United States
          Environmental Protection
          Agency
Health Effects Research
Laboratory
Cincinnati OH 45268
EPA-600, 1-80-025
May 1980
           Research and Development
          Potential Health
          Effects from
          Persistent  Organics in
          Wastewater and
          Sludges Used for Land
          Application
EP 600/1
80-025
              U.S.
              EDISOJf.ir.j.  08817

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                RESEARCH REPORTING SERIES

Research reports of the Office of Research and Development, U.S Environmental
Protection Agency, have been grouped into nine series. These nine broad cate-
gories were established to facilitate further development and application of en-
vironmental technology.  Elimination of traditional grouping  was consciously
planned to foster technology transfer and a maximum interface in related fields.
The nine series are1

      1   Environmental  Health  Effects Research
      2   Environmental  Protection Technology
      3   Ecological Research
      4   Environmental  Monitoring
      5.  Socioeconomic Environmental Studies
      6   Scientific and Technical Assessment Reports (STAR)
      7   Interagency Energy-Environment Research and Development
      8   "Special" Reports
      9   Miscellaneous Reports
This report has been assigned to the ENVIRONMENTAL HEALTH EFFECTS RE-
SEARCH series This series describes projects and studies relating to the toler-
ances of man for unhealthful  substances or conditions This work is generally
assessed from a medical viewpoint, including physiological or psychological
studies. In addition to toxicology and other medical specialities, study areas in-
clude biomedical  instrumentation and  health research techniques utilizing ani-
mals — but always with  intended application to human health measures
 This document is available to the public through the National Technical Informa-
 tion Service, Springfield, Virginia 22161.

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                                          EPA-600/1-80-025
                                          May 1980
POTENTIAL HEALTH EFFECTS FROM PERSISTENT
   ORGANICS IN WASTEWATER AND SLUDGES
        USED FOR  LAND APPLICATION
                   by

            Vimala A. Majeti
                   and
             C. Scott Clark
   Department of Environmental Health
University of  Cincinnati Medical Center
         Cincinnati,  Ohio   45267
          Grant No. R805445-01
             Project Officer

           Herbert R. Pahren
         Field Studies Division
   Health Effects Research Laboratory
         Cincinnati, Ohio  45268
   HEALTH EFFECTS RESEARCH LABORATORY
   OFFICE OF RESEARCH AND DEVELOPMENT
  U.S. ENVIRONMENTAL PROTECTION AGENCY
         CINCINNATI,  OHIO  45268
                          ',.

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                                DISCLAIMER
     This report has been reviewed by the Health Effects Research Laboratory,
U.S. Environmental Protection Agency, and approved for publication.  Approval
does not signify that the contents necessarily reflect the views and policies
of the U.S.  Environmental  Protection Agency, nor does mention of trade names
or commercial products constitute endorsement or recommendation for use.

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                                  FOREWORD
     The U.S.  Environmental  Protection  Agency  was created  because  of in-
creasing public and government  concern  about  the dangers of pollution to the
health and  welfare of the American  people.   Noxious  air,  foul  water, and
spoiled  land  are  tragic  testimony  to the  deterioration  of  our  national
environment.  The complexity of that environment and the interplay  between its
components require a concentrated and  integrated attack on the problem.

     Research  and  development  is  that  necessary first  step  in  problem
solution and  it  involves defining the problem,  measuring  its  impact, and
searching for solutions.   The primary mission of the Health Effects Research
Laboratory in  Cincinnati (HERL)  is to  provide a sound health effects data base
in support  of  the regulatory activities  of the EPA.  To this end, HERL conducts
a research  program  to  identify, characterize, and quantitate  harmful effects
of  pollutants that may   result  from  exposure  to  chemical, physical,  or
biological  agents  found  in  the environment.   In  addition  to  the  valuable
health information  generated by these activities, new research techniques and
methods are being developed that contribute to better understanding of human
biochemical and physiological functions, and  how these  functions  are altered
by low-level insults.

     This  report  provides a general  assessment of the  potential  problems
which may occur when persistent organics contained in municipal sludges are
applied to land.   Since  information  on this  subject is sparce, examples of
problems which might occur if organic concentrations are excessive are drawn
from other  sources  such as refuse.  With a better understanding of any health
effects, measures can  be  developed to reduce  exposure to potentially harmful
materials.
                                   Director
                                   Health Effects Research Laboratory
                                    m

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                                  ABSTRACT


    The potential  health problems associated with the presence of persistent
organic chemicals  in wastewater and sludge,  when applied to agricultural
lands, are reviewed.  The type and amounts of organic chemicals present in
wastewater and sludge, their fate on land,and available control measures  are
discussed.  The potential health effects of organic chemicals  on workers/
populations who come in contact with them during wastewater treatment,  trans-
portation, and/or application are considered.  Examples are given from known
cases of acute exposure - Louisville, Kentucky;  Memphis, Tennessee;
Bloomington, Indiana; Toone-Teague, Tennessee; Love Canal, New York;  etc.,
since there is no direct information available on effects of long-term ex-
posure to organic chemicals in wastewater and sludge applied to agricultural
land.

    The effects of organic chemicals on the quality of ground  and surface
waters and on the food chain including the uptake by plants, animals, and
humans are also considered.  Examples are cited from known cases of  ground
and surface water contamination from leachates from chemical waste landfills
and from industrial waste discharges.  For the effect on the food chain,  the
Japanese incident of rice oil contamination by PCBs and the accidental  dairy
cattle feed contamination by PBBs in Michigan are reviewed.  It is emphasized
that the examples cited represent effects of acute exposure and, therefore,
may not be representative of potential contamination by organic chemicals of
food chains from land application.  It is believed that they might serve the
purpose of providing some insight into the effect of consuming low levels of
these chemicals through food chains over a long period of time.

    The review concludes that there is not sufficient information at present
to assess the full extent of long-term health risks of exposure to orgam'cs
in the wastewater treatment plants or at land application sites.  Recommen-
dations are made concerning guidelines and further research.  Further research
is recommended on the uptake of organic chemicals by food crops.  It is also
recommended that health surveys be carried out on populations that are known
to have consumed food grown on land application facilities.  Long-term follow-
up is also recommended for populations who have had acute short-term exposure
to organic chemicals from waste materials.

    This report was submitted in partial fulfillment of Grant No. R 805445-01
by the Department of Environmental Health, University of Cincinnati, under the
sponsorshop of the U.S. Environmental Protection Agency.  This report covers
the period February 22, 1978 to February 21, 1980.
                                     IV

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                                 CONTENTS
Foreword	,	  i i i
Abstract	,	,	,	   i v
Figures and Tab! es	   vi
Acknowl edgments	vi i i

   1.  Introduction	,	,	,	,	   1
   2.  Conclusions	,	   2
   3.  Recommendations	   3
            Policy/guidelines	   3
            Further research	,	,	   4
   4.  Characterization of Organic Chemicals in Wastewater  and  Sludge   5
   5.  Fate of the Organic Chemicals on Land	,	  15
   6.  Control of the Organic Chemicals	  17
   7.  Effect of the Organic Chemicals 	  23
            Effect on wastewater treatment plant workers	  23
            Effect on other populations	  24
            Water pollution	  25
                Surface water pol 1 uti on	  25
                Groundwater pollution	  27
            Effect on food chain	  29
                Physical contamination	  36
                Uptake by plants	  36
                Uptake by animals	  38
                Uptake by humans	  41

References	  45

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                             FIGURES AND TABLES
Number                             Figures                             Page
  1     Insecticide cycle	   30

                                   Tables
  1     Ranges of Concentrations of Organic Compounds in Municipal
          Wastewater Treatment PI ant Ef f 1 uents	    6
  2     Organic Compounds Identified in Muskegon System Wastewater....    8
  3     Concentration of Organic Compounds in Domestic Sludges	   10
  4     Curene 442 (MOCA) Levels in Wastewater, Sludge, River Water
          and Sediment, Soil and Air in Adrian, Michigan	   12
  5     National Interim Primary Drinking Water Standards	   18
  6     Toxic Pollutant Effluent Standards	   18
  7     Ambient Water Quality Criteria Proposed by EPA for Some
          Toxic Organic Pollutants	   19
  8     Maximum Acceptable Daily Intakes for Some Pesticides	   22
  9     Soil Pollutant Limit Values (Provisional)	   22
 10     Pesticides in the Environment and Their Toxicity	   31
 11     Human Health Criteria Proposed by EPA for Some Toxic
          Organic Chemicals in Ambient Water	   32
 12     Interim Human Health Effects Criteria Proposed by EPA
          for Some Carcinogenic Organic Chemicals in
          Ambi ent Water	   34
 13     FDA Tolerances for PCBs in Food and Food Packaging	   37
 14     FDA Recommendations to EPA on the Land Application of Sludge..   39
                                      VI

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                       FIGURES AND TABLES (continued)


Number                                                                 Page

 15     Some Pesticide Residues in Adipose Tissue of Cattle
          Fed Irradiated Sludge	   40

 16     Liver Function Tests of Michigan and Wisconsin Dairy
          Farm Residents	   43
                                     vii

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                             ACKNOWLEDGMENTS
    We wish to acknowledge the assistance provided by Mr. A. Komrichwarakool,
graduate student in the Department of Environmental Health, University of
Cincinnati, in searching the literature pertaining to this report.

