed to be harmless by reliable manufacturers should
be used in the manufacture of confectionery (p. 555).

WHY COAL-TAR COLORS SIIOU'LD NOT BE BARRED.
4. Coal-tar colors, as a class, should not be prohibited; but all those coal-tar colors
generally found to be poisonous, or which are hard to produce without containing
poisonous properties when ready for use, should be forbidden the privilege of being used
or offered for sale for use in food (pp. 116, 117).
5. I ought to put in a plea for the use of coal-tar colors, harmless, of course, for the
ra,-on that we have not as yet been able to find any vegetable coloring that is suitable
tltm will give us the results that we require. Coal-tar colors, as everybody knows,
are much stronger and are more soluble and not acted upon by acids, whereas the
vegetable colors, with but one exception, which is a dark red, we have found great
difiic-ulty in making use of for bottled soda water. Almost all the vegetable colors
either fade out or change on account of the citric acid in the syrup or food, or form in t
little while a precipitation which renders the goods unsalable (pp. 119, 120).
6. * aniline butter colorings are superior to all vegetable colors
in the following points: (1) Shade and brilliancy. (2) Strength, by which less
foreign material is introduced into the butter. (3) Permanency when exposed to
light arid cold storage. (4) No effect on the taste or flavor. (5) A clear solution






RECOMMENDATIONS BY COLOR INDUSTRIES. 49

without sediment or mud which gives the butter a uniform tint without specks (pp.
176, 177).
7. We recommend * that the use of harmless coal-tar colors, such as
chrysoidine, tropweoline, azoflavine, rocelline, ponceau, Bordeaux, Biebrich red,
sulphonated fuchsin and naphthol yellow S be allowed, subject to declaration on the
label of the quality and quantity of the color used (p. 226).

RELATION. OF LABEL TO COLORED FOOD PRODUCTS.
8. * if it seems wise in the opinion of the commission to allow certain color-
ing matters in food products, then the names of the coloring matter ought to be stated
on the article (p. 109').
9. * I suggest that the use of aniline colors should be made proper if it is
so stated on the label (p. 127).
10. We recommend * that the use of harmless coal-tar colors * be
allowed subject to declaration on the label of the quality and quantity of the color
used (p. 226).
LABELING OF FOOD COLORS AS DISTINGUISHED FROM COLORS FOR OTHER USES.

11. We recommend that if by any means the Government has the power under
the food laws to compel color manufacturers so to do, they be compelled to label all
packages containing colors intended to be used in articles of food as colors intended
for such purposes as distinguished from colors intended for other purposes; * *
(pp. 555, 555a).
THE TEST OF A HARMLESS COLOR.
12. A harmless color is one "which will neither retard digestion nor have special
physiological effects when consumed in quantities corresponding to two grains per
day per adult" (p. 106).

QUANTITY OF COLOR TO BE CONSIDERED IN DETERMINING HARMLESSNESS.

13. The quantity of 2 grains is mentioned here because in confectionery where
these harmless colors are more used perhaps than in any other product, it would be
a proportion of one part of color to 3,500 parts, representing 1 pound of color to :3.a5jo
pounds of confectionery, and that is why that was accepted, because that is practi-
cally the maximum quantity used in confectionery (p. 106).
14. In the very minute quantities in which the colors are used in carbonated bev-
erages, it would seem a great hardship to prevent us from using coal-tar colors. One
ounce of coal-tar red will color satisfactorily from 1,000 to 2,000 gallons (of soda water.
Of yellow and orange 1 ounce will color from 1,000 to 8,000 gallons. It is readily
seen that unless the coloring used is absolutely a violent poison it can have abso-
lutely no effect on the consumer who takes it in an 8-ounce glass, and who could
not possibly consume half a gallon or a gallon of that product (p. 119).
15. On this ba.,is 1,()0 pound, of butter would contain 4120 grains of aniline color
(p. 183).
16. One ounce of color to 30 pounds colored food (p. 135).
THE NUMBER OF DIFFERENT COAL-TAR COLORS REQUIRED.

17. And if I were on this committee I would advocate taking out twn or three
dyestuffs ,which beyond any shadow of doubt are harmless, and which have been
experimented upon, and which would be sufficient for all the purpLIoses of the indu.-try
* * none of these colors are patented, anybody can manufacture them i pp.
147, 148).
972910-Bull. 147-12-----4






50


COAL-TAR COLORS USED IN FOOD PRODUCTS.


18. You have been told that the food commission of the State of Pennsylvania is
going to rule that seven colors shall be allowed in the State of Pennsylvania. That
is not enough, because it is not possible to reproduce all of the required shades with
those colors unless you take the seven primary colors, when you can reproduce any
colors. But it is absolutely necessary to have about three yellows to meet the require-
ments of the trade. Some of the articles that are put out have an organic acid nature,
and the anilines will stand that. * On that account the character of the
food product must be taken into account in the use of the color, and the confectioners
have about 30 colors that I know positively of * (p. 160).
19. We recommend that * chrysoidine, tropaeoline, azoflavine, rocelline,
ponceau, Bordeaux, Biebrich red, sulphonated fuchsin, naphthol yellow S be
allowed * (p. 226).
MANUFACTURING REQUIREMENTS WHICH COAL-TAR COLORS MUST FULFIL.
20. Coal-tar colors, as everybody knows, are much stronger and are more soluble
and are not acted on by acids. * Almost all the vegetable colors either fade
out or change on account of the citric acid in the syrup or food, or form in a little
while a precipitation which renders the goods unsalable (p. 119).
21. There are many of these colors (coal-tar colors) that will not stand the natural
acids produced in manufacturing foods. For instance, in making confectionery, in
boiling candy you make a certain grade of candy where the mixture is boiled to
230. A certain color will stand that temperature. Then you take another candy
and that is boiled to 320 or 340 F., and the colors that will stand 230 will in many
cases not stand the temperature of 340, while another class of colors will stand that
temperature. So you have got to distinguish and get a color that will stand these
difficult requirements (pp. 159, 160).
GUARANTEES AND GOVERNMENT CONTROL.
22. Only such colors as are guaranteed to be harmless by reliable manufacturers
should be used in the manufacture of confectionery (p. 555).
23. We recommend * that the Government procure samples of such colors
from time to time, wherever they have jurisdiction so to do, and if such colors be not
legal for such purposes under the food law, that the same be prosecuted and driven
off the market in so far as the Government has the power to do so; and if no means
can be devised to compel such labeling of colors intended for food purposes, then
that the Government procure such evidence as possible as to the purpose for which
a color is intended to be used, and if such evidence shows a food purpose, that such
color be prosecuted if illegal under the food law (pp. 555, 555 a).
24. See page 13.
25. The chemical test is the first, and that might throw out a color on account of
its containing a little tin or zinc, or some substance foreign to the food product.
Whether that is deleterious in the quantity in which it is present or not is immaterial
(p. 160).
26. In a brief filed the following suggestions were made:
It must be stated that all the chemist can determine is whether or not the colors
contain some impurities that are known to l)be of poisonous nature. Aniline colors are
or can be made entirely free of such impurities, and with this fact established the task
with the chemist is exhausted. When it conimes to decide the question whether or not
a color by itself, when free of all impurities, is injurious to health or not, then the
chemist is not the proper authority; it is for the physiologist and for the medical pro-
fession to pass on such questions. Chemical theories go for nothing in deciding such
questions. It would not even do to classify colors or other substances according to
their makeup, as it has been shown again and again that substances belonging to the
same chemical class arc entirely different in regard to the physiological conduct.






INVESTIGATIONS ON HARMFULNESS. 51

Reliable information on this subject can be gained only by physiological experiment,
as we can not say definitely whether a substance, color or any other, is injurious or
not without finding out for every substance by experiment. This has been done for a
considerable number of aniline colors, and these experiments are the only things that
deserve any attention. Everything else is idle talk. * There are a very
large number of aniline colors that have not been treated yet, and we are safe in saying
that among these will be also some harmless and others injurious. As they have not
been experimentally tested, we do not know which are harmless and which are not;
It will therefore be clear that a law forbidding the indiscriminate use of aniline color
for the purpose of coloring articles of food is necessary and useful.
But if the meaning of the law is to prevent only the use of injurious colors, as it
appears to be, then the way to proceed would be very definitely outlined. Besides
physiological colors, all such colors should be forbidden that have been found to be
injurious and such aniline colors as have not been tested sufficiently. There will
then be left over a number of aniline colors which have been proven by experiment
to be entirely harmless, even if taken in large doses.
The experimenters were quite impartial. They had no preconceived ideas, but
started simply to find out the true state of affairs. Their reports are therefore very
reliable, and it will not do to overlook or to ignore them. The colors that they found
harmless can be considered perfectly safe, so much the more as the doses conveniently
taken with food would be much smaller than the doses that have proven to be harm-
less. These harmless aniline colors carry all the shades wanted in the food industry.
The law should provide that one of these colors (or mixtures of these) must be used
when a food article is being colored, because these few aniline colors are the only
colors that can be considered perfectly safe as far as our present knowledge goes.
Nothing should be left to guesswork or experimenting, as is the case just now. The
colors that are permitted should be enumerated by their scientific as well as by their
commercial names, and only such colors should be listed as permissible for coloring
food products as have been proven to 1Ie harmless, even in large doses. Provision
should be made to insure the purity of the colors sold for coloring food; the manner
of packing such colors and the labeling of same should le laid down clearly, and all
colors now listed, aniline as well as physiological colors, should be strictly forbidden.
If the problem is viewed without preoccupation and prejudice, the facts given above
will speak for themselves.

VIII. INVESTIGATIONS, OTHER THAN ON ANIMALS, BEARING ON
THE HARMFULNESS OF COAL-TAR COLORS.
PFEFFER.

Pfeffer, writing on tlhe Absorption of Anilin Colors by Living
Cells, summarizes his results as follows:
The relatively little poisonous Methylene Blue does damage protoplasm in a solution
of 0.001 per cent.
Methyl Violet: This coloring matter is not only stored up in the juices of the cell.
but is also able to color the living protoplasm, and care is necessary, on account 4of ith
poisonous nature of Ihe Mtethyl Violet, to prevent damage; these cautions are based
upon solutions of 0.0003: to 0.00001 per cnrt i strength.
Methyl Violet hles poisonous than t'yvanin.
Bismarck Brown about as pIsonMus as Miethvlyl(en. Blue.
Fuchsin as poisonous as Methylene Blue.
Safranin as poisonowis as Methylent, Blue.
Methyl Orang is poiso.nous (inly to a slight degree.
Tropwolin 000, Tropauolin 00, and RIoolic Acid are not poisonous.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


Methylene Green as poisonous as Methyl Violet.
Nigrosin as poisonous as Methyl Violet.
Eosin (Tetraiodo fluorescein) kills in 0.1 per cent solution, but lets live 24 hours in
0.01 per cent solution. (Untersuchungen aus demn Botanischen Institut zu Tuebingen,
1886-88, mol. 2, pp. 179-331.)
WINOGRADOW.
*
Winogradow reports on the influence of certain coal-tar colors on
digestion, which experiments were carried out in glass. The con-
clusions arrived at are as follows:1
The twelve colors, Safranin (584L, Azo Fuchsin G. (93), Coerulein S. (527), Jodeosin
(516), Magdala Red (614), Benzopurpurin (277, 278, 279, 307), Ponceau 2R (55),
Orange II (86), Phloxin RBN (?), Chrysanilin (532), Azoflavin (92), and Cerise
(mixture of 448 and 532), even in amounts of a few milligrams, which in relation to
thedigestive fluid make up only few tenths or hundredths of a per cent, exercise a
strongly retarding, almost completely inhibitive, action upon the peptic digestion of
albumen.
The thirteen colors, Chinolin Yellow (667), Acid Green (434, 435), Azo Acid Yellow
(92), Naphthol Yellow (4), Primulin (659), Anilin Orange (87), Metanil Yellow (95),
Methylene Green (651), lodin Green (459), Yellow T (84), Anilin Green (?)
Auramin 0 (425), and Martius Yellow (3), retard the digestive action noticeably,
although to a slighter degree than the first 12 colors; in any event they are not indif-
ferent. (Zts. N(ahr. Genussm., 1903, v. 6, p. 589.)
HEIDENHAIN.
Heidenhain, in his book entitled "Ueber chemische Umsetzungen
zwischen Eiweisskorpern und Anilinfarben" (Bonn, Germany, 1902),
reports on the behavior of 70 different coal-tar colors, 3 intermediate
products, and 4 raw materials toward various albuminoids such as
serumalbumen, albumen, and casein.
Of these 70 colors, 21 have been investigated physiologically, and
the results embodied in this report; and of these 21, 17 were on the
United States market as food colors and 4 were not on this market.
Limiting the attention to the 17 that were offered, 4 of them are
among the 7 permitted colors of Food Inspection Decision 76.
In the cases where albumen and casein were used, they were
employed in 0.5, 0.1, 0.02, 0.01, and 0.005 per cent solutions, acidified
with acetic acid; the coloring matter was employed in a 1 per cent
solution in the first strength, in 0.1 per cent solution in the second
ad(l third strengths, and in a 0.02 per cent solution in the fourth and
fifth strengths, and one volume of coloring-matter solution was
brought in contact with five volumes of albuminoid solution.
The following colors s precipitated the albuminoid in all the strengths.
The numbers in parentheses indicate the Green Table numbers;

I It 19 not iialways posible to identify the trade narnmieq given by Winogradow with specific numbers in
the (Irefn 'rIl11-4; the I lnmbers in pairendhi.4es after the name Indicate the number in the Green Tables
where vcr thaIt lilntiific.tion could he minaile with any reasonable certainty; wherever two or more numbers
appear, the context indicates that the name might apply to any one or all of them.


52






INVESTIGATIONS ON HARMFULNESS.


the numbers in italics are those of the permitted list of Food Inspec-
tion Decision 76: (55) Ponceau 2 R, (65) Fast Red B, (434) Light
Green SF bluish, (56) Ponceau 3 R, and (106) New Coccin.
The following precipitated in all but the fifth strength: (107)
Amaranth.
The following precipitated only the first three strengths: (14)
Orange G and (85) Orange I.
The following precipitated only the first two strengths: (462) Acid
Magenta.
For the basic colors the method of testing was different from thliat
described for the acid colors and the amounts employed were not so
definitely set forth. A 1 per cent solution of serum albuminoid was
employed; the solution of coloring matter used varied in strength
from 0.5 to 1 per cent (b), a "very dilute solution" (a) being also
employed. The annotations given by tlie author (p. 114) arel herewith
reproduced in full:
(17) Chrysoidin Y. (a) In a very dilute solution the yellow ba-e i- at nicu liber-
ated, and when sufficient color is added albumen precipitation lakes place. No color
change on heating. (b) Turns yellow at once. Further additional culor prduicc:- a
brown and albumen precipitation.
(201) Manchester Brown. (a) Becomes yellow at once, due to separation if the
free base. On heating no change. (b) Becomes a discolored brown, and produces a
nice brown albumen precipitate.
(425) Auramin 0. (a) No change. (b) Precipitates albumen strongly.
(427) Malachite Green. (The oxalate of the color was used.) (a) Clhr chlianigs
from a blue-green to a more pure green. (b) Cold, no prccipiiatiiui idf albumen;
heated, sudden precipitation of albumen.
(428) Brilliant Green. (A sulphate of the color was i.-sd.) (a) B.i,',in,- milky.
(b) Immediate precipitation of albumen.
(448) Magenta. (Acetate and nitrate were u1.ed, and ill b1,tl :icleil Ilie .amc.) (')
Color changes from yellowi.h-red to ro-e-red. (b) Albiiuiii'ii pr.'ipiilalin :uldlhant,
even in the cold.
(451) Crystal Violet. (a) The color loses its reddi-h '1C.-I ai 1(1 c'ilaIgets to 1,Ir',' 1blue.
(b) Albumen precipitated by the us.e of much ciil,,r.
(4) Naphthol Yellow S was tested as tlie frev-rcl,,r aiii aani ii, n, t;ll, .- iiin ,r pItas-
sium salt, which is its commercial form. It ipr following solutions: 1. 1 per cent. serum a.1 lIIumIen il water. 0.5 ].'"r u'lit .-,'riim
albumen in 10 per cent acetic acid. 3. Caseiii, 0.7- plr 'ciit inl P) ,,r ,ciit .t,-tio- ,ril.
4, Serum albumen; 5, ('Caseii; 6, Nurlein, all in 03 ) percent h'>liitii in 0 2 p14r cilit
sodium hydroxid. 7. Nucleinim acid il (11.5 per 'tiii W'tI r T S,1i ,,i'.n
The relationship between the aniounits of ,olor-acid an1d albuininmid
solution here used(l loes linot alppel r ldeflinitelV ill ttie hook.
Ilmving reference no)w, to tlie literatiutre a1H lit h ,e jisio li I
action, as compiled lhereiln, it will l)be )observ.1 lithat ithe aliiilt to III-
cipitate all)u n, nit )reitltae it, lltd'r til rciiIllili,,iis of
Ileidenlhaiin, a)pea.rs Inot It o laI'e any dlirIt' ('0111)ti,11111 Nwith, t!1,
results obtained by actuatil phlisiologictl test.t oII aJimals (W or 1an.1.
For instance, among the five that precipitated iall live st rentgths of


53






COAL-TAR COLORS USED IN FOOD PRODUCTS.


albumen and casein, No. 65, Fast Red B, of the Green Tables, has
been found to be not harmful by tests actually described; No. 56,
Ponceau 3 R, belongs to a class of colors generically permitted by the
law of Austria; Nos. 55, Ponceau 2 R, and 106, New Coccine, have
been reported on both favorably and unfavorably by different experi-
menters; No. 434, Light Green SF bluish on physiological examina-
tion hlias been described as suspicious.
From this it appears that two colors, physiologically probably
harmless, precipitated all the five strengths of albumen, and three
colors, which are perhaps no more than suspicious, likewise precipi-
tated all five strengths of albumen.
No. 107, Amaranth, which has been examined with favorable
results by two different experimenters, precipitates four out of the
five strengths.
Of the two colors precipitating the first three strengths, both have
been examined physiologically with favorable results, namely, Nos.
14,.Orange G, and 85, Orange I.
The color wlich precipitated only the first two strengths, namely,
No. 462, Acid Magenta, has likewise been examined physiologically,
and the reports are favorable.
Thus it would seem that there is no definite connection between the
physiological action and the ability to precipitate albumen from
acetic acid solution in the case of acid colors.
In the case of basic colors the situation seems to be somewhat
different.
OTHER AUTHORS.
Rosenstiehil (Fifth International Congress of Applied Chemistry,
Vol. III, p. 700) states that when tle color is present in an excess,
yeast absorbs 8 per cent of Magenta (448) and 5 per cent of Malachite
Green (427, 428). The Acridins (528-538), the Thionins (649-657),
the Safranins (583, 584), and the Rosanilins (447-448) dye yeast the
best; solutions containing 3 per cent by weight of the dry weight of
the yeast are completely ldecolorized by such yeast and at ordinary
temperatures. Tle Eosins and( Phlithaleins dye the yeast only incom-
pletely, whereas Azo dyes (7-393) (witli tlhe exception of Benzo Pur-
purin, 277, 278, 279, 309) do not (lye yeast at all. Such dyed yeast,
however, is not (lead; it has merely lost its power to cause fermenta-
tion. The numbers in parentlieses are tie corresponding numbers in
the Gr(een Tables as nearly as they could be identified.
Bokorniy (Chem. Ztg., 1906, v. 30, p. 217) examined Magenta (448),
Stif'anin (584), Victoria Blue (487, 488 or 490), Methylene Blue (650),
and Alizarin Blue (562 or 563) (tlhe numbers in parentheses are the
probable Green Table numbers) as to their effect on micro-organisms
such as yeast cells, infusoria, and the like, and found that these dyes


54






INVESTIGATIONS ON HARMFULNESS.


