• TABLE OF CONTENTS
HIDE
 Title Page
 Acknowledgement
 Table of Contents
 List of Tables
 List of Figures
 Abstract
 Introduction
 Literature review
 Plan of research
 Materials and procedures
 Pollution of the Floridan...
 The Gainesville water system
 Summary and conclusions
 Bibliography
 Biographical sketch














Title: Iodination of public water supplies
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Permanent Link: http://ufdc.ufl.edu/UF00098211/00001
 Material Information
Title: Iodination of public water supplies
Physical Description: xiv, 155 leaves. : illus. ; 28 cm.
Language: English
Creator: Bonner, William Paul, 1921-
Publication Date: 1967
Copyright Date: 1967
 Subjects
Subject: Water supply -- Florida -- Gainesville   ( lcsh )
Iodine   ( lcsh )
Purification -- Water   ( lcsh )
Genre: bibliography   ( marcgt )
non-fiction   ( marcgt )
 Notes
Thesis: Thesis -- University of Florida.
Bibliography: Bibliography: leaves 148-154.
General Note: Manuscript copy.
General Note: Vita.
 Record Information
Bibliographic ID: UF00098211
Volume ID: VID00001
Source Institution: University of Florida
Holding Location: University of Florida
Rights Management: All rights reserved by the source institution and holding location.
Resource Identifier: alephbibnum - 000568614
oclc - 13686661
notis - ACZ5352

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Table of Contents
    Title Page
        Page i
    Acknowledgement
        Page ii
        Page iii
    Table of Contents
        Page iv
        Page v
    List of Tables
        Page vi
        Page vii
        Page viii
        Page ix
    List of Figures
        Page x
        Page xi
    Abstract
        Page xii
        Page xiii
        Page xiv
    Introduction
        Page 1
        Page 2
        Page 3
        Page 4
    Literature review
        Page 5
        Page 6
        Page 7
        Page 8
        Page 9
        Page 10
        Page 11
        Page 12
        Page 13
        Page 14
        Page 15
    Plan of research
        Page 16
        Page 17
        Page 18
        Page 19
        Page 20
        Page 21
        Page 22
        Page 23
        Page 24
        Page 25
        Page 26
        Page 27
        Page 28
        Page 29
        Page 30
        Page 31
        Page 32
        Page 33
        Page 34
        Page 35
        Page 36
        Page 37
        Page 38
        Page 39
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        Page 41
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        Page 43
        Page 44
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        Page 46
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        Page 48
        Page 49
        Page 50
        Page 51
        Page 52
        Page 53
        Page 54
        Page 55
        Page 56
    Materials and procedures
        Page 57
        Page 58
        Page 59
        Page 60
        Page 61
        Page 62
        Page 63
        Page 64
        Page 65
        Page 66
    Pollution of the Floridan aquifer
        Page 67
        Page 68
        Page 69
        Page 70
        Page 71
        Page 72
        Page 73
        Page 74
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        Page 108
        Page 109
        Page 110
        Page 111
        Page 112
        Page 113
        Page 114
        Page 115
        Page 116
        Page 117
    The Gainesville water system
        Page 118
        Page 119
        Page 120
        Page 121
        Page 122
        Page 123
        Page 124
        Page 125
        Page 126
        Page 127
        Page 128
        Page 129
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        Page 131
        Page 132
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        Page 135
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        Page 137
        Page 138
        Page 139
        Page 140
        Page 141
        Page 142
        Page 143
        Page 144
    Summary and conclusions
        Page 145
        Page 146
        Page 147
    Bibliography
        Page 148
        Page 149
        Page 150
        Page 151
        Page 152
        Page 153
        Page 154
    Biographical sketch
        Page 155
        Page 156
        Page 157
Full Text










IODINATION OF PUBLIC WATER SUPPLIES











By

WILLIAM PAUL BONNER


A DISSERTATION PRESENTED TO THE GRADUATE COUNCIL OF
THE UNIVERSITY OF FLORIDA
IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE
DEGREE OF DOCTOR OF PHILOSOPHY











UNIVERSITY OF FLORIDA
June, 1967










ACKNOWLEDEGMNTS


I would like to express my sincere appreciation to Dr. A. P.

Black, my committee chairman, who provided the guidance, assistance

and inspiration which were required to complete this dissertation. His

competent teaching and advice have been most valuable in training me for

my profession; likewise, his expression of enthusiasm toward life and

work hae provided an excellent example which I shall try to follow.

The contributions made by others who served on my committee, namely,

Dr. H. A. Bevis, co-chairman, Professor J. E. Kiker, Jr., and Dr. B. G.

Dunavant are also gratefully acknowledged.

I am indebted to R. P. Vogh, J. B. Warrington, J. J. Smith, Jr.,

Margaret Whittle, G. P. Whittle, Michael Keirn, Patricia Green and

others for rendering valuable assistance in carrying out this work. My

thanks to Mrs. Janice Larson for her fine help during the performance

of this work and for typing the final manuscript.

Appreciation is extended to my wife, Marjorie, who, as she always

has in our life, helped and encouraged me in this work. Her patience

and understanding while providing a home in the absence of a husband

and the inspiration of my two sons through cheerful greetings and

wanting a father at home are also greatly appreciated.

To Union Carbide Corporation, Nuclear Division, for making this

study possible by granting me a leave of absence, and to Mr. E. G.

Struxness, Drs. T. Tamura and F. L. Parker of Oak Ridge National








Laboratory, for their guidance and encouragement, sincere appreciation

is extended.

Many thanks go to my parents and relatives who have helped in

every way possible to provide the opportunity of attending college and

easing the financial strain. Financial support is also acknowledged

through a traineeship from the United States Public Health Service under

Training Grant No. 2T1RH3-06(66), and support of the project through

Demonstration Grant WPD-19-04-66 awarded by the Federal Water Pollution

Control Administration of the Department of the Interior.










CONTENTS


Page

ACKNOWLEDGMENTS . . . . . . . . . . . . ii

LIST OF TABLES . . . . . . . . . . . . vi

LIST OF FIGURES .................. ..... x

ABSTRACT. .. . . . . . . . . . . . . xii

CHAPTER

I. INTRODUCTION . . . . . . . . . .. 1

II. LITERATURE REVIEW . . . . . . . . . 5

Iodine . . . . . . . . . . . 5
Historical . ... . . . . . 5
Formation of Iodates .. . . . . . 6
Chemistry of Iodine in Dilute Aqueous Solutions 7
The Iodide Content of Natural Waters . . . 7
Pollution of Ground Water from Surface Sources 10
Indicators of Pollution . . . . . 11

III. PLAN OF RESEARCH . . . . . . . . . 16

Preliminary Work at Marietta, Ohio . . . 16
Description of Problem . . . .. . 16
Source of Water . . . . . . . .. 16
Water Treatment . . . . . . . 17
Laboratory Studies . . . . ........ 17
Studies Conducted at Marietta, Ohio . . . 24
Possible Pollutants . . . . . . . 34
Summary and Conclusions . . . . .. 34

Gainesville Study . . ... . . . . .. 36
Floridan Aquifer . . . . . . . 36
Piesometrio Surface and Flow of Ground Water . 39
Pollution of Aquifer. . . . . ... 41
Selection of Sample Points . . . . 49
Description of Water Treatment Facilities and
Distribution System . . . . . . 53
Methods of Iodination . . . . . 54








Page

IV. MATERIALS A!D PROCEDURES . . . . . . . 57

V. POLLUTION OF THE FLORIDAN AQUIFER . . . . . 67

Introduction . . . . . . . . . 67
Discussion of Results . . . . . . . 67
Corollary Studies at Lowell, Florida . . . 105
Summary . . . . .. . . . . . 117

VI. THE GAINESVILLE WATER SYSTEM . . . . . . . 118

Introduction . . . . . . . . . 118
Change in the Bacteriological Quality of Water
from the Well to the Consumer . . . . 118
Laboratory Studies . . . . . . ... 127
Detention Time of the Distribution System . . 138
lodination of the Gainesville Water Supply . . 140

VII. SUMMARY AND CONCLUSIONS . . . . .. . 145

BIBLIOGRAPHY . . . . . . . . . . . . . 148

BIOGRAPHICAL SKETCH . . . . . . . . . . ... 155









LIST OF TABLES


Table Page

1. Iodine Content of Water from Four of the Great Lakes . 8

2. Iodine Content of Water from Some United States Rivers . 9

3. Iodine Content of Water from Some Pennsylvania Wells . 10

4. Chemical Analysis of Plant Water Supply, Union Carbide
Corporation, Metals Division, Marietta, Ohio, June 4, 1965 18

5. Taste Test No. I. Averaged Preferences of Nine
Observers . . . . . . . . . . . . 20

6. Taste Test No. I. Individual Preferences of Nine
Observers for Waters of Table 5 . . . . . . 20

7. Taste Test No. II. Averaged Preferences of Eight
Observers . . .. .. . . . . . . . 21

8. Taste Test No. II. Individual Preferences of Eight
Observers for Waters of Table 7. . . . . . . 22

9. Comparison of Taste Produced by Chlorine and Iodine in
Marietta, Ohio Well Water Containing .05 ppm Phenol . 23

10. Comparison of Taste Produced by Chlorine and Iodine in
Marietta, Ohiq Well Water Containing 2.0 ppm Phenol . 24

11. Taste and Odor of Raw Water . . . . . . . 26

12. I1, HIO, and Cl2 Residuals in Raw Water . . . . 28

13. Taste of Aerated Samples Treated with C12, 12 and HIO . 30

14. Observed and Calculated Oxygen Demands of Several Waters 30

15. Calculated and Observed Halogen Demands of Water from
Five Wells at Marietta, Ohio. . . . . . . . 32

16. Level of Water in the Upper and Lower Strata of the
Floridan Aquifer. Well No. 6, City of Gainesville . . 42

17. Characteristics of Wells from Which Water for the City
of Gainesville Is Obtained . . . . . . . 43







Table Page
18. Chemical Characteristics of Water from Wells in the
City Well Field, March, 1967 . . . .. . . 44

19. Drainage Wells at West End of Lake Alice . . . . 46

20. Characteristics of Three Wells Owned by the University
of Florida ........................ 49

21. Location of Sample Points . . . . . . . . 50

22. Pertinent Data Relative to Sampling Points . . . .. 52
23. Analytical Data Sheet . . ... . . . . 58

24. Nitrate-N Content of Water Within the Gainesville
Area (ppm as N) . . . . . . . . . ... 69

25. Free Ammonia-N in Water Within the Gainesville
Area (ppm as N) . . . . . . . . ... 71
26. Organic Ammonia-N in Water Within the Gainesville
Area (ppm as N) . . . . . . . . . . 73

27. Nitrite-N Content of Water Within the Gainesville
Area (ppm as N) . . . . . . . . . . 75
28. COD of Water Within the Gainesville Area (ppm) . . . 78

29. Total Phosphate in Water Within the Gainesville
Area (ppm as PO) . . . . . . . . . . 80

30. Chloride in Water Within the Gainesville Area (ppm) . 83

31. Chlorine Demand of Water in the Gainesville Area (ppm) . 86
32. Iodine Demand of Water in the Gainesville Area (ppm) . 88

33. Carbon Chloroform Extractables in Water Within the
Gainesville Area (ppb) . . . . .. .. . 90
34. Carbon Alcohol Extractables in Water Within the
Gainesville Area (ppb) . . . . . .. . . 91

35. Coliforms in Water Within the Gainesville Area
coliformss per 100 ml) . . .. . . . 94

36. Standard Plate Count for Water Within the Gainesville
Area (colonies per ml) . .. .. -. . . . 95







Table Page

37. Color of Water in the Gainesville Area (units) . . . 97
38. Iodide Content of Water in the Gainesville Area (ppb) . 99

39. Iodide Content of Water from Wells in the City's Well
Field, March 22, 1967 . . . . . . . . . 101

40. Characteristics of Three Sources of Water in the
Ocala Area . . . . . . . . . . . .. 102

41. Chemical Characteristics of Water from the Ocala Area .. 103

42. Total Hardness of Water in the Gainesville Area
(ppm as CaCO3) .. . . . . . . . . . 107
43. Total Alkalinity of Water in the Gainesville Area
(ppm as CaCO 3) . . . . . . . . . . . 109

44. The pH of Water in the Gainesville Area . . . . 111

45. Hydrogen Sulfide in Water in the Gainesville Area (ppm) 112

46. 131I Content of Well Water from Well No. 2, Girls'
School, Lowell, Florida . . . . . . . . 116