    The assistance provided by Miss E. Widner, Head, Bibliographic Research
Division, Department of Environmental Health, University of Cincinnati, in
editing this report is also gratefully acknowledged.

    We also wish to extend our appreciation to Dr. G. L. Braude of the U.S.
Food and Drug Administration, Washington, D.C.,and Dr. G. F. Lee of the
Colorado State University, Fort Collins, Colorado, for their review of this
document and their comments and suggestions.

    We are also thankful to the Health Effects Research Laboratory, U.S.
Environmental Protection Agency, Cincinnati, Ohio, for providing financial
support for this work under Grant No. R 805445-01.
                                   vm

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                                 SECTION 1

                               INTRODUCTION


    Among all constituents of concern that are present in wastewaters and
sludges, the effects of the toxic organic chemicals are the least known.   Of
the chemical contaminants, heavy metals and persistent organic compounds  are
of most concern.  Most attention has been paid to the fate and effect of
heavy metals, little to the impact of persistent organic compounds.  Since
many heavy metals and organic chemicals will be in more concentrated form in
sludge than in wastewater, the latter may be considered less hazardous than
sludge, but there may be exceptions.  The potential problems that may be
caused by persistent organic compounds to the workers/populations who come in
contact with them during wastewater treatment, transportation, and/or appli-
cation; their effects on the food chain, on the quality of ground and surface
waters; and recommendations for the regulation of them will be considered in
this report.

    Little information is available on direct health effects of organic chem-
icals in wastewater and sludge applied to land.  Examples of known health
effects on wastewater treatment plant workers from acute exposure to toxic
organic chemicals are included where applicable.  Similarly, since there  is
no information available on groundwater and surface water pollution from
organic chemicals in wastewater and sludge applied to land, effects of toxic
organic chemicals leaching from industrial chemical waste landfills are
discussed briefly because of their potential for groundwater pollution.

    The reports of Jones and Lee (1), Dacre (2), Lennette and Spath (3),
Chang and Page (4), and Braude (5) form the background materials for parts
of this report.

    In order to assess the potential health risks of the organic chemicals
in wastewaters and sludge for the practice of the various forms of land
application and disposal, a number of factors need to be understood:

    (1)  The type and amounts of the organic compounds present in wastewaters
         and sludge;

    (2)  Their fate and potential environmental contamination;

    (3)  Available control measures; and

    (4)  Their effects on wastewater treatment plant workers, on populations
         living near land application facilities, on ground and surface water
         pollution, and on the food chain.

                                     1

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                                 SECTION 2

                                CONCLUSIONS
    At present there is not sufficient information to assess the long-term
health risk associated with exposure to organics in the wastewater treatment
plants or at land application sites.  Acute toxic effects are readily recog-
nizable.   The harmful  effects thereof can be most directly reduced by en-
forcement of appropriate pretreatment requirements.  If these are not
effective, harmful effects can possibly be reduced by removal of workers from
the source of toxic fumes, by proper ventilation and by the use of appropriate
respirators and protective clothing, etc., since the exposure to organic
chemicals is mainly by inhalation.   Effects of exposure to low levels of
organics over a long period of time (chronic exposure) including dose-
response relationships and health effects are not known at this time.

    Land application systems tend to concentrate chemicals in the soil en-
hancing the possibility of uptake by plants and animals.  If more complete
information on the concentration and fate of the organic chemicals in the
environment (water, air, food crops, animals, etc.) were known, it would be
possible to make an assessment of the potential hazards associated with the
land disposal of wastewaters and sludges containing hazardous organic
chemicals.  At the present time, sufficient information is not available to
do this.

    The potential for groundwater pollution from leaching of waste landfills
is a serious problem and adequate preventive measures should be instituted.
The potential for air pollution from landfills that have received a variety
of substances which may interact with each other has been given very little
attention.

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                                 SECTION 3

                              RECOMMENDATIONS
POLICY/GUIDELINES

    (1)  Pretreatment' standards for the discharge of industrial  wastes to
municipal sewerage systems should take into account downstream uses of the re-
ceiving body of water such as for crop irrigation; the nature of the specific
municipal wastewater treatment processes; the type of industrial waste; and
the prevalence of combined sewer discharges.

    (2)  Unless adequate pretreatment requirements are being enforced, land
application of wastewater or sludge containing relatively high concentrations
of hazardous contaminants should be limited to land not involved in food
production because there is only very limited information available on the
uptake of organic chemicals by vegetation.

    (3)  Sludges containing more than 10 ppm PCBs and/or significant amounts
of other toxic organic chemicals should not be permitted to be applied on
the surface of grazing lands since sludge may be ingested by animals and be-
cause of the tendency of many organics including PCBs to accumulate in lipid-
rich tissues and milk.

    (4)  Sludges containing high levels of persistent organic compounds should
not be used as animal feed supplement after disinfection alone.

    (5)  Wastes containing relatively high levels of persistent organic con-
taminants should be classified into categories such as:  (1) those suitable
to disposal in secure landfills, (2) those suitable only for destructive-
type disposal because of their hazardous nature or potential to produce
hazardous substances upon contact with other wastes, and (3) those suitable
under certain conditions for land application.

FURTHER RESEARCH

    (1)  Uptake of organic chemicals by food crops should be studied in de-
tail.  Since very little is known about the organics uptake by plants, all
parts of the plant should be studied.  (Some selectivity regarding the parts
of the plant can be exercised depending upon which parts of a given crop are
edible.)

    (2)  Full extent of groundwater pollution by organic chemicals leaching
from landfills and/or lands with buried sludge should be studied further.

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    (3)  Long-term follow-up should be initiated on populations who have had
acute short-term exposure to organic chemicals from waste materials.   Ex-
amples of such populations are those associated with exposures  at Love Canal,
New York, Toone-Teague, Tennessee,  and the Louisville,  Kentucky, and  Memphis,
Tennessee, wastewater treatment plants.

    (4)  The potential health effects of utilizing domestic sewage sludge as
a cattle feed supplement for both beef and dairy cattle should  be studied
further from the standpoint of organics passing through the food chain.

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                                 SECTION 4

       CHARACTERIZATION OF ORGANIC CHEMICALS IN WASTEWATER AND SLUDGE


    The presence of organic matter in raw and treated wastewater is highly
variable and dependent upon the source of wastewater and the degree of
treatment.  Attempts to characterize organic matter in wastewaters in the
past have not been very successful.  It is only recently that the extensive
identification of organic compounds in waters, drinking water in particular,
has been undertaken.  A summary listing of some 1000 organic compounds in
effluent waters has been published by the Horld Health Organization (WHO)
(6).   Many of these organics have been identified in raw sewage.
Some of these compounds are very toxic and some of them are known or sus-
pected carcinogens as reviewed in a research report to Congress by the Na-
tional Academy of Sciences, National Research Council (7).   Chlorination of
treated wastewater results in the formation of a wide range of chlorinated
derivatives (8).   Many of the organic chemicals present in wastewater are
toxic and potentially carcinogenic, teratogenic,or mutagenic to humans.  A
relatively large number of organic compounds survive the conventional treat-
ment process and are present in the treated effluent in the yg/1 range.  The
sources of these compounds are difficult to trace except when there is an
accidental spill such as from the local industrial plants.

    In the past few years there have been significant efforts toward de-
termining the nature and concentrations of the organic compounds present in
wastewaters and sludges.  Some work in this area has been devoted to
chlorinated hydrocarbons, pesticides, and PCBs.  EPA Office of Research and
Development has been conducting a survey of chlorinated hydrocarbons in
municipal wastewater effluents which showed the presence of chlorophenols,
chlorobenzenes, chloralkanes, and chloroalkenes (9).   Table 1 lists some of
the organic compounds together with the range of concentrations found in
municipal wastewater effluents (1,10,11).  A number of new compounds have been
found in the Muskegon untreated wastewaters in addition to some of the com-
pounds identified by others (11) (Table 2).  The concentration of chlori-
nated hydrocarbon pesticides and other organic compounds identified in
several wastewater sludges are presented in Table 3 (1,12,13).