55


in a concentration of 1:100,000 killed them, whereas strychmin
nitrate in the same concentration is substantially without effect.
Death is caused by absorption of the dye by the albumen of the
protoplasm. The dyes seem to be absorbed not only by living albu-
men, but also by living nerve cells and fibers. Pure anilin or coal-
tar colors, however, are not poisonous in the ordinary meaning of the
words, that is, humans are not likely to be easily injured by them.
Houghton (J. Amer. Chem. Soc., 1907, v. 29, pp. 1351-1357) shows
that Bismarck Brown (197, 201) and Crocein Scarlet (160?) hinder
the peptic digestion of fibrin, casein, and albumen.
Stilling (Anilinfarbstoffe als Antiseptica, 1890, v. 2, pp. 55-56) states
that he found the animal cells to be affected by pure coal-tar colors
in the same way that vegetable cells were affected.
Penzoldt, based upon the experimental work of Beckh (Archiv.
Exp. Path.. Pharmak. 1890, v. 26, p. 310), reports as follows:
Of the 15 dyes-
Green Table
Name. number.
1. Malachite Green.......................................... 427
2. Hofman's Violet (methyl variety)......................... 450
3. Methyl Violet........................................... 451
4. Rose Bengal (Erythrosin)................................ 517
5. Phenyl Blue............................................. 480
6. Methylene Blue......................................... G50
7. Fuchsin.................................................. 448
8. Coralline................................................. 1844
9. Eosin................................................... 512
10. Methyl Orange........................................... 87
11. Vesuvin................................................. 197
12. Tropaeolin.............................................. SS
13. Scarlet Red..... ....................................... (?)
14. Congo Red............................................... 240
15. Indulin sulpho acid....................................... 601
all of which are water soluble and when u:.ecd werc free from arsenic, nliy the first six
in saturated solution arrested the development of Staphylococus pyogems iiurus, and
of these six all but the Erythrosin and Methyl.i, Blue uarreted the growth ,f mithrax
bacillus.
Of these six when injected into ralbbits su.iibt.,iol.ilsly the following pridurCAd no
changes of consequence: Erythrusin (250), PlicnIl Bl1t (100), Mtlthylene Blue (75).
The numbers in parentheses show tht inumlcr ,,f millignms 4f dye per kill) body
weight of the rabbit..
Methyl Violet (50) produced only local (changt.s, nii'h as gangrtwn,.
Malachite Green (100) and llofman's Violht (20) produiL. d inusular jparalysi.s, which
in the case of Malachite Grtnri resulted fatally on the ninth day: in thei c'a.* o(f llf-
man's Violet the paralysis was (oniplete on the tenthi day.
The remaining nine colors are apparently of no t.ffect upon t, htaphylovciue or upon
anthrax.
II. W. Williams (A Manual of Bacteriology, 19.06, p. 200), under
"Disinfectants and Germicides," says:
Aniline dyes. Many of these substances, notably pyoktanin (M.thvl Vi' 1.4t), pIs-
sees germicidal propertiv4. A solution of 1:5000 will kill tho anthrax bacillus in two






56


COAL-TAR COLORS USED IN FOOD PRODUCTS.


hours. A much stronger solution, 1:150, is required to kill the typhoid bacillus in
the same time. Malachite Green is said to possess even greater germicidal power than
pyoktanin. Methylene Blue also possesses considerable germicidal power.

IX. COMPILATION UNDER THE GREEN TABLE NUMBERS OF ALL
INFORMATION AVAILABLE AS TO THE SUITABILITY OF COAL-
TAR COLORS FOR FOOD.

GENERAL STATEMENTS.

Before entering upon a detailed study of what has been published
for and against specific coal-tar colors, it is probably well to consider,
for whatever they may be worth, some of the general statements that
have been made, from time to time, in the literature relative to coal-
tar colors, considered either as a whole or as subdivisions or classes
thereof, and their physiological action or their suitability for use in
foods.
1. Schultz (Die Chemie des Steink'ohlenthcers, Brunsuwick, 1887-1890,
Vol. II, p. 35), after discussing the regulations of the German Empire
in respect to food coloring, says:
With respect to these regulations the artificial organic coloring matters can be
regarded, in general, as harmless. For the purposes of dyeing magenta made by
means of arsenic acid, further picric acid, and those coloring matters which occur as
oxalates or zinc chlorid double salts, such as Methylene Blue and Bitter Almond Oil
Green, can be used. The use of the substances named for the coloring of food products
is, however, suspicious and should not be permitted.
2. Stilling (Anilinfarbstoffe als Antiseptica, Strassburg, 1890, Vol.
II, pp. 55-56) says:
In view of the fact that the most innocent substance, such as distilled water or com-
mon salt, when introduced in large quantities into the organism can act fatally, the
anilin coloring matters therefore, particularly if they be free from all admixtures, such
as arsenic, copper, and chlorid of zinc, are to be regarded as wholly nonpoisonous.
All experience gathered since my first publication has likewise fully confirmed this
nonpoisonous nature.
3. Stilling (Ber. PJin. Wochensch. 1890, p. 581) also says:
Proceeding from purely theoretical views, and based upon these botanical and
physiological experiments, I have recommended anilin colors as antiseptics for the
following reasons:
1. They are to be designated as absolutely nonpoisonous. This will be confirmed
by every chemist acquainted with the relevant details, and also from the medical aide
this has long ago been determined by Grandhomme. The publications of this author,
who made extensive observations and experiments in the anilin factory of Meister,
Lucius & Bruening, appeared in the beginning of the eighties, and has hardly become
known in medical circles. However, I was first made acquainted with this by my
colleague, Prof. Rose, in Strasburg.
2. That it is possible to bring about death in experimental animals by introducing
large amounts of the coloring matter into the peritoneal cavity proves nothing against






COMPILED DATA UNDER GREEN TABLE NUMBERS.


the nonpoisonous nature of these substances. This action is to be regarded as a purely
mechanical one, a view which I will thoroughly confirm in my second communication.
With respect to the anilin colors not soluble in water, Ehrlich long before me, in his
excellent publication on the oxygen requirements of the organism, has arrived at this
view, and has excellently described it as merely a penetration of the organs.
4. Lehmann (Methoden der Prak-tischen Hygiene, Wiesbaden, 1890,
p. 543) says:
The hygienic significance of coal-tar colors has heretofore been judged quite vari-
ously. When the intensely poisonous nature of the first impure and particularly
arsenic-containing coloring matters became known the inclination was to judge the
coal-tar coloring matters very strictly; when it was subsequently recognized that
the contaminations were largely the cause of the harmfulness to health, there followed
a period in which no poisonous coal-tar coloring matter was known in any pure con-
dition. (Eulenberg & Vohl, 1870.) More recent investigations, however, have
disclosed a series of coal-tar coloring matters which, as a matter of fact, possess a con-
siderable poisonous action, and already cases, although not numerous, have become
known in which serious and even fatal poisonings by means of pure coal-tar colors
have arisen. Alongside of this there still continue to exist the possibilities described
by Eulenberg and Vohl (Viertel-Jahressch. fur Gerichtliche Mediz, 1870), whereby
harmless coloring matters become harmful; but the realization of these po)(.i-
bilities has become essentially more seldom through improvements and changes in
manufacture.

5. Stilling (Arch. Exper. Patrol. Pharmak%., 1891, v. 28, p. 352), in
speaking of the anilin colors as antiseptics, says:
It is the nonpoisonous nature of thee substances, their easy solubility and dif-
fusibility, and above all their inability to coagulate albumen which lends them their
importance, which now can be only difficultly denied.
NOTE.-The work of Heidenhain abstracted iii Section VIII does
not fully bear out this article.
6. Erdmann (Pharm. 'Centrall., 1S92, v. J, p. 37) says:
The sulphonated as well as the carboxylated coal-tar dyes will not have any pro-
nounced action on the organism. Acid dyes may therefore bie regarded in gecnral
as nonpoisonous, whereas in the case of basic dyes a physiological examination is to lie
recommended before they are permitted to be applied to articles in daily u.se or
indeed to be used in food or drink.
NOTE.-Out of tlhe 80 different dyes on the food-color market in
the summer of 1907 whose composition was avowedt, 15 were basic
and 65 were acid.

7. Tschirchi ex)pressed himself as follows:
1. The coal-tar colors, and in a narrower sense the aniliii clhrs, are no longer
harmful on account of their arsenic content, since at the present liit thie grte11 niaj.,ri\
of them are prepared freo from arsvnic.
2. Some colors have ehown themselves to be hliarniful t, the .-y.-tem.
3. Coal-tar colors, in general, should therefore be permitted ftor lieh v i' irrti.w i it' ,,,i l,.
but those that have been found to be harmful should be expremly aund ,,jt.t'tli('lly
forbidden.


57






COAL-TAB COLORS USED IN FOOD PRODUCTS.


4. The amount of coloring matter which has been determined quantitatively in
bonbons and liqueurs is so small that even the ones regarded as poisonous would not
be able to develop their harmful effects. (Zts. Nahrs. Unters. Hygiene Waarenk.,
1893, v. 7, p. 338.)
8. Georgievics (Lehrbuch der Farbenchemie, Leipzig, 1895 p. 10)
says under "Poisonous nature of the coloring matters:"
It is a little known fact that of the very large number of organic coloring matters
only a few have been found to be poisonous; these are Picric Acid, Victoria Orange
(Saffron-surrogate), Aurantia, Metanil Yellow, Orange II, and Safranin. The preju-
dice which is still quite widely accepted that most of the artificial coloring matters
are poisonous dates from the early periods of anilin-color manufacture, at which time
magenta and the coloring matters made from it occurred in commerce highly con-
taminated with arsenic. At present, however, these coloring matters are prepared
absolutely free from arsenic, and are, as such, nonpoisonous. A few coloring mat-
ters which occur commercially as zinc chlorid double salts, such as Methylene Blue
and Malachite Green, may be harmful in consequence of their zinc content, and
should therefore never be employed in the coloring of food products. * In
consequence of their physiological activity some coloring matters are employed as
medicines, indeed principally Methyl Violet, Auramin and Methylene Blue. The
first two, known as blue and yellow Pyoctanin (pus-destroying) are, owing to their
great antiseptic action and diffusibility, valuable medicines; on account of the
unpleasant coloring effect accompanying them they are but little used. Methyl
Violet was first recommended as an antibacterial remedy in diseases of the eye by
Stilling; subsequently it has been employed in other special cases; its principal
use, however, is in surgery for the prevention of malignant proud flesh.
The use of Auramin is entirely analogous.
Methylene Blue (as a free base) is used principally as an analgesic (pain-relieving
remedy) and is given internally; on account of its ability rapidly to diffuse through
the tissues of the nervous system; it can also be introduced by injection. It is used
as a remedy against malaria, carcinoma, Bright's disease, etc.
The following have been tested as remedies or as antiseptics: Safranin, Lydin
(Mauvein), Vesuvin, Anilin Blue, Carbolic Magenta, Alizarin Yellow C (Gallaceto-
phenone), etc. The potassium salt of Dinitro-ortho-cresol was brought into com-
merce by the Farbenfabriken vorm. Friedr. Bayer & Co., under the name of Anti-
nonnin, and has given excellent results as a means against formation of mold in
cellars and against wood fungi.
9. Weyl (FHandbuch der Hygiene, 1896, p. 378) says:
A few organic coloring matters, but only a very few, possess poisonous properties.
A rule by means of which the poisonous or nonpoisonous nature of organic coloring
materials can be determined without experiment is unknown even for those coloring
matters whose constitution has been determined and experiments on the poisonous
nature of organic coloring matters are very few in number.
10. Lewin (Leirbuch der Toxicologie, 1897, p. 230) says:
In the use of various fabrics or of foodstuffs, which are colored with anilin or
coal-tar colors, or min commercial contact with such colors, local and general symptoms
of poisoning, such as eczema, swelling of the face, vomiting, diarrhea, anesthesia,
paresis, etc., have been observed. These are generally due to the toxic nature of
the coloring matters, frequently to harmful ingredients of the same, and hardly ever
to poisonousu muordants. Many workmen in anilin factories show permanent spots;
for example, on the cornea and conjunctiva, head, chest, face, and neck, without


58






COMPILED DATA UNDER GREEN TABLE NUMBERS.


59


any interference with their general condition. Local changes of more serious nature
have more frequently been observed in the mucous membranes and on the skin.
Thus, in one case, a camel's-hair pencil, soaked with anilin color, accidently entered
the eye, and at first nothing was noticed buta violet blue coloration, later inflamma-
ion and chemosis took place. I have observed local swelling and indurations of the
skin, particularly on the cheeks, in the case of children after they had worn caps
colored with anilin dye.

11. Winton (Connecticut Agric. Exper. Sta. Report, 1901, p. 181)
says:
Although there is evidence that most of the coal-tar dyes are not injurious to some
of the lower animals, it is not safe to assume that they are entirely harmless to human
beings. The dog, an animal used in most of WVeyl's experiments, has a proverbially
strong stomach, and eats with no apparent discomfort many things which would
disturb the digestion of a man.

12. Chlopin, in his book published in 1903 (see p. 75), states as
follows:
(Page 114.) * All the dyes examined by me I divided into three categories:
Dyes which caused striking general symptoms of poisoning and led to the death of
the animal, or would have led to it if the experiments were not purposely discon-
tinued, I designate by the term poisonous; dyes which induced some separate and
temporary symptoms of disease, for instance, vomiting, diarrhea, separation of albu-
men in the urine, the general condition remaining normal, I designate as suspicious:
lastly, the dyes which caused no apparent disturbance during the experiments arc
designated by the term nonpoisonous. I purposely do not call the last category
harmless, because by our experiments the question could not be decided negatively
as to whether the nonpoisonous dyes did not cause some finer pathological changes in
the organism and functions which could not be detected by simple observation.
(Pages 219-221.) Thus, according to all the investigators quoted, there were found
altogether 22 poisonous and harmful dyes, out of about 60 dyes examined; which
makes 36.7 per cent of poisonous and harmful dyes among those? Examined.
My investigations gave 30 per cent of poisonous and 40 per cent of suspicious dyes.
The percentages above given have a fairly well established basis, since they were
obtained by the examination of 100 dyes, which is about one-fifth of all the dyes in
commerce. Further, considering the distribution of the poisonous and harmful dyes
according to various chemical groups, we find that they occur in 12 of the IS groups,
and we can not note any regularity in this distribution; it is impossible to say that
there is any definite connection between the fact that t1' dye belongs to a certain
chemical group and its action on the animal organi:m. Usually among the dyes of
one and the same group there arc some harmful ones, but there are also sonic harmless
ones, and the ones and the others have very similar colnpositin,. This or that action
of the dyes on the animal organism, as we shall pre'sently see', is di tirinmiwd inumre Iby
the delicate difference in the internal structure of their mIolechule4 than by those
differences on which is based, at the present timni. the: clasificatin o'f the aromatic
dyes.
On the basis of the whole experimental material on hail--mii.e Mnd that of other
investigators-I can make only the following very few and purely empirical generaliza-
tions:
1. According to the shade produced, the poisonous aimi harmful colors are distributed
as follows: Most of all poisonous dyes are found among the Yellows and then ()ranges;
then come the Blues, then the Browns and thu Blacks; there are very few harmful
dyes among the Violets and Greens; among the Reds was found only one suspicious
one, and no poisonous ones.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


2. The most poisonous dyes belong to the Nitro, Azo, Triphenyl, and Thiazin
groups, and also to the Auramins.
3. A whole group of poisonous and harmful dyes is formed by the new sulphid dyes
known as Vidal's dyes.
(Page 224.) By the facts and observations quoted above is corroborated the opinion
that in general the coal-tar dyes, according to the composition and properties, appear
as substances foreign to the animal organism, and may influence harmfully the vital
functions, even in those cases when they do not possess distinctly poisonous properties.
For this reason many hygienists make it a principle not to allow the coloring of food
products or of beverages with coal-tar dyes, independently of the fact whether they
prove in actual experiments on animals poisonous or not.
We must therefore agree with M. Rudner that food of the masses require the most
far-reaching protection, maintaining them free from foreign additions.
13. Koenig (Die Menschlichen Nahrumgs- und Genussmittel, Berlin,
1904, Vol. II, p. .162) says:
Even though the majority of the anilin coloring matters, in view of the small
amounts in which they are generally employed, can not be regarded as directly harm-
ful to health, yet the objections to their use in the coloring of food products for the
purpose of substituting or strengthening a natural color lies in the deception con-
nected therewith * *.
14. Firaenkel (Arzneimittel-Synthese, Berlin, 1906, p. 570) says:
It is clear that the coloring property of these chemical substances stands in no
relation to their physiological actions, but, on the contrary, the physiological actions
depend only upon the general structure of these substances, and therefore upon their
membership in definite chemical groups.
(Pages .574-5.) We see, even in considering this group of substances, that they do
not possess any specific action, but they are capable of use, preferably by external
application, as antiseptic materials, as materials which in their action stand somewhere
between carbolic acid and corrosive sublimate, and whose coloring property, in conse-
quence of which they were primarily selected, is directly a hindrance in this use,
sine the coloring of the bandages and the hands of the operators and the skin of the
patients certainly can not be regarded as a pleasant, occurrence; that the antiseptic
action stands in some relationship to the properties of the substances as coloring matter
must be positively contradicted. It depends only on the general structure of the
substance, and does not stand in any direct relation to the chromophore and auxo-
chrome groups of the substances, but more closely to the aromatic nucleus. Indeed,
it may happen that an auxochrome group diminishes the antiseptic activity of such a
substance.
NoTrE.-I'he dyes referred to belong to tlhe Monazo, Disazo,
Triphinyl-inetlane, Xanthin, Azin, and Thiazin classes.
(PaIge 9.!.) The investigationsof Ehrlich have shown that basic dyes color the brain
gray, and, moreover, they color nerve fiber very well, and are therefore to be regarded as
iieurot rop!s;. The dye acids, on the other hand, do not dye nerve fiber, and in particu-
lar the substit.uted sulphonic acids do not d(lye tissue at all.
1i. Mycr, in his paper on "A preliminary communication on the
toxicity of so.,m aniline dyestuffs" (J. Amer. ('hem. Soc., 1907, vi. .'2?9,
p. 892), says:
(PI'age 89..) "A manufacturing confectioner of this city, for whom I made examina-
tiin of colors uCsed by him, informs me that a yellow color sold as Auramin has such