47. Location of Sample Points in the Water Treatment Plant . 119

48. Changes in Bacteriological Quality, pH and Chlorine
Residual as Water Passes Through the Water Treatment
Plant, 3 to 5 AM, Nov. 29, 1966 . . . . . 121

49. Changes in Bacteriological Quality, pH and Chlorine
Residual as Water Passes Through the Water Treatment
Plant, 5 to 6 AM, Nov. 29, 1966 . . . ... . . 122

50. Changes in Bacteriological Quality, pH and Chlorine
Residual as Water Passes Through the Water Treatment
Plant, 3 to 4 AM, Dec. 20, 1966 . . . . . . 123

51. Changes in Bacteriological Quality, pH and Chlorine
Residual as Water Passes Through the Water Treatment
Plant, 4 to 5 AM, Dec. 20, 1966 . . . . .... 124

52. Sampling Points in Distribution System for
Bacteriological Analyses . . . . . . . . 125

33. Coliform and Standard Plate Count in the Distribution
System During a Period of Chlorination . . . . . 126


viii








Table Page

54. Concentration of Iodide and lodate irn Iodinated Water . 131

55. Halogen Residuals in Water Collected from the
Distribution System During the Period of lodination . . 143









LIST OF FIGURES

Figures Page

1. Foaming at the Water Treatment Plant Due to Pollution
of City Wells . . . . . . . . . . 12

2. Iodine Demands of Marietta, Ohio Well Water After
Several Days Standing . . . . . . . . 25

3. Immediate Chlorine and Iodine Demands of Marietta,
Ohio, Well Water, Oct. 7, 1966 .. . . . . . 33

4. Summary of Information From Water Supply Well No. 4,
City of Gainesville, Florida, September, 1965 . . . 38

5. Contours of the Piesometric Surface in the Top Part of
the Floridan Aquifer and Relative Location of Sample
Points .. . . . . . . . . . . 40

6. Relative Location of Sample Points . . . . . 51

7. Removal of H2S From Water with Copper Turings . . 62

8. Removal of H2S From Water with Copper Wire . . 63

9. Nitrate-N Content of Water Within the Gainesville
Area (ppm as N) . . . . . . . 68

10. Free Ammonia-N in Water Within the Gainesville
Area (ppm as N) ............. . . ... 70

11. Organic Ammonia-N in Water Within the Gainesville
Area (ppm as N) ... . . . . . . .. . 72

12. Nitrite-N Content of Water Within the Gainesville
Area (ppm as N) . . . . . . . . . 7. 4

13. COD of Water Within the Gainesville Area (ppm) . 77

14. Total Phosphate in Water Within the Gainesville
Area (ppa as PO0) . . . . . . . . . 81

15. Chloride in Water Within the Gainesville Area (ppm) . 82








Figure Page

16. Chlorine Demand of Water Within the Gainesville
Area (ppm) . . . .. . 85

17. Iodine Demand of Water Within the Gainesville Area (ppm) 87

18. Coliform and Standard Plate Count for Water Within
the Gainesville Area . . . . . . . . 93

19. Color of Water Within the Gainesville Area (units) . 96

20. Iodide Content of Water Within the Gainesville Area (ppb) 100

21. Diagrammatic West to East Cross-Section Indicating
Possible Path of Pollution . . . . . . . 104

22. Total Hardness of Water Within the Gainesville
Area (ppm as CaCO3) . . . . . . . . 106

23. Total Alkalinity of Water Within the Gainesville
Area (ppa as CaCO3, P alkalinity = 0) . . . 108

24. The pH of Water Within the Gainesville Area (units) . 110

25. Rainfall During the Period of Investigation . . . 113

26. 131I in Water From Well No. 2 (Girls'School,
Lowell, Fla.). . . . . . . . . . . 115

27. Persistence of HIO and Chloramine in the Removed Pipe 129

28. Persistence of HIO and Chloramine in the Removed Pipe 130

29. Persistence of Halogen Residuals in Gainesville Tap
Water Stored in Glass Containers . . . . . ... 132

30. Persistence of Chloramine Without KI . . . . . 133

31. Persistence of Halogen Residuals in the Newer Pipe . 135

32. Persistence of Halogen Residuals in the Older Pipe . 136

33. Iodine Demand of Dechlorinated Gainesville Tap Water . 137
34. Detention Time (hrs.) Non-Carb Hardness Tracer . . 139

35. Iodine Residuals 24 hrs. After KI First Added . . 142








Abstract of Dissertation Presented to the Graduate Council in
Partial Fulfillment of the Requirements for the Degree of
Doctor of Philosophy


IODINATION OF PUBLIC WATER SUPPLIES

By

William Paul Bonner

June, 1967

Chairman: Dr. A. P. Black
Major Department: Bioenvironmental Engineering

A comprehensive sampling program which included both- surface and

ground water was conducted to show the extent to which the Floridan

Aquifer is receiving pollutants from surface sources on the periphery

of the City of Gainesville. The primary routes by which pollutants

enter the ground near the city are Alachua Sink and two drainage wells

near the west end of Lake Alice. Each is located about three miles

from the city's well field, Alachua Sink to'the south and Lake Alice to

the west.

Both chemical and bacteriological determinations show that pollu-

tants of sewage origin are present in wells comprising the city's well

field. The presence of iodides in water from Lake Alice provided a

unique tracer to show that water entering the ground through the two

shallow drainage wells travels east past wells owned by the University

of Florida and into the city's well field. The highly colored water

which is entering the ground through Alachua Sink is believed to be

traveling northward in the upper stratum of the aquifer into the

shallower wells in the city's well field.








After successful studies at three state correctional institutions

at Lowell, Florida, had shown iodine to be an effective and desirable

disinfectant for water, its use in other systems was investigated. The

iodination of a private water supply at Marietta, Ohio, provided valu-

able background data by showing that a low HIO residual could be main-

tained in the presence of high concentrations of ammonia and other

industrial pollutants.

The size of the Gainesville water system as well as the polluted

water which serves as its source of supply made the Gainesville system

a desirable one on which to conduct further studies. Laboratory studies

using pipe which were removed from the distribution system showed that

a low HIO residual could be maintained in the presence of chloramine,

tubercules, scale and organic matter. Both taste and odor slowly

developed,with at least 48 hours required before either became objection-

able.

The detention time of water within the distribution system was

determined to be less than 48 hours except for a few areas served by

dead-end mains.

Iodination of the supply for a brief period was accomplished by

adding iodine as the iodide ion to the chloramine residual leaving the

treatment plant. Maximum use of the iodine was obtained through reoxi-

dation of the iodide ion by obhloramines as the water passed through the

distribution system.

Iodination of the supply was terminated 12 hours later due to

the presence of an objectionable taste and odor in the water which had


xiii








not been predicted by laboratory studies.

Present laboratory studies are centered around elucidating the

agent or agents responsible for the taste and odor.










I. INTRODUCTION


Water, our most indispensable natural resource, has long been

looked upon as a symbol of purity and health. However, the installation

of the first municipal water supply system in the mid-1800's witnessed

an increase in the incidence of gastrointestinal diseases, and typhoid

fever took its share of victims. The use of polluted water sources for

such systems accelerated the cycle of enteric pathogens from man to

water to man.1 This paradoxical situation, however, served to call

attention to the part played by public water supply systems in either

disseminating or protecting against water-borne diseases.

Since the late 1800's, much progress has been made in water

treatment in America. America's first municipal filtration plant was

built in 1872. The turn of the century witnessed the development of

the American rapid sand filter as a substitute for the older English

slow sand filter. Lime-soda softening was first used in 1908. In the

same year bleaching powder was first used in this country for continuous

chlorination, and in 1910 liquid chlorine was introduced as a disin-

fectant for water.

A combination of these events and an understanding of the mode

of infection has reduced the death rate due to typhoid fever from 59 per

100,000 in 1881-1885 to less than 0.1 per 100,000 today. Outbreaks of

other gastrointestinal diseases caused by enteric pathogenic bacteria

have decreased. Of all of these factors, however, continuous


- 1 -








- 2 -


chlorination has probably been the most important single factor in

dramatically reducing the incidence of water-borne diseases. Its use

for water disinfection is without question one of man's greatest

advances in the field of preventive public health.1'2

In addition to numerous strains of bacteria, over 100 different

viruses are known to be excreted with feces by man.2'3,''5 Since

viruses are found in human waste, they, like bacteria become water-borne,

spread through water systems and have been known to cause disease.6

Berg recently reported that at least six viruses have been isolated

from four different areas of the water distribution system of Paris,

France. The outbreak of infectious hepatitis in New Delhi, India, in

1955 is a classic example of a water-borne enteric virus outbreak occur-

ring when the treated water met accepted standards of bacterial quality.8

Recently, evidence has accumulated to indicate that chlorine is

not the ideal disinfectant for water.9 As pointed out in the Gross

Report9 to the Surgeon General, chlorine is ineffective against certain

microorganisms in the concentrations normally used for the disinfection

of public water supplies. Nematodes, slime bacteria, certain viruses and

cysts of Entauoeba histolytiea, some of which are pathogenic, are known

to be somewhat resistant to chlorine in low concentrations. Further

drawbacks to the use of chlorine include its decreasing bactericidal

effectiveness with increasing pH values, its reactions with ammonia and

its high chemical reactivity, which makes it difficult to maintain

stable residuals and frequently results in the formation of tastes and

odors when certain impurities are present.








- 3-


Some authors 910911 have suggested that a reassessment of the

sense of security concerning accepted water treatment practices is

needed. Specifically, the present methods of disinfection warrant

research effort. At the present time, the best defense against an out-

break of water-borne disease is the presence of sufficient effective

disinfectant in the water to insure that it is safe to drink.12

Since 1953, iodine has been recognized as a potential disinfec-

tant for water.13 Iodine may be the preferred disinfectant in situa-

tions where chlorine is relatively less effective, namely, for waters

whose pH is above pH 8.0 and for waters containing high concentrations

of organic material and/or ammonium compounds. By virtue of the fact

that iodine is a fast-acting viricide and has advantages in areas where

chlorine has disadvantages, it has been suggested that under field con-

ditions iodine may be the better disinfectant.11

Iodine has been shown to be effective as a disinfectant for swim-

ming pool water, for emergency water supplies, and for public water

supplies.13'14'15 Studies carried out in conjunction with the iodina-

tion of the water supply at three state institutions at Lowell, Florida,

have shown no adverse physiological effects on a human population as a

result of drinking iodinated water.

The next logical step in the development of iodine for use in

public water supplies is to demonstrate that iodine can be used in a

large and more highly polluted water supply. The water supply for the

city of Gainesville, Florida, meets these requirements and has been

selected for the present study. This study was designed and initiated








-4-


to accomplish the following objectives:

1. Determine the extent and magnitude of organic pollution in

the Gainesville area by evaluating:

(a) The bacteriological quality of local surface and ground

waters.

(b) The presence and amount of organic pollutants in area

well water.

(c) The recycle of iodide from the distribution system back

into area wells by observing the change in base-line

iodide levels resulting from the use of iodine for dis-

infecting the water of the University of Florida swimming

pool for the past three years.

2. The addition of iodine to the treated water of the City of

Gainesville in order to determine:

(a) The persistence of 12 or HIO residuals throughout the

system.

(b) The rate of buildup, if any, of iodates in the distribu-

tion system.

(c) Any change in bacteriological quality of water in the

distribution system.

While stable iodine was used in this study, it should be remembered

that radioactive iodine would be expected to take the same route should

it enter the cycle of water from any source.

The data and conclusions derived from both the applied and labora-

tory studies are presented and described in the following pages.










II. LITERATURE REVIEW


Historical

A brief look at a time table of events quickly reveals the extent

to which the importance of iodine has been recognized. For example:

1811 Discovered by Bernard Courtoit.16

1816 First used in the treatment of goiter by Proust.17

1833 Iodized salt recommended by Baussengault for goiter

prevention.17

1839 Tincture of iodine used for the treatment of wounds by

Davies.18
19
1867 Used for treatment of gonorrhea by Watson.

1873 Davaine demonstrated the sporicidal activity of iodine.20

1915 Used for the disinfection of drinking water.

1922 1967 During this period more than 30 technical papers

were published on the use of iodine for water disinfection.

A few of the more important papers are briefly summarized.

Iodine as a disinfectant for drinking water. Chang and Morri13'

in 1953, reported that elemental iodine is a suitable agent for the

emergency disinfection of water supplies. Their work showed iodine to

be effective against most types of pathogenic organisms within a reason-

able time at a concentration of a few parts per million.