    Sludges from Schenectady, New York, and Bloomington, Indiana, were found
to contain 23.1 ppm(14)and 300 ppm(15)pCBs, respectively.  General
Electric Company in Schenectady, New York, and Westinghouse Electric in
Bloomington, Indiana, both manufacture electrical capacitors in which PCBs
are used as insulating fluids.  Further, the sediments from Hudson River
below Schenectady and other streams near Bloomington were found to be con-
taminated with PCBs (15,16).  PCBs levels as high as 2980 ppm were found in

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-------
TABLE 2. ORGANIC COMPOUNDS IDENTIFIED IN
MUSKEGON SYSTEM WASTEWATER (11)

Pollutant5
Wastewater Sampled3
Aerated Holding
lagoon lagoon
Influent effluent effluent

Final
effluent
Dichloromethane (c)
1,2-Dichloroethane (c)
1,2-Dichloroethylene (c)
Toluene
Xylene (d)
Acetone
Dimethyl sulfide
3-Pentanone
Dimethyl disulfide
Dichlorobenzidine (c)
Phenol (c) (d)
Ethyl benzene (c)
Trichlorobenzene (c)
Diazobenzene
Dichlorobenzophenone
Aniline (d)
N-Ethylaniline
N,N-Diethyl aniline
N,N-Dimethylaniline (d)
Chloroaniline (d)
Benzothiazole
Benzyl alcohol (d)
Cresol (d)
Methoxy phenol (d)
Hydroxymethoxyacetophenone
Dimethoxyacetophenone
Chloropropiophenone
Hexanoic acid
Decanoic acid (d)
Dodecanoic acid
Tetradecanoic acid
Hexadecanoic acid
Heptadecanoic acid
Octadecanoic acid
a-Pinene
3-Pinene
a-Terpineol
Trithiapentane (d)
Tetrathiahexane (d)
2-Ethyl-l-hexanol
Isoborneol
                                (continued)

                                     8

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                             TABLE 2 (continued)

Wastewater Sampled3
Pollutantb Influent
Decanol +
Dodecanol +
Tetradecanol +
2-(2~(2-ethoxyethoxy)ethoxy)ethanol +
Tetradecene
Trimethyl i socyanurate
Atrazine
Heptanoic acid (e)
Octanoic acid (e) +
Nonanoic acid (e) +
Pentadecanoic acid (e)
0-Phenyl phenol (e) +
Benzoic acid (e) +
Phenylacetic acid (e) +
Salicylic acid (e) +
Phenylpropionic acid (e) +
Vanillin (e) +
Acetovanillin (e) +
Homovanillin (e) +
2-(4-Chlorophenoxy)2-methyl +
propionic acid (e)
Aerated Holding
lagoon lagoon Final
effluent effluent effluent
_ _ _
+ - +
- - +
_
+
+ +
- - +
(f) +
(f) +
(f) +
(f) +
(f)
(f) +
(f)
(f)
(f)
(f)
(f)
(f)
(f) +


a.  Presence or absence of pollutant in wastewater is indicated by + or -
    "?" indicates presence suspected but not confirmed beyond reasonable
    doubt.

b.  Unless  noted otherwise, listed compounds were identified in daily
    samples at RSKERL.

c.  Compounds appearing on the EPA "List of Dangerous Pollutants."

d.  Identified in both daily samples at RSKERL and composite samples at AERL.

e.  Identified in composite samples at AERL.

f.  Composite samples of aerated lagoon effluent were not obtained.

-------
TABLE 3.  CONCENTRATIONS OF ORGANIC COMPOUNDS IN DOMESTIC SLUDGES (l,12,13)a
                            yig/1  LIQUID SLUDGE

Compound
% Solids in sludge
Chlorinated hydrocarbon
pp'DDT
op 'DDT
pp'DDE
pp'DDD
Total DDD/DDE/DDT
DDT
a-Chlordane
y-Chlordane
Total chlordane
isomers
Heptachlor
Heptachlor epoxide
Total heptachlor
Aldrin
Dieldrin
Lindane
Toxaphene
Total organochlorine
pesticides
PCBs
(Arochlor 1254)d
North
Toronto1"1
6.25
pesticides
1.33
6.87
•7.18
4.31
19.69
-
15.79
12.56

28.35
5.37
3.04
8.41
2.03
3.03
1.48
-

63

214
Point
Edward b
6.90
and PCBs:
0.77
4.11
3.68
3.98
12.54
-
12.51
11.41

23.92
2.29
1.77
4.06
1.09
1.69
1.16
-

45

108
Newmarket^
12.2

1.12
1.15
2.18
1.60
6.68
-
5.69
2.84

8.53
0.70
0.58
1.28
0.70
1.65
0.63
-

20

74
Sarniab
16.19

2.70
5.25
20.77
6.41
35.13
-
16.99
12.92

29.91
14.95
6.78
21.73
9.40
3.23
3.22
-

103

1122
MSDGCC


-
-
-
-
-
< 100
-
-

< 10
< 200
< 200
-
< 10
< 10
< 500
< 10

-

-
Other pesticides and organics:
Orthophosphates and
carbamate insecticides
2,4-D
2,4,5-T
2,4,5-TP

-
-
-
-

-
-
-
-

-
-
-
-

-
-
-
-

< 10
<1000
< 5
< 30

Dash (-) indicates no data found (none detected).
a.  Reprinted from "Risk Assessment and Health Effects of Land Application of
    Municipal Wastewater and Sludges" with permission of B.P.  Sagik and C.A.
    Sorber, eds., The University of Texas at San Antonio, San Antonio, TX (1978).
b.  Chawla et al. (12).  Mean levels of organochlorine pesticides in digested
    chemical sludges in four Ontario treatment plants using  lime (Newmarket),
    iron (North Toronto, Sarnia) or alum (Point Edward) treatment.
c.  McCalla et al. (13).  Concentrations in sludges from five  sludge sources
    in the Metropolitan Sanitary District of Greater Chicago (MSDGC), solid
    content of the sludges unknown.
d.  Mean.monthly levels (12).
                                     10

-------
Hudson River sediment (17).  PCB concentrations in sludges from 33 munici-
palities in Ontario, Canada, were surveyed by Shannon et al. (18).  PCB levels
in untreated wastewater ranged from<0.1 to 1.8 ppb, while the levels in
digested sludge ranged from 0.6 to 76.6 ppm (dry weight).  Municipal sludge
in Hopewell, Virginia, was found to be contaminated by kepone, a chlorinated
pesticide manufactured by Life Science Products which discharged kepone waste
into the city sewage system (19).   Kepone levels of 0.1 - 10 ppm were found
in the sludge samples from the holding pond and from the landfill near the
Hopewell Sewage Treatment plant.  Fish and shellfish from the James River near
Hopewell were found to contain 0.1 - 20 ppm kepone (20).  The concentration
of two PCBs in sludge from a number of municipal wastewater plants in
Michigan ranged from less than 0.1 mg/1 to 352 mg/1 (21,22).  As would be
expected, the concentrations of the organics are considerably greater in
sludges than in wastewater.

    The wastewater and sludges at  the wastewater treatment plant, Raisin
River water and sediment, roadside soil and air in Adrian, Michigan were
found in early 1979 to be widely contaminated with Curene 442 (MOCA, 4,4'-
Methylene-bis(2-chloroaniline), a  potential human carcinogen (23).  Curene
442 is used as a curing agent for  isocyanate-containing polymers and
polyurethane elastomers.  The source of contamination was traced to discharges
received by the Adrian Wastewater  Treatment Plant from Anderson Development
Company over a period of several years.  Curene 442 is not very soluble in
water and therefore tends to accumulate in sludges and soils.  The Anderson
Development Company also has a highly contaminated storage lagoon.  Soil
samples taken in April 1979 at the Anderson Development Company plant site
and in the adjacent neighborhood showed concentrations of up to 590 ppm of
Curene 442.  Anderson Development  Company has discontinued production of
Curene 442 in February 1979 by order of Michigan Department of Natural Re-
sources.  The amounts of Curene 442 (MOCA) found in the wastewater treatment
plant effluents and sludges, Anderson Development Company lagoon water and
sediment, Raisin River water and sediment, roadside soil and air in Adrian,
Michigan are listed in Table 4 (23).  As can be seen from Table 4, the Curene
442 (MOCA) contamination in Adrian, Michigan is widespread.

    Although the list of compounds shown in Tables 1-3 is quite extensive,
it is by no means exclusive, as to the total number or types of organic com-
pounds present.  At present the identification of organic compounds in waste-
waters and sludges is limited by the volatility of the compounds and the
available analytical techniques.  Most organic compounds which come directly
from industrial effluents or are metabolites or degradation products can
not be readily detected or determined by the available analytical procedures.
This is especially true for compounds with high molecular weights and with
more hydrophilic compounds.
                                      11

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  TABLE 4.   CURENE 442a (MOCA)b LEVELS IN WASTEWATER,  SLUDGE,  RIVER WATER
 	AND SEDIMENT. SOIL AND AIR IN ADRIAN,  MICHIGAN  (23)	
 Date         Type and location
sampled	of sample	
                            Curene 442a
                              (MOCA)b
                 Source/Comments
2/7/79
2/28/79


3/12/79 to
3/13/79
3/13/79



3/13/79




5/12/79



2/7/79
3/13/79


5/12/79
Wastewater (yg/1)
Adrian WWTPC
  Influent
  Effluent
  Lagoon effluent
Adrian sanitary sewer
  at ADCe lagoon outfall
Adrian eastside drain
  water
Adrian eastside drain
  sediment
Adrian WWTPC
  runoff from sludge field
Adrian eastside drain
  water
Adrian eastside drain
  sediment
Process wastewater dis-
  charged by ADCe to
  Adrian WWTPC
     3.00
     4.10
  2800.00

  1200.00

     2.00

  1200.00


   140.00


     6.80

11,000-95,000.