60






COMPILED DATA UNDER GREEN TABLE NUMBERS.


high tinctorial power that 1 ounce will color 2,000 pounds of candy to the highest yel-
low tint required in his business. It is obvious that the toxicity of such a body would
have to be very high to render it harmful in such use." Conclusions of this kind do
not take into account the possible detrimental action ensuing on healthy as well as
diseased persons from long-continued use of small quantities of foreign substances.
(Page 909.) The same author raises objection to feeding experiments on the ground
that substances are thereby introduced greatly in excess of the amounts generally
found in foods and that the ill effects "are liable to be due to the excess and in long-
continued experiments due to a cumulative action of the excess." Surely if excessive
amounts have a cumulative action, small amounts may also finally show toxic effects
due to retention and accumulation of the poison. To declare a substance entirely
innocuous would require evidence as to its nontoxicity both to normal and diseased
persons after its long-continued administration in both small and large doses. The
most extreme contingencies would have to be provided for. The above objections to
feeding experiments are therefore not valid. It is hoped that a study of the effects
on metabolism of some of these substances will help to further elucidate the subject.
He summarizes the results of his physiological investigations of
seven different coal-tar colors as follows:
1. Several commercial organic dyestuffs (Curcumin S, Tartrazin, Naphthol Red S,
Carmois in B, Naphthol Yellow S, Gold Orange, and Ponceau 2 R) were studied as
to their general effects on dogs when administered in varying amounts and during
fairly long periods (two weeks).
2. None of these dyestuffs under the conditions above indicated exhibited any
marked degree of toxicity. There was only one fatal result, which may have been
due to influence independent of the action of the colorant.
Similar quotations from the literature could be added to the fore-
going, but these are beyond question sufficient to show that a wide
divergence of opinion as to the harmless or harmful nature of the
coal-tar colors as a class does exist among scientific men, and that all
those above quoted agree that there are some at least of tlhe coal-tar
colors which even in a pure state may be harmful to humanL heltllh,
and that the question of actual harmfulness under the conditions
of actual use in foods and the consumption of foods is regarded by
some as being properly answered in tlhe negative and by oth ers as
being properly answered in the affirmative. The question of amount
of color employed in thle food products an(l t lie amountris o(f such food
normally eaten are therefore raised by some as tle decidiiir. factors.
In this connection the following statement from page 41) of tilie
arguments before the committee e on Patents in the House (if Repre-
sentatives, April 8, 15, 16, 22, 29, 1908, may 1be of interest:
S* It should )be remembered that after a new chemical- has been dis,'iovred
and patented it requires as many as three years of experiment lit4iret, wet dart offer it
in this country as a medicine for human beings. Th,'se eXl]TrimenIts are tnmlut teil
abroad before we receive it here. It is first tried on animals anl gradulzally, with great
caution, extended to human beings in the foreign hospitals, so as tI) :acertan iiits
physiological effects quantitatively upon the various organs, lith whn ihi itse irguins
are in the healthy state and when they are affected by various disorders * *.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


A search of the literature herein compiled fails to disclose any such
searching physiological examination of any of the coal-tar colors
recommended for use by human beings in food products, as is asserted
in the above quotation to be necessary in the case of a new chemical
intended for use as a drug. If Fraenkel, as quoted on page 60, is
correct in his statement that coal-tar colors act physiologically
because they are chemicals and not because they are coloring matters,
then coal-tar coloring matters prior to use in foods, in which they are
used by the young and the old, the well and the sick, without restric-
tion and without supervision, should also be thoroughly tested, and
very few, if any, coal-tar colors seem to have been examined with
the thoroughness set forth in the above quotation. That uniformity
and purity of product is necessary in order to be sure that the chem-
ical is going to act physiologically in the same way every time is
obvious. According to Fraenkel, what is true of a chemical is just
as true of a coal-tar color, and if uniformity of strength and cleanli-
ness of product are desirable when a chemical is to be used as a medi-
cine, such properties are equally desirable when a chemical is to be
used as an ingredient in food.

CLASSIFICATION OF OPINIONS IN LITERATURE AND IN LEGAL
ENACTMENTS SHOWING CONDITION OF THE MARKET IN 1907.

The literature and legal enactments hereinafter grouped under the
relevant Green Table numbers have been classified as (1) unfavora-
ble-i. e., only unfavorable reports found in the literature; (2) favor-
able, and (3) contradictory reports, as each case required; so that
under each Green Table entry there is not only the relevant literature,
but also the character assigned to it for tlhe purpose of coming to a
conclusion as to the propriety of the use of such color in foods as
based on such literature, which conclusion formed in that respect
the basis for Food Inspection Decisions Nos. 76, 77, and 106.
However, it does not follow that all dyes placed in the "favorable"
list are actually harmless; the investigations or opinions reported of
each may very well be based upon insufficient data. This classifica-
tion, therefore, is merely intended to reflect the present state of the
literature with respect thereto, and is not necessarily final nor con-
clusive.
In substantially all the recorded cases the observers directly or
indirectly assert the absence of arsenic and mineral poisons in the
dyes subjected to physiological test, but the kind of other impurity,
if any, is not stated.
For thle purpose of a coiln)rellensive survey of the literature and
legal enact ents, tie following tabulation is presented:


62








COMPILED DATA UNDER GREEN TABLE NUMBERS.


63


Condition of the United States color market in the summer of 1907.

[x=not on market. Figures indicate number of dealers offering sample. Cross lines separate the several
groups.]


Favor-!
able.





10
x










x


2


Green
Table
number.


1
2
3
14
5
6

8
9
11
13
14
15
16
17
18
28
41
43
55
65
70
78
84
86
86
87
88
89
92
93
94
95
97
102
103
105
106
107

138
160
163


Con-
tradic-
tory.








5
1
2
6
2


x
x
x


x
I
Ir


I


Unfa-
vor-
able.


Unfa- Favor- Con-
vor- avor-ble. tradic-
able. ale tory.


x ..... ..


x
..........x



........ ... 1
2 ......1

..... .. .. ... ..


..... .........


Green
Table
number.


164
166
169
188
197
201
240
269
277
287

394
398

399

425

427
428
433
434
4.35
448
450
451
457
459
462
467
477
478
479
480
483
488,490

502
504
512
516
517
520


1

4





2
x
x








2
2


1
4
...........................i...







2


2
3


4
x
5
x


Green
Table
number.


521
527
530
532

5W3

572
574
576
5S 4
593
599
6i00
fA~l
W }2
614

<62n
I ,20N
b.J9

649
ti50
651
654


659 x


....... 667


.......................................i c s;'
'.'.'.'.'.'.'.' 6(70
I 675
!1 fiA9
692


........ 1 106
..... Iot ils


U afa-
vur-
able.


Favor- Con-
able. tradic-
tory.


........ ........
.. .. X .. .. .. .


X ....... ...... . .......

S' I
I . . . . . . . .
I




. . . . X . . . .
. . . . . .
. . . . . x . . . .

x .. .. .. . . . ...
x . . . .. . . . . .
xI
x. . . . . 2... .

x ......... ........
S... ..... ........
A : ;

"Y ;-A ::::


I

X
X





18


3


:32
i 1i.


x


41
'26


Italicized figures are colors in the permitted list, Food Inspection Decision 76.
% On United States market in 1907.

This table shows that of the 106 coal-tar dyes exanineld pllysiolog-

ically only 50 were on the United States market; further, out of 33
"unfavorable" dyes 8, or one-fourth, were on tile I'nited States

market; out of 32 "favorable" dyes 16, or one-hlialf, were on tile

United States market, and finally that out of 41 "contradictory"

dyes 26, or very nearly two-thirds, were on the U'nited States market

in the summer of 1907.

Assuming this classification to be substantially and essentially fair,

the only Green Table numbers which are of interest for the present

discussion are those classified under "favorable," because any color

positively injurious or of doubtful character is o-misidered as being
properly excluded from use in food products. 'The Green numbers

classified as ''favorable" are 32 in number, as follows. 4: 5-; 2S :

65; 85; 89; 92; 93; 102;, 103; 105; 107; 166; 169; 240; 3941; 399; -133;

4385; 462; 467; 477; 51 512; 17; 520; 521; 527; 576; 593; 5991; 600; 692.


3



1
' i



x


X
x



X
2

1" i


2

x

2
8
x
X



2





x

x
x
X
X


x ........


....... .. .. .
2




.... ^ i '" i":: :
........ x
........ 6..x
...... ......
6 ........


6
.. .... .. ... ....
6

........ 1.. .

7
.. .. ........* ** *
.. . . . .







COAL-TAR COLORS USED IN FOOD PRODUCTS.


Of these 32, 16 were on the United States market in the summer
of 1907 and their composition disclosed; they are presented in the
following table, together with the number of dealers, out of a possible
12, offering them for sale.

Distribution of "favorable" colors on the American market in 1907.


Gr en Number
Table of dealers
number, handling.,

4 10
65 2
85 2
89 1


Green Number Green Number Green Number
Table of dealers Table of dealers Table of dealers
number, handling. number. handling.', number, handling.

103 6 240 1 512 3
105 1 433 1 517 5
S107 7 I 435 4 520 2
169 1 4-62 2 69 3


From among these 16, six of the seven permitted colors of Food
Inspection Decision No. 76 were selected. The process of selection
and of elimination is described on page 166.

CLASSIFICATION ACCORDING TO CHEMICAL COMPOSITION AND
SUITABILITY.

In the following table the chemical composition of thesubstances
corresponding to the Green Table numbers is given, and their classi-
fication according as the literature is regarded as being (1) unfavor-
able, (2) favorable, or (3) contradictory in regard to the color. The
colors are also arranged in the groups to which they belong chemically,
so that this table shows: (1) The number of groups reported on in the
literature, (2) the number and composition of members of each group
so reported on, and (3) the interpretation here placed upon such
reports in literature. This table is given in the expectation that it
will be of use to chemists and physiologists.

Opinions (is to suitability, classified according to groups and chemical composition.

(The chr-mical riornenclature is that of the (Gireen Tables; "a" is used for alpha and "b" for beta.)

U unfavorable. Favorable. Contradictory.

NITRO COLORS.


1. Symmetrical trinitrophenol.
2. Dinitro o and p-cresol.
:1. 1)nitro-a-naphl hol.
6. Ilexanltro-d I phenylamin.
MONOAZO COLORS.
7N. Met hyl-benzenyl-amldo-t hlo-
xylhnol-azo,-a-naphthol dli-
sulphoni, wril.
94. Benzene-uzo- pv razalone -car-
boxy-fllsulihloniu awlIl.
97. Sulpl1o-tohlLcn.C-iaLzo-b- naph-
thol.


4. Dinltro-a-naphthol-b-mono-
sulphonic acid.
5. Dlnitro-a-naphthol-a- mono-
sulphonic acid.



28. p-nltro-benzene-azo-a-naph-
thylamin p-sulphonic acid.
t5. a-naphthalene-azo-b-naph-
t hol-disulphonic acid.
M5. p-sulphobenz ene-azo-a-
naph t hol.
89. p sulphohenzene azo dl -
phenylamln-su 1 p h o n i c
lu-id.
92. Dlphenylamln yellow with
nitro-dlphenylamln.


8. Amido-azo- henzene-dl- and
monosulphonic acid.
9. Amido azo toluene disul-
phonic arid.
11. Bcnzene-azo-b-naphthol.
13. Benzene-azo-b- naphthol b
sulphonic acid.
14. Benzeneazo-b-naphthol dl-
sulphonio acid G.


64







65


Opinions as to suitability, classified according to groups and chemical composition-Con.


Unfavorable. Favorable. Contradictory.


MONOA.ZO COLORS---continued.























DISAZO COLORS.
164. Sulphobenzene-azo-sul p h o -
benzene-azo-b-naphthol -
sulphonic acid.
201. Hydrochlorid of toluene dis-
azom-tolylene-dlamin.
277. Ditolyl-dsazo-binaphthion I c








NITROSO COLORS.

8TILBENE COLORS.

DIPH3NTLMETHANE COLORS.
425. Hydrochlorid of Imildo-tetra-
methyl-diamldo-dlphenyl-
methane.
TRiPNTLFNMETHANE COLORS.
434. DImethyl-dibenzyl-diamldo.
triphenyl-carbinol-tris u I-
phonic acid.
459. Chlorld ofheptamethyl-rosan-
ilin chloride.

478. Trlphenyl-pararosanllin dl-
and trisul phonic acid.
479. Triphenyl-pararosanilin-t r i -
sulphonic acid.
488.490. Hydrochlorid of pho-
nyl-tetra- (penta) methyl-
trlamido.d lphenyl-aph-
thyl carbinol.


93. p-sulphobenzene-azo dioxy-
naphthalene sulp ho n i c
acid.
102. p-sulpho-paphthalene azo -
b-anphthol.
103. p-sulpho-napht hsalene-azo-a-
naphth ol-p-sul phonic acid.
105. p-sulpho-naphthalene azo -
b-naphthol m o n o s u 1-
phonic acid.
107. p-sulpho-naphthalene azo -
b-naphthol-dis u I p h o n ic
acid.














166. Sulphobenzene azo-sulpho-
benzene-azo- p- tolyl b-
naphthylamin.
169. Sulphotoluene-azo-toluene-
azo b naphthol a sul-
phonic acid.
240. DIphenyl disazo binaph -
thlomc acid.







394. Dlnltroso-resorclnol.

399. A zoxy-stllbene-di-sul phonic
acid.





43. Diethyl-dibenzyl diamido-
triphenyl carbinol-disul-
phonic alcid.
435. Diet hyl dlbenzyl-dlamldo-
triphenyi-carbinol-tris u 1-
phonic acid.
4Q2. Trisulphonic acid of rosani-
lin and ararosanilin.
477. Triphenvl rosainilin -i mono-
sulphonic acid and triphe-
nyl- pararosanilin mono-
suLilphonic acid.
467. Dlsulphonicacid ofdlrmethyl
dibenizyldi-ethyl triamido
triphenyl carbinol.


15. Benzene-azo-b-naphthol di-
suiphonic acid R.
16. Dimethyl-amido azo ben-
zene.
17. Hydrochlorid of diamido-azo-
'benzene.
18. Hydrochlorid of beazene-azo-
m-tolvlene-diamin.
41. Hydrochlorid of toluene-azo-
m-tolylene-diamin.
43. Toluene-azo b-naphthol-sul-
phonic acid.
55. Xylene-azo-b-naphthol-disul-
phonic acid.
70. Dichloro-phenol-azo-b- naph-
t hol.
84. p-sulpfbobenzene-azo resorci-
nol.
86. p-sulphobenzene-azo- b-naph-
thol.
87. p-sulphobenzene-azo-dimet h-
ylanilin.
88. p-su Jphobenzene-azo diphe-
n yl amin.
95. m-siuphobenzene azo-diphe-
nvlamin.
106. p-sulphonaphthalene azo-b-
naphthol-disulphonic acid.

138. Bisulphobenzene disazo a-
naphbthol.
160. Sulphobenzene-azo-benzene -
azo b naphthol mono-
sulphonic acid.
163. Sulphobenzene azo sulpho-
benzene-azo-b-napht hol.
188. Disulpho-b-naphthalene-azo-
a-naphbthalene azo b -
napht hol-disulphonic acid.
197. Hydrochlorid of benzene-dis-
azo-phenv lene-dianmin.
269. Ditolvi disazo bl salicylic
acid.
287. Dltolyl-disazo-bl-a-naphthol-
p-sulphonic acid.
398. Nitroso-b-naphthol-b-monoo -
sulphonic acid.


427. Chlorid of tetra-methyl dl-p-
amnido-iriphenyl-carbinol.
42:. Sulphate or chlorid of tetra-
et h v Iy dianido triphenyl-
carbinol.
448. Hlvdrochlorid or acetate of
ararosanltin and roant-
fn.
450. Ilydrochlorlds or acetates of
miono-li or Irimehyl (or
ethyl) rosanillns and p-ra-
rosanilins.
451. Ilydrochlorld of penta- and
hexanimethvl-pararosa.ilin.
457. Ilydrochlor'd. stiulphle orT
acetate of triphetnyl rutani-
ltin and triphenyl paruaros-
arnillln.
4I. Trn henvl-rosanllin and trl-
phaenyI-purn-rt~nailin sul-
phonic acids.
483. Aurln cnrhlnol, oxydlre', au-
rin. naiPhyl u in, and
pseudo roaulle aclil.


97291 -Bull. 147-12-----6


COMPILED DATA UNDER GREEN TABLE NUMBERS.







66 COAL-TAR COLORS USED IN FOOD PRODUCTS.

Opinions as to suitability, classified according to groups and chemical composition-Con.


'Unlivorable.


Favorable.


Contradictory.


XANTIIENE COLORS.

502. Triethylrhodamin.
516. Diiodo fluorescein.




ACRIDIN COLORS.

530. Ilydrochloridofdiamido-phe-
nyl-dimethyl-acridin.
532. Nitrate of chry-sanilin and
homologues.

ANTETRACENE COLORS.


INDOPHENOL COLORS.

572. Tin compound of dimethyl
p-amido phenyl-p-oxy-
a-naphthylamin.
574. Hydrochlorids of p-pheny-
lene-diamin-p-amidophe -
nol and diamido-dipheny-
lamin.

AZIN COLORS.
602. Spirit Nigrosines.
614. Amido naphthy I -naphtha -
zonium chlorid and dia-
mido naphthvl-naphtha-
zonium chlorid.

OXAZIN COLORS.

620. Dimethylamido dioxy phe-
nazoxonium carboxylate.
639. Chloride of dimethyl-amido-
naphtho phenoxazonium
chlorid.
N
THIAZIN COLORS.