-5-








-6-


In the same year, Morris, Chang, Fair, and Conant22 reported

that several iodine-releasing compounds were suitable for field use in

disinfecting water with iodine. Their studies were primarily responsible

for its adoption by the military for the disinfection of canteen water in

the field.22

Later, studies conducted at Lowell, Florida, contributed much to

the present knowledge of iodine as a disinfectant for water supplies.14

The studies have demonstrated that the consumption of iodinated water by

the inmates of three state institutions over a period of more than three

years has had no detrimental effect on general health or thyroid

function. 1423 Iodine was also shown to be as effective as chlorine as

a bactericide.

In a very recent publication, Berg shows that iodine is an

effective viricide and suggests that under field conditions it could be

a better disinfectant than chlorine.

Iodine as a disinfectant for swimming pool water. Swimming pool

studies likewise have shown iodine to be an effective disinfectant with

few disadvantages and many desirable qualities which chlorine does not

possess.15,24,25,26

Formation of Iodates

Wyss and Strandskov2 found that in buffered solutions and at

relatively high pH values HIO is rapidly converted to iodate. Chang2

showed that the iodate ion had no disinfecting ability. These findings

raised serious questions concerning the possibility of maintaining stable

residuals throughout distribution systems carrying water of high pH values.







-7-


However, the high concentrations of iodine used in the iodate studies

cast some doubt on the results which might be obtained if lower concen-

trations were used.

Subsequent laboratory studies conducted by Black, Kinman, Thomas,

Freund, and Bird14 showed that in a potable water environment iodate

formation at pH values as high as pH 9.0 is not significant. When 1.0

ppm iodine was used the maximum concentration of iodate ion found over

periods of from 4 to 17 days was 0.05 ppm.

Jabero29 showed that iodate formation was not significant at pH

9.0 in a small distribution system.

Chemistry of Iodine in Dilute Aqueous Solutions

The chemistry of iodine in dilute aqueous solutions as it applies

to a potable water environment has been fully discussed by Chang,8 who

points out that there are important differences between the behavior of

chlorine and iodine which would be expected to markedly alter- their

effectiveness as sanitizing agents.

The Iodide Content of Natural Waters

Available data show that the concentration of iodide in natural

waters in the United States varies widely. Tables 1, 2, and 330'31 give

the concentration of iodine found in the waters of certain lakes, rivers

and wells in the United States. These data show that although iodine is

widespread in nature, its concentration in most waters is extremely low.

Because of the low concentrations of iodine found in most fresh

water sources and the prevalence of endemic goiter, this country wit-

nessed the first trials of the addition of iodine to public water supplies







-8-


Table 1

Iodine Content of Water from Four of the Great Lakes30


Lake Iodine (ppb)


Lake Superior at Duluth, Minn. 0.01

Lake Superior at Marquette, Mich. 0.02

Lake Michigan at Milwaukee, ias. 0.015

Lake Michigan at Winnetka, Ill. 0.10

Lake Michigan at Chicago, Ill. 0.12

Lake Erie at Cleveland, Ohio 0.86

Lake Ontario at Toronto, Canada 1.45

Average 0.37



for the prevention of that disease during the 1920's. Supplies at

Rochester, N. L., Anaconda, Mont., Sault Ste. Marie, Mich., and Virginia,

Minn. were iodized by the addition of low concentration of sodium iodide

to the water for a short interval of time prior to the general accep-

tance of iodized salt.32'33'34

lodination of water supplies is not new. Only the form of iodine

and the. purpose of addition has changed.

Although the concentration of iodide in surface waters and most

ground waters is only a few parts per billion, some natural brines con-

tain iodides in concentrations ranging from three to 65 ppm.35 By









- 9 -


Table 2

Iodine Content of Water from Some United States Rivers30


River Iodine (ppb)

Mississippi River at Minneapolis, Minn. 0.88

Mississippi River at St. Paul, Minn. 0.83

Mississippi River at St. Louis, Mo. 3.52

Mississippi River at New Orleans, La. 7.70

Me.ssouri River at Kansas City, Mo. 1.69

South Platte River at Denver, Colo. 0.77

Scioto River at Columbus, Ohio 0.21

Cumberland River at Nashville, Tenn. 0*22

Susquehanna River at Harrisburg, Pa. 0.23

James River at Richmond, Va. 0,60

Potomac River at Washington, D. C. 0.72

Oconee River at Atlanta, Ga. 3.20

Average 1.71



recovering the iodide these sources could provide an almost inexhaustible

supply of iodine should the demand for iodine warrant the exploitation

of this vast source.







- 10 -


Table 3

Iodine Content of Water from Some Pennsylvania Wells31


City Iodine (ppb)


Allentown 2.4

Bethlehem 2.5

Warren State Hospital 2.5

NMcees Boaks 1.0

Meadville 1.7

Beaver 0.0

Alliquippa 0.3

Average 1.5



Pollution of Ground Water from Surface Sources

While the presence of pollutants in streams may be readily

noticeable, pollutants may also exist in ground water and present an

equally great hazard to the health of its users. The Broad Street Well

in London, 1854, is an historic example of ground water pollution and

its role in the spread of disease.36 An early example of the pollution

of well water as evidenced by the presence of detergents occurred in 1958

on Long Island.37 Many other cases were soon reported. 3839,0,41,l42

In areas underlain by limestone aquifers short circuiting is

frequently encountered through numerous channels, sink holes or even







- 11 -


caverns resulting from the solvent action of surface water containing

carbon dioxide on the underlying limestones. This is called "Karst" or

solution-type topography. In such areas the physical, chemical, and

bacteriological quality of ground water is variable, fluctuating with

rainfall and waste disposal practices in the area. 3

A series of typhoid outbreaks in southeast Minnesota between 1939

and 1943 were shown to be due to pollution entering porous limestone

strata from surface sources.

The gastroenteritis epidemic at Riverside, California, in May,

1965, reportedly affected 18,000 out of a population of approximately

130,000. Although a great many questions relative to the epidemic remain

unsolved, contaminated water from a well which had been known to show

evidence of surface contamination is suspected as being the cause of the

outbreak.45

In the City of Gainesville, Florida, ground water pollution has

become evident. In January, 1964, the presence of detergents in the

well water caused foam to build up as high as nine feet over the re-

carbonation basin as shown-in Figure 1. 6 A thorough discussion of the

pollution problem which exists in the Gainesville area will be pre-

sented later in this work.
Indicators of Pollution

ABS and LAS. Alkyl benzene sulfonate (ABS), the primary surface

active agent used in detergents for many years, is not a substance which

naturally occurs in nature. Since it is widely used as a household

detergent its presence in water is thus an indication of pollution by


















'i.
10 a~iiw
Now .^


-S.


Fig. 1 FOAMING AT THE WATER TREATMENT PLANT
DUE TO POLLUTION OF CITY WELLS


-12-


I:


'S











11r'








- 13 -


sewage or other man-made wastes.41,47

The replacement of the original branched chain nonbiodegradable

detergents (ABS) with the newer straight chain and more biodegradable

materials (LAS) has reduced the problem of pollution by detergents to

a considerable extent. 49 However, along with the elimination of

complaints due to the presence of detergents in water has gone a

valuable indicator for the presence of sewage pollution.

Phosphates. Closely associated with the presence of ABS or LAS

in domestic wastes is the presence of phosphates. Phosphates are used

in detergents as "builders" and are usually added in the form of sodium

tripolyphosphate, sodium hexametaphosphate, tribasid sodium phosphate,

or tetra sodium pyrophosphate.42,50 Collectively, these forms of phos-

phate are called polyphosphates.

Apparently, a combination of biological action and hydrolysis is

responsible for the degradation of polyphosphates through sewage treat-

ment. Engelbrecht and Morgan51 report that 90 percent of the phosphate

present in the sewage effluent is already in the orthophosphate form.

Polyphosphates are likewise subject to hydrolytic degradation in natural

waters, the rate of reversion varying with the different chemical and

physical characteristics of the water.51

As an indicator, the presence of polyphosphates is associated

with fairly recent sewage pollution. Orthophosphates on the other hand

may indicate the presence of pollution from either domestic waste or

drainage from agricultural land.51 It is important, therefore, to con-

sider the results of other chemical analyses and a survey of the drainage








- 14 -


area in evaluating the source of phosphates in water.

Carbon-chloroform extract (CCE) and carbon-alcohol extract (CAE).52

The absorptive power of activated carbon has long been know .53 Through

the years it has found many applications in industry as a deodorizer and

decolorizing agent.5 Its remarkable ability to absorb organic from

water is the basis for two determinations known as "carbon-chloroobrm

extract" or CCE and "carbon-alcohol extract" or CAE.

By running several thousand gallons of water through a bed of

activated carbon a sufficient quantity of the organic material can be

recovered by drying and then extracting first with chloroform and then

with ethyl alcohol.55'56 Its use as a quantitative measure of pollution,

however, is unjustified since recoveries from the chloroform extraction

are reported to range from only 50 to 90 percent, and ethyl alcohol

extraction from 20 to 30 percent.57 58'59'60

One of the most significant contributions which CCE and CAE deter-

minations can make as indicators of pollution is their use as a monitor

to determine undue stress on a stream from pollutants arising from indus-

trial or domestic sources. By determining both CCE and CAE it is possible

to determine the relative quantities of different types of pollutants.

Organic pollutants arising from the various chemical manufacturing indus-

tries, as well as petroleum-based pollutants, are mainly recovered in the

chloroform extract. The alcohol extract contains detergents, as well as

materials originating from algal activity, organic matter in soil, decay

of vegetation, decomposition of sewage and other natural sources.52,58961

Field studies have shown that where the primary pollutants are











- 15 -


from chemical industries, the CCE exceeds the CAE, and when sewage is the

predominant pollutant, the CAB exceeds the CCE by a factor of from four

to six.52.57.58s61

Together, CCE and CAB values are a valuable index for determining

the relative organic content of water and the relative quantities of

different types of pollutants. Where concentrations of 200 ppb have been

found, the taste and odor of the water are usually poor.62

The sampling program of the national water quality network has

provided valuable information regarding the quality of finished waters in

the United States and Puerto Rico. Much of the earlier data which have

been obtained have been recently published by Taylor. 63 Of 172 water

supplies checked, only two values for CCE were greater than the 200 ppb

limit set by the 1962 Drinking Water Standards. The mean was deter-

mined to be 66 ppb with the range extending from 7 to 267 ppb.

Organic color. Gainesville, Florida, is located within a 300-

square-mile area in the southwest section of Alachua County which has no

surface outflow. 65 The few small streams in the area terminate in sink

holes and most rainfall leaves as underground flow. Most lakes and

streams in the area contain waters with high organic color; thus, the

presence of high organic color in ground waters indicates the possibility

of local surface water pollution.










III. PLAN OF RESEARCH


Preliminary Work at Marietta. Ohio

Description of Problem

In response to a request from the Mine and Metals Division of the

Union Carbide Corporation at Marietta, Ohio, an investigation of their

plant water supply was made to determine the feasibility of disinfecting

it with iodine. The water was believed to contain phenol since chlorina-

tion was producing highly objectionable tastes and odors. Since it has

been shown that no odor or taste is produced by phenols in the presence

of iodine in low concentrations and in view of the highly successful

studies at Lowell, Florida, it was felt that iodination of the supply

might solve the problem. A request for permission to iodinate the

supply was approved by the Ohio Department of Health.

Source of Water

The water supply is derived from four wells penetrating an un-

consolidated glacial formation. Recharge of the aquifer is primarily

from local rainfall and from the Ohio River which flows from 125 to 600

feet from the four wells. A comparison of the water level in the wells

and the observed water level in the Ohio River indicates that the two

levels are approximately the same, and from the nature of the formation

it is suspected that the ground water level in the aquifer rises and

falls with the level of water in the river.


- 16 -








- 17 -


Water Treatment

Water usage averagesapproximately 1.4 agd. Present equipment

permits a maximum pumping rate of 1500 gpm with a 75,000 gallon elevated

storage tank floating on the system to meet peak demands. The only

treatment consists of the addition of approximately four ppm of chlorine

in the form of gaseous chlorine.

Laboratory Studies

Analysis of water. Chemical analyses of the water from two of

the four wells and of a composite sample from all wells were available

from Hall Laboratories in Pittsburgh, Pa. These data are shown in

Table 4. Phenol was found in one of the samples, which indicated that

ohlorophenole might be the source of the observed tastes and odors.

While the concentration of ammonia reported seemed unreasonably high

for a potable water, its effect on taste and odor should obviously be

included in any evaluation.

Methods. A series of laboratory experiments were run in order

to compare the action of both chlorine and iodine on synthetic waters

containing known amounts of ammonia and phenol.