   230-440.00
Water Quality Division,
MDNRd
Environmental Services
Division, MDNRd
Environmental Services
Division, MDNRd
                                                    00
Adrian WWTPC effluent          1.00
Adrian eastside drain water    1.00
ADCe lagoon water            250-350.00


Adrian WWTPC influent          0.50
Adrian WWTPC effluent          0.30

Sludge (mg/kg)
ADCe lagoon sludge          2000,00

Adrian WWTPC
  Return sludge                0.006
  Digested sludge              1.70

ADCe lagoon sediment      16,000,00
Adrian WWTPC sludge           18.00

Adrian WWTPC sludge
  from dry beds               86.00
Environmental Pro-
tection Bureau,
MDNRd
Analytical Laboratory
Division of Chemical
Technology, U.S. FDA,
Washington, D.C.

Environmental Pro-   .
tection Bureau, MDNR
                 Water Quality Division,
                 MDNRd
                 U.S.  FDA, Washington,
                 D.C.

                 Environmental  Pro-
                 tection Bureau, MDNRd
                                 (continued)


                                     12

-------
                              TABLE 4 (continued)
 Date
sampled
   Type and location
       of sample
  Curene 4429
    (MOCA)b
Source/Comments
3/12/79 to
3/13/79
2/7/79


2/28/79


3/13/79


6/27/79 to
6/28/79



2/28/79




4/5/79


5/4/79
5/8/79



5/29/79
River Water and Sediment

South branch Raisin
  River water
South branch Raisin
  River sediment

Groundwater (yg/1)

ADCe well water


Adrian WWTPC dewatering
  well
ADCe well water

Adrian WWTPC observation
  well

Soil
Adrian WWTPc-soil sample
  near well A
Adrian WWTPc-soil sample
  near well B
Adrian public roads,
  surface soil
Adrian public roads
  surface soil
  4/10 mile from ADCe
  3/4 mile from ADCe
  over 1 mile from ADCe
    <0.10 yg/1
 1.30-9.60 mg/kg
   200.00



    <0.10

     1.50



     0.30




   1600 yg/kg

   6500 yg/kg

<0.05-590 ppm
  W/W
                                         13 ppm W/W
                                        1.3 ppm W/W
                                        2.1 ppm W/W
Environmental Services
Division, MDNRd
Adrian residential sampling-
  vacuum cleaner dust from
  homes near ADCe          1.8-21 mg/kg
Garden soil from homes
  near ADCe
   Soil surface
   Soil 2-6" subsurface
   Soil 6-10" subsurface
                                       0.08-2.90 ppm
                                       0.02-0.86 ppm
                                       0.01-0.07 ppm
Water Quality Division,
MDNRd

Environmental Services
Division, MDNRd

U.S. FDA, Washington,
D.C.

Water Quality Division,
MDNRd
Environmental Services
Division, MDNRd
Air Quality Division,
MDNRd

Environmental Enforce-
ment Division, MDNRd
                 Environmental Enforce-
                 ment Division, MDNRd
                 Michigan Department
                 of Agriculture
                                 (continued)


                                     13

-------
                             TABLE 4 (continued)

Date
sampled
5/24/79 to
6/6/79
Type and location
of sample
Air
Air samples in Adrian
surrounding ADCe
Adrian area dust
surrounding ADCe
Curene 442a
(MOCA)b
4.57 ng/rn^
23 ppm
Source/Comments
Air Quality Division,
MDNRd

a.  Anderson Development Company's trade name for 4,4'-methylene-bis(2-
    chloroaniline).
b.  Dupont Company's trade name for 4,4'-methylene-bis(2-chloroaniline)
c.  Wastewater treatment plant.
d.  Michigan Department of Natural Resources.
e.  Anderson Development Company.
                                     14

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                                 SECTION 5

                FATE OF THE ORGANIC CHEMICALS ON LAND (4,24)


    Several investigations have been conducted to determine the fate of
disease-causing microorganisms, nitrogen, and phosphorus in the wastewater
during the course of land application.   Little is known at the present time
about the fate of potentially toxic chemicals in the wastewater and their
possible pathways in soils.  Hazardous  substances in wastewater that are not
removed during the treatment process may pose a present or potential long-
term danger  to human health or to other living organisms because they are
often  nonbiodegradable, bio-accumulate,or persistent in the environment.

    The concentrations of organic chemicals are usually low (vg/1) in treated
wastewater effluents and sludges.  Repeated application on land may result in
accumulation of organic chemicals in soil.  The ionizability, water solu-
bility, and structure-function relationships (25) of the organic chemicals
determine to a great extent their ultimate fate and behavior in soil and
the environment.

    The behavior and decomposition pathway of many pesticide residues which
constitute a significant fraction of the persistent organics in soils has
been studied for many years (26).  Organic chemicals in wastewater and
sludge applied to land could be expected to be influenced by the same pro-
cesses that affect the fate and behavior of organic pesticides.  Some of the
processes that can cause the breakdown  of pesticides are photodecomposition,
chemical and microbiological decomposition, and detoxification by crop plants
or weeds.  Several factors such as pH,  surface activity and solubility affect
the degradation rate.  Microbial degradation is influenced by the microbial
population and by factors affecting microbial activity.  Simple organic com-
pounds such as aliphatic and phenolic acids, amino acids and sugars are
readily decomposed by soil microorganisms.  Highly chlorinated or halogenated
compounds, and compounds with branched  chains and higher molecular weight,
are more resistant to biodegradation and require longer periods of time to
decompose in soils.   Transfer processes move and dilute the pesticides keeping
their chemical structures intact..  These include:

    (1)  volatilization,

    (2)  movement into and out of plants by adsorption and exudation,

    (3)  retention by crop plants and weeds in small amounts,

    (4)  runoff into streams and lakes,

                                     15

-------
    (5)  movement downward into the soil  in percolating water and upward
         from lower depths by capillary flow, and

    (6)  adsorption and inactivation by soil  constituents (24).

    The adsorption phenomena of soils could increase the organic chemical  con-
centration at the soil  surface and, therefore, make them more susceptible   to
microbial decomposition.   The adsorption generally decreased in  the order:
organic matter > vermiculite > montmorillonite > illite > chlorite >
kaolinite (4).  Adsorption of organic pesticides by soil also characteristi-
cally increases as the  concentration of functional groups such as primary,
secondary and tertiary  amines, amides, carboxyl, and phenolic groups increase.
The presence of organic substances usually increases the adsorption affinity.
The pesticides can also be effectively bonded with iron and aluminum oxides
at proper soil pH ranges  (4).  Both laboratory and field studies indicate
that many pesticide residues adsorb to surface soils with only a few migrating
to depths of 30-60 cm in  soil (27).  Besides adsorption of organic pesticides
and other chemicals by  soil, chemical reaction with functional groups on
humates can also occur.  The immobilized organic substances in soils are
subsequently subject to chemical  or photochemical decomposition, volatil-
ization and microbial decomposition.  With existing data it is difficult to
project the long-term effectiveness and the consistency of soil  mantle to
immobilize and detoxify hazardous substances in wastewater.  Therefore,
adequate studies should be done to determine the actual fate of the chemical
contaminants present in wastewaters and sludges.

    The study conducted at Muskegon, Michigan, focused on the behavior of
many of these compounds in land disposal  (11).  The study showed that the
concentrations of many  of the chemicals present in raw wastewater following
spray irrigation were reduced below the detection limits in the effluent by
treatment consisting of an aerated lagoon and filtration through several
feet of sand.  From Table 2, it appears that the majority of the removal
took place in the storage lagoon and in the spray irrigation-percolation
system.
                                     16

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                                 SECTION 6

                      CONTROL OF THE ORGANIC CHEMICALS
    Control of organic chemicals can be in the form of discharge standards
for organics in wastewater effluents.   EPA has proposed standards for
drinking water (Table 5) (28) and for some toxic effluents (Table 6) (29,30).
Water quality criteria proposed by EPA for some toxic organic chemicals that
would form the basis for state water quality standards and EPA toxic effluent
standards are listed in Table 7 (31-33).  These criteria are an indication of
the maximum concentration of a pollutant in water which, when not exceeded,
will insure protection of specified water use.  Dacre proposes SPLVs (soil
pollutant limit values) to control the hazard loads of toxic chemicals in
soils (2).  These values may be compared with Threshold Limit Values (TLVs),
which refer to airborne concentrations of substances and represent conditions
under which it is believed that nearly all workers may be repeatedly exposed
day after day without adverse effect.   The control measures should take into
account acceptable daily intake (ADI)  values.  ADI values estimated by World
Health Organization for some pesticide chemicals to which man may be exposed
are shown in Table 8 (34,35).  The ADI values and SPLVs could possibly be
adapted for municipal wastewater effluents and sludges.  Table  9 lists
SPLVs for some of the insecticides identified in sludges (2).
                                    17