649. Zinc-double-chlorid of di-
methyl diamido-phenaz-
thionium chloride.
6.51. Nitromethylene lBlue.
654. Chiorid of dimethyldiamido-
toluphenazthionium.
TrIOBENZENYL COLORS.

659. Dphydrothiotoliiidin.

QUINOLIN COLORS.
667. Quinophthalone.

SULPIHD COLORS.

670. Sulphohydro derivative of a
polythiazin.
675. Thioeatechin S (composition
unknown.

INDIGO COLORS.


512. Tetrabromofluorescein.

517. Tetraiodofluorescein.
520. Tetraiododiehlorofluorescein.
521. Tetrabromotetrachloro fluor-
escein.
527. Sodium bisulphite corn-
pound of corulein.











576. New Gray (composition un-
known).







593. Phenyl- and tolyl-safranins.
599. Mixtures of dianilido-amido-
trianilido-, and tetraani-
lido phenyl phenazo -
nium chlorids.
600W. Indulins and fluorindins.


504. Hydrochlorid of diethyl-m-
amido-phenol-phthalein.












563. Dioxy-anthraquinone-b-qui-
nolin.


584. Diamnidophenyl and
tolazonium chlorids.
601. Sulphonated indulins.


tolyl-


650. Chlorid of tetramethyl-di.
amido-phenazthionium.


692. Indigotln disulphonic acid.


689. Indigotin.







COMPILED DATA UNDER GREEN TABLE NUMBERS.


67


PHYSIOLOGICAL ACTION OF COAL-TAR DYES.

SUMMARY OF SYMPTOMS.


A rough summary of the symptoms noted or positively deter-
mined to be absent, the number of the deaths produced, and the
number of cases in which nothing abnormal was noticed may serve
as a convenient guide in considering the detailed statements herein-
after given relative to all the symptoms, clinical data, legislative and
other publications, or permissions.
In the following tables are brought together most, if not all, of the
recorded observations with respect to the humans and other animals
upon which the physiological action of coal-tar dyes has been studied
as well as the results of autopsies when recorded. The columns
headed "Unfavorable," "Favorable," and "Contradictory" have the
same significance as in the preceding table; italicized numbers
are those of the permitted colors of Food Inspection Decision No. 76.
Asterisked numbers indicate that the dye was administered
hypodermically.

EXPERIMENTS ONi DOGS.

TABLE I.L-Observations on dogs.

(Reference to Crecen Table numbers.)


Symptoms. Unfavorable. Favorable.


Deaths..................

Autopsies...............
Stained skin..............
Stained conjunctiv a?......
Respiration difficulties....
Temperature normal ...
Temperature high........
Temperature low.........
General depression.......
Weakness...............
Loss of weight...........
Emaciation...............
Paralysis of heart.........
Loss of appetite..........
Aversion to food..........
Colored urine............


Colorless urine............


1; 2: 3; 488or490; 574; 639
(2); 649.
3; 488 or 490; 572: 574; 620;
639; 649.
I ..................
1........................
1; 3.................
2; 620; 64.19...........
488 or 490; 3............
48 or 490..............
425; 649; 675...........
1; 3; 97; 649; 659.......
1: 4,M or 490: 639 .......
4.s or 490; 639...........
2;3; 97; 425; 53; 649; 69.7.1;
667; 670.
649; 3...................
3; 6; 7s: 94; 97: 277; 42:,:
4:i4; 4.744; 47k; 47!1; .rlA)'
516; 5-30; 532; 614; 6;.Ni;
651 ; 659; 667; 670.


103: 105; 399; 44i7. 477; 593;


...,.............. ........






.4H1; ;394 .......... .......
4i .... .. .:" ; .. .i;....:1.
I1'66: 2440; 3'.4; :14.: 4.:,;;
5'..21: 5.7; >57;;99.
2411... .....................


Urine not alffalcil........ 4% or 49u;: 641 ........... 4e.7. 477...............
Albuminuria ............. 1; 3: 7:s; 94; 97: 4"25: 431. 4; ,.. 2. I1.; 2111; :24...
459: 471; 516; 5I |; t:,l;
65;9: G',7.
Albuminuria doubtful.... 7s; 47 .................. ......................
Alkaline urine............ t70....................
Bloody urine...................................... .......................
Phenol in urine ......... ........................ .........................
Kidney Irritation........ I ....................... ..........................
Bladder irritation ....... .................. .........................
Thirst.......... ..... ..3... 3 ............. ...... ... ....................
Colored feces ............ 94; 42.'7; 4h, or 413; (I2rL'... 13; 105; 399; 477 .......
Thin stool.......... 425; 2: ,1 ....... 7..................
Diarrhea ............... 1: 3. 94; 97; 479; 425; .'Ai:; 4: r.'; P1;3; l'L.; 31.; 5'27;
Il l; I,I ;: (;19; U1' 1. 6i711. ,>'l.t.
Softened fec ...................................... .............. ......
Bloody stool............. ...................... ... ...... ....................


Contradictory.


16 (2); 55;: 70"*1;; 6;S 7:.9 2"
1,W; 428 (1j; 451 (2);
4,qO; 601; 6"74.
16: 55; 70*; 87 (2): 45 (2);
457; 4S'0 (2); 601; 650.
39s.
39,.

451; 601.
457.
451.
6.1().
650.
16i; 483.
17; l; 41;95; l:3R;431 :650.
I.1i; 451.
16; 87; 42S.
16; S7: 11%; 197; 42s; 451;
4,,1: 670.
451.
!; 4: 11: 13; 14; *16: V:; %4;
si; 7: $s; '5; 1 Ls; 197;
2fi6i: 2.S7; 3IRt ; 42.%; 44,N;
4.3; 504; 601; 6:A).
'%,7.
4.,1: 40): tll.
.<. 9: 1: 17, !N. or 41: 70;
; 95; IK,; 197; -'40;
2 7.
I:ik.
14; S.S'; 2N9; 2N7.
451.
11; i1
!1. t^.
Mi.
ti 'fl.
S7.; W; 3h; 4N.); l. l; iWl i
16 51-14.
11: It.. 10-4: hfi. S47: I;I. N.
42s; 4.%3; 'AH; &,%4. l'.:J.
15.
1 Ix .







COAL-TAR COLORS USED IN FOOD PRODUCTS.

TABLE I.-Observations on dogs-Continued.


Unfavorable.


Favorable.


Pus in stool.................................................................
Stool desires.............. 02...................... ..........................
Vomiting................ 1; 2;3; 6; 97;277;425;479; 399; 433; 467; 576; 69S...
I 488 or 490; 516;532;574;
S614; 639; 649; 670; 675.
Retching ................. 675...................... 2 ......................
Salivation................ I 488 or 490; 639; 649; 675....'... ...............
Anemia..................t 488 or 490; 639 ....................................
Stupor ................... ............................ .........................
Desire to sleep ............................................. .......................
Catarrh of eyes and nose. ...................... ..........................
Cramps................... 1; 2 ................. ..... ...................... ...
Convulsions.............. 2; 675.............................................
Tremors .................. ... ..........................
Congestion................... ... ..........................
Paralysis of limbs....... 1; 675.............................................
Destroys coloring matter 1; 2...............................................
of blood.
Loss of sight.............. ....................................................
Loss ofhearing ..................... ..........................
Internal disorders ........
Interna disord rs. .I ..... ... .. .... .. ...... .... .. .. .. .. ........ .. -----------.


Contradictory.


650.
11; 16; 86; 87; 95; 197; 269;
428; 448; 451; 483; 650.
16; 86.
584.
601.
451.
451.
601.
87.
16; 55; 87; 428; 450.

87; 601.
601.
650.


The following table discloses the results of the autopsies made and
reported on dogs.

TABLE II.-Autopsies on dogs.


Symptoms. Unfavorable. Favorable. Contradictory.


No change in internal
organs.
Nothing abnormal.......
No change except whole
interior colored red.
LIVER.
Fatty degeneration.......
Blood-poor..............
Pale.....................
Swollen.................
Inflamed................
Blood-filled..............
KIDNEYS.
Congested...............
Filled with decomposed
blood corpuscles.
Colored..................
Soft.....................
Blood-poor...............
Blood-filled..........
Swollen....... ......
Thickened...............
Inflamed................
STOMACH.
Colored.................
Catarrh...................
Inflamed mucous mem-
brane.
Punctured mucous mem-
brane.
Contracted and filled
with colored mucous.
LUNGS.


572; 620; 639...........
488 or 490..............
574 .....................
649......................
574......................


105; 399; 467; 477; 93......
103....................


3; 639; 649.........................................
639........... ..........................


488 or 490 ..........................................
574...................... ..........................
620; 639................. 692......................


488 or 490...............
488 or 490...............
574; 649................


639............ ..........................


Filled with blood ......... 574...................... ........................
Punctured........................................ .. ........................
HEART.
Swollen ... .............. 574...................... .........................
Paralyzed................574......... ..........................


87.
87 III; 457.




601; 650.
451 (2); 480 II*; 601.
451(2).
650.



451 (2); 480* (II).
451 (2).
480 (1); 601; 650.
480* II.
601.

650.
650.


650.
650.

601.






601.



16 (2); 87 I; 428; 87 I.


68


Symptoms.


..........................
..........................
..........................






COMPILED DATA UNDER GREEN TABLE NUMBERS. 69

TABLE II.-Autopsies on dogs-Continued.
[
Symptoms. Unfavorable. Favorable. I Contradictory.

INTESTINES.
Colored ................... 488 or 490................................... ....... 650.
CatarrhL .................. 488 or 490.............. ..........................
COLORED.
Brain .................... I ......................... ........................... 650.
Fat ...... ... .. .. I 6,50.
8Fat......... ..... ... .... ....................... ......................... 650
Skin .................... .... ......................................
H eart sac ................ .................................................. 650.
Diaphragm............... I................ ...... ........................ 650.
(Esophagus.......... ..... 488or 490............... ......................... 650.
All organs colored ......... .................................................. 480* II.
All organs swollen......................... ...................... ........ 480* 11.
General congestion...... 3 (II).....................................
Peritonitis............................................................................ 70*.
Fat all disappeared....... 639..................................................... ...
Flabby muscles.......... 639................................................

In this connection it may be of interest to note that out of 16 dyes
producing death when administered through the mouth to dogs, 7
were on the United States market in the summer of 1907. Their
Green Table numbers are as follows, the numbers in parentheses
indicating the number of makers or importers, out of a possible 12:
offering them: 55 (2); 86 (8); 95 (2); 428 (3); 451 (5); 601 (1); 650 (2).
The following table gives the Green Table numbers of coal-tar dyes
which on administration to dogs positively did not in certain specific
cases produce the particular disturbances recited, although the case of
the several colors as a whole is regarded in the literature as "favor-
able," "unfavorable," or "contradictory," as stated.

TABLE III.-Observations on dogs showing definite negative results in spi lic cases
grouped under the general verdict of the literature as a whole.

Symptoms. Unfavorable. Favorable. ('ontratdictorv.
I-
Vomiting................ 614 ...................... 1 4: 105; 462 .............. 95; 101.
Diarrhea................ ....................... 4; 105; 462 ............... 95; 504.
Albuminuria ............ 6; 97; 277; 434; 532; 614; 4; 92; 93; 1U.5; 433; 4-k2; 14: 16; 55; 84: '; .s7: sS:
651; 659. 521; 527; 576. 197; 398; 448: 5(1: 1411.
Sugar In urine ............ ......................... 4;' 394 ................... I
Phenol in urine ........... ............. ............ I 2 7.
Loss of weight............... ...................... 19 ........... .......... t i,.

That is, when these dyes were tried on dogs the observers reported
in certain specified cases, positively and definitely, the absence of any
of the symptoms named.
It is stated of the following colors that theyproduced no bad effects
in certain specified cases: 4; 9; 65; 86; 105; 18S; 197; 240; 457; 572;
593. No bad effect except colored urine: 13, 95. No bad effect
except albuminuria: 88, 287. No bad effect except loss of weight:
12.5 per cent (17, 18, or 41).
It is therefore true of all of these coal-tar dyes that there are 'ondi-
tions under which they have been observed not to produce tihe bad






70 COAL-TAB COLORS USED IN FOOD PRODUCTS.

effects as above set forth; but this tabulation must not be taken to
mean that these dyes can not, under any conditions whatever, produce
untoward results; the reverse is true in most cases.

EXPERIMENTS ON HUMAN BEINGS.

The Green Table numbers of those colors concerning which experi-
mental data are available on humans are as follows: 1; 2; 3; 4; 6;
9; (17, 18,41); 55; 65; 85; 86; 95; 102; 103; 105; 106; 107; 197;
427; 428; 448; 462; 532; 602; 650.
The symptoms produced are classified in the following list:

Internally administered.


Not poisonous ................... 4;
9; 55; 65; 85; 95; 102;
103; 105; 106;107; 448;462
Poor general condition......... 86; 650
Fever........................... 2
Loss of appetite .................. 2
Vomiting .................. 3; 532; 650
Intestinal irritant ................ 650
Diarrhea ...................... 532; 650
Bladder irritant ................. 650
Colored urine............... 86; 95; 650
Albuminuria .................... 650
Increased micturition ............ 650
Irritant ......................... 532
Inflammation .................... 532
Dryness of throat ................ 86


Bad taste in mouth .............. 86
Restlessness ..................... 86
Rush of blood to head........... 86
Vertigo ........................ 86; 650
Headache ....................... 650
Delirium ........................ 650
Twitching of muscles ............ 650
Yellow coloration of skin ......... 3
Yellow-colored mucous membrane. 3
Food colored with it made a family
sick ........................... 3
Adults withstand ................. 1
Children and weak adults do not
withstand..................... 1
Deaths .......................... 2; 3
Autopsy ........................ 3


It should be noted that of the 13 dyes here classed as not poisonous


to humans all but No. 102 were on
summer of 1907, as is shown in the


the United States market in the
following table:


Number of dealers offering these nonpoisonous colors in 1907.

Green Sources Green Sources I Green Sources Green Sources
Table offering Table oTffering Table offering Table offering
numbers, same. numbers, same. numbers, same. numbers, same.

14 10 65 2 103 6t 107 7
9 1 s5 2 105 1 448 4
55 2 95 2 106 5 462 2

1 On permitted list, Food Inspection Decision 76.
Symptoms produced by external application of certain colors (Green Table numbers).


Burning ................... 2;
Itching ......... ........ 2; 6;
B listers .......................
Sw elling......... .............


427; 428
427; 428
.. 2; 6
4127; 428


Dermatitis ....................... 4
Eczema ........ (17, 18, or 41); 197; 602
Inflammation .................. 427; 428


It should Ie tnot(, telat No. 86 has been tried on humans and has
been found not to Ipro(Iuce diarrheaa or vomiting.

SIHemorrhagic gastritis.






COMPILED DATA UNDER GREEN TABLE NUMBERS. 71

G. T. 3 has apparently killed a human at 60 mg per kilo and the
autopsy disclosed hemorrhagic gastritis. G. T. 448 has been sug-
gested as a possible remedy for Bright's disease. It should also be
borne in mind that adults can stand G. T. 1 in doses of 540 to 900 mg
daily for a long time, whereas children and weak adults stand that
substance only poorly.
EXPERIMENTS ON SMALL ANIMALS.
Results of experimenting on rabbits with 10 coal-tar dyes whose
Green Table numbers are 1, 2, 86, 89, 107, 427, 448, 504, 517, and
563 have been tabulated as follows:
Death ................. 1; 2; 427*; 563* Paralysis ......................... 427*
Diarrhea ........................ 1 Cramps .......................... 427*
Colored urine-------------------................... 86 No harm produced. SO; oj:; 44.!; 5044; 517
Softened feces ................... 86
In the case of the numbers marked with an asterisk the color was
administered hypodermically. In this connection reference should
also be had to the paper of Penzoldt abstracted in Section VIII,
page 55.
The four coal-tar dyes 55, 103, 425, and 480 have been tested on
guinea pigs and no disturbance was noticed in all, but in the case of
103 occasional thirstiness was observed. No. 448 has been fed to
hens without damage, and No. 2 has been recommended as an insect-
icide, a fungicide, and a mouse poison.
GENERAL STATEMENTS.
The following statements may be of interest before thle detailed
compilation is read:
1. 0. Buss (Forschungsber. uiber Lebensnsmittd, 1896, vol. 2, pp.
163-197, 237), in a paper entitled "Contributions to the Spectrum
Analysis of some Toxic and Pharmacognostically Important Coloring
Matters, with Special Consideration to the Ltra-Violet," cites as
poisonous the following (Green Table numbers follow in parentheses
wherever connection could be satisfactorily established):
Picric Acid ...................... (1) Metanil Yellow ................... 5)
Dinitro o- and p-Cresol ............ (2) Corallin .......................... ( 3)
Martius Yellow .................. (3) Safranin .......................... r -)
Aurantia ........................ (6) Methylene Blu-.-.................. (( ))
Fast Yellow. ................ (8) lodin Green ...................... (4.l9)
Orange II...................(86) Alizarin Blue S................... )
As nonpoisonous:
Naphthol Yellow.................. (4) Naphthul Green................... I1S)
Eosin ........................... (512) Malachite Green .............. (427,428)
Erythrosin....................(517) Dahlia....(4.. -4.'51)
Anilin Blue..................(457)
As doubtful:
Methyl Violet ................ (451,454) 1 Vesuvin....................... (197,201)






72 COAL-TAR COLORS USED IN FOOD PRODUCTS.

On the following Buss is noncommittal:
Auramin........................ (425) Magenta .......................... (448)
Biebrich Scarlet ................. (163) Aurin ........................... 1(483)
Water blue....................... (480) Acid Green...................... (435)
Naphthol Black of various brands, which seemed to be mixtures.
2. It has been pointed out that the following nine colors are harm-
less:
Naphthol Yellow .................. (4) Wine Green ...................... (?)
Naphthol Brown............. (?) Milling Red ..................... (?)
Chinolin Yellow ................. (667) Azo-acid Blue ................... (36)
PyrotinRRO.................. (115) Fastrose....................... (?)
Acid Green................. (434,435)
Most of these have not been examined experimentally, but scien-
tific studies have been made of the poisonous qualities of Azo-Blue
and Naphthol Yellow. (Zts. angew. Chemie, 1896, p. 24.)
3. Chlopin in his monograph (see p. 75) says:
On the basis of my personal experience I consider the testing of the action of coal-
tar dyes on man not permissible, since such experiments may induce in the subjects
of experiment more or less serious symptoms of poisoning, for which in some cases
there are no antidotes at our disposal. To such accidents, in my opinion, only the
experimenter himself may subject himself, because he knows what he is doing. Pre-
liminary tests of dyes on dogs and other animals afford no guaranty of escape from dis-
agreeable accidents which may take place in the testing of the dye on man. (Page 111.)
These data and calculations convincingly prove how erroneous the current opinion
is that for the coloring of food substances and beverages only exceedingly small,
almost unweighable, quantities of dyes are used. (Page 113.)
On page 221 et seq., the following general discussion of this subject
is found:

THE MANNER OF ACTION OF POISONOUS DYES ON THE ANIMAL ORGANISfM.