Water for use in evaluating each variable was prepared from

demineralized water by passing it through a column of activated carbon

to remove all taste and odor. Reagents added to the water were ACS

reagent grade with stock solutions and subsequent dilutions prepared

from taste-free water. All stock solutions and dilutions were prepared

immediately prior to use.





- 18 -


Table 4
Chemical Analysis of Plant Water Supply
Union Carbide Corporation, Metals Division
Marietta, Ohio June 4, 1965


Well No. 2 Well No. 6 Tap in Lab

pH value 25C 7.2 7.2 7.0
Bicarbonate (HCO3) 267 206 224
Sulfate (30S) 485 275 355
Chloride (Cl) 146 94 123
Nitrate (NO3) 25 < 5 15
Silica (Si02) 16 12 14
Phenol < 0.005 < 0.005 0.015
Hardness (as CaCO,) 740 480 600
Calcium (Ca) 236 149 184
Magnesium (Mg) 37 26 34
Iron (Fe) < 0.05 0.15 < 0.05
Manganese (Mn) 0.25 2.3 0.8
Sodium (Na) 82 54 68
Chromate < 0.1 < 0.1 0.1
COD 3.6 3.0 2.7
Cr3 Chromate 0.1 0.1 0.1
Potassium 11 4.4 7.6
Syndet 0.1 0.1 0.1

Suspended Solids (eat) < 5 < 5 < 5

Ammonia (NH3) 22 3 13








- 19 -


Taste and odor. The tests were conducted by selecting a taste

panel and letting each member taste the water without knowing its con-

tents. To prevent tiring of the members' taste buds the tests were con-

ducted in two parts. Test I was designed to determine the preference of

panel members for water containing phenol and treated with chlorine; with

iodine released from KI by chloramine; and with iodine released from KI

by chlorine (HOC1). Test II was designed to determine the preference of

panel members for waters containing phenol and treated with chlorine,

chloramine, elemental iodine, and elemental iodine plus ammonia. In each

test taste-free water was used as a control. The results of these tests

are tabulated in Tables 5, 6, 7, and 8.

These data suggest that:

1. There is a definite preference for iodinated over chlorinated

water when phenol is present.

2. Taste is slightly enhanced when chlorine is used to oxidise

I" to HIO in the presence of ammonia and phenol.

3. Iodination using elemental iodine is preferred over iodina-

tion using potassium iodide plus chlorine.

Marietta. Ohio well water. Samples of water which were shipped

from Marietta, Ohio, were used in laboratory tests to determine whether

iodinating the water would produce an objectionable taste. Since phenol

is unstable in water57 and since the water was en route four days, it

was assumed that all phenol was gone. Therefore, phenol was added to

the samples immediately prior to adding other reagents used in the test.

Taste tests using 50 ppb phenol were conducted to determine the







- 20 -


Taste Test No. I.


Table 5
Averaged Preferences of Nine Observers


Materials added to taste-free
denineralized water ppm
Sample Preference Order of
No* No. (Avg) Preference Phenol Ammonia Iodide Chlorine

1 3.1 2 .01 0 1.0 .224
2 3.67 4 .01 .1 1.0 .224

3 3.13 3 .001 0 0 .224
4 3.89 5 .01 0 0 .224

5 1.67 1 0 0 0 0



Table 6
Taste Test No. I. Individual Preferences of Nine
Observers for Waters of Table 5


Sample
No. 1 2 3 4 5 6 7 8 9

1 2 2 3 4 5 4 5 2 1
2 5 3 5 5 4 2 4 3 2

3 3 5 2 2 1 3 1 5 4
4 4 4 4 3 2 5 2 4 5

5 1 1 1 1 3 1 3 1 3

No order stated both alike.
















- 21 -


Table 7
Taste Test No. II. Averaged Preferences of Eight Observers


Materials added to taste-free
demineralized vater ppm
Sample Preference Order of
No. No. (Avg) Preference Phenol Ammonia Iodine Chlorine

1 3.29 2 .001 0 0.8 0
2 3.72 3 .010 0 0.8 0

3 3.0 1 .010 0 0 0
4 5.0 6 0 0 0 0

5 4.0 4 .010 .1 0.8 0
6 5.6 7 .010 0 0 .224

7 4.25 5 .010 .1 0 .224








- 22 -


Table 8
Taste Test No. II. Individual Preferences of Eight
Observers for Waters of Table 7


Sample No. 1 2 3 4 5 6 7 8

1 6 2 5 1 1 2 1* 6
2 7 1 6 2 2 3 2 5

3 1* 3 3 3 3 4 j 2
*
4 2 4 4 7 5 1 47 1

5 3* 5 1 6 6* 5* 5 4
6 4* 6 7 4 4 6* 60 7

7 5 7 2 5 7 7 7 3

No preference or all tastes the same.
xl.2,3 no preference as to order but best.
Y4,5 no preference but intermediate.
z6,7 no preference but worst.


relative effects of the two halogens. The results are tabulated in
Table 9. These data suggest that lodinated water is preferred over
chlorinated water. Comments expressed by the taste panel showed that
each water was palatable and that a five in order of preference was still
an acceptable water.









- 23 -


Table 9

Comparison of Taste Produced by Chlorine and Iodine in Marietta, Ohio
Well Water Containing .05 ppm Phenol


Reaaents Added to Marietta. Ohio Well Water
Sample Order of (ppm)
No. Preference Phenol Iodide Iodine Chlorine

1 5 .05 1.5 0.42

2 3 .05 1.5

3 4 .05 0.42
4* 1 .05 1.5

5 2 .05 0.42

Demineralized water used as controls*


Since no objectionable taste was observed when 50 ppb of phenol

was used, it was felt that perhaps a different ratio of halogen to

phenol should be used. From works published by Burttschell, Rosen,

Middleton, and Ettinger6 maximum taste is produced when the ratio of

chlorine to phenol is 2:1. As reported earlier in this section, the

normal dosage of chlorine is four ppm:; thus, the dosage of phenol should

be two ppm.

The results of taste tests using the above concentrations are

shown in Table 10.







- 24 -


Table 10

Comparison of Taste Produced by Chlorine and Iodine in Marietta, Ohio
Well Water Containing 2.0 ppm Phenol


Reagents Added to Marietta, Ohio
Order of Well Water (ppm)
Sample No. Preference Phenol Iodine Chlorine

1 1 2.0

2 2 2.0 4.0

3 3 2.0 1.5

Demineralised water included as a reference.


All observers termed the tastes produced as extremely bad.

The results of the laboratory studies suggested that some agent

other than phenol was present in the water, causing taste to develop.

Iodine demand data on the well water with and without added

phenol add strength to the hypothesis that something other than phenol

was responsible for the observed tastes. See Figure 2. The results

obtained clearly indicated the need for similar tests on samples imme-

diately after pumping from the wells, and arrangements were made for a

trip to Marietta in order that such tests could be made.

Studies Conducted at Marietta. Ohio

Taste and odor of raw water. Immediately after collecting water

from each of the four wells, the presence of taste and odor was deter-

mined using plant personnel as panel members. Water from a private well







- 25 -


e-e J
0 -
a 0 .0
E u0 N
n 4 z


0 -" 0
< O S E <






0
o-a w
iI I--
000










o 0
Spw



0



IODINE, ppm







- 26 -


in the same aquifer and located one mile southwest of the wells of primary

interest was included for comparison purposes. This well is designated

as "One-Aile Well." The results are shown in Table 11.


Table 11

Taste and Odor of Raw Water


Well No. Taste Points Odor Points

2 astringent 65 none 0

3 slightly less 60 none 0

5 strongest 100 strong 100
6 less 85 moderate 70

Composite intermediate 80 slight 30

One-Mile
Well good 0 none 0

Points assigned on the basis of 100 points for Well No. 5.

Identified by R. P. Vogh as the characteristic odor of
ohlorobenzene.


An inspection of the chlorination equipment revealed that the

water supply was not being chlorinated and had not been for several days

due to a strike of operating personnel. Even without the addition of

chlorine, the taste of the water was highly objectionable, so much so

that no one had noted the absence of chlorine in the treated water.

Even though it was apparent that nothing would be gained by iodinating the









-27-


water, it was felt that data of great value might result from efforts

to determine the nature and amounts of organic materials present in the

water and a comparison of its chlorine and iodine demands.

Halogen residuals. The first test was planned to determine the

persistence of low halogen residuals in water from individual wells.

Wells No. 3 and No. 5 were selected,with "One-Ale well" as the control.

Tob samples of water from each of these wells was added, in one series,

4.0 ppm of chlorine; in a second series, 0.50 ppm of 12; and in a third

series, 0.50 ppm of HIO. The 12 and HIO residuals were determined over

a period of 20 hours since this portion of the test was started soon

after arriving at Marietta. The chlorine residual was determined only

once, at the end of three hours, as that portion of the test was not

begun until late in the second day of the plant visit. The data are

shown in Table 12. They show that in these waters HIO residuals were

quite persistent; that free 12 residuals disappeared quickly, and that

of the three well waters, that from Well No. 5 had the greatest parent

chlorine demand. This point will be referred to again later.

These data suggest that the water contains enough ammonia to tie

up all chlorine as chloramine an4 in addition, pollutants are present

which have an iodine, HIO and chlorine demand.

lodination of the plant water asumlv. Realizing that iodination

would perform no miracle, Company officials requested that the water

supply be iodinated for a short period of time in order to evaluate

some of the variables involved.







- 28 -


Table 12

12, HIO, and C12 Residuals in Raw Water


we C 2 (ppm) 12 (ppm) HIO (ppm)
No. 3 hr. 3 hr. 8 hr. 20 hr. 3 hr. 8 hr. 20 hr.


3 3.73 0 0 0 0.48 0.48 0.2?

5 1.76* 0 0 0 0.15 0.14 0.07
One-mile
Well 3.85 0.48 0.46 0.30 0.53 0.51 0.45

Initial
Concen. 4.0 0.50 0.50

Combined chlorine.

Free chlorine.


Iodine was fed into the system as a solution of potassium iodide,

using an automatic proportioning. hydraulically driven Wallace and
Tiernan hypochlorinator. The strength of the potassium iodide solution
fed was adjusted to one pound per gallon. Gaseous chlorine fed by the

existing chlorinator was used to oxidize the iodide ion to HIO. The
exact feed of chlorine could not be determined since the rotometer was
not accurately calibrated below ten pounds per 24 hours.

A check of the residual in the distribution system showed that a
residual of 0.17 ppm (HIO) was maintained to the administration and

laboratory building.









- 29 -


Additional laboratory studies. Additional laboratory studies

were initiated in an effort to determine more about the taste and odor

present in the water. Two methods of treatment which were used to shed

light on the nature of-the agents are:

1. Superchlorination to oxidize the organic material.

2. Aeration to remove gaseous components.

Superchllorination. A composite sample of water was dosed with

10, 20, 40, 60, and 120 ppm of c12 in an effort to oxidize the organic

matter present in the water. While the odor and taste of chlorine were

pronounced, the odor and taste present in the raw water were either

considerably reduced or masked by the chlorine. A yellow color appeared

in the water containing greater than 20 ppm chlorine and a brown pre-

cipitate formed when samples were allowed to stand for from tw to four

hours. Chromate and chlorinated organic are possible sources of the

color, but the presence of neither of these has been confirmed. It is

also possible for diaminobenzene or related compounds to produce a yellow

color when oxidized by chlorine.6 This is similar to the orthotolidine

test for chlorine.70

Aeration. A composite sample of water was aerated for three

hours by bubbling air through the water at the rate of 75 bubbles per

minute. If the water prior to aeration was assigned a taste rating of

100, the aerated water would be rated at 20.

The results obtained after adding C12, I2, and HIO to the aerated

water are tabulated in Table 13.









- 30 -


Table 13

Taste of Aerated Samples Treated with C12, 12 and HIO


Dosage Taste in One Hour Order of Preference

4.0 ppm Cl2 Not objectionable 3

0.5 ppm I2 Not objectionable 2
0.5 ppm HIO Not objectionable 1



Ammonia and COD. The ammonia content of water from each well

was determined by KJeldahl distillation.57 As shown in Table 14, some

extremely high values were obtained.


Table 14

Observed and Calculated Oxygen Demands of Several Waters


Parts Per Composite Demineralized
Million of Sample "One. Water Plus
Determined Well Well Well Well From Four Mile 27 ppm 112 ppm
Criterion No.2 No.3 No.5 No.6 Wells Well" NH3-N NH3-N

Ammonia
Nitrogen 80 112 0.38 27 54 0.04 -- -

COD 17 8.7 4.2 4.4 4.5 2.8 4.7 14







- 31-


While it was realized that aromatic hydrocarbons, pyridine and

ammonia would not be oxidized by dichromate to an appreciable extent,

it was felt that COD data would be beneficial in determining the presence

of other organic in the plant water supply.71 From Table 14 it will be

noted that the higher COD values were obtained on waters having a high

concentration of ammonia. Water from "One-mile well" and demineralized

water containing a known concentration of ammonia were included for com-

parison.purposes.