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TABLE  5.  NATIONAL INTERIM PRIMARY DRINKING WATER STANDARDS  (28)
          MAXIMUM CONTAMINANT LEVELS (mg/P
       Endrin                               0.0002
       Lindane                              0.004
       Methoxychlor                         0.1
       Toxaphene                            0.005
       2,4-D                                0.1
       2,4,5-TP                             0.01
 TABLE  6.   TOXIC  POLLUTANT  EFFLUENT  STANDARDS  (29,30)
	(yg/D	
       Aldrin/Dieldrin                      0.003
       DDT  (ODD,  DDE)                       0.001
       Endrin                               0.004
       Toxaphene                            0.005
       PCBs                                0.001
       Benzidine                            0.1
                           18

-------
    TABLE 7.  AMBIENT WATER QUALITY CRITERIA PROPOSED BY EPA
	FOR SOME TOXIC ORGANIC POLLUTANTS (31-33)	
                            Freshwater aquatic lifeSaltwater aquatic life
                            24 hr. average (ceiling)  24 hr. average (ceiling)
Organic Pollutant                   yg/1                      pg/1

Acenaphthene110 (240)7.5 (17)~

Acrolein                         1.2 (2.7)                   0.88 (2.0)

Acrylonitrile                    130 (300)                   130 (290)

Aldrin/Dieldrin                  0.0019 (1.2)                0.0069 (0.16)

Benzene                         3100 (7000)                  920 (2100)

4-Bromophenyl phenyl ether       6.2 (14)

Carbontetrachloride              620 (1400)                 2000 (4600)

Chlordane                        0.024 (0.36)                0.0091 (0.18)

Chlorinated benzenes

  Chlorobenzene                 1500 (3500)                  120 (280)
  1,2-Dichlorobenzene             44 (99)                     15 (34)
  1,3-Dichlorobenzene            310 (700)                    22 (49)
  1,4-Dichlorobenzene            190 (440)                    15 (34)
  1,2,4-Trichlorobenzene         210 (470)                   3.4 (7.8)
  1,2,3,5-Tetrachlorobenzene     170 (390)                   2.6 (5.9)
  1,2,4,5-Tetrachlorobenzene      97 (220)                   9.6 (26)
  Pentachlorobenzene              16 (36)                    1.3 (2.9)

Chlorinated ethanes

  1,2-Dichloroethane            3900 (8800)                  880 (2000)
  1,1,1-Trichloroethane         5300 (12,000)                240 (540)
  1,1,2-Trichloroethane          310 (710)
  1,1,1,2-Tetrachloroethane      420 (960)
  1,1,2,2-Tetrachloroethane      170 (380)                    70 (160)
  Pentachloroethane              440 (1000)                   38 (87)
  Hexachloroethane                62 (140)                   7.0 (16)

Chlorinated phenols
  2-Chlorophenol                  60 (180)
  4-Chlorophenol                  45 (180)
  2,4,6-Trichlorophenol           52 (150)
  Pentachlorophenol              6.2 (14)                    3.7 (8.5)

Chloroform                       500 (1200)                  620 (1400)

                                (continued)


                                     19

-------
                        TABLE 7  (continued)
Organic pollutant
Freshwater aquatic life
24 hr. average (ceiling)
        yg/1
Saltwater aquatic life
24 hr. average (ceiling)
        yg/1
1 -Chi oronaphthalene

Cyanide

DDT and metabolites

Dichloroethylenes
  1,1-Dichloroethylene
  1,2-Dichloroethylene

2,4-Dichlorophenol

Dichloropropanes
  1,1-Dichloropropane
  1,2-Dichloropropane
  1,3-Dichloropropane

1,3-Dichloropropene

2,4-Dimethylphenol

Dinitrotoluenes
  2,3-Dinitrotoluene
  2,4-Dinitrotoluene

1,2-Diphenylhydrazine

Endosulfan

Endrin

Fluoranthrene

Halomethanes
  CH3C1
  CH3Br
  CH2C12
  CHBr3

Heptachlor

 Hexachlorocyclopentadi ene
      29 (67)

     1.4 (3.8)

     0.00023 (0.41)
     530 (1200)
     620 (1400)

     0.4 (110)
     410  (930)
     920  (2100)
    4800  (11,000)

      18  (250)

      38  (86)


      12  (27)
     620  (1400)

      17  (38)

     0.042  (0.49)

     0.002  (0.10)

     250  (560)


    7000  (16,000)
     140  (320)
    4000  (9000)
     840  (1900)

     0.0015 (0.45)

     0.39 (7.0)

    (continued)
    2.8 (6.4)



    0.0067 (0.021)


   1700 (3900)
    400  (910)
     79  (180)

    5.5  (14)
    4.4  (10)
     0.0047  (0.031)

     0.3  (0.69)
    3700  (8400)
     170  (380)
    1900  (4400)
     180  (420)

     0.0036 (0.05)
                                      20

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TABLE 7 (continued)

Freshwater aquatic life Saltwater aquatic life
24 hr. average (ceiling) 24 hr. average (ceiling)
Organic pollutant yg/1 yg/1
Isophorone
Lindane
Nitrobenzene
Nitrophenols
2-Nitrophenol
4-Nitrophenol
2,4-Dintrophenol
2 ,4-Di ni tro-6-methylphenol
2 ,4 ,6-Tri ni trophenol
2100 (4700)
0.21 (2.9)
480 (1100)

2700 (6200)
240 (550)
79 (180)
57 (130)
1500 (3400)
97 (220)
--
53 (120)

53 (120)
37 (84)
150 (340)
PCBs                              0.0015 (6.2)            0.024 (0.20)



Phenol                            600 (3400)



Tetrachloroethylene               310 (700)                79 (180)



Toluene                          2300 (5200)              100 (230)



Toxaphene                         0.007 (0.47)            0.019 (0.12)



Trichloroethylene                1500 (3400)
                                      21

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TABLE 8 .  MAXIMUM ACCEPTABLE DAILY INTAKES FOR SOME PESTICIDES (34,35)
                        (rag/kg body wt/day)
        Aldrin                      0.0001
        Dieldrin                    0.0001
        Endrin                      0.0002
        Chlordane                   0.001
        DDT                         0.005
        Heptachlor                  0.0005
        Lindane                     0.0125
        2,4-D                       0.3
     TABLE  9.  SOIL POLLUTANT LIMIT VALUES (PROVISIONAL)  (2)
                          (mg/kg dry soil)
        Aldrin                      0.0024
        Dieldrin                    0.0024
        Endrin                      0.0048
        Chlordane                   0.024
        DDT (ODD, DDE)              0.0000002
                                 22

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                                 SECTION 7

                     EFFECT OF THE ORGANIC CHEMICALS


EFFECT ON WASTEWATER TREATMENT PLANT WORKERS

(a)  The workers at the wastewater treatment plant in Adrian, Michigan were
exposed to Curene 442 (MOCA, Methylene-bis(2-chloroaniline)) in wastewater
and sludges over a period of several years (23).  The source of Curene 442 was
discharges from Anderson Development Company in Adrian, Michigan.  Based on
tissue culture carcinogenicity tests and animal test studies in mice, rats,
and female beagle dogs, National Institute of Occupational Safety and Health
(NIOSH) considered Curene 442 (MOCA) a potential human carcinogen (36).
Curene 442 has a very low solubility in water.   It also has very low vapor
pressure.  Therefore Curene 442 tends to accumulate in sludges and soils.  It
is reported to be readily absorbed through skin.  Workers handling sludge
would, therefore, be at a potential risk from exposure to Curene 442.  The
Michigan Department of Public Health analyzed urine specimens from Adrian
wastewater treatment plant operators for Curene 442 in May 1979 but found no
evidence of its presence.  However, Curene 442 was detected in the blood and
urine specimens of Anderson Development Company's workers.  There are no con-
clusive epidemiological studies at present on which an evaluation of the
carcinogenic risk to Adrian wastewater treatment plant workers can be based.

(b)  Several acute toxic effects have been reported by the treatment plant
workers at the Morris Forman Plant in Louisville, Kentucky, and at the North
Treatment Plant in Memphis, Tennessee, when exposed to toxic pesticide
chemical wastes.  In Louisville, Kentucky, the exposure was a result of un-
authorized use in March 1977 of a combined sewer for the dumping of a highly
toxic pesticide waste material  containing hexachlorocyclopentadiene (Hexa)
and octachlorocyclopentene (Octa) (37-39).  Workers involved in the steam
cleaning of the mechanical screen complained of eye irritation, burning skin
above the arms and face, sore throat and symptoms similar to bronchitis.
Airborne concentrations of Hexa at the time of exposure were unknown but four
days after the episode, the air concentrations in the primary treatment areas
(screen and grit chambers) ranged from 270-970 ppb.  By comparison, the
recommended TLV for occupational exposure to Hexa is 10 ppb (40).  The in-
cident forced the treatment plant to shut down the operation voluntarily
from March 29, 1977 to June 5,  1977 resulting in the discharge of untreated
sewage containing toxic chemical waste directly into the Ohio River.