The mechanism and the chemistry of the action of the artificial dyes of the aromatic
series on the animal organism remains to the present day, with few exceptions,
exceedingly slightly and superficially studied. The same can be said also concern-
ing the pathological and anatomical changes which are induced by these dyes.
More than the others there have been studied in the toxicological respect the dyes
belonging to the Nitro group; Picric Acid; Martius Yellow (Dinitro-naphthol potas-
sium), and Saffron substitute (Dinitrocresol potassium.)
According to Kobert, these dyes belong to the poisons acting on the blood. Accord-
ing to the same authority, Methylene Blue, which belongs to the other chemical
group o(if Thiazins, acts similarly.
In the fundamental works on the sanitary investigations for the dyes, by Cazeneuve
and l-pine, by Weyl, and by Santori, we find almost no material relating to the
explanation of the manner of the action of the dyes. These investigators limiting
themselves to a very cursory description of the symptoms of poisoning, and reciting
in most general terms the results of autopsy, not even indicating the cause of death.
Such, for instance, are the reports of autopsies made by T. Weyl and some other
investigators, as quoted above.

I Apparently a purified form of Corallin.






COMPILED DATA UNDER GREEN TABLE NUMBERS. 713

We may expect that more detailed investigations in this respect will be made at the
proper time by pharmacologists, since study of the mechanism and chemistry of the
action of the poisonous substances on the animal organism is their province; for the
hygienist it is quite sufficient merely to establish the fact that a given substance is
poisonous or harmful, and he need not go any further. For this reason, in those cases
in which I desired to clear up the causes of death of the animals in my experiments,
and to cord pathological and anatomical changes (although by the terms of the regu-
lations governing this competition, a close study of the action of the dyes, and the
ascertainment of the mechanism and chemistry of their action was not required), I
called in a person more competent than myself on these questions.
Not counting the duplicates we made five autopsies all told. In all these cases death
resulted from paralysis of the heart. The pathological and anatomical changes in all
cases, except one, did not present anything specific, and finally reduced themselves to
a feebly expressed turbid swelling of the heart and of the liver, a rush of blood to the
stomach, and a congestion of the internal organs.
The exception was the autopsy of a dog, which died from Methyl Orange; this dog
died with the symptoms of paralysis of a cerebro-spinal nature. This experiment was
made twice, and the autopsies of both animals showed hyperrnmia in the lowest part
of the spinal column, on the border of the anterior and the lateral columns.
As to the symptoms of poisoning not resulting in acute death, here most frequently
was observed vomiting, diarrhea, and albumen in the urine, showing disturbance of
the functions of the digestive tract, and an affection of the kidneys.
A highly typical picture of poisoning is presented by the sulphid Vidal dyes. They
cause rapid, almost instantaneous, deafening of the animal, whereupon the animal falls
on one side in convulsions and lies, not moving its body, but convulsively and rapidly
twitching its anterior limbs during several minutes. The tongue hangs out of the
mouth, a strong secretion of saliva is noted, then vomiting begins, and the dog gradu-
ally begins to revive; with difficulty he arises onhis frontfeet and sits down, not being
able yet to stand on his posterior extremity, which is in a state of paresis. After a few
hours the dog becomes normal. The symptoms of poisoning, just described, are exceed-
ingly similar to the supposed "apoplectic form" of poisoning by hydrogen sulphid,
which had been studied on animals by K. Lehmann, and which was observed in per-
sons who inhaled air containing a few per cent of this gas. Air containing 0.1 to 0.3
per cent of hydrogen sulphid kills cats and dogs in 10 minutes.
In our experiments in which were introduced substances containing sodium sulphid,
the poisoning must have been caused by hydrogen sulphid which was liberated from
the dye by the acid of the gastric juice, and which could cause poisoning also through
the stomach and through the respiratory apparatus.
Fortunately Vidal dyes, owing to their repulsive odor, will scarcely lind a wide
application in coloring food and beverages.
SOME REFLECTIONS REGARDING FURTHER INVESTIGATIONS OF I)YES FROM A SANITARY
STANDPOINT.
The present investigation, as well as all the investigations (f tin action of dyes on
animals by previous investigators, had for its object the solution of the question in
what number there exists among the dyes of the aromatic series dyes which possess
poisonous, or more or less pronounced harmful properties (answering essentially the
sanitary toxicological question). From the practical point of view such investigations
presented and do present the most important interest, inasmuch as they afford a possi-
bility of protecting the public from the use of obviously poisonous and harmful sub-
stances, but by such investigations questions of exceedingly sanitary imlpoxrtance are
not answered, namely:
1. Ought we to consider as quite harmless those dyes which do not induce pro-
nounced symptoms of poisoning and which are designated herein by the term non-
poisonous?






COAL-TAR COLORS USED IN FOOD PRODUCTS.


2. Is the usual answer which is given to the hygienist by the defenders of the unre-
stricted use of the coal-tar dyes for coloring food products and beverages, namely, that
in practice the dyes are introduced into the human organism in so small quantities
that their properties can be neglected, justified?
To both questions, besides the facts and considerations which I gave above in my
investigations, we may reply experimentally in two ways:
(a) By prolonged investigations continued over a period of years of the action of
very minute quantities on the animal organism, which has so far, owing to the incon-
veniences of such long experiments, not been done by anybody; and
(6) By investigation of the action of small doses of dye on some physiological func-
tions, and first of all on the activity of the digestive organs, which is first of all dis-
turbed upon the introduction of dyes into foods and beverages. The solution of the
last question can be best promoted, in my opinion, by experiments made on dogs and
by exploratory examination of the body according to the method of Prof. Pawlow.
Unfortunately, experiments such as these, owing to the difficulty of the Heidenhain-
Pawlow operation, are inaccessible to the majority of investigators.
As a very useful substitute of such investigations may serve observations on the
action of dyes on the activity of the digestive juices outside the body of animals.
On my proposition Dr. A. E. Winogradow began in my laboratory experiments on
the action of small doses of dyes of the aromatic series on the digestion in vitro. Dr.
Winogradow so far examined 25 coal-tar dyes in this respect according to the method of
Metta and convincingly proved that in insignificant doses coal-tar dyes (from one-half
to 4 milligrams) entirely stopped the digestion of albumen by artificial gastric juice.
It was found that the capacity to depress the digestion is possessed not only by poison-
ous dyes, but also by dyes which proved in my experiments on animals nonpoisonous.
It is quite possible, therefore, that an admixture of coal-tar dyes will exert an unfa-
vorable influence on the digestion and assimilation of food prepared from products col-
ored by them. Experimental proof of the last supposition can be given only by experi-
ments on the influence of dyes on the metabolism of substances in animals and man.
COMPLETE DETAILED STATEMENT OF ALL COMBINED DATA.

ABBREVIATIONS OF AUTHORITIES CITED.

The data hereinafter given is brought together as nearly as pos-
sible under the Green Table numbers to which it is pertinent. It is
believed that the literature has been quite thoroughly searched, and
that nothing of substantial importance has escaped recording in this
compilation; certainly whatever may have escaped can hardly serve
to change the general conclusion to which this compilation leads.
In order to avoid repetition min the following tabulation, "Weyl"
is to be understood as referring to the book entitled "The Coal Tar
Colors, with Especial Reference to their Injurious Qualities, etc.," by
Theodor Weyl, translated by Leffmann and published in Philadel-
phia, Pa., in 1892.
"Licber" refers to the book entitled "The Use of Coal Tar Colors
in Food Products," by Ihugo Lieber, published in New York in 1904.
"Fraenkel" refers to the book entitled "Arzneimittel Synthese,"
by Dr. Sigmund Fraenkel, published in Berlin in 1906.
"Confectioners List" refers to the Official Circular from the Exec-
utive Committee of the National Confectioners' Association of the


74






COMPILED DATA UNDER GREEN TABLE NUMBERS.


United States entitled "Colors in Confectionery" and reprinted, in
part, in the book entitled "Food Inspection and Analysis," by Albert
E. Leach, published in New York in 1906, pages 630-634.
"Resolutions of Swiss Analytical Chemists" refers to these reso-
lutions as published in Zeitschrift fuir Nahrungsmittel Untersuchung
und Hygiene, 1891, page 293.
"Schacherl" refers to Schacherl's publication entitled "Die Zulaes-
sigkeit Kuenstlicher Farbstoffe zum Farben von Lebensmitteln,"
published in Vol. III, pages 1041-1048, of the Report of the Fifth
International Congress of Applied Chemistry held in Berlin June 2
to 8, 1903.
"Chlopin" refers to Chlopin's monograph published in Russian
and entitled "Coal Tar Dyes. Classification, properties, and action
of artificial dyes on the animal organism, etc.," published at Dorpat
in 1903, or to the abstract of Chlopin's paper printed at page 169-172
of Vol. IV of the Report of the Fifth International Congress of Ap-
plied Chemistry held in Berlin, 1903.
"Canton of Tessin" refers to the publications of the Tessin regula-
tions published in 1897 in Zeitschrift fiur Untersuchung der Nahrungs
und Genussmittel, page 414.
Whenever possible the doses administered have been given in mil-
ligrams per kilo and grains per 100 pounds of body weight of animal.
In the case of the tabulations taken from Chlopin's monograph this
was not done; but in order to render such comparative data easily
available factors have been placed at the head of each tabulation;
for example, under G. T. 6 (1 gram=106 mg=74.2 grains), which
means that each gram administered amounts to 106 mg per kilo or
74.2 grains per 100 pounds of body weight of animal; by nm ultiJ)lying
the doses given by either of the factors the corresponding compara-
tive information is obtained.
In addition to the 106 Green Table numbers that have been
examined physiologically, there are reported thle results of the phli-s-
iological examination of S coal-tar colors not in the Grecil T"I'les, of
which 3 are said to be nonpoisonous, 3 are called poisonous. 1 is
called harmful, and the last is said to be "not (iUite larmless."
These 8 dyes are not included in this compilation.
TABULATION BY GREEN TABLE NUMBERS OF IIIYsiOLI)GIC.'A AN)
OTIHEIt D1).ATA..
G. T. 1.
Trade namrnes.-Picric acid; carbazotic acid.
Scientific namne.-Synmmtrical trinitrophenol.
Discovered.-1771.
Shade.-Yellow. Not offered.


75






76


COAL-TAR COLORS USED IN FOOD PRODUCTS.


FAVORABLE.
Nothing.
UNFAVORABLE.
1. Prohibited by Confectioners' List.
2. WEYL (p. 30): "The injurious character of picric acid has long been known."
3. "In Germany its employment for coloring food is forbidden by the imperial enact-
ment of 1888, on account of its poisonous character." (pp. 68-71.)
4. "The foregoing statements show that while the acid must be considered poisonous,
its injurious character is far less than has generally been assumed, nevertheless,
the legal prohibition of its use as a coloring matter for food or drink is just."
(p. 71.)
5. "Erb gave a rabbit weighing 1,700 grams, 0.06 gram of potassium picrate (24.5
grains per 100 pounds) daily for 90 days; slight loss of weight and occasional
diarrhea were noted, but nothing more serious." (p. 69.)
6. A rabbit weighing 2,065 grams died at the end of 19 days, after having taken 2.52
grams of the substance, or 854 grains per 100 pounds body weight; number of
doses not stated. (p. 69.)
7. Weyl's experiment on a dog, weight not given: April 21-26, 0.24 gram (3.7 grains)
sodium picrate daily; April 28-May 9, 0.36 gram (5.5 grains) daily; total, 5.76
grams (8.9 grains) sodium picrate; no serious disturbance; May 13, 1.2 grams
(181 grains) sodium picrate at one dose; weakness marked, diarrhea and dyspnea
next day; May 14, 0.6 gram (91 grains) caused vomiting; evening of same day,
0.36 gram (5.6 grains) given; May 15, animal lively; 0.24 gram (3.7 grains)
again given, and on evening of same day 0.72 gram (11.2 grains); May 16,
marked weakness of animal, and 0.16 gram (2.5 grains) given, causing vomiting;
May 17, 0.17 gram (2.6 grains) given; May 18 and 19, animal definitely recovered,
and aside from strong yellow tinge of the conjunctiva and skin, no abnormal
conditions manifest. Animal died May 20 after receiving 1.32 grams (20.4
grains) potassium picrate. Weyl concludes, therefore, that dogs are resistant
to this substance, notwithstanding the prostration and the blood disorganiza-
tion.
8. Weyl summarizes the effect on humans from therapeutic and poisoning cases to
the effect that daily doses of from 0.54 to 0.90 gram (8.3 to 13.8 grains) of potas-
sium picrate are easily borne by healthy adults for a considerable time; children
and weak adults bear picric acid badly. (p. 70.)
9. "Picric acid * is poisonous * *." (p. 96.)
10. FRAENKEL (p. 572): "On the other hand, this substance is not usable for internal
administration on account of its decomposing the red blood corpuscles, and of
its energetic cramp production, as well as on account of its disturbance of the
kidneys, and the ultimate paralysis of the respiratory centers; nevertheless,
picric acid is not to be considered a violent poison * *."
11. SCHACHERL (p.1044):' "Picric acid * (is), according to numerous state-
ments in the literature, poisonous even in small doses, and (is) therefore un-
qualifiedly to be declared as unpermissible."
12. LIEBER (p. 16), where it is stated to be forbidden by the German law, and is also
otherwise substantially the same as Weyl above quoted.
13. Resolutions of the Society of Swiss Analytical Chemists, September, 1891: "The
following are to be regarded as coloring matters harmful to health: * *
picric acid *."
14. Prohibited by the Belgian law of June 17, 1891.
15. LEwIN (Lehrbuch dcr Torikologie, 1897, p. 232): "Picric acid is poisonous. Rab-
bits can stand daily 10 milligrams of a green containing picric acid, but not 20
milligrams. Their death is accompanied by paralysis."
16. Buss lists it as poisonous.






COMPILED DATA UNDER GREEN TABLE NUMBERS.


G. T. 2.
Trade names.-Victoria Yellow; Victoria Orange; Golden Yellow;
Saffron Substitute; Anilin Orange; Di-nitro-Cresol.
Scientific name.-Di-nitro-o-and-p-cresol.
Shade.-Yellow. Not offered.
Discovered.- 1869.
Used for coloring butter, liqueurs, etc.
FAVORABLE.
Nothing.
UNFAVORABLE.
1. Prohibited by Confectioners' List.
2. FRAENKEL (p. 572): "On the other hand dinitro-cresol is much more intensely
poisonous (than picric acid), which is probably caused by its greater solubility
in water."
3. SCHACHERL (p. 104.4): * Dinitro-cresol [is], according to numerous state-
ments in the literature, poisonous even in small doses, and [is] therefore unquali-
fiedly to be declared as unpermissible."
4. Resolutions of the Society of Swiss Analytical Chemists, September, 1891: "The
following are to be regarded as coloring matters harmful to health * *
Dinitro-cresol * *."
5. Forbidden by the Canton of Tessin.
6. WEYL (p. 31): "I have shown the same (poisonous nature) for Dinitro-cresol (Saf-
fron Substitute). (See Zts. angew. Chem., 1888, No. 12, for confirmation of my
results by Gerlach.)"
7. "The reverse is the case with the poisonous dinitro-cresol (Saffron Substitute)."
(p. 55.)
8. WE.YL describes experiments with this compound. (pp. 71-85.)
9. Fourteen rabbits were experimented on, of which 13 died. Amounts administered
in the fatal cases.per 100 pounds body weight were (p. 74):
Grains. Grains.
189 175
175 168
175 175
175 168
175 168
175 175
175
Of 12 experiments on dogs, 5 receiving the color by the mouth and 7 hypoder-
mically, 3 cases resulted fatally; the fatal case by the mouth requiring 38.4S grains
per 100 pounds body weight; the 2 fatal cases h)ypodermically represented 11 and
20grains per 100 pounds body weight, respectively, although 140, 38.5,31.6, and
35 grains per 100 pounds body weight by the mouth were borne without fatal
effect; and 241, 11.9, 9.8, and 4.9 grains per 100 pounds body weight, hypo-
dermically, were also borne without fatal effect (p. 75).
10. WEYL (p. 96): "* * Dinitro-cresol * are [is]poisonous; *"
11. Prohibited by the Belgian law of June 17, 1891.
12. (Zta. Nahr. Genussm., 189?, p. 353): Recommended as an insecticide, 1500 being
sufficient for all ordinary purposes. One milligram is sufficient to kill a mouse;
2 milligrams recommended for killing mice.
13. WEYL (Handbuch der Hygiene): For humans, the fatal dose, when administered by
the stomach, appears to be 60 milligrams per kilo body weight, or 43 grains per
100 pounds.


77






78


COAL-TAR COLORS USED IN FOOD PRODUCTS.


14. "The president of the Council of Oppein forbids on April 19, 1899, the use of Saf-
fron Surrogate for coloring food products."
15. LEWIN (Lehrbuch der Toxikologie, 1897, p. 232): "Saffron Surrogate * 4,
which is used for coloring foodstuffs, is poisonous. It appears to attack the
coloring matter of the blood, and produces, in the case of dogs, vomiting, cramps,
and convulsions. * Feathers colored with Saffron Surrogate cause
burning and itching, and finally blisters on the hands of the women working
with them; the faces were also similarly affected, and this was accompanied by
loss of appetite and fever."
16. Buss lists it as poisonous.

G. T. 3.

Trade names.-Martius Yellow; Naphthol Yellow; Naphthylene Yel-
low; Naphthylamin Yellow; Manchester Yellow; Golden Yellow; Saf-
fron Yellow; Jaune d'Or; Jaune Naphthol.
Scientific name.-Dinitro-alpha-naphthol.
Discovered.-1864.
Shade.-Yellow. Not offered.