These data suggest that ammonia was responsible for most of the

observed COD and further suggest that if organic which are oxidizable

by dichromate were present in the water, they were present in relatively

low concentrations.

Halogen demands. Halogen demand was determined by adding suf-

ficient halogen to yield the desired initial concentration and immediately

determining the halogen residual. This initial halogen concentration was

increased until a measurable free residual was obtained* The chlorine

and iodine demands of the waters are tabulated in Table 15 and presented

graphically in Figure 3. The calculated chlorine demand of each water

based on its ammonia content and the following equation are shown in

Table 15.

2NH3* 3 2 6HC1. +N



As previously mentioned, data which are presented in Table 12

show that water from well No. 5 had a higher chlorine demand than that

from well No. 3 and "One-mile well." Quite a different conclusion must








- 32 -


Table 15

Calculated and Observed Halogen Demands of Water from Five
Wells at Marietta. Ohio


Chlorine Demand. pvm Measured Iodine Demand, ppm
Sample Calculated Observed As 12 As HIO

Well No. 2 607 806 0.07 0.11

Well No. 3 850 1179 0.07 0.12

Well No. 5 2.8 4.2 1.66 0.57

Well No. 6 207 221 1.32 0.36

Composite* 410 490 0.82 0.26

"One-mile well" 0.33 1.0 0.03 0.05

Dosage yielding measurable free halogen residual within five
minutes.
**
Composite sample prepared by mixing equal volumes of water from
each of the four plant wells.


be drain, however, when the results shown in Table 15 are considered.

It is interesting to note that the iodine demands are quite dif-

ferent from those for chlorine, not only in magnitude but in relative

demands as well. While well No. 5 has a relatively low chlorine demand

it has the highest HIO and 12 demand. These data show that while much

of the chlorine demand can be accounted for from the ammonia content of

the water, other pollutants are present which also have a chlorine demand.

These data further suggest that either the pollutants which are present







- 33 -


LEGEND
i.ooo- -_ U IODINE


[ CHLORINE


2 3 5 6 COMPOSITE ONE-
MILE
WELL NUMBER WELL
FIG. 3 IMMEDIATE CHLORINE & IODINE DEMANDS OF
MARIETTA,OHIO, WELL WATER OCT. 7,1966
i i











in wells No. 5 and No. 6 are different than those found in wells No. 2

and No. 3, or the high concentration of ammonia or other pollutants

present in wells No. 2 and No. 3 inhibit the reaction of 12 ahd .H1 with

certain pollutants which would otherwise show an 12 and HIO demand.

Possible Pollutants

A brief survey of the plant's waste disposal practices was made

in an effort to gather more information regarding possible pollutants.

A Union Carbide plant operated by its Plastics Division is located

adjacent to the plant operated by its Mine and Metals Division. It was

disclosed that phenol and styrene monomer are produced from chlorobenzene

in the plastics plant. The principal waste products of the plant are

tars which are disposed of in a waste disposal area located uphill from

the well field. Some chlorobenzene, phenol and styrene monomer are con-

tained in the tars and are necessarily dumped in the waste disposal area

along with the tars. Since chlorobenzene and phenol are solvents and

miscLble with water, it is highly probable that a mixture of these waste

products finds its way into the aquifer and well field.

This limited survey of waste products is obviously incomplete

since an analysis of the water shows a high concentration of ammonia in

most of the wells. Company officials gave no indication as to the

source of ammonia.

Summary and Conclusions'

As indicated by preliminary laboratory studies, iodination of a

Marietta, Ohio, well water without preliminary aeration did not produce

a palatable water. While the presence of phenol in the raw water was








- 35-


believed to be responsible for the taste in the treated water, there are

several indications that it is not the sole source of taste and odor.

Three observations which lead to this conclusion are:

1. The raw water, before treatment, has an objectionable taste

and odor. The odor has bean identified as the characteristic odor of

chlorobenzene which is one of the raw materials used in the production

of phenol.

2. Even though the water supply had not been chlorinated for

several days due to a strike of operating personnel, plant personnel

had detected no difference in the taste of the water.

3. With ammonia present in the raw water, all chlorine exists as

chloramine which would be expected to react too slowly with phenol to

cause an appreciable buildup of chlorophenols during the very short time

which the water remains in the distribution system.72

The 0OD of the raw water suggests that the major contaminants are

aromatic hydrocarbons and ammonia. Both chemical analyses and a know-

ledge of the plant's waste products substantiate this hypothesis.

While aeration and subsequent disinfection of the raw water pro-

duced a water having an acceptable taste, it was recommended that

another source of water be obtained before iodinating the supply on a

continuous basis.

The work done toward iodinating this water supply has been of

great value in demonstrating the potential which iodine has as a disin-

fectant for water. It has clearly demonstrated that a low HIO residual

can be maintained in the presence of high concentrations of ammonia and










other industrial pollutants as had been predicted from the chemical

properties of iodine.73

Gainesville Study


Floridan Aauifer

General characteristics. The City of Gainesville is located

over one of the most productive ground water formations in the conti-

nental United States. This formation, called the Floridan Aquifer,

underlies most of the Florida peninsula with numerous recharge areas and

sufficient head to prevent serious salt water intrusion.7 It is the

primary source of fresh water for Florida and serves as the source of

water supply for most municipalities. This aquifer is the source of

water supply for the City of Gainesville.

In the Gainesville area, the Floridan Aquifer is composed primarily

of limestones and dolomites to a depth of several thousand feet. The

cover of sands and clays extends from the surface to a depth of about

150 feet,becoming thinner to the southwest and thicker to the northeast.65

Characteristics in the Gainesville area. Well drillers' logs show

that the characteristics of the FloridanAquifer in the Gainesville area

are substantially the same as those encountered in the City of Gaines-

ville well No. 4. These characteristics are as follows 6

1. The aquifer begins at approximately 100 to 150 feet in depth.

2. It extends beyond 1,020 feet in depth.

3. The permeability of the aquifer varies considerably due to the

presence of several beds of permeable, cavernous limestone

separated by other beds of practically impermeable limestone


- 36-







-37-


and dolomites.

4. The most cavernous and porous beds are found between 100 and

200 feet and at 300 to 350 feet.

5. Relatively permeable beds are again found between 650 to 800

feet and from 960 to at least 1020 feet.
6. Between 350 and 650 feet there are layers of practically

impervious limestones and dolomites which, at least in the

Gainesville area, impede direct communication between the
upper and lower permeable beds.

7. The water in the upper part of the aquifer is moderately

hard (200 ppm as CaCO ), low in chlorides (10 ppm as Cl),

and low in sulfates (15 ppm as S04). The quality of the

water derived from these strata remained relatively constant

until recent years, when a notable deterioration in quality

has been observed. Pollution from surface water and sewage
has become increasingly evident, especially during periods of

heavy rainfall.
8. Water in the lower part of the aquifer (650 to 850 feet) is

slightly harder (226 ppm as CaOO ) and slightly higher in

sulfates (84 ppm as S0o). So far this stratum has remained

relatively uncontaminated.

9. Water from a still deeper part of the aquifer (3015 feet) is
even harder (346 ppm as CaCO3) with a noncarbonate hardness
of 180 ppm as CaCO.

Figure 4 is a graphical representation of geological characteristics











- 38 -


uar or ernma .m n.on warn Iws.v w-LL o. a
CIT or oIiUi r.r .LO..O.


























a.5 obA L 4ULyT ws av0PU0m Or 1T11I. u 1 1
5 414 414 m**































4F*W *ig -4 (Ref 46)







rFig. 4 (feroe 46)













IIS l inlO l i s m as -








- 39 -


and water quality in the Floridan Aquifer as derived from data obtained

during drilling and testing city well No. 4.46.65

It should be noted that the aquifer can be considered as being

primarily composed of three strata as follows

1. An upper permeable stratum extending from 100 feet to approxi-

mately 350 feet in which cracks, crevices and caverns are

numerous.

2. An impervious stratum between 350 and 650 feet.

3. A lower permeable stratum beginning at about 650 feet and

extending to about 800 feet.

Piezometric Surface and Flow of Ground Water

A hydrological study of a four-county area which included Alachua

County was conducted by the Florida Geological Survey in 1958-1960.75

The piezometric levels in the upper permeable stratum of the Floridan

Aquifer in the Gainesville area were redetermined in August, 1965, and

found to be six to eight feet higher than at the same points in 1960.6

The higher elevations were probably due to heavy rains during June, July,

and August, 1965. Substantially the same gradients were found in

August, 1965, indicating that the direction of underground water move-

ment remains the same regardless of whether the piezometric level rises

or falls.

Figure 5 shows the contours of the piezometric surface in the

top part of the FLidan Aquifer as of August, 1965, as well as pertinent

points for future reference. These contours suggest that:

1. Ground water flows from a wide area around Gainesville to the










AUGUST 30-31, 1965
SPERRY RAND


6 6. MUNICIPAL AIRPORT


4AESVILLE --- 1RONWOOD



ORMAN ANNIS CITY WELL NO. 3


LAKE ALICE CITY WELL NO. 6


UNIV. OF FLA. WELL/ ALAmUA SINK




CONTOURS OF THE PIEZOMETRIC SURFACE IN THE TOP PART OF THE
FLORIDAN AQUIFER AND RELATIVE LOCATION OF SAMPLE POINTS


Fig. 5 -








- 41-


city's well field which is located in the southeast section

of the city.

2. East of Gainesville water flows from east-northeast to west

toward Gainesville.

3. To the west and north ground water flows from southeast to

northwest.

Very few wells in the Gainesville area penetrate both the upper

and lower permeable strata and even fewer penetrate the lower permeable

stratum with the upper stratum cased out. Without the upper stratum

cased out it would be difficult if not impossible to determine the

piezometric level of water in the lower permeable stratum. City well

No. 6, however, penetrates both the upper and lower permeable strata

with the upper permeable stratum cased out. Measurements made on city

well No. 6 over a three-year period include the random measurement of

the piezometric level of water in both the upper and lower permeable

strata. These data, which are tabulated in Table 16, show that the

water level in the upper permeable stratum is higher than that in the

lower stratum. 466 These results indicate that there will be a down-

ward flow of water from the upper to the lower stratum where connections

between the two strata exist.

Pollution of Acuifer

Source of water. The source of water for the City of Gainesville

is a series of seven wells located near the water treatment plant in the

southeast section of the city. While all wells penetrate the Floridan

Aquifer, depths of the wells vary from 365 feet to 872 feet; thus, the







- 42 -


Table 16

Level of Water in the Upper and Lower Strata of the Floridan
Aquifer. Well No. 6, City of Gainesville


Depth From
Surface to
Water Level Aug. 26, Oct. 29, Aug. 31, Apr. 25,
(feet) 1964 1964 1965 1967

Lower stratum 87.9 85.1 86.2 86.4

Upper stratum 86.8 84.3 81.3 86.0

Difference 1.1 0.8 4.9 0.4



water obtained from each well may have different characteristics depend-

ing on the depth from which the water is obtained. The physical charao-

teristics of these wells are summarized in Table 17 and the chemical

characteristics in Table 18.

In time, well No. 1 was turned over to the City of Gainesville

Power Plant for use as a source of cooling water. Wells No. 2 and No. 3

are old wells with antiquated equipment, showing evidence of pollution,

and are not in regular use.

Evidence of pollution. Until recent years (prior to 1960) wells
No. 4, No. 5, No. 6, and No. 7 produced water of good quality. About

1960, wells No. 4 and No. 6 began to show an increase in color and bac-

teriological count during periods of high rainfall.4

In November, 1963, the quality of water in wells No. 4 and No. 6






- 43 -


Table 17

Characteristics of Wells from Which Water for the City of
Gainesville Is Obtained


Total Casinr Draw-
Well Depth Dia. Depth Yield down
No. (ft) (in) (ft) gpm (ft) Remarks

1 365 12 266 1200 5 Old well, abandoned
2 407 18 128 1800 16 Not in regular use
3 421 18 170 2000 1 Not in regular use

4 464 30 173 5100 7 Polluted. Had to be
relined and deepened

4 872 20 375 3800 46 Relined and deepened

5 742 24 152 4300 13 Needs to be relined
6 750 24 163 4000 12 Polluted. Had to be
relined
6 750 20 331 2800 46 Relined

7 713 24 157 3500 3 Needs to be relined



deteriorated rapidly, reaching a peak in January, 1964, after several

days of abnormally high rainfall which had been preceded by several

months of very dry weather.75 The presence of high organic color (150

units), high coliform counts (100#) and a high concentration of deter-
gents in well No. 6 suggested the presence of sewage pollution. A blan-

ket of detergent foam several feet thick, produced by recarbonation of

the treated water passing to the filters is shown earlier in this study

in Figure 1.
