    In Memphis, Tennessee, the situation is not a one time dumping of toxic
chemical waste but an apparent continuous entry of the wastes into the
treatment plant from a pesticide formulator  since it was first opened in


                                     23

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1977.  Ironically, the waste material  that was dumped into  the Louisville
sewer system is believed to have originated from the same company.   The ex-
posure at both plants is to the same pesticide material,  except that in
Memphis, Tennessee, there are many other chemicals present besides Hexa.  Also
in Memphis, Tennessee, the exposure is one of an almost continuous nature to
variable but generally low levels of these chemicals whose  long-term toxic
effects are not known.  Acute effects were reported when the discharge was
heavy (41,42).

(c)  Eight workers at the wastewater treatment plant in Bloomington, Indiana,
were exposed to PCBs discharged by the Westinghouse Corporation.   Analyses of
tissue samples showed that PCBs were present in all  eight workers.   Two of
these workers, who had previously worked at the Westinghouse plant, had PCBs
levels of 10.4 and 10.1 ppm (lipid basis).  The other six had an average
level of 6 ppm.  The levels found in these workers are higher than levels
found in a national  monitoring survey in which only 5% out  of a total 637
tissue samples tested had levels higher than 2 ppm.   Even though the acute
toxicity of PCBs is  low, the long-term effects of exposure  to PCBs are not
known and experiments with laboratory animals have associated PCBs with still-
births, miscarriages and various metabolic disorders.  The  toxic effects of
ingestion of PCBs on humans had been demonstrated in a 1968 episode in Japan
where a batch of rice oil was accidentally contaminated by  PCBs (discussed on
page 41) (15,43).

    There is no information available at present on the health effects of
organics on workers  involved in the transportation and/or land spreading of
wastewater or sludge.

    Information from the study of health effects of pesticides in agricultural
use may be useful in this respect.  An evaluation of agricultural exposure
was not included in  this review.

EFFECT ON OTHER POPULATIONS

(a)  No information  is available at present on the effects  of organics in
wastewaters and sludge on populations living near wastewater treatment plants.

(b)  No information is available at present on the health effects of organics
on populations living near facilities where land application is practiced.
At present there are only a few epidemiological studies being conducted on
the potential health risks associated with the land application of waste-
water and/or sludge to agricultural lands, some of which follow:

      (i)  A retrospective and a prospective study in Israel on populations
           engaged  in land application of wastewater (44);

     (ii)  A prospective study by Ohio Farm Bureau on potential health effects
           to farmers involved with land application of sludge (45);

     (iii)  A short-term prospective study of the workers at a wastewater spray
           irrigation facility in Muskegon, Michigan (46).


                                      24

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Of these, only the study at Muskegon, Michigan, is taking into consideration
the potential health effects of organic chemicals.

(c)  Two examples of populations affected by leachates from industrial waste
landfills are:

      (i)  In Toone, Tennessee, residential drinking water supplies were con-
           taminated by chlorinated pesticide waste chemicals leaching from
           an old landfill that was used by Velsicol Chemical Corporation for
           dumping chlorinated pesticide residues from its Memphis, Tennessee,
           operation (47,48).  Some of the symptoms that have been noticed
           since the fall of 1977 which the residents associate with the con-
           tamination of their water supplies are - skin and eye irritation,
           weakness in joints and persistent cough (49).

     (ii)  In Love Canal, Niagara Falls, New York, where houses and an
           elementary school were built on an old Hooker Chemical Company
           landfill site, the chemicals leached into the groundwater and were
           brought back to the surface by rising water tables causing ground-
           water and air pollution.  The rate of miscarriages in this commu-
           nity are reported to be one to five times higher than expected and
           an excess of birth defects was also noticed (5.0).  However, data
           to support their conclusions have not yet been published.  Many
           of the residents of this community were evacuated from their homes.

Even though these landfills are not in use now, they are discharging long-
abandoned toxic waste chemicals into air and water.  Ironically, Hooker
Chemical waste and Velsicol Chemical waste in the past were very similar since
some of their products were similar.


WATER POLLUTION

(a)  Surface Water Pollution:  Lateral  dispersion by runoff can cause surface
water pollution by organic chemicals with the possibility of contaminating
drinking water supplies.   However,  there are no published accounts of
situations where surface drinking water supplies  have been contaminated by
organic chemicals in wastewaters and sludge used  for land application.   Sur-
face water pollution by organic chemicals can also result from chemical waste
discharges from industries.   Some examples follow:

      (i)   Raisin River Pollution by Curene 442 (MOCA)  in Adrian. Michigan
           (1979) (23): The wastewater and sludges at the wastewater treatment
           plant in Adrian,  Michigan,were contaminated with Curene 442 (MOCA)
           which was discharged by Anderson Development Company.   The waste-
           water treatment plant discharges effluents into the Raisin River.
           The water and sediment of the Raisin River wece found to be con-
           taminated with Curene 442 (MOCA)  (Table 4).   The Michigan De-
           partment of Public Health has expressed concern for the com-
           munities of Blissfield,  Deerfield,and  Dundee who use the Raisin
           River as a drinking water supply.


                                     25

-------
 (ii)   Hudson  River  Pollution  by  PCBs  (1974)  (16):  Hudson River has been
       contaminated  by  PCBs discharged from two General Electric plants  in
       Fort  Edward -  Hudson Falls area about  40 miles north of Albany.
       The General Electric plants manufacture electrical capacitors in
       which PCBs are used as  insulating fluids.  General Electric was
       one of  the largest users of PCBs manufactured by the Monsanto
       Company, and  about 30 pounds of PCBs were discharged into the
       Hudson  River  every day.  The discharges appear to have declined
       to less than  10  pounds  per day  in recent years.  PCBs are
       chlorinated hydrocarbons similar to DDT.  They are insoluble in
       water,  highly resistant to heat, and not readily decomposed, thus
       making  them very persistent environmental contaminants.  They
       accumulate in river-bottom sediments because of their insolubility
       in water.  Analyses of  water and sediment samples in Hudson River
       during  the years 1973 and  1974  by U.S. Geological Survey showed
       0.3 to  3.0 ppb of PCBs  in  water and up to 18,000 ppb of PCBs in
       the sediment.  A later  survey by EPA,  Region II showed 2.2 - 3.1
       ppb of  PCBs in water and 540 -  2980 ppm  of PCBs in the sediment
       near  the General Electric  plant discharges, with 660 ppm being
       detected several miles  downstream  (17).  Fish were found to be
       contaminated  not only near the  General Electric plants but also
       several hundred  miles south of  the plants indicating long-range
       transport of  PCBs discharged by industrial activities.  The toxic
       effects of ingestion of PCBs on humans had been demonstrated in a
       1968  episode  in  Japan where a batch of rice oil was accidentally
       contaminated  by  PCBs  (discussed on page  41).

(iii)   Clear Creek Pollution by PCBs in Bloomington,  Indiana  Q976)  05):
       Waste discharges by the Westinghouse Electric Corporation in
       Bloomington,  Indiana, into the  city sewer system and storm water
       runoff  from outdoor facilities  at  the  Westinghouse plant have
       contaminated  the Clear  Creek and other streams  in the area with
       PCBs.  The Westinghouse plant manufactures electrical capacitors
       in which PCBs are used  as  insulating fluids.  The company dis-
       charges about one to eight pounds  of PCBs per day into the city
       sewer system.  The wastewater effluents  of the  Bloomington, Indiana,
       sewage  treatment plant  which were  discharged into Clear Creek
       contained  19-47  ppb of  PCBs.  The  sediment of Clear Creek,was
       found to contain 18 ppm of PCBs.   This creek flows into Salt Creek
       which flows  into the  East  Fork  of  the  White River, a tributary
       of  the  Ohio  River.  The fish  in Clear  Creek, Salt Creek, and the
       West  Fork  of  White  River were all found to be contaminated with
       PCBs  thus  making them unsuitable for human consumption  (15).