FAVORABLE.
Nothing.
UNFAVORABLE.
1. Prohibited by Confectioners' List.
2. WEYL (p. 31): "Cazeneuve and Lepine pointed out the poisonous nature of
Martius Yellow * *."
3. "This body (Chamber of Commerce at Sonneberg) recommends for the prepara-
tion of children's toys three colors, the poisonous character of which I can
demonstrate. These are Martius Yellow * *." (p. 34.)
4. "For instance, for preliminary researches, dogs and rabbits have value for
chemical reasons. The conclusions derived from such experiments must be
accepted with great deliberation, since it happens that rabbits will bear without
injury doses which will seriously, nay, even fatally, act upon the dog, as I
have already shown to be the case with Martius Yellow." (p. 56.)
5. Where two experiments by Cazeneuve and L6pine are referred to, in which
diarrhea, vomiting, and albuminuria were produced by this substance.
(pp. 85-89.)
6. Weyl's own experiments on 4 dogs showed weakness, vomiting, diarrhea, and
albuminuria resulting from the use of this color; the amounts of color admin-
istered per kilogram of body weight were 73, 17.5, 17.5, and 11.3 milligrams,
which amount to 51, 12, 12, and 8 grains, respectively, per 100 pounds of
body weight. (p. 87.)
7. "Martius Yellow, therefore, belongs to the injurious colors. As a coloring matter
for food and drink its use should be wholly prohibited." (p. 89.)
8. * and Martius Yellow are poisonous; * *." (p. 96.)
9. LEWIN (Lehrbuch der Toxikologie, 1897, p. 231): "Like Saffron Surrogate, it is
poisonous. In an experiment on myself, using large doses, I noticed among
others the general yellow coloration of the skin. In a poisoning resulting
fatally after 5 hours with Martius Yellow, vomiting, yellow coloration of the
skin and mucous membranes were observed; whereas the autopsy revealed,
among other things, hemorrhagic gastritis. (Jacobson, Hosp. Tid., 1893, p.
765.)"






COMPILED DATA UNDER GREEN TABLE NUMBERS. 79

10. Such small amounts as are used for the coloring of pastry are said to be non-
poisonous. (Vitalil boll. chim.farm., 1893, p. 738.)" (p. 231.)
11. CAZENEUVE AND LUPINE (Compt. rend., 1885, v. 101, pp. 1167-1169) say: I. "A
dog received 71 milligrams per kilogram of body weight, or 50 grains per 100
pounds daily. On the second day diarrhea and vomiting ensued; loss of
appetite except for milk. Thereafter it experienced difficulties in breathing;
suffered albuminuria; its urine was colored; it died on the sixth day. The
autopsy disclosed considerable congestion. II. A dog weighing 22 kilos
received 400 milligrams (19 milligrams per kilo or 13 grains per 100 pounds);
this caused a yellow vomit; next day it received 500 milligrams (27 milligrams
per kilo or 17 grains per 100 pounds), which caused violent diarrhea, fever,
thirst, disinclination for all food. The animal was killed; the autopsy showed
badly congested kidneys."
12. Prohibited by the Belgian law of June 17, 1891.
13. SCHACHERL (p. 1044): "* * Martius Yellow * [is], according to
numerous statements in the literature, poisonous even in small doses, and [is]
therefore unqualifiedly to be declared as unpermissible."
14. Prohibited by law in Italy. (See Lieber, p. 24.)
15. FRAENKEL (p. 572): "This substance also shows poisonous properties, although
it is less poisonous than dinitro-cresol."
16. Resolutions of the Society of Swuiss Analytical Chemists, September, 1P91: "The
following are to be regarded as coloring matters harmful to health * *
MartiusYellow * *."
17. Forbidden by the Canton of Tessin.
18. DIETRICH (Zts. Nahr. Genussm., 1902, v. .5, p. 364): "A lot of groats, after eating
which a family became sick, was found to be free from ordinary poisons, but
had been colored with Martius Yellow."
19. Buss lists it as poisonous.
DOUBTFUL.
1. WINOGRADOW (Zts. Nahrs. Genussm., 1903, r. 6, p. 589) says it noticeably retards
digestive action; is not indifferent.

G. T. 4.

Trade names.-Sulphur Yellow; Sulplhonaphthol Acid Yellow;
Succinic; Solid Yellow; Saffron Yellow; Jaiune AcideC.; J iune Acidle;
Fast Yellow; Citronin; Anilin Yellow; Acid Yellow S.
Names under which it was offered on 1the Unitfd States market a.% a
food color in 1907.-Naphthol Yellow SLOZ; Naplithol Yell(w S;
Naphthol Yellow; Naphthol Yellow L; Yellow F Y; Lemion Yelhow.
Scientific namne.-Dinitro-iilplia-naphtlol-1)et ti-inoniisulplolnic acid.
Discovered and patentcd.-1879.
Shade.-Yellow. Offered ,by 10 out of 12 sources.

I A VO It A It L.E.

1. Permitted by Confectioners' l.ist.
2. ('AZENEUVE AND LAPINE (('omft. rid., IS1s5, r. 101, pp. 1167-!169): "A di,
received each day for 5 days 32 milligrams per kilogram (if ,odlv W.iydl. ,r
23 grains per 100 pounds; frar the 10 days next lsuceeding it rci,'ivel fii r tihi'N
that amount, that is, 133 milligrams 1e-r kilogram of odyl weiht. ,r 93 grail.






80 COAL-TAR COLORS USED IN FOOD PRODUCTS.

2. CAZENEUVE AND IEPINE (Compt. rend., 1885, v. 101, pp. 1167-1169)-Continued.
per 100 pounds; for the 10 days next succeeding it received daily twice the last
amount, or 266 milligrams per kilogram of body weight, that is, 186 grains per
100 pounds. It received altogether in the 25 days 621 grams, or 964 grains.
There was no vomiting, no diarrhea, and no albumen in the urine at any
time."
3. WEYL (p. 31): "* * not poisonous to human beings and dogs: Naphthol
YellowS. * "
Weyl describes his own experiments on 3 dogs, giving them, respectively,
417, 34, and 100 milligrams per kilo body weight, or per 100 pounds 292, 24,
and 70 grains, respectively. Whether the color was administered by the mouth,
or injected subcutaneously, all bodily functions appeared to remain normal,
and it was only in the case of repeated doses of 417 milligrams per kilogram
of body weight, or 292 grains per 100 pounds, that albuminuria appeared.
S (pp. 89-92.)
4. "Only the sulphonated colors Naphthol Yellow * are harmless and appli-
cable to the coloring of food and drink." (p. 96.)
5. Permitted by the laws of Austria.
6. Permitted by the law of Italy.
7. Permitted by the law of France.
8. SCHACHERL (p. 1044): "* * Naphthol Yellow S * possesses no poi-
sonous properties."
9. FRAENKEL (p. 572): "Naphthol Yellow S is an entirely nonpoisonous substance."
10. MEYER (J. Amer. Chem. Soc. 1907, v. 29, p. 900): One hundred milligrams per
kilogram of body weight for the initial administration, and subsequent admin-
istrations increased geometrically. After the second administration intermit-
tent diarrhea resulted, emphasized by increased amounts with no albumin or
sugar in the urine; continued for 14 administrations; so that in 14 administra-
tions 147.58 grams of color had been given; the initial dose is 70 grains per 100
pounds of body weight, and the average daily dose of the total administered
is 394 grains per 100 pounds of body weight. Urine only slightly yellow col-
ored after small doses, but red after larger doses.
11. LIEBER (p. 143): A dog received 36 milligrams per kilogram of body weight, or
25.2 grains per 100 pounds once a day seven times every other day; during the
whole period the dog was apparently in good condition with no bad effects
from the color.
12. Buss lists it as nonpoisonous.
13. CAZENEUVE AND LAPINE (Compt. rend., 1885, v. 101, pp. 1167-1169): Three
chronic invalids received daily from 2 to 4 grams of the dye in cochets; except
slight colic and diarrhea nothing abnormal.
DOUBTFUL.
1. LEWIN (Lehrbuch der Toxikologie, 1897, p. 232): "Acid Yellow S is said to be able
to produce dermatitis on frequent contact-therewith."
2. WINOGRADOW (Zts. Nahr. Genussmn., 1903, v. 6, p. 589) says it noticeably retards
digestive action; is not indifferent.

G. T. 5.

Trade name.-Brilliant Yellow; Naphthol Yellow S or RS.
Scientific name.-Dini tro-alpha-naphthol-alpha-monosulphonic acid.
Discovered and patented.-1884.
Shade.-Yellow. Not offered.







COMPILED DATA UNDER GREEN TABLE NUMBERS.


FAVOiPABLE.

1. Permitted by Confectioners' List.
2. WEYL (pp. 92-94): Describes experiments on 2 dogs, in which the initial dose
was 532 milligrams by the mouth, and 17 milligrams hypodermically, per kilo-
gram of body weight, respectively, 372 and 12 grains per 100 pounds of body
weight; in both cases the urine was colored, in the second ce traces of albu-
minuria resulted. In the first case the albuminuria was doubtful.

3. "Brilliant Yellow is not poisonous, even in large doses, when administered by the
stomach * the albuminuria was very slight. (p. 94.)
4. "Only the sulphonated colors * Brilliant Yellow, arc harmless, and
applicable to the coloring of food and drink." (p. 96.)
5. SCHACHERL (p. 1044): * Brilliant Yellow * possesses no
poisonous properties."
6. FRAENKEL (p. 572): "For the same reason * Brilliant Yellow * *
is without effect."

G. T. 6.


Trade names.-Aurantia; Nitrodiphenylamin;
Kaiser Yellow.
Scientific name.-Hexanitro-diphenylamin.
Discovered.-l 873.
Shade.-Yellow. Not offered.


Imperial Yellow;


FAVORABLE.
Nothing.
UNFAVORABLE.

1. WVEYL(p. 96): Aurantia suspicious."
2. SCHACHERL (p. 1044):" Aurantia [is] according to numerous statements
in the literature poisonous even in small doses, and [is] therefore unqualifiedly
to be declared as unpermissible."
3. CHLOPIN (p. 116) as results of his experiments considers it injurious. Thlie exlperi-
mental data are as follows:

E.xperimenlal data jql ( "ilopin.

11 graTm-= lk; rng=74 2 grains.]


Date. Dose. Weight ur.4?i'
Iuri une.


I Grama. Kilo. co.
1 9. 4 4:5
3 ......... 4VK

33 ......... 410
3 ........ 410



,. I
3 4 N


S;neranal condition uo aninial aiid urine.


Before exprirlmentI urine anil 'l rinorrim.l
\'ulli tedl sef iral t tlllii'. lrilne' ijr iltir" .iril no 1 l''tiiin'?i.
Repeated \uriif11i g; urine ditrk Iro\iwn, wiu'l, no :llmi t ieni: tjoiZ
No VumII1 in i' urine alnimst 1 lack: Wu' I: ii., all'iini*
No vunlliig: uriTIn dark tbrown. 1t idl. 11i .i3l|tiIlt'II.
Voim iting; urinte iilint.st fil,- 'k. : hti'l. 1 ,11 111 (tll'iii .
No vonilllriig, urint almost lhu-k. .'tll,. rio :illiuriwn
Same; urine clwxulate 1ruwn. uacdl: no all 'ulitii. get,.nI .',ndiii-
tlun iliortuiml.
Gnridully etlur of LrIne I ttcomes nornial: in 'Tv cry ter re.i'et-
dig Is w'ell.


972910 Mull. 1 17 12


1902.
Mar. 12
13
14


15
s18
19
20
21
22-26
Total






82 COAL-TAR COLORS USED IN FOOD PRODUCTS.

4. FRAENKEL (p. 573): "The coloring matter called Aurantia, which is a salt of
hexanitro-diphenylamin, appears to be poisonous on account of the nitro groups,
which is on the other hand denied by a few observers."
5. Resolutions of the Swiss Analytical Chemists, September, 1891: "The following are
to be regarded as coloring matters harmful to health * Aurantia

6. Forbidden by the Canton of Tessin.
7. LEWIN (Lehrbuch der Torikologie, 1897, p. 232): "Aurantia has a poisonous action.
After wearing gloves for 8 hours made with so-called dogskin, which were col-
ored with Aurantia, a man suffered confluent blisters, accompanied by itching.
The workmen with this material get blisters on the face and on the hands.
Ptrspiration increases the tendency to such blisters."
8. Buss lists it as poisonous.
G. T. 8.

Trade names.-Acid Yellow; Fast Yellow G; Acid Yellow G; Fast
Yellow; Fast Yellow extra; Jaune Acide; New Yellow L.
Names under which it was offered on the United States market as a
food color in 1907.-Fast Yellow Y; Fast Yellow G; Acid Yellow G
pat.; Fast Yellow 053.
Scientific na me.-Amidoazobenzene-disulphonate with some sodium
amidoazobeniizene-monosulphonate.
Discovered.-1878.
Shade.-Yellow. Offered by 5 out of 12 sources.

FAVORABLE.
1. Permitted by Confectioners' List.
2. CAZENEUVE AND LAPINE (Bull. de l'acad. de mied., April 27, 1886, p. 643), where
it is classified among the "nontoxic" colors.
3. FRAENKEL (p. 575), where it is stated to be nonpoisonous.
4. Permitted by the law of Austria.
UNFAVORABLE.
1. WEYL (p. 115): "Poisonous to human beings. (?)"
2. CHLOPIN (p. 151) considers that the work of others makes this a suspicious color.
His own experimental data are as follows:
Experimental data by Chlopin.
C. T. 8 AND 9.
[1 granm = 152 mRg- 106 grains.]


urine.

1V(11. Grains. Kilos. rM.
Mar. I 1;- .......... ......... :10i Dog normal; color urine normal; acid; no albumen.
14 6 .6 ............ Do.
1-, ******.... . .. . . D o.
I .......... .................... Urine greenish brown; reddens with 11SO4 and C1I; no
ii albuimen.
17 .................... 305 Color same; traces of albumen.
S.......... .......... 3K) Color less Intense; trace of albumen.
N9 3 fi.4 32) Do.
S.......... .......... 2) Urine greenish brown; albumen gone; dog is lively.
21 ........6 22 Everything normal.
Total..... 4

Conclusion: "SupiciouM."






COMPILED DATA UNDER GREEN TABLE NUMBERS.


3. Buss (Forschungsber. iber Lebensmittel, 1896, Vol. III, p. 173): Is regarded as
poisonous.
4. KOBERT (Lehirbuch der Intoxicationen, 1893, p. 335): Listed as poisonous.
5. LEWIN (Lehrbuch der Toxikologie, 1897, p. 231) says "produces eczema," and
cites Deutsche Med. Wochenschr., 1891, p. 45.

G. T. 9.

Trade names.-Fast Yellow R; Fast Yellow; Yellow W.
Name under which it was offered on the United States mark-(et as a
food color in 1907.-Fast Yellow 034.
Scientific name.-Sodium salt of amidoazotoluene-disulphonic acid.
Discovered and patented.-1878.
Shade.-Yellow. Offered by 1 out of 12 sources.

FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYL (p. 31): * not poisonous to human beings and dogs * *
Solid Yellow."
3. CAZENEUVE AND LAPINE (Compt. rend., 1885, v. 101, pp. 1167-1169): A. A dog
received 42 milligrams per kilogram of body weight, or 29 grains per 100 pounds,
for 5 days; thereupon received four times that amount for 5 days, or 168 milli-
grams per kilogram body weight, or 117 grains per 100 pounds; for the 10 days
next succeeding it received daily twice the last dose, or 336 milligrams per
kilogram of body weight, that is, 235 grains per 100 pounds; it then received
in 1 day 20 times the original dose, or 840 milligrams per kilogram body
weight, that is, 596 grains per 100 pounds, and during the entire period nothing
abnormal was noticed. B. Three chronic invalids received from 2 to 4 grains
of the dye daily; except colic without diarrhea nothing abnormal. They con-
cluded that this dye is no more harmful than Naphthol Yellow S (G. T. 4).
4. CAZENEUVE AND LEPINE (Bull. de V'acad. de m7ed., 1886, p. 643): Tolerated by
man, well or sick.
UNFAVORABLE.
1. WEYL (p. 115): "Poisonous to human beings. (?)"
2. CHLOPIN (p. 151): Where he considers that the work of others makes this a suis-
picious color. For his experimental data thereon see table under G. T. 8;
Chlopin's chemical description of the dye used applies to both G. T. 8 and 9.
3. KOBERT 'Lchrbuch der Inloxicationen, 1893, p. 336): Listed as poisonous.

G. T. 11.

Trade names.-Sudan I; Carminapli.
Names under which it was ojffcnd on. the Un1ited Staftes mnarkt as a
food color in 1907.-Oil Orange 7078; ('erasin Orange I.
Scientific name.-Benzeniie-azo-betanaphlithol.
Discovered.-1i 883.
Shade.-Orange Yellow. Offered by 2 out of 12 sources.
FAVU'RABLE.
1. WEYL (p. 115): "Nonpoisonous * Soudan I * *."
2. "Other Azo-colors, * fur instance Soudan I I are entirely non-
poisonous." (p. 148.)


83






84


COAL-TAR COLORS USED IN FOOD PRODUCTS.


UNFAVORABLE.

1. Prohibited by Confectioners' List.
2. WEVEYL (p. 119): Dog received 18 grams in 6 doses in 17 days, and remained under
observation 5 days longer; 4 doses of 168 milligrams per kilogram body weight
(118 grains per 100 pounds) and 2 doses of 420 milligrams per kilogram body
weight (294 grains per 100 pounds) produced colored urine, phenol in urine,
vomiting and distinct albuminuria beginning with the third dose. From the
foregoing Weyl concludes as follows: "The color in the doses administered is
not entirely harmless, since a limited albuminuria seems to be brought about."
3. FRAENKEL (p. 576): "It is not wholly harmless, since this coloring matter seems
to produce a slight albuminuria."

G. T. 13.

Trade names.-Ponceau 4 G B; Crocein Orange; Brilliant Orange;
Orange G R X.
Names under which it was offered on the United States market as a
food color in 1907.-Crocein Orange 10234; Crocein Orange; Crocemin
Orange G; Ponceau 4 G B.
Scientific name.-Anilin-azo-betanaphthol-monosulphonic acid.
Discovered.-1878.
Shade.-Orange Yellow. Offered by 6 out of 12 sources.

FAVORABLE.

1. Permitted by Confectiorers' List.
2. WEYL(p. 115): "Nonpoisonous * Ponceau 4 G B * *."
3. Experiment on dog in doses of 161 milligrams per kilogram body weight; that is,
113 grains per 100 pounds body weight, apparently produced no disturbance
aside from coloring of the urine. (p. 124.)
4. WEYT, (p. 1-8): "Other Azo-colors * for instance * New Coc-
cmin * are entirely nonpoisonous."
5. Weyl's coiicliusion reads as follows: "This color can be regarded as nonpoisonous."
6. FRAENKEL (p. 577): "Ponceau 4 G B can be regarded as nonpoisonous."

UNFAVORABLE.

1. Excluded by law of Avstria.

G. T. 14.

Trade narnes.-Orange G; Orange G G.
Names. under which it was offered on the United States market as a
food color in 1907.-Orange G G crystals; Orange G.
Scie ntfic name.-Aniilin-azo-betanaphthol-disulphonic acid G.
Discovered and patented.-1878.
Shade.-Orange Yellow. Offered by 2 out of 12 sources.