Table 18
Chemical Characteristics of Water from Wells in the City
Well Field, March, 1967


Parts Per Million
Well Well Well Well Well Well
Constituent No.2 No.3 No.4 No.5 No.6 No.7

Total dissolved solids 277 195 309 248 331 280
Total hardness, as CaCO 212 178 256 180 266 200
Carbonate hardness,
as CaCO3 173 80 202 152 192 166
Noncarbonate hardness,
as CaOO3 39 98 54 28 74 34
Alkalinity, as CaCO3 173 79 202 152 192 166
Calcium, as CaCO3 139 127 184 120 190 140
Magnesium, as CaCO 73 51 72 60 76 60
Chlorides, as Cl 11 11 8 13 12 12
Iodides, as I 9*5 11.4 12.0 7.0 15.5 12.4
Sulfates, as SOj4 13 5 50 8 84 24
Organic Color (units) 10 27 3 37 7 20
pH (units) 7.60 6.90 7.52 7.55 7.4 7.50







-45-


Possible sources of pollution. Two possible sources of sewage

pollution existed on the periphery of the city; (1) the effluent from

the university sewage treatment plant as well as wastes from the Teaching

Hospital which at that time emptied into a sink hole on the University

of Florida campus, and (2) effluent from the city's sewage treatment

facility which eventually enters Alachua Sink via Sweet Water Branch.

Both of these sinks are located approximately three miles from the city's

well field, Alachna Sink to the south and the sink on the. University of

Florida campus to the west.

On four occasions prior to 1964, the effluent of the University of

Florida Sewage Treatment Plant had been traced through the sink on the

University of Florida campus to the city well field.75 An isotope spill

at the University of Florida Teaching Hospital in August, 1962, provided

an excellent tracer to show that water entering the sink reached the

city's water treatment plant in less than ten hours, which means that the

water traveled the straight-line distance of approximately 9,500 feet at

a minimum velocity of 16 feet per minute.7

After the evidence of sewage pollution in city well No. 6 in

January, 1964, the University of Florida diverted the sewage effluent

from the sink into Lake Alice and sealed off the sink. Lake Alice, how-

ever, is drained by two drainage wells located at the west end of the

lake. Both of these drainage wells penetrate the upper permeable stratum

of the Floridan Aquifer as may be seen from Table 19.

Dye tests conducted by adding 25 pounds of Rhodamine-B dye in the

west drainage well at Lake Alice in January, 1964, failed to show any







- 46 -


Table 19

Drainage Wells at West End of Lake Alice


Well No. 1 Well No. 2

Total depth, feet 235 450

Casing diameter, inches 24 24 20

Casing depth, feet 83 243



connection between the drainage wells and the city's well field.

Likewise, the addition of 20 pounds of Uranine-B dye into Alachua

Sink failed to positively show a direct connection between the sink and

the city well field. Samples of water collected from well No. 6 after

dye was added to the sink were analyzed by two different laboratories

using three different methods. The results were conflicting so that no

definite conclusion could be drawn. The addition of 50 pounds of

Rhodamine-B dye to Haile Sink, a straight-line distance of 29,400 feet

from city well No. 6, likewise failed to show a connection between the

sink and the city well field. The results, however, are not surprising

since the dyes used in these tests have been shown to have a rapid photo-

chemical decay.77 Organic color, almost always present, fluoresces

brilliantly, and some of the materials present in treated sewage are

known to be fluorescent.78

Samples of water were collected from the various sinks and surface








- 47 -


waters in the area in an effort to use a comparison of nematode and

algae forms as indicators of the source of pollutants. Professor W. T.

Calaway of the University of Florida Department of Entomology reported

that while the algae forms in Lake Alice and Alachua Sink were differ-

ent, no definite conclusions could be drawn regarding the source of

pollutants in the city wells.76

In brief, after the sink hole on the University of Florida campus

was sealed off and effluent from the campus sewage treatment facility

and Teaching Hospital diverted to Lake Alice, no direct connection

between known sources of sewage pollution and the city's well field

could be proven.

Hydrological investigation. Hydrological investigations were

made in wells No. 4 and No. 6 in order to determine the point of entry -

of the polluted water. These investigations consisted of:4

1. Electric logging.

2. Temperature logging.

3. Depth sampling.

4. Deep well current meter traversing.

The results showed that the polluted water was entering each well

from the lower portion of the upper permeable stratum of the Floridan

Aquifer.

Corrective measures. Polluted water was prevented from entering

these two wells by relining well No. 6 to a depth of 331 feet and

deepening well No. 4 to 872 feet and relining it to a depth of 375 feet.

Essentially the stratum from which the polluted water was entering the











- 48 -


wells was cased out so that water pumped from these two wells entered

the well from the lower permeable stratum.

While the problem of grossly polluted water entering the city's

wells has been somewhat relieved, polluted water still persists in the

upper permeable stratum.

Threat of additional pollution. Apparently both Alachua Sink

and the drainage wells at Lake Alice penetrate only the upper permeable

stratum. In the absence of cracks, crevices or other means of commnni-

cation between the upper and lower strata, the lower stratum should con-

tinue to provide a supply of good quality water. However, a potential

threat to the lower stratum exists on the campus of the University of

Florida as described below.

The University of Florida has three deep wells for use in conneo-

tion with its steam and air conditioning plant. These wells are located

immediately west of the Teaching Hospital and approximately 1.5 miles

west of the city's wells. As shown in Table 20, these wells penetrate

the lower permeable stratum and are open to both the upper and lower

strata. Tests conducted in the city's wells show that water is prefer-

entially pumped from the upper stratum even though a well may penetrate

both. These wells thus present a serious potential route for polluted

water to enter the lower stratum.













Table 20

Characteristics of Three Wells Owned by the University of Florida


U. S. Geological Survey No.

938-221-1 938-221-2 938-221-3

Total depth, feet 916 700 909

Casing diameter, inches 20 20 24

Casing depth, feet 290 188 183



Selection of Samle Points

Sample points were selected to establish the baseline iodide con-

centration in the water prior to the possible initiation of iodination

of the city's water supply and to determine the source and extent of

sewage pollution in the Floridan Aquifer near the City of Gainesville*

The locations of sample points are given in Table 21 and represented

graphically in Figure 6. Samples of water entering the ground at Alachua

Sink and the drainage wells at Lake Alice were included to show the

quality of water entering the ground at these points.

From Table 22 one may observe that the wells whioh vwre selected

are pumped frequently if not continuously and at a rate much greater
than the usual home owners' well. These wells should serve as an excel-

lent source of water representative of water in the aquifer in that par-

ticular area.







- 50 -


Table 21

Location of Sample Points


Name or
Number Identification Location

1 City well No. 3 605 SE 3rd Street

2 City well No. 6 Approx. 800 SE 5th Street

3 University of Florida West of Teaching Hospital
on Archer Road

4 Ormon Annis properties 29th Place at NW 22nd Street

5 Sperry Rand Corp. Waldo Road
6 Municipal Airport Waldo Road

7 West drainage well at
Lake Alice Univ. of Florida campus

8 Alachua Sink Camp Ranch SE of 41st Avenue
and 15th Street SE



The wells at Sperry Rand Corp. and the Municipal Airport were

selected not only for their geographic location with respect to the city

wells but should be representative of wells which will comprise the city's

new well field to be located in that area.

The University of Florida well was selected partially because of

its geographic location but primarily because of its possible role in

providing a route fbr pollutants to enter the lower permeable stratum

from the upper stratum.























ORMAN ANNIS CITY WELL NO. 3


LAKE ALICE CITY WELL NO. 6


UNIV. OF FLA. WELL ALACHUA SINK





Fig. 6 Relative Location of Sample Points







- 52-


Table 22
Pertinent Data Relative to Sampling Points


Total Casing Pumping Frequency of
Name or Idea- Depth Depth Diameter Rate or Pumping or
No. tification (ft) (ft) (in) Flovw(gd) Flow

1 City well No. 3 421 170 18 2.9 As needed
2 City well No. 6 750 331 24 20 4.0 Frequently

3 Univ. of Fla. 909 183 24 2.5 Continuously
4 Ormon Annis 330 175 6 0.3 As needed

5 Sperry Rand Corp. 350 160 12 0.72 Continuously
6 Municipal Airport 447 175 10 Unknown Frequently

7 Drainage well at
Lake Alice 235 83 24 4.2 Continuously
8 Alachua Sink -- 40.0 Continuously

Average of three flow checks made by using an electric current
meter manufactured by W. and L. E. Gurley Co., Troy, N. Y.


In the northwest section of the city, wells which were pumped con-

tinuously could not be found. Instead, several wells were available
whose primary use is as a source of water supply for a small residential
area. The south well located on Oman Annis' property was selected
because of accessibility and the amount of data available on this well.46.75
While it would have been desirable to sample each well used as a

source of supply for the City of Gainesville, it was felt that perhaps








- 53 -


typical walls could be used to obtain the same information. City well

No. 3 was selected as a typical well extending only into the upper

permeable stratum of the Floridan Aquifer, while well No. 6 was selected

as a typical well extending into the lover stratum with the upper stratum

cased out. Henceforth in this study wells owned by the City of Gaines-

ville will be referred to as well No. 3 or well No. 6., etc.

Description of Water Treatment Facilities and Distribution System

The water treatment plant is designed for lime-soda softening of

the water. Facilities include two upflow solids-contact units, recarbo-

nation, rapid sand gravity filters, and chlorination. Raw water is

pumped directly into the solids-contact unit where the sludge, activated

silica and lime slurry are thoroughly mixed. The softened water is

separated from the sludge in the clarification zone and then passes by

gravity through the recarbonation basin where the pH is reduced from

pH 10.3 to its stabilization pH of about 8.6. The stabilized water is

filtered through six rapid sand gravity filters into a 200,000 gallon

clear well, and subsequently transferred to either a 500,000 or a

1,000,000 gallon ground storage reservoir.

Excess sludge is processed in a vertical Fluosolids calciner or

dewatered in a centrifuge for disposal. The treatment capacity of the

solids-contact units is 15 mgd with filter capacity rated at 13.5 mgd

at a loading rate of three gpm per square foot. The entire plant will
process water at a maximum rate of 15 mgd.

The water is chlorinated by the addition of from 9-12 ppm of

chlorine to the solids.-contact unit. Ammonium sulfate is added to the







- .5 -


softened water to provide a chloramine residual of at least to parts

per million leaving the plant.

The distribution system consists of about 185 miles of mains

greater than four inches in diameter. High service pumps deliver water

from the ground storage reservoir into the distribution system with two

elevated storage tanks, having a total capacity of 1.5 million gallons,

floating on the system.

Methods of lodination

Data available show that accidents do happen in public water

supplies which result in explosive outbreaks of disease. They frequently

affect large proportions of a population with cases numbering in the

thousands.79

Highly polluted water used as a source of water supply may like-

wise cause widespread disease. The outbreak of infectious hepatitis

which occurred in Delhi, India, in 1955-56, is a classic example of a

viral disease outbreak occurring when conventional treatment produced a

water meeting the bacteriological criteria of the USPHS Drinking Water

Standards. The low chloramine residual which was maintained in the

distribution system was evidently effective in producing a bacteriolog-

ically safe water but was ineffective against the virus of infectious

hepatitis.8

The addition of ammonium sulfate to the treated water in the

Gainesville plant, which converts the free chlorine present during treat-

ment to combined chlorine, is not through choice but through necessity.

It is realized that this conversion from the more active to the relatively








- 55 -


inactive form of chlorine very greatly reduces the bactericidal effective-

ness of the element, but experience has shown that consumers will not

tolerate the very pronounced tastes and odors produced when a free

chlorine residual is added. It was hoped that the relatively low chem-

ical reactivity of iodine might make it possible to maintain an iodine

residual throughout the distribution system without the production of

tastes and odors, and thus provide an additional factor of safety by

possibly inactivating viruses which may be present in the treated water.

Iodine might possibly be added to a municipal water supply by any

of the following procedures.

1. By vaporizing through accurately controlled heat input.

2. In the form of a saturated solution prepared by slowly passing

water through a bed of crystalline iodine, as is being done

at the Lowell institutions.