 (iv)   James River  Pollution by  Kepone in Virginia  (1975)  (51,52):   Fish
       and  sediment  in  James River,  near  Hopewell, Virginia, were found
       to  be contaminated with kepone, a  chlorinated  pesticide used
       mainly  against potato beetles  in Europe.  The  river was closed  to
       commercial fishing  from Hopewell,  Virginia,to a point 84 miles
                                 26

-------
           downstream where it enters  Chesapeake Bay.  Kepone was manufactured
           by Allied Chemical  from 1968  to  1973  intermittently  at  the  Hopewell,
           Virginia, plant.   A  new company called Life  Science Products,  formed
           by two former  Allied Chemical  employees,  resumed production of
           kepone under a subcontract  from  Allied Chemical.  During  1968 to
           1973,  Allied Chemical  discharged its  waste  from kepone  manufacturing
           plant  into James River without a permit.  The  Life Sciences Pro-
           ducts  discharged its waste  into  Hopewell's  sewerage  system, which
           eventually discharged into James  River. Life Science's discharge of
           kepone waste into the city sewerage system resulted in closing  down
           the sewage treatment plant  because kepone inhibited  the normal
           bacterial  action required for sewage  treatment, and  the untreated
           sewage wastes  were  discharged into the James River.  Kepone has been
           found  to be widely  distributed throughout the  Hopewell, Virginia,
           area and the James  River was  closed to fishing in December  1975.
           Even though there is no known evidence of short-term health
           effects in the general  population and the long-term  effects of ex-
           posure to kepone are not known,  the toxicity of kepone  is well
           documented in  workers of Life Science Products. They had symptoms
           of severe headaches, tremors, memory  loss,  liver  damage, slurred
           speech, and involuntary rolling  of eyes.  Many of them  had  become
           sterile.   The  half-life of  kepone in  human  body is 165  days.

      (v)   Ohio River contamination by CCU (1977) (53):   For several  years,
           FMC Corporation in  Huntingdon, West Virginia,  had been  discharging
           2000 to 4000 pounds of CC14 every day into  the Kanawha  River  which
           flows  into the Ohio River.  The  discharges  were in violation  of a
           court-ordered  consent decree  by  EPA designed to end  excessive dis-
           charges of CCU into the Kanawha River.  The largest spill  to date
           in February 1977 of 70 tons,  raised the levels of CC14  in
           Cincinnati drinking water to  80  ppb.   The effects of long-term ex-
           posure to low  levels of CCl^  are not  known  but studies  have shown
           CC14 to be carcinogenic in  laboratory animals  (7).

     (vi)   The illicit dumping of toxic  chemical waste into the Louisville,
           Kentucky, sewerage system forced  the treatment  plant  to  shut down
           operation from March 29, 1977 to June 5,  1977  resulting in  dis-
           charging of untreated sewage  containing toxic  chemical  waste
           directly into  the Ohio River  (37-39).

(b)  Groundwater  Pollution: Groundwater contamination can occur from
collection, treatment,and disposal of  municipal  wastewater by the  following
routes:

    - leakage from collecting  sewers
    - leakage from treatment plant lagoons
    - land disposal of treatment plant effluents and disposal to surface
      water bodies that recharge aquifers
    - land disposal of sludges that are  subject  to leaching.
                                      27

-------
Although the volume of wastewater entering the groundwater system from these
various sources may be substantial,  there have been few documented cases  of
hazardous levels of constituents of  sewage affecting well  water supplies,
largely because the subject has not  been studied in detail.   A large pro-
portion of the sewage treatment plant effluents discharged to land do not
meet secondary treatment standards (54).

    The impact on groundwater of diffuse land spreading of municipal sludge
is practically unknown because fewer than 1% of the present municipal sludge
land spreading disposal facilities are monitored for effect on water quality.
(59).  Groundwater pollution by organic chemicals can also occur from
leaching of toxic chemicals from industrial waste landfills, municipal solid
waste disposal sites, or agricultural use of pesticides.

      (i)  Industrial waste landfills are a source of serious groundwater
           contamination because of  their large number and potential for
           leaking hazardous substances that are relatively mobile into the
           groundwater environment.   The contaminants cover the full range
           of organic and inorganic  chemicals normally present in industrial
           wastewaters.  Those documented as having degraded groundwater
           quality include phenols,  acids, heavy metals, chlorinated hydro-
           carbons and cyanide (54).  Hazardous chemicals are often present
           in the leachate from industrial waste landfills (e.g., CM, Cd, Cr,
           chlorinated hydrocarbons, and PCBs).  The particular make-up of the
           leachate is dependent upon the industry using the landfill or
           dump (54).  This source of contamination is one of the most
           frequently reported in spite of the almost complete lack of ground-
           water monitoring.  Toone, Tennessee, described in an earlier
           section, is an example where groundwater pollution has occurred from
           leachates from a toxic waste landfill.

               Dover Township, New Jersey, is another example where ground-
           water pollution had occurred from industrial waste landfill.
           Residents of this community noticed taste and odor problems with
           their drinking water in 1974.  Tests showed petrochemicals in  the
           water in the ppm range, and as a result 148 wells were permanently
           condemned.  Three years earlier, several thousand drums of toxic,
           flammable, explosive,and  oxidizing wastes had been dumped on near-
           by property.  Damages for capping wells, removing drums, drilling
           deeper wells, emergency water, water analysis, extension of public
           water and installing observation wells came to over $400,000 (55).

     (ii)  Land disposal sites for municipal solid wastes can be sources  of
           groundwater contamination because of the generation of the
           leachates caused by water percolating through the bodies of refuse
           and waste materials.  Leachate can be a highly mineralized fluid
           containing such constitutents as chloride, Fe, Pb, Cu, Na, nitrate,
           and a variety of organic  chemicals (54).

               Many problems with leachates in groundwaters have been at
           least partially documented.  A recent report for the northeastern


                                    28

-------
           U.S., for example, documented 60 cases in which well  supplies were
           made unsuitable for domestic consumption (56).

    (iii)  A study of the extent of pesticide levels in rural  drinking waters
           of two counties in South Carolina was carried out to  determine the
           role of agricultural practices and other possible sources (57).
           One of the counties was known to have received a higher amount of
           the pesticides over a period of several  years than  the other from
           the information obtained from the County Extension  Service.  The
           study showed that the pesticide levels found in the drinking
           waters of the county that received a higher amount  of the pesticides
           were lower than in the county that received a lower  amount of the
           pesticides.   Such factors as well location, depth or  type of con-
           struction were found to have little or no direct bearing on the
           residue levels.  The authors believed that local environmental
           conditions other than agricultural pesticidal use may have some
           bearing.   The pesticidal residues observed were the chlorinated
           hydrocarbons with DDT, lindane, dieldrin,and mi rex  being most
           common.  Although the study concluded that the pesticidal residues
           found in  the drinking waters of the two  counties were well below
           the accepted limits, a comparison with the national interim
           primary drinking water standards (28) revealed that some are above
           the recommended levels and therefore caution should be exercised
           in using  the affected water supplies.

EFFECT ON THE FOOD CHAIN

    Only a limited amount of information is available on the effects of the
food chain of the organic chemicals present in wastewater and  sludge used in
land application.  Wastewater application methods are important  in assessing
potential food contamination.  Methods of field application of wastewater and
sludge can be one of a variety of surface or subsurface application methods
(58).   The choice of the methods depends on the individual land  application
facility, geographic location, and climate.

    Primary attention should probably be given to organic compounds that are
known to be potentially toxic and carcinogenic such as organochlorine
pesticides, polycyclic aromatic hydrocarbons, PCBs, etc. (Tables 5-7).
The organochlorine compounds are of particular concern because most of them
have been found to be known or suspected carcinogens in animal models, are
highly resistant to  degradation,and are lipid soluble.  This accounts for
their accumulation and translocation to animals and humans via food chain
(Figure 1, Insecticide Cycle)(2,59).  The toxicological properties of some of
the pesticides - LDgo, fatal dose and the levels at which chror.ic poisoning
and acute poisoning, etc. occur are summarized in Table 10 (60-62).

    The ambient water quality criteria proposed by EPA for the protection of
human health from the adverse health effects caused by ingestion of toxic
organic chemicals in water are shown in Table 11 (31-33).   EPA has recommended
human health criteria in water of zero for carcinogens, but since this is not
feasible at present. EPA provided criteria for achieving various levels of
protection on an interim basis as shown in Table 12 (31-33). Tolerance

                                     29

-------
                         Insecticide
Atmosphere
                                                 Atmosphere
                       Microorganism

                           Worm
            Plankton and
            Microoranism
Atmosphere
 Animal'

Insecticide
                                                 Atmosphere
      Figure 1.  Insecticide cycle (2,59)a
     a)
        Reprinted from C.M. Tu and J.R.W.  Miles,  Residue
        Reviews, 64, 17-65 (1976), with permission of
        F.A. Gunther, Ed., Springer-Verlag,  New York, N.Y.
                             30

-------

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-------
     TABLE 11.  HUMAN HEALTH CRITERIA PROPOSED BY EPA FOR SOME
	TOXIC ORGANIC CHEMICALS IN AMBIENT WATER (31-33)

                                              Human health effects
     Organic compound	criterion (yg/1)
Acenaphthene                                          20.00

Acrolein                                               6.50

Bis(2-Chloroisopropyl) ether                         175.80

Chlorinated benzenes
  Chlorobenzene                                       20.00
  Trichlorobenzene                                    13.00
  Tetrachlorobenzene                                  17.00
  Pentachlorobenzene                                   0.50