85


COMPILED DATA UNDER GREEN TABLE NUMBERS.

FAVORABLE.

1. Chlopin examined this color, and his experimental data are as follows:

Experimental data by. Chlopin.

No. 1 (p. 128).
[1 gram=73 mg=51 grains.]


Date. Dose. Weight. 24-hours' General condition of animal and urine.
urine.

1901. Grams. Kilos. cc.
Apr. 4 1 13.7 525 Nothing abnormal; no albumen.
5 .................... 600 Urine light chocolate brown, acid; no albumen.
6 2 .......... 990 Urine clear, yellow, blackish sheen; no albumen.
7 ................... 550 Urine clear, dark brown; no albumen; faintly alkaline.
8 .................... 680 Do.
9 ................... 730 Nothing abnormal.
10 ................... 755 Do.
Total. 3

No. 2 (p. 14).
[1 gram= 119 mg= 103 grains.]


.3


3
3
3
3


8&4
.... ......



..........
..........
..........
.. ........


315
...... 4..
370O


320
210
225
295


Nothing abnormal; no albumen.
Do.
Urine orange in color, acid, no albumen; in other respects nothing
abnormal.
Do.
Do.
Do.
Do.
Do.
Do.


Conclusion: Nonpoisonous.


1. Excluded by Austrian law.


UNFAVORABLE.


G. T. 15.


Trade names.-Ponceau 2 G; Orange R.
Scientific name.-Sodium salt of benzene-azo-beta-naphthol-disul-
phonic acid R.
Shade.-Bright Red. Not offered.


FAVORABLE.

1. Permitted by Confectioners' List.

UNFAVORABLE.

1. Excluded under Austrian law.
2. Excluded under Swiss laws.

G. T. 16.

Trade names.-B utter Yellow; Oil Yellow.
Scientific name.-Dimethyl-amido-azo-benzene.
Discovered.-1875.


Shade.-Yellow.


1901.
Nov. 8
12
13-14
15
16
17
18
20
21
Total.


Not offered.







86


COAL-TAR COLORS USED IN FOOD PRODUCTS.


FAVORABLE.

1. WEYL (p. 31): "Butter Yellow produces no disturbance in rabbits."

UNFAVORABLE.

1. CLmoPi (p. 138): Where as a result of his own experiments he considers it poi-
sonous. His experimental data are as follows:

Experimental data by Chlopin.
No. 1.


[(1 gram=159 mg= 111 grains.]


Date. Dose. Weight. General condition of animal and urine.

1902. Gra ms. K ilos.
May 6 3 6.3 Before experiment urine normal; after a few hours vomiting; urine not
collected.
7-8 ................. No vomiting; eats poorly; more tired than usual.
9-15 ................... Dog gradually becomes normal.
16 3 .......... Vomiting; loss appetite.
17 .................... Repeated vomiting.
18 .......... ........ Vomiting continues.1


No. 2.
[1 gram =96 mg=67 grains.]

1903.
Feb. 5 2 3 10.4 Before experiment dog quite normal; acid; no albumen.
6 .................... Vomiting during night; dog does not eat, but drinks; urine more yellow
than normal; acid; no albumnen; in the evening the dog walked and
drank water.
7 ................. Died during the night; thin excreta in kennel; autopsy showed paralysis
of heart as causing death.

No. 3.
[1 gramn= 167 mg= 117 grains.]

1903.
Feb. 8 2 6 Five hours after administration vomiting and involuntary thin feces.
9 .................... Dog does not eat; drinks much; weak; urine dark yellow; no vomiting.
10 .................... Do.
11 ................... Dog lies in cage; moves slowly when allowed out of cagp; In the evening
retching.
12 .......... .......... Dog is still weak, but general condition somewhat better; urine strikingly
colored; acid; no albunien.
13 .......... .......... Began to eat; no albumen.
14-16 .................. Geapral condition improving and almost normal; lassitude continues
more than usual; urine normal color; acid; no albumen.
17 3 2 .......... Tn the evening repeated vomiting; loss of appetite.
18 2 .......... No vomiting; in the evening bothersome; does not eat.
19 ........ ..7 Stools normal; striking disturbance of movements; paralysis of legs; must
spread hind legs to stand; when pushed not only falls, but turns on his
back; sight and hearing are normal; dog died at night.


' This dug ran away.


SGruelelr's make.


* Berlin make.


G. T. 17, 18, 41.

17. Trade narnes.-Chrysoidin Y; Chrysoidin crystals.
Name 'under which it was offered on the United States market as a
food color in 1907.-Chrysoidin Y.
Scientific namrne.-Anilin-azo-mneta-phenylene-diamin.
Disco vered.-1875.






COMPILED DATA UNDER GREEN TABLE NUMBERS.


Shade.-Orange. Offered by 2 out of 12 sources.
18. Trade names.-Chrysoidin R; Cerotin Orange; C extra; Gold
Orange for cotton.
Name under which it was offered on the United States market as a
food color in 1907.-Chrysoidin R.
Scientific name.-Anilin-azo-meta-tolylene-d iamin.
Shade.-Yellow brown. Offered by 1 out of 12 sources.
41. Trade name.---Chrysoidin R.
Scientific name.-Hydrochlorid of toluene-azo-meta-tolylene-di-
amin.
Discovered.-1876.
Shade.-Orange Brown.

(NOTE.-It has not been possible accurately to differentiate in the literature as to
whether Nos. 17, 18, or 41, or all three, were referred to.)

FAVORABLE.
1. VWEYL(p. 115): "Nonpoisonous * Chrysoidin * *."
2. Permitted by the law of Italy.

UNFAVORABLE.
1. Prohibited by Confectioners' List.
2. WEYL (p. 126): Experiment on dog, giving him 113 milligrams per kilogram body
weight, or 79 grains per 100 pounds body weight, produced a slight albuminuria.
In a second experiment a dog receiving "1 grain" ("grain" is evidently a
misprint for "gram" and will be so treated), that is, 105 milligrams per kilogram
body weight, or 74 grains per 100 pounds body weight, daily for one month, did
not produce albuminuria, but caused a loss of body weight of about 12.5 per cent.
A third dog receiving about 2 milligrams per kilogram body weight, or about 1.5
grains per 100 pounds body weight subcutaneously, suffered a loss of 20 per cent
of its body weight in 23 days; dose repeated 24 days after and animal kept
under observation seven days longer when animal was normal.
3. Weyl in summarizing experiments on these three dogs concludes as fdllows:
"Chrysoidin produces, according to my investigations, a slight albumiinuria,
and notable reduction in body weight, but further disturbance has nuot beenl
noted." (p. 127.)
4. FRAENKEL (p. 577): "The abovo-mentioned ('Chrysoidin * produtio. a
slight albuminuria, and a notable decrease of body weight, and prldicis factory
eczema."
5. LEWIN (Lehrbuch der Tozikologie, 1897, p. 231): "Produces eczrna," and cites
Deutsche Med. Wochenschr., 1891, p. 4.5.

G. T. 28.

Trade name.-Archil Substitute V.
Scientific name.-Sodiumni salt of para-nitrol)benzene-azo-ulp IlIL-na)IpIl-
thylamin-para-suiphonic acid.
Discovered and patented.-1S78.
Shade.-Red. Not offered.


87






COAL-TAR COLORS USED IN FOOD PRODUCTS.


FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYt(p. 115): "Nonpoisonous * Archil Substitute * *
Describing experiments on three dogs, as follows: A. 430 milligrams per
kilogram body weight, or 301 grains per 100 pounds body weight, on each of two
successive days, and double the dose on the fourth day, producing no vomiting,
but a tendency to vomit, a slight albuminuria and colored urine. B. 182 mil-
ligrams per kilogram body weight, or 127 grains per 100 pounds body weight,
administered daily for one month; results similar to foregoing, but no colored
urine. C. 105 milligrams per kilogram body weight, or 116 grains per 100 pounds
body weight administered subcutaneously, produced only slight albuminuria,
and no reduction in body weight. (p. 125.)

G. T. 43.

Trade names.-Orange GT; Orange RN; Orange 0; Orange N.
Scientific name.---Sodium salt of toluene-azo-beta-naphthol-sulpho-
nic acid.
Discovered.-1879.
Shade.-Orange. Not offered.

FAVORABLE.
1. Permitted by Confectioners' List.
UNFAVORABLE.
1. Excluded by Austrian law.
2. Excluded by Swiss laws.
G. T. 55.

Trade names.-Ponceau R; Ponceau 2 R; Ponceau G and GR;
Xylidin Red; Xylidin Scarlet.
Names under which it was offered on the United States market as a
food color in 1907.-Scarlet; Orange R.
Scientific name.-Sodium salt of xylene-azo-beta-naphthol-disul-
phonic acid.
Shade.---Scarlet. Offered by 2 out of 12 sources.

FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYL (p. 31): "According to Cazeneuve and LUpine's experiments the follow-
ingarenotpoisonous tohumanbeingsanddogs * PonceauR * *."
3:. "Ponceau R (Ponceau 2 R, Xylidin Red, Xylidin Ponceau), not poisonous to dogs
neither by administration by stomach nor injection into blood." (p. 115.)
4. "()thlier Azo colors * Xylidin Red * are entirely nonpoisonous."
(p. 14s.)
5. FILAENKEL(p. 575): "That the monazo coloring matters examined by Cazeneuve
and LUpine, as already above stated, were nonpoisonous, can be easily explained
by the coIHtitution of these substances. These two investigators examined
* Ponceau R * *."


88






COMPILED DATA UNDER GREEN TABLE NUMBERS. 89

6. LIEBER (p. 140): A guinea pig received 310 milligrams per kilogram body weight
or 217 grains per 100 pounds body weight, once a day six times every other day;
the appetite appeared to remain good, and no disturbances were noted.
7. Permitted by Austrian law.
8. Permitted by Swiss laws.
9. CAZENEUVE and LgPINE (Bull. de l'acad. de mid., 1886, p. 643): Tolerated by
man well or sick.
10. CHLOPiN (p. 150) classes it as nonpoisonous on his own experiments. His experi-
mental data are as follows:

Experimental data by Chlopin.
(1 gram= 141 mg=99 grains.]


Date. Dose. Weight. 24-hours' General condition of animal and urine.

1902. Grams. Kilos, cc.
May 3 2 7.1 370 Dog and urine normal and no albumen.
4 .......... .......... 351 Urine rose-colored; no albumen.
5 2 .......... .420 Color normal; no albumen.
6 ........- .......... 290 Rose-colored urine; no albumen.
7 2 ........... 359 Normal color; no albumen.
8 .................... 360 Rose-colored; no albumen.
9 .................... 330 Color and composition normal.
Total. 6
________I______________________________________

UNFAVORABLE.
1. Prohibited by the ordinance of the police commissioner in France. (S-e Lieber,
p. 80.)
2. MEYER (J. Amer. Chem. Soc. 1907, v. 29, pp. 900-901): The dog experimented
on showed signs of paralysis on the morning of the seventh day at 8 o'clock,
and died at 10.40 a. m., after having received a total of 32 grams of color, (if
which 16 had been given on the last day. The initial dose was 70 grains per
100 pounds body weight; the total weight of color was 5,818 milligrams per
kilogram body weight, or 4,073 grains per 100 pounds; the average daily dse
was therefore 582 gains per 100 pounds, or 831 milligrams p)Cr kilogram body
weight.
DOUBTFUL.

1. WINooaGRADow (Zts. Nahr. Genussmn., 1903, v. 6, p. .5'9) says it almost comcputely
inhibits digestion.

G. T. 65.

Trade names.-Fast Red B; Bordeaux B; BordeaCLux B11; Bordeaux
R extra.
Names under which it was offered on (iMe I'nited States market ia. a
food color in 1907.-Bordeaux B; Claret Reld.
Scientific name.-Alphanaptthytlanizl-z,)-bct anapthol-disull di-
nic acid.
Discovered.-1878.
Shade.-Red. Offered by 2 out of 12 sources.






COAL-TAR COLORS USED IN FOOD PRODUCTS.


FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYL (p. 115): "Bordeaux Red (Fast Red B) not poisonous to human beings."
3. "Other Azo colors * Fast RedB * are entirely nonpoisonous."
(p. 148.)
4. FRAENKEL (p. 575): "That the monoazo coloring matters examined by Cazeneuve
and Lepine, as already above stated, are nonpoisonous, can be easily explained
by the constitution of these substances. These two investigators examined
* Bordeaux B."
5. ARLOING AND CAZENEUVE (Archires de physiologie, 1887, pp. 356-393): As a result
of this work, which is divided into three parts-(1) Stating the effect of direct
introduction of the color into the circulation; (2) intravenous injections; (3)
comparing the effects of injections of color and of salt; and (4) feeding by the
mouth-these investigators conclude that these coloring matters are toxic only
in extremely large doses; that when given to dogs with their food that no incon-
venience of any kind results; this is based upon experiments on three dogs,
covering 145 days, where each dog received per kilogram of'initial body weight
in the first case 20,307 milligrams, or 14,213 grains per 100 pounds initial body
weight; in the second case, 29,590 milligrams, or 20,713 grains per 100 pounds
initial body weight; and in the third case, 28,154 milligrams, or 19,758 grains
per 100 pounds initial body weight. Per day this means 98 grains per 100
pounds initial body weight in the first case; in the second case, 143 grains per
100 pounds initial body weight; and in the third case, 137 grains per 100 pounds
initial body weight.
6. CAZENEUVE (Arch. gin. de med., 1886, p. 753) says it may be taken without effect
by man or animals, sick or well, in large doses.
7. CAZENEUVE AND LUPINE (Bull. de l'acad. de med., 1886, p. 643): Tolerated by man
well or sick.
G. T. 70.
Trade name.-Azarin S.
Scientific name.-Ammonium bisulphite compound of dichloro-
phenol-azo-beta-naphthol.
Shade.-Red. Not offered.
FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYL (p. 115): "Nonpoisonous * AzarinS * *."
3. Experiments on five dogs; three fed by the mouth; two treated hypodermically,
of which latter one died. The first dog received 1,367 milligrams per kilogram
body weight in 25 days; that is, 54.7 kilograms per day on the average, or a total
of 957 grains per 100 pounds of body weight; that is, 38 grains per 100 pounds
body weight per day. The second dog received a total of 1,942 milligrams per
kilogram body weight in 20 days, or 97 milligrams per kilogram body weight per
day, which amounts to a total of 1,359 grains per 100 pounds body weight, or 68
grains per 100 pounds body weight per day. In both cases a distinct amount of
albumen was present in the urine, and the urine evolved sulphurous acid on treat-
ment with hydrochloric acid. The third dog received hypodermically three
doses in eight days, each (lose being 213 milligrams per kilogram body weight;
that is, 1.19 grains per 100 pounds body weight; no bad effects. (p. 133.)
3. "Administered by the stomach Azarin S is harmless." (p. 184.)
4. "Other Azo colors, * for instance Azarin S, are entirely nonpoisonous."
(p. 148.)
5. FRAENKEL) (p. 578): "A zarin S administered by the stomach is entirely harmless."


90






COMPILED DATA UNDER GREEN TABLE NUMBERS. 91

UNFAVORABLE.

1. WEYL (p. 134): Dog; weight not given; received 5 cc of Azarin S paste by injec-
tion into the abdominal cavity, and survived three days. "The cause of death
was considered to be peritonitis without effusion. The result of this post-
mortem is of much interest. The red spots consisted, as was determined by
chemical analysis, of the azo color which is the basis of the Azarin S. Conse-
quently in the peritoneal cavity the same splitting up of the Azarin S had
occurred which takes place when it is attached to textiles."
2. FRAENKEL (p. 578): To the same effect.

G. T. 78.
Trade name.-Erika B.
Scientific name.---Sodium salt of methyl-benzenyl-amido-thio-
xylenol-azo-alpha-naphthol-disulphonic acid.
Discovered and patented.-1889.
Shade.-Rose Pink. Not offered.

FAVORABLE.
Nothing.
UNFAVORABLE.

1. CHLOPIN (p. 153): Based onhis own experiments considers it as not harmless. The
experimental data are as follows:

Experimental data by Chlopin.
[1 gram=125 mg=87.5 grains.]

Date. Dose. Weight. 24 hours generall condition of animal andi urine.
I urine.
1901. Grams. Kilos. cc.
May 9 2 8.0 392 Dog normal; urine acid; no albumen.
10 .................. 400 Urine of rose shade; insignificant traces of albumen; acid.
11 .......... .......... 420 Color same; no albumen.
12 2 .......... 360 Do.
13 .................... 390 Do.
14 .................... 293 Urine yellow, greenish shade; traces of albumen.
15 .......... ......... 350 Color normal; no albumen.
16 2 8.2 390 Do.
17 .................... 402 Urine wine yellow. orange, acid: no albumen.
18 .......... .......... 350 Dog quile well; urine orange: no albmnen.
Total. 6


G. T. 84.

Trade names.-Resorcin Yellow; Tropaolin 0; Tropaeolin R;
Chrysoin; Chryseolin; Yellowv T; Gold Ye oAei Yellow; Ac Ylw.
Names under which it u'was o/fircd on the U'nitd Sitcts nimarkt (s a
food color in 1907.-Clirysoin REZ; Resorcin 0275.
Scientific name.-Sodiumn salt of para-suIphoLcnzeile-azo-resorcinl.
Discovered.-l S75.
Shade.-Reddish yelh)low. Offered by 2 out, of 12 sources.







92 COAL-TAR COLORS USED IN FOOD PRODUCTS.

FAVORABLE.
1. CHLOPnr (pp. 131-2) examined this color physiologically, and has classified it as
harmless. The experimental data are as follows:

Experimental data by Chlopin.
No. 1 (p. fr7).
[1 gram=43 mg=30 grains.]

Date. Dose. Weight. 24 h Sur' General condition of animal and urine.
I urine.

1901. Grams. Kilos. cc.
Apr. 9 .......... 23.00 500 Dog quite well; urine normal color, acid; no albumen.
10 11.21 .......... ........ Do.
11 0.70 .................... Urine acid; no albumen.
12 1 2.00 .................... No symptoms of poisoning; eats.
13 .................... 480 Urine dark brown; no albumen.
14 .................... 520 Do.
17 .................... 580 Urine normal color; no albumen; dog is well.
Total.. 13.21
20.70

No. 2.
[1 gram= 156 mg= 109 grains.]