3. To employ an excess of an oxidant such as chloramine to

oxidize the iodide ion (I-1) to HIO. This procedure would

obviously take full advantage of the principle of reoxidation

and reuse, within the time and geometry limits of the distri-

bution system.

The first two methods are more applicable to iodination when iodine

alone is to be added to the supply, that is, when iodine is to be used to

replace chlorine as the disinfectant. The third method, however, has

many possibilities. Studies of the iodination of swimming pool water

have shown that when I reacts with oxidizable matter in water, much of

the I+1 is reduced to I"1 which, in the presence of excess oxidant, will




















be reoxidized to I31.67 Calculations have been made which show that in

swimming pool water the iodide ion is used as many as 13 times before it

is eliminated from the pool by all types of loss.14 It seems reasonable

that by maintaining a chloramine residual in the distribution system the

iodide ion would be immediately reoxidized should it be reduced by oxi-

dizable matter in the water. Laboratory studies which will be presented

later in this report confirm the assumption that a low iodine residual

can be maintained for a long period of time in the presence of chloramines.

By using the last method both excess chloramine and iodine (as HIO)

would be present in the water to provide a combined disinfecting action.

This method has the further advantage of satisfying most of the halogen

demand of the water with less expensive chlorine, thus minimizing the

dosage of iodide ion required in order to maintain an HIO residual for

a sufficient length of time for water to reach the ends of the distribu-

tion system. This last method was chosen as the method to be used in a

brief trial run in the Gainesville water supply.


- 56 -










IV. MATERIALS AND PROCEDURES


General. The analyses to be made on samples collected from

each sampling point were carefully selected to give meaningful informa-

tion on water quality. At the beginning of the test period, 28 differ-

ent determinations were made on each sample. However, a review of the

data revealed that several of the determinations could be omitted with-

out limiting the objectives of the study, as may be seen in Table 23.

The materials and procedures used for each analysis are described

in the following paragraphs. Unless otherwise specified, all analyses

were as given in the 12th edition of Standard Methods for the Examina-

tion of Water and Wastewater.57 All reagents used in this study were

ACS reagent grade.

When photometric measurements were necessary, a Beckman Model B

Spectrophotometer was used.

pH. All pH measurements were made with a Beckman Model G pH

Meter.

Free NH -N and organic NH -N. Both free and organic ammonia-N

were determined on the same sample. Free ammonia was determined by

method A (distillation method) and organic ammonia by Kjeldahl digestion

and distillation.


Manufactured by Beckman Instruments, Inc., South Pasadena, Calif.
Manufactured by Beckman Instruments, Inc., Fullerton, Calif.
Manufactured by Beckman Instruments, Inc., Fullerton, Calif.


- 57 -






- 58 -


Table 23

Analytical Data Sheet

Sample #_ location Date: From to -

Date & time begin e; end No. of hours__

Meter reading begin end ______________

Pumping rate or flow of stream ________________


Analysis .

pH

COD

Free NH3-1N

Organic NH,-N

Nitrite

Nitrate

Iodide

Turbidity*
H2S

Alkalinity*

Total hardness*

Chloride

Organic color
ABS*

Phosphate

Halowne demands

C3


Analysis Result

CAE


Ether insolubles

Water solubles

Neutrals

Weak acids*

Strong acids

Bases

Total

Bacteriolory

MT (oolifbrm)/100 ml

WMT (non a.)/100 ml

SPC colonies/i __________


After evaluation of the initial data these analyses were dis-
continued.


Result






- 59 -


Nitrate-N. Nitrate-N was determined by method B (brucine-

sulfanilic acid).

Hydrogen sulfide. Hydrogen sulfide was determined as total

sulfide (H2S + HS~) by method A (titrimetric method).

Chloride. Chloride was determined by method A (argentometric

method). The interference from hydrogen sulfide was eliminated when its

presence was detected by odor.

Organic color. Color was determined using a Hellige Aqua

Tester* Model 611.

Alkylbenzene sulfonate (ABS) and linear alkylate sulfonate (LAS). -

ABS and LAS were determined as total anionic detergents using the methyl
80
green method described by Moore and Kolbeson. The method is simple

and much more applicable to a large number of samples than other methods.

Phosphate. Phosphates were determined by the stannous chloride

method which is described in Standard Methods with minor modifications

to speed up the oxidation and hydrolysis of organic bound phosphorous.81

Halogen demands. For the purpose of this study halogen demand

is defined as the initial concentration of the halogen (either chlorine

or iodine) which is necessary to give a 1 ppm free residual at the

end of 24 hours.

Stock solutions of chlorine and iodine were prepared and stan-

dardized by phanylarseneoxide** titration using a Wallace and Tiernan


Manufactured by Hellige, Inc., Long Island City, N. Y.
**
Standard phenylarseneoxide solution, 1 ml = 0.2 mg available Cl.
W. H. Curtin Co., Jacksonville, Fla.








- 60 -


Amperometrio Titrator.*

Samples of water were collected in acid-washed glass bottles and

the demand studies were set up within a few hours after sample collec-

tion. Two-liter samples were placed in acid-washed glass bottles.

Measured dosages of iodine or chlorine were added and the solutions

thoroughly mixed andstored in a closed cabinet out of contact with

light except during brief periods of sample withdrawal. Two-hundred

milliliter samples were withdrawn at predetermined time intervals and

halogen residuals determined by amperometric titratio, using a titrator

which had previously been sensitized to the halogen for which a titra-

tion was to be made. Samples containing hydrogen sulfide were aerated

for one hour prior to setting up the demand study. Halogen demands

determined in this manner gave a betterindication of the organic content

of the water than could have been obtained with hydrogen sulfide present.

Carbon chloroform extract (CCE) and carbon alcohol extract (CAE). -

Both the materials and methods used for CCE determinations were as

described in Standard Methods57 except for one additional piece of equip-

ment which is described below. CAE was determined as per instructions in

USPHS Publication No. 1241.52

The presence of hydrogen sulfide in water posed a problem. Its

presence in concentrations much higher than those of the organic would

most likely cause fouling of the activated carbon long before the

desired volume of water had passed through the carbon absorption unit.


*
Manufactured by the Wallace and Tiernan Co., Belleville, N. J.








- 61 -


Its presence could also reduce the efficiency of the absorption unit by

being preferentially adsorbed.
82
Personal communications with Dr. Breidenbach of the Federal

Water Pollution Control Administration at Cincinnati, Ohio, revealed

that no effort was made to remove hydrogen sulfide from water sampled

routinely by the National Water Quality Network. However, crystalline

sulfur was frequently observed in the CCE.

The results of laboratory studies quickly revealed that when

water containing hydrogen sulfide was passed through a bed of clean

copper turnings the hydrogen sulfide concentration was reduced to a

very low level due to the formation of insoluble CuS. Data which are

presented in Figure 7 show the results which were obtained over a period

of 23 days of continuous service using a small glass column filled with

copper turnings. Calculations based on these data showed that a column

four inches by five feet should provide sufficient contact surface to

remove H2S from approximately 3400 gallons of water.

Sections of PVC pipe four inches by five feet filled with copper

wire were similarly tested for H S removal. The results which are given

in Figure 8 show that by using four columns in series,at least 24 hours

of operation could be obtained before the column required cleaning.

These data suggest that the surface area of the copper wire in the pipe

was considerably less than had been predicted. The copper was easily

cleaned with a 25 percent solution of nitric acid and reused.

As a result of these experiments four pieces of PVC pipe four

inches by five feet filled with copper wire were placed in the line










GLASS COLUMN 0.62"x 43" FILLED WITH COPPER TURNINGS
---- H2S IN INFLUENT (RIGHT SCALE)
a8. --- FLOW (ml PER MIN)(LEFT SCALE)
S HS IN EFFLUENT (RIGHT SCALE)
2 7 TOTAL FLOW 38 GAL. 414


2 4 6 8 10 12 14
TIME (DAYS)


16 18 20 22


FIG. 7- REMOVAL OF H2S FROM WATER WITH COPPER TURNINGS











4"x5' PVC PIPE FILLED WITH COPPER WIRE
.--- HSS IN INFLUENT
HS IN EFFLUENT OF ONE COLUMN
H S IN EFFLUENT OF FOUR COLUMNS IN SERIES
FLOW 0.25 gpm
1.4

1: .2 -:------------------^-- -------------------




0.8-






0.2-


2 4 6 8 to 12 14 1s 18 20 22 24
TIME (HOURS)
FIG. 8 REMOVAL OF H2S FROM WATER WITH COPPER WIRE












immediately preceding the carbon absorption unit where waters containing

H2S were to be sampled. The copper was cleaned once each day to insure

maximum efficiency of the unit. It was assumed that the removal of

organic by the copper was negligible since copper is an approved

material for use in the installation of carbon absorption units.

Bacteriology. Coliform determinations were made by Black Lab-

oratories, Gainesville, Florida, using the membrane filter technique

(MFT).

The Earle B. Phelps Sanitary Engineering Research Laboratory

determined the 24-hour standard plate counts (SPC) at 35C.

Iodine in the Dresence of chloramine. In all studies requiring

the determination of iodine (HIO) in the presence of chloramine, the

colorimetric method developed by Black and Whittle was used. When

determinations were made in the laboratory, concentrations were precisely

determined by using a Beckman Model B Spectrophotometer. A Hach

iodine test kit Model ID-1 was used when determinations were made in

the field.

Iodate. In the absence of obhloramine, iodates were determined
83
colorinetrically, using the method developed by Black and Whittle.

When chlorine, chloramine. or iodine was present, iodates were

determined by amperometric titration. All chlorine, chloramine and

iodine were first titrated and then the pH was lowered to pH 2 and


*
Manufactured by Beckman Instruments, Inc., South Pasadena, Calif.

Manufactured by Hach Chemical Co., Ames, Iowa.


- 64 -








- 65 -


excess potassium iodide added. After standing for three minutes the

pH was raised to pH 4 and the iodine equivalent of iodate titrated with

phenylarseneoxide..

Iodide. Iodides in concentrations greater than 0.05 ppm were

determined colorimetrically, using the procedure developed by Black and

Whittle.83 The determination of iodide in natural waters, however,

required the use of a much more sensitive method. Samples were concen-

trated 10:1 and the iodide content determined by a procedure used for

the determination of protein bound iodine as described by Sunderman.

The method is based upon evaluating the catalytic effect of the iodide

ion on the rate of oxidation of the arsenite ion by ceric sulfate, under

rigidly controlled conditions. All low.level iodide determinations were

made by the Clinical Laboratories of Shiands Teaching Hospital.

Radioactive iodine (1311). 131I was determined on samples

collected from well No. 2 at Lowel] using the whole body counting

facilities of the Department of Radiology at the University of Florida

Health Center. Facilities were such that a fairly large sample could

be counted. For this reason a five-gallon sample contained in a glass

bottle was used.

Counting equipment consisted of a four-inch by nine-inch Nal

(TII) crystal and a Packard Model 116 multichannel analyzer. The

analyzer was calibrated for 10 key/channel. Frequent checks of the

calibration were made by counting a 40K source.


Manufactured by Packard Instrument Co., Inc., La Grange, Ill.



















- 66 -


Count data showed that decay products of 226Ra were present in

the water. Correction of the count data for their presence was neces-

sary since the energy spectrum for both 131I and daughters of 226Ra

overlap in the 0.3 to 0.4 Mev range. Count data from a sample of water

collected prior to the time 131I was administered to test subjects was

used to strip the spectrum of those components due to 226Ra daughters.
A 1311 standard containing 0.425 pCi 131I was prepared in the

same type container as was used for the samples. The overall counting

efficiency based on this standard was determined to be 0.77 percent.

The 131I content of both the standard and samples was based on the

summation of counts in the corrected energy spectrum between 0.3 and

0.4 Mev.









V. POLLUTION OF THE FORIDAN AQUIFER


Introduction

As previously stated, polluted water is known to be entering the

ground at two locations on the periphery of the city. Further, it is

known that polluted water is entering some of the wells in the city's

well field.

This -so-called baseline study has been designed to determine the

extent to which the Floridan Aquifer is polluted in the Gainesville area.

It is also designed to provide other information on water quality which

will be useful in selecting the site for the development of a new well

field in an area where the water is relatively free from pollution and

of good chemical quality.

Discussion of Results

YbrMs of nitrogen. Figures 9 through 12 and Tables 24 through

27 show the concentrations of nitrate, free ammonia, organic ammonia and

nitrite, all expressed as nitrogen, in water from each sampling point.