1901.
Oct. 9 .......... 6.4 30 Dog well; urine yellow; no albumen.
10 2 .......... 350 Do.
11 2 ................... Urine brown, acid; no albumen.
12 .......... .......... 300 Urine light brown, acid; no albumen.
13 2 ............. 335 Do.
14 .................... 290 Do.
15 .................... 290 Do.
16 2 .......... 375 Do.
17 .................... 300 Do.
18 2 ................ Do.
19 .................... 320 Urine light brown, acid, no albumen; diarrhea.
20 ................... 360 Brown yellow, acid, no albumen no diarrhea.
21 .................... 360 Urine normal; dog is well.
22-26 ......... 7.0 ......... Do.
Total... 10

1 Internally. 2 Subcutaneously.
2. Permitted by the law of Italy.
UNFAVORABLE.
1. Forbidden by the Confectioners' List.

DOUBTFUL.

1. WINOGRADOW (Zts. Nahr. Genussm., 1903, v. 6, p. 589) says it noticeably retards
digestive action; not indifferent.

G. T. 85.

Trade names.-Orange I; Alphanaphthol Orange; Naphthol Orange;
Tropaolin 000; Orange B.
Names under which it was offered on the United States market as a
food color in 1907.-Orange RZ; Orange 027.
Scientific name.-Sodium salt of para-sulphobenzene-azo-alpha-
naphthol.
Discovered.- 187 6.
Shade.-Orange. Offered by 2 out of 12 sources.






COMPILED DATA UNDER GREEN TABLE NUMBERS.


93


FAVORABLE.
1. Permitted by Confectioners' List.
2. WEYL (p. 31): "According to Cazeneuve and Lepine's experiments, the following
are not poisonous to human beings and dogs: * Orange * *."
3. "Orange I (Alpha-naphthol Orange, Tropaolin 000) not poisonous to dogs neither
by administration by stomach, nor by injection into blood." (On authority of
Cazeneuve and Lepine.) (p. 115.)
4. WEYL (pp. 123, 148) refers to this as not poisonous.
5. Permitted by the law of Italy.
6. Permitted by the law of Austria.
7. CAZENEUVE (Arch. gin. de md., 1886, Vol. I, p. 753) says it may be taken without
effect by man or animals, sick or well, in large doses.
8. CAZENEUVE AND LEPINE (Bull. de l'acad. de med., 1886, p. 64-3): Tolerated by man,
well or sick.
G. T. 86.

Trade names.-Orange II; Betanaphthol Orange; Tropseolin 000
No. 2; Mandarin G extra; Chrysaurein; Gold Orange; Orange extra;
Atlas Orange; Orange A.
Names under which it was offered on the United States market as a
food color in 1907.-Naphthol Yellow SLOZ; Orange II; Orange;
Orange Y; Mandarin G extra; Orange A 1201; Orange A extra.
Scientific name.-Sodium salt of para-sulphobenzene-azo-beta-
naphthol.
Discovered.- 1876.
Shade.-Orange. Offered by 8 out of 12 sources.

FAVORABLE.
1. Permitted by law in Italy.
2. FRENTZEL(Zts. Nahr. Genussm., 1901, v. 4, p. 974) says that according to his experi-
ments this color, in the small amounts in which it is used in food products and
which can enter the human system in the course of 24 hours, can hardly, even
with frequent administration, cause a harmful effect.
3. FRENTZEL(Zt8. Nahr.Genuasm., 1901, v. 4, pp. 968-974): Experimented on rabbits,
giving dye with food, a total of 21 grams in 19 days, a total of 8,748 millig-rams
per kilogram body weight, or 6,133 grains per 100 pounds body weight, in doses
of 1 grm each, daily for the first 15 days, or about 417 milligrams per kilogram
of body weight, or 292 grains per 100 pounds body weight per dose for these 15
doses; the color could only be detected in the urine, and the feces becanime
softer. A dog was given 1,020 milligrams per kilogramn body weight, or 714
grains per 100 pounds body weight, and showed distinct kidney irritation, great
thirst, and diarrhea; recovery required about one week; and thereafter the same
animal was fed by the mouth one-twentieth of the above dose each day for 9
successive days without any untoward effect. A second dog received per kilo-
gram of body weight 172 miilligranms, (or 121 graiiLs per 100I pounds body weight,
and it, like the first dog, in the first experiment, showed kidney irritation,
diarrhea, and great thirst. (On humans 100 milligrams, or 1 grains, colored
the urine within 15 minutes, and this color remained fur 24 hours; there was no
sign of vomiting or diarrhea; the bitter taste of the color was noticeable.






94


COAL-TAR COLORS USED IN FOOD PRODUCTS.


UNFAVORABLE.

1. Forbidden by Confectioners' List.
2. Forbidden by Swiss Analytical chemists.
3. WEYL (p. 115): "Poisonous Orange II. * *"
4. "Betanaphthol Orange is, therefore, according to Experiment I, poisonous in
small doses when administered by the stomach, and suffices to kill an ordinarily
large strong dog." (p. 123)
5. A. Weyl's own experiments on two dogs, the initial dose in one case being 476
milligrams per kilogram body weight, or 333 grains per 100 pounds body weight;
the animal receiving in the course of 20 days, in four doses, 1,333 milligrams
per kilogram body weight, or 933 grains per 100 pounds body weight; or 335
milligrams per dose per kilogram body weight; that is, 225 grains per dose per
100 pounds body weight. The animal died, and suffered diarrhea and albumi-
nuria, and its urine was colored red throughout the entire period. B. The
second dog received hypodermically per kilogram body weight, 116 milligrams,
or 61 grains per 100 pounds body weight; its urine was colored; albuminuria,
diarrhea, loss of hair, abscesses, and loss of weight occurred. It required 36
days to recover from four doses administered during one week. C. A rabbit
received 1,333 milligrams per kilogram body weight, or 933 grains per 100
pounds body weight, and died within 12 hours. (p. 122)
6. "Of the 23 Azo colors subjected to examination only two * Orange II
produces) such effects when administered by the stomach that we can con-
sider it poisonous. With dogs the lethal dose is less than 1 gram per kilo of
the body weight of Orange II * *." (p. 147.)
7. "Further Orange II, which is poisonous * *"
8. "The poisonous qualities of Orange II."
9. "Further, in spite of the presence of the sulpho groups, colors may be poisonous,
as is shown with Orange II." (p. 148.)
10. CHLOPIN (Zts. Nahr. Genussm., 1902, v. 5, p. 241): A. A dog received 349 milli-
grams per kilogram body weight, or 244 grains per 100 pounds body weight for
the first day of experiment, which dose was repeated on the third and fourth
days; nothing untoward is noted for the first three days in the condition of the
dog; the urine was dark red but free from albumen; on the fifth and sixth days
two-thirds of the above amount was given, and on the seventh and eighth days
the original dose was given. On the fourth day the animal was frisky and had
a good appetite but was vomiting; on the fifth day vomiting stopped, but
diarrhea ensued, which diarrhea continued for one week; the weight remained
practically constant; the urine was colored throughout from dark red to orange
red and dark brown and became normal the fourth day after the last administra-
tion. B. Humans: Chlopin took 200 milligrams, or 31 grains, in a gelatin capsule
at 3 p. m.; at 4.30 p. m. the urine was colored a strong red orange; at 6 p. m.
a dryness of throat and bad taste in mouth appeared; at 6.30 p. m. felt very
badly; vertigo and unable to remain seated and continue writing; blood rushed
to head; the general condition very poor; somewhat improved by moving
about in open air; 7.30 felt so poorly took Glauber's salt as an antidote; 11 p. m.
ill condition still continuing; urine normal yellow; midnight recovered.
('hlopin states that he would not repeat this experiment on himself, or on
any other human, and he concludes therefore that this color must be regarded
as harmful.
11. CnLoPN (p. 1.33) classes it as "harmful." The experimental data are as follows:







95


COMPILED DATA UNDER GREEN TABLE NUMBERS.


Experimental data by Chlopin.
[1 gram=l16 mg=81 grains.]


I i 24-hours'
Dose. Weight. urine.


General condition of animal and urine.


Grams. Kilos.
3, 8.6
......... ..........I
3 ...........
3 .........
2 ..........
2 ........ .
3 ..........
3 8.2


cc.
3.50
340
3.50
350
325
330
350
315


.. .... 375
8. 59 ..........
...... 350


Dog is quite well; urine normal.
Urine brown red, acid; no albumen.
Do.
Diarrhea and vomiting at night, no albumen; urine orange red,
acid, no albumen.
Diarrhea continues; no albumen; no vomiting.
Diarrhea continues; dog lively, eats with relish; no albumen.
Urine brown orange, acid, no albumen; diarrhea continues.
Urine clear; no albumen: diarrhea continues.
Urine dark brown; no albumen; diarrhea decreases.
Diarrhea sti!l less:; no albumen.
Diarrhea very slight; urine slightly orange, no allbuminen.
Urine normal in color and composition; diarrhea stopped.


Total.. 19


12. Buss lists it as poisonous.
DOUBTFUL.
1. WINOOGRADOW (Zts. Nahr. Genussm., 1903, r. 6, p). 589) says it almost completely
inhibits digestion.
G. T. 87.
Trade names.-Orange III; IIelianthin; Tropteolin D; Methyl
Orange; Dimethylanilin Orange.

Scientific name.-Sodium salt of para-sulp)hobenzenc-azot-dimnet hyv-
lanilin.
Discovered.- 1876.


Shade.-Orange Yellow.


1. Permitted by the law of Italy.


Not offered.

FAVORABLE.

UNFAVORABLE.


1. CHLOPIN (pp. 145, 146) on his own experiments classes it as poisnfiu.is.
experimental data are as follows:
Experimental data by ('hlopin.
No. 1.
[1 gramn= 1'3 Tng= 114 grains.]


Weight.


24-houirs'
u-ine.


Kilos. cr.
6. 14 31it}
.......... 2"50
. ......... ;3 0
. ... ...... T305
.......... 305


. .. . .. . I. l e .
. .. .... .. .. .little.
.......... L little .
.......... L little.


General connlilion o)f aiiiii.il :n,'l irin'.


Before experiment 'lug 1iiilti noniri.LI; color uriinn IuIsal,. acidl.
no alburmen.
)Do.
rolor of urine dlark yellow; no .ulll,'iaiiu.
Urine brown; reddish with i sulphuric acidl: no alblmIen.
Do.
S )o.
D o.
Do.
Urine dark brown: no alhinmen: vuomiing.
Paresis of hind legs: dog dor,4 not val. bult Irink. with :ii!ily.
(Complete alaxia, whirli lie'cai' gel lier tilln I hie h: ol c'in Tlinot
move In straight line, anti waIlk-. in circles, andml dtrop hii' b':Il
on things and falls; afler falling arises withlli dTilllltv :n,
stands with widely spretl! feet. .ontintinziilfv liing not0w o1
then the other; extremilie's shake; on llth ,i:>y sat with h!ilt.-
culty; plUedl on his feet, maintained equillritim wit ii if-.
flhnt'ty: Involuntatrlly lifts one paw anrl Inuuves It iihout In the
air; animal cain still'swa.illow; cv"s re,,nk-,i to lighl; dtits n1,[
eat; on the 12th the hintl legs in ilrfvly parlni7NId; on Ifit
14th vomiting andi paralysis of the frt'nt legs; lie's iulh'lyv
without moving; Is killed. .Atilop'.y shtiws no change In in-
ternal organs excPpt hypirnmnin in the luintmr region of the
"spinal column (?) Imrlurlng Itwwee'n nnterlr andi littertl
colIimmni," ciausing death by piralysLs of the heart.


Total..j iD


Date.


1901.
May 27
28
29
30
31
June 1
2
3
4
5
6
8


I..........


The


Date.

1901.
Aug. 29
30
31
Sept. I
2
3
4
5
fl
A
7
8-9


Dose.

Grams.



2


*,
2
2|






96


COAL-TAR COLORS USED IN FOOD PRODUCTS.


Experimental data by Chlopin-Continued.
No. 2.
[1 gram=-149 mg=104.3 grains.]

Date.Dose. Weight ur' General condition of animal and urine.

1901. Grams. Kilos. cc.
Dec. 3 3 6.7 .......... A few hours after giving color dog in tremors; does not eat.
4 .................. Little. Urine black; acid; no albumen; paralysis of the extremities.
5 ................... Little. Dog lies in cage in full paralysis; died before dinner; no albu-
men in urine; cause of death, paralysis of heart.

2. MIEYER (J. Amer. Chem. Soc., 1907, v. 29, p. 900): Dog receiving 113 milligrams
per kilogram body weight; that is, 79 grains per 100 pounds body weight. Result,
diarrhea, which continued throughout 17 days, although only 3 doses of the
same size were given in 6 days; thereafter the dose was increased geometrically;
the diarrhea continued; the coloring matter was discharged in the urine and
the feces; there was no abnormal condition revealed by the autopsy.
DOUBTFUL.
1. WINOGRADOW (Zts. Nahr. Genussm., 1903, v. 6, p. 589) says it noticeably retards
digestive action; is not indifferent.

G. T. 88.
Trade names.-Diphenylamin Orange; Orange IV; Tropeolin 00;
Orange M; Fast Yellow; Orange G S; New Yellow; Orange N; Acid
Yellow D.
Scientific name.-Sodium salt of para-sulphobenzene-azo-diphenyl-
amin.
Discovered.- 1876.
Shade.-Orange Yellow. Not offered.

FAVORABLE.
1. WVEYL (p. 115): "Nonpoisonous * Diphenylamin Orange * *
2. * Diphenylamin Orange is * nonpoisonous." (p. 132.)
3. "For instance, the poisonous Metanil Yellow corresponds to the nonpoisonous
Diphenylamin Orange." (p. 148.)
4. The experiments on which Weyl based the conclusions above may be summarized
as follows: A. A dog received 183 milligrams per kilogram body weight, or
128 grains per 100 pounds body weight. The urine was rendered black, and
contained traces of phenol and abundant albumen; this condition lasted for
72 hours, at the end of which 110 milligrams per kilogram body weight, or
77 grains per 100 pounds body weight, were administered; urine became
colorless and albumen diminished. Five days afterwards a total of 10 grams,
or 366 milligrams per kilogram body weight, or 256 grains per 100 pounds
body weight, were administered; the urine became abundant, was strongly
black, alkaline, contained albumen. The loss of weight was 1 kilogram, or
about 3| per cent. B. A dog received 308 milligrams per kilogram, or 216 grains
per 100 pounds body weight, as the initial dose; albuminuria did not result
until after repeated dosing same as initial dose, and administered for 2 weeks.
5. Weyl's conclusions are as follows: "According to the above investigations,
Diphenylamin Orange causes albuminuria, but further disturbances did not
appear during the several weeks' observations on the animals used,"







COMPILED DATA UNDER GREEN TABLE NUMBERS. 97

6. CHLOPIN (p. 148) examined this color and classes it as nonpoisonous. The ex-
perimental data are as follows:
Experimental data by Chlopin.
[1 gram= 145 mg= 100 grains.]

Date. Dose. Weight. 24 nehours' General condition of animal and urine.
__ _____ __I________ ____

1901. Grams. Kilos. cc.
Oct. 27 3 7 300 Dog quite normal; urine color normal; no albumen.
28 ................... ...........Urine dark brown; acid; no albumen.
29 3 ........ ..... .......... D o.
30 3 ......... .......... D o.
31 3 ........... ....... Do.
Nov. 1 3 .................Urine yellow, with sulphuric acid red; no albumen.
2 3 .......... 340 Orange with orange sheen; no albumen.
3 3 6.5 .......... Do.
4 .......... .......... 275 Urine brown yellow; acid; no albumen.
5 3 ....... 300o Do.
6 .......... 6.7 .......... Do.
Total. 24

7. FRAENKEL (pp. 577,578) to the same effect as WVeyl, as above.
8. Permitted by the law of Italy.

UNFAVORABLE.

1. Prohibited by Confectioners' List.

G. T. 89.

Trade names.-Brilliant Yellow S; Yellow WR; Curcumin.
Names under which it was offered on the United States market as a
food color in 1907.-Brilliant Yellow S.
Scientific name.-Sodium salt of para-sulphobenzene-azo-diphenyl-
amin-suphonic acid.
Shade.-Yellow. Offered by 1 out of 12 sources.

FAVORABLE.

1. LIEBER (p. 136): A very young rabbit received six doses on alternate days, each
dose amounting to 320 milligrams per kilogram of body weight, or 224 grains per
100 pounds of body weight. No untoward symptoms are recorded; the body
weight increased almost 10 per cent in 11 days.

L'NFAVORABLE.
Nothing.
G. T. 92.

Trade names.-Azo Acid Yellow; Azoflavin: Azo Yellow; Indian
Yellow.
Scientific nam.e.-Mfixture of nitrate diplhenylaminii yellow with
nitro-diphenylamin.
Discovered.- 1 SSO.
Shade.-Yellow. Not offered.


97291-Bull. 147-12-- 7







98 COAL-TAR COLORS USED IN FOOD PRODUCTS.

FAVORABLE.

1. CHLOPIN (p. 128) examined this color and classifies it as nonpoisonous. The ex-
perimental data are as follows:

Experimental data by Chlopin.
No. 1.
[1 gram=125 mg=87.5 grains.]

Date. Dose. Weight. 24 hours' General condition of animal and urine.
urine.

1901. Grams. Ko. Cc.
Apr. 6 2 8 370 Dog normal; urine acid; no albumen.
8 ....... .......... Little. Urine reddish orange; acid; no albumen.
10 3 .......... .......... Do.
S 11 .................... 600 Urine red; no albumen.
12 .................... 430 Urine almost normal color; acid; no albumen.
Total. 5

Conclusion: Nonpoisonous.
No. 2 (p. 129).
[1 gram=143 mg= 100 grains.]

Date. Dose. Weight. 24 hours' General condition of animal and urine.
urine.

1901. Grams. Kilos. cC.
Apr. 12 2 7 430 Dog normal; urine acid; no albumen.
14 3 .......... 610 Do.
15 .................... 600 Urine dark yellow; acid; no albumen.
16 ................... 400 Urine almost normal color; acid; no albumen.
Total.. 6

Conclusion: Showed no harmful effects.
2. Permitted by law in Italy.
UNFAVORABLE.
Nothing.
DOUBTFUL.

1. WINOGRADOW (Zts. Nahr. Genussm., 1903, v. 6, p. 589) says it almost completely
inhibits digestion; noticeably retards digestive action; is not indifferent.

G. T. 93.

Trade name.-Azo-fuchsin G.
Scientific name.-Sodium salt o(f para-sulphobenzene-azo-dioxy-
naphthalene-sulphonic acid.
Discovered.-1889.
Shade.-Reddish brown. Not offered.

FAVORABLE.

1. CHLOPIN (pp. 126, 127) examined this color and classifies it as nonpoisonous. The
experimental data arc as follows:




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