Except for two sampling points a decrease in the concentration of

nitrates was observed over the sampling period. Values for both free

and organic ammonia-N fluctuated during the period with perhaps a gen-

eral trend upward during January and February. A measurable concentra-

tion of nitrite was found only twice, ones at Alachua Sink and once at

Orman Annis' well. High values for the three most prevalent forms of

nitrogen were found in water from Lake Alice, Alachua Sink and well No. 3.


- 67 -
























ORMAN ANNIS L CITY WELL NO. 3 ,
.00 .04
.23 o-. .06

LAKE ALICE /CITY WELL NO.6
.05
.05 o.4 .oo
.04 .05 .00oo
UNIV. OF FLA. WELL ALACHUA SINK
.04 .08 .05
.05 .00 .15
.23


Fig. 9 Nitrate-N Content of Water Within the Gainesville Area (ppm as N)
















Nitrate-N Content of


Table 24

WJater Within the Gainesville Area (ppm as N)


Nov. 2 Nov. 11 Nov. 21 Nov. 26 Dec. 3 Dec. 10 Dec. 17 Jan. 6


City well No. 3 0.04 0.06

City well No. 6 0.05 0.04 0.05 0.05 0.00 0.00

Univ. of Fla. well 0.04 0.05 0.08 0.00

Lake Alice 0.05 0.04

Alachua Sink 0.05 0.15 0.23

Orman Annis 0.00 0.23

Municipal Airport 0.05 0.06

Sperry Rand Corp. 0.15 0.00








































Fig. 10 Free Ammonia-N in Water Within the Gainesville Area (ppa as N)














Table 25

Free Ammonia-N in Water Within the Gainesville Area
(ppm as N)


Nov.2 Nov.11 Nov.21 Nov.26 Dec.3 Dec.10 Dec.17 Jan.6 Jan.12 Jan.18 Feb.8


City well No. 3 0.29 0.27 0.20 0.24

City well No. 6 0.37 0.49 0.34 0.42 0.42 0.44 0.46

Univ. of Fla. well 0.08 0.02 0.09 0.04 0.12 0.04

Lake Alice 0.86 0.05 0.11 0.47

Alachua Sink 0.30 0.57 0.15 1.25 1.13

Orman Annis 0.06 0.004 0.06 0.03

Municipal Airport 0.01 0.01 0.05

Sperry Rand Corp. 0.07 0.10 0.14





















ORMAN ANNIS CITY WELL NO. 3 '
.003 .14 -"-- .25 .42
.02 -39
.09 .._.33
LAKE ALICE CITY WELL NO.6
.75 .30 16 .00 .09 .21
.31 .06 .06
.30 .21 .08
UNIV. OF FLA. WELL ALACHUA SINK
.1 .09 .75 .58
.02 .16 1.65 1.38
.03 .16 .16


Fig. 11 Organic Ammonia-N in Water Within the Gainesville Area (ppm as N)
















Organic Ammonia-N


Table 26

in Water within the Gainesville Area
(ppm as N)


Nov.2 Nov.11 Nov.21 Nov.26 Dec.3 Dec.10 Dec.17 Jan.6 Jan.12 Jan.18 Feb.8


City well No. 3 0.25 0.39 0.33 0.42

City well No. 6 0.00 0.06 0.21 0.09 0.06 0.08 0.21

Univ. of Fla. well 0.10 0.02 10.03 0.09 0.16 0.16

Lake Alice 0.75 0.31 0.30 0.30

Alachua Sink 0.75 1.65 0.16 0.58 1.38

Oman Annis 0.003 0.02 0.09 0.14

Municipal Airport 0.03 0.09 0.06 0.11

Sperry Rand Corp. 0.002 0.02 0.11




































.00 .00
.00 .00
.00 .93



Fig. 12 Nitrite-N Content of Water Within the Gainesville Area (ppm as N)














Table 27

Nitrite-N Content of Water Within the Gainesville Area (ppm as N)


Nov. 2 Nov. 11 Nov. 21 Nov. 26 Dec. 3 Dec. 10 Dec. 17 Jan. 6


City well No. 3 0.00 0.00

City well No. 6 0.00 0.00 0.00 0.00 0.00 0.00

Univ. of Fla. well 0.00 0.00 0.00 Trace

Lake Alice 0.00 Trace

Alachua Sink 0.00 0.00 0.93

Orman Annis 0.00 0.02

Municipal Airport 0.00 0.00

Sperry Rand Corp. 0.00 0.00

*
Present but concentration less than 0O'1 ppm







- 76 -


The presence of organic ammonia, free ammonia and nitrate-N in

the concentrations found indicate that nitrogenous organic matter and

its products of decomposition are present in waters to the west and

south of the present well field. The absence of nitrite-N and the

presence of nitrate-N suggest that the process of decomposition is

stabilized and that the pollutants are not of recent origin.

Two hypotheses seem to have merit in explaining the relatively

high free ammonia-N content of water from well No. 6: (1) pollution of

very recent origin by sewage, or (2) the biological or chemical reduction

of nitrates. Coliform organisms which are occasionally found in the

water add strength to the first hypothesis, while the low concentrations

of nitrate-N, absence of nitrite-N and the presence of hydrogen sulfide

add strength to the latter hypothesis.

Low values for all forms of nitrogen were found in waters from

sample points northeast of the city. This was to be expected since the

piezometric level of water in this area is higher than that found in

other areas of Gainesville.

OR. Data which are presented in Figure 13 and Table 28 show

that the highest COD values were obtained for Lake Alice, Alachua Sink

and well No. 3. Intermediate to low values were obtained for well No. 6

and the University of Florida well,with still lower values obtained for

sample points northeast of the city.

The ODD of 20.6 ppm for the Orman Annis well is believed to be due

either to a sampling or analytical error since such a high COD is highly

unlikely without gross pollution. The low COD of 5.0 ppm for Alachua





















ORMAN ANNIS / *- CITY WELL NO. 3
0.00 "17.2
20.6 3.9

LAKE ALICE GITY WELL NO.
17.2 0.13 8.1
25.0 3.3 0.oo
UNIV. OF FLA. WELL ALACHUA SINK
0.00 7.3 39.1
0.00 1.7 5.0
1.6 46.7


Fig. 13 COD of Water Within the Gainesville Area (ppm)


















Nov. 2 Nov. 11 Nov. 21 Nov. 26 Dec. 3 Dec. 10 Dec. 17 Jan. 6 Jan. 12


City well No. 3

City well No. 6

Univ. of Fla. well

Lake Alice

Alachua Sink

Orman Annis

Municipal Airport

Sperry Rand Corp.


17.2

6.4 .13

0.00 0.00

17.2

39.1


0.00

2.5

0.00


2.6 8.1


0.00


7.3

25.0


46.7

20.6


0.00


0.00 0.00







- 79 -


Sink occurred at the same time a low of 3.9 ppm was obtained for well

No. 3.

These data, and those previously given, suggest that organic

pollutants are present in ground water both south and west of the present

well field. They further suggest that water northeast of the city is

relatively free of organic pollutants.

Phosphate and chloride. Both totalphosphate and orthophosphate

determinations were made on all samples collected during the first two

months of this study. The results showed that orthophosphate was equal

to total phosphate, indicating that no polyphosphates were present.

As may be seen from Table 29, the concentration of phosphates

tended to increase during the sampling period except for the two sample

points northeast of the city. Again, high concentrations were found in

Lake Alice, Alachna Sinks and well No. 3,with lower values at well No. 6,

University of Florida well and Orman Annis' well (Figure 14).

Figure 15 and Table 30 show that chlorides remained relatively

constant during the sampling period. Higher values were obtained for

Lake Alice and Alachua Sink, with intermediate values for the University

of Florida well, wells No. 3 and No. 6 and the Orman Annie well.

The higher value fobr phosphates at the Orman Annis well on Feb-

ruary 8 is believed to be an error since other analyses to not confirm

the presence of pollutants in the water on that date.

It is interesting to note that well No. 6 and the University of

Florida well show similar values for phosphates, chloride and nitrate

as shown in Figures 11, 14, 15 and Tables 26, 29 and 30.

















Nov.2 Nov.11 Nov.21 Nov.26 Dec.3 Dec.10 Dec.17 Jan.6 Jan.12 Jan.18 Feb.8


City well No. 3 .75

City well No. 6 .14

Univ. of Fla. well .18

Lake Alice 2.9

Alachua Sink

Orman Annis

Municipal Airport

Sperry Rand Corp.


.16 .19


.24

1.5


2.7 2.9


< .01


"< .01


1.07 1.55

0.25

0.30

3.1

4.2 4.5

0.18 1.25

< .01

0.03























ORMAN ANNIS CITY WELL NO.
0.12 0.18 r 0.75 1.07
0.15 1.25 0.76 1.55

LAKE ALICE N.,.,CITY WELL NO. 6
2.9 1.5 0.14 0.16 0.25
2.4 3.1 0.17 0.19
0.15 0.24
UNIV. OF FLA. WELL ALACHUA SINK
0.18 0.25 2.7 4.2
0.12 0.24 2.9 4.5
0.20 0.30 3.3



Fig. 14 Total Phosphate in Water Within the Gainesville Area (ppm as PO)




















0.


ORMAN ANNIS *CITY WELL NO. 3
- 12 ._I 15 19
19 11

LAKE ALICE CITY WELL NO. 6
28 16 12 11 13
20 13 14 10

UNIV. OF FLA. WELL ALACHUA SINK
13 12 16 29
11 11 18 28
12 15 7


Fig. 15 Chloride in Water Within the Gainesville Area (ppm)














Table 30

Chloride in Water Uithin the Gainesville Area (ppm)


Nov.2 Nov.11 Nov.21 Nov.26 Dec.3 Dec.10 Dec.17 Jan.6 Jan.12 Jan.18 Feb.8


City well No. 3 15 12 15 19

City well No. 6 12 14 11 11 10 12 13

Univ. of Fla. well 13 11 12 12 11 15

Lake Alice 28 20 16 13 a

Alachua Sink 16 18 7 29 28

Orman Annis 9 19 12 11

Municipal Airport 5 4 5 8

Sperry Rand Corp. 8 7 12











ABS-LAS. The results obtained from the first few samples shoved

that the ABS-LAS content of the waters was near the lower limit of

detection and its determination on the remaining samples was omitted.

Apparently the biodegradability of the new detergents has virtually

eliminated ABS-LAS pollutants in this area.

Halogen demands. The chlorine demand of waters remained quite

unibfom during the sampling period except for Alachua Sink and Lake

Alice where substantial decreases were noted. Data which are presented

in Figure 16 and Table 31 show that the higher demands were found in

water from Lake Alice, Alachua Sink and well No. 3 with a lower demand

in well No. 6. Minimum values of from two to four ppm were obtained at

all other points.

Data from Figure 17 and Table 32 show that except for values

obtained at Lake Alice, the iodine demand of the waters increased during

the sampling period. Of particular interest is the three-fold increase

for well No. 3, the fbur-fold increase for well No. 6, and the increased

values at Alachua Sink. As shown in Figure 17, higher values were

obtained fbr Alachua Sink, Lake Alice and wells No. 3 and No. 6. All

other values ranged from two to six ppm.

The increase in iodine demand without a corresponding increase in

chlorine demand is difficult to understand. Chlorine being chemically

more active than iodine would be expected to show the greater increase.

In evaluating these data it is well to remember that even though the

iodine demand of the water at times was equal to or greater than the

chlorine demand on a ppm basis, the actual "kinetic" demand of iodine on
























ORMAN ANNIS *.,_CITY WELL NO.3
I. o 14.
3.0 14.0
3.0 13.0
LAKE ALICE CITY WELL NO.6
25.0 5.8 / .0 8.0 9.5
7.0 7.0 7.5
5.5
UNIV. OF FLA. WELL ALACHUA SINK
3.0 2.0 40.0 28.5
3.0 2.6 36.0 28.8
3.0 2.5 28.0



Fig. 16 Chlorine Demand of Water Within the Gainesville Area (ppm)
i














Table 31

Chlorine Demand of dater in the Gainesville Area (ppm)


Nov.2 Nov.11 Nov.21 Nov.26 Dec.3 Dec.10 Dec.17 Jan.6 Jan.12 Jan.18 Feb.8


City well No. 3

City well No. 6

Univ. of Fla. well

Lake Alice

Alachua Sink

Orman Annis

Municipal Airport

Sperry Rand Corp.


14.0

7.0

3.0

25.0


14.0

7.0 8.0 8.0

3.0


40.0 36.0


28.0

3.0


13.0 14.0

9.5

2.5

5.8

28.5 28.8

3.0 2.6

1.5

4.4




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