Chlorinated naphthalenes

  Trichloronaphthalene                                 3.90
  Tetrachloronaphthalene                               1.50
  Pentachloronaphthalene                               0.39
  Hexachloronaphthalene                                0.15
  Octachloronaphthalene                                0.08

Chlorinated phenols
  2-Chlorophenol                                       0.30
  3-Chlorophenol                                      50.00
  4-Chlorophenol                                      30.00
  2,5-Dichlorophenol                                   3.00
  2,4,5-Trichlorophenol                               10.00
  2,4,6-Trichlorophenol                              100.00
  2,3,4,6-Tetrachlorophenol                          263.00
  Pentachlorophenol                                  140.00

Cyanide                                              200.00

Dichlorobenzenes                                     230.00
  (all  isomers combined)

2,4-Dichlorophenol                                     0.50

Dichloropropanes                                     200.00

Dichloropropenes                                       0.63

Endosulfan                                           100.00

 Endrin                                                1-00

Ethyl benzene                                         110.00
                            (continued)

                                32

-------
                         TABLE 11 (continued)
                                              Human  health effects
     Organic compound                           criterion  (yg/1)
Fluoranthrene
Halomethanes
CH3C1
CH3Br
CHBr3
CHCl2Br
CC12F2
CF3C1
Isophorone
Naphthalene
Nitrobenzene
Nitrophenols
Dinitrophenols
Trinitrophenols
Dinitrocresols
200.00

2.00
2.00
2.00
2.00
2.00
3000.00
32,000.00
460.00
143.00
30.00

68.60
10.00
12.30
Phenol                                               340.00

Phthalate esters
  Dimethyl ester                                 160,000.00
  Diethyl ester                                   60,000.00
  Di butyl ester                                     5000.00
  Di-2-ethyl  hexyl  ester                          10,000.00

Toluene                                           17,400.00

1,1,1-Trichloroethane                             15,700.00
                               33

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TABLE 12.  INTERIM HUMAN HEALTH EFFECTS CRITERIA PROPOSED  BY  EPA FOR  SOME
           CARCINOGENIC ORGANIC CHEMICALS IN AMBIENT  WATER (31-33)

Levels that would permit one case of cancer in
specified population size exposed people (yg/1)
Organic carcinogen
Acrylonitrile
Aldrin
Benzene
Benzidine
Carbontetrachloride
Chlordane
Chloroalkyl ethers
Bis(2-chloroisopropyl ) ether
8is(2-chloroethyl) ether
Bis(chloromethyl ) ether
Chlorinated ethanes
1,2-Dichloroethane
1 ,1 ,2-Trichloroethane
1 ,1 ,2,2-Tetrachloroethane
Hexachloroethane
Chloroform
DDT
3,3 -Dichlorobenzidine (DCB)
1 ,1-Dichloroethylene
Dieldrin
2,4-Dinitrotoluene
1 , 2-Di phenyl hydrazi ne
Heptachlor
Hexachlorobenzene
Hexachl orobutadi ene


1/10 Million
0.0008
0.46 x 10"6
0.15
1.67 x 10"5
0.026
0.012

0.115
0.0042 ,
0.2 x 10"°

0.07
0.027
0.018
0.059
0.021
0.98 x 10"5
0.001
0.013
0.44 x 10"6
0.0074
0.004
0.23 x 10"5
1.25 x 10"5
0.0077
(continued)
34
1/1 Million
0.008
0.46 x 10"5
1.5
1.67 x 10"4
0.26
0.12

1.15
0.042 ,
0.2 x 10"b

0.7
0.27
0.18
0.59
0.21
0.98 x 10"4
0.01
0.13
0.44 x 10"5
0.074
0.04
0.23 x 10"4
1.25 x 10"4
0.077


1/100,000
0.08
0.46 x 1
15
1.67 x 1
2.6
1.2

11.5
0.42
0.2 x 10

7.0
2.7
1.8
5.9
2.1
0.98 x 1
0.1
1.3
0.44 x 1
0.74
0.4
0.23 x 1
1,25 x 1
0,77




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-------
TABLE 12 (continued)

Levels that would permit one case of cancer in
specified population size exposed people (yg/1 )
Organic carcinogen
Hexachlorocyclohexane (HCH)
a-HCH
B-HCH
Y-HCH
p-HCH
Nitrosamines
N-Ni trosodimethyl ami ne
N-Ni trosodiethyl ami ne
N-Ni trosodi-n-butyl ami ne
N-Ni trosopyrol i dine
PCBs
1/10 Million

1.6 x 10~4
2.8 x 10"T
5.4 x 10";
2.1 x 10~4

2.6 x 10~4
0.92 x 10/1
1.3 x 10"4
0.0011
2.0 x 10~6
1/1 Million

1.6 x 10"?
2.8 x 10~^
5.4 x 10"^
2.1 x 10"-5

2.6 x 10~3,
0.92 x 10:J
1.3 x 10"-3
0.011
2.0 x 10"5
1/100,000

0.016
0.028
0.054
0.021

0.026
0.0092
0.013
0.11
2.0 x 10"4
Polynuclear aromatic hydrocarbons
Benz-a-pyrene (BaP)
Dibenzanthracene (DBA)
TCDD
Tetrachloroethylene
Trichloroethylene
Vinyl chloride
0.97 x 10"!
0.43 x 10"H
0.455 x 10"8
0.02
0.21
5.17
0.97 x 10~3
0.43 x 10"J
0.455 x 10"7
0.2
2.1
51.7
0.0097
0.0043
0.455 x 10"6
2.0
21
517
        35

-------
limitations set by FDA for various pesticides and toxic organic chemicals in
food products should be used for selective monitoring of vegetation grown on
sludge-treated  lands.  Tolerance limitations set by FDA for PCBs in a variety
of food products in 1973 and subsequently modified in 1979,  are shown in Table
13 (63,64).

(a)  Physical Contamination (5):  Chaney and Lloyd (65) have shown that sewage
sludges are effectively retained on the top of the vegetation when applied by
spraying, and that they are not well  removed by rain.  Because of the more
dilute nature (and lower viscosity) of wastewater and effluents, lower con-
tamination levels on vegetation would be expected.  However, evaporation and
repeated application may provide sufficient buildup of contaminants to be a
cause for concern.  Contaminants physically retained on crops may be ingested
by animals,or possibly directly by humans if improper practices are followed
(66).

(b)  Uptake by Plants:  The extent to which organic chemicals in wastewaters
and sludge, at the levels indicated in an earlier section,  will be taken up by
plants and may be toxic to human beings through food crops  is not well under-
stood (5,67).

    The Michigan Department of Agriculture has analyzed fresh produce grown in
household gardens close to Anderson Development Company in  Adrian, Michigan
(23).  As mentioned in an earlier section, Curene 442 (MOCA), a potential
human carcinogen, was found in discharges from the Anderson Development
Company and in samples of garden soils in the residential area surrounding the
Anderson Development Company (Table 4).  It is believed that these household
gardens did not receive municipal sludge from the Adrian wastewater treatment
plant as a fertilizer, even though the wastewater treatment plant sludge was
given away to home gardeners up until 1977.  In a press release dated July 13,
1979, the Michigan Department of Agriculture stated that the results of
analysis of limited samples tested in their laboratory showed no evidence of
Curene 442 (MOCA) residues in thoroughly washed samples of  onion tops and
bulbs, zucchini and radishes.

    The uptake of pesticides and PCBs from soils into plants has been studied
to a limited extent.  Plants do take up many pesticides through roots and
translocate them within the plant (68).  Some pesticides are taken up but
others are not or are taken up at low levels (69).  The pesticides heptachlor,
dieldrin, and chlordane are taken up by soybean plants from soil, translocated
to the seed and stored at low levels  in the oil (70).  PCBs on the other hand
are not carried to the top of the soybean plants if direct  vapor transmission
is prevented by a barrier over the soil (71).  Uptake of PCBs by root crops,
however, has been demonstrated under field conditions.  It  was shown that
carrot peel contained 97% of the root residue and very little was found in
the foliage (72).  Lawrence and Tosine (73) reported that the PCB concentration
in the leaves of corn and grass grown on sludge-treated land was comparable to
that in the sludge, whereas the Center for Disease Control  (CDC) found
negligible amounts of PCBs in vegetation grown in land treated with sludge
containing PCB levels as high as 300 ppm in Bloomington, Indiana (15,74).  For
example, CDC found that beets grown in sludge-amended soil  containing 4 ppm
PCBs were found to have 0.6 ppm PCBs  (l/7th of that in the  soil), grass from a

                                      36

-------
     TABLE 13. FDA TOLERANCES  FOR  PCBs  IN  FOOD
              AND FOOD PACKAGING  (PPM)  (63,64)

Mi 1 ka
Dairy products
Poultry
Fish and shell fishb
Eggs
Infant and junior food
Complete and finished animal feed
Animal feed components
Paper food-packaging material
1.5
1.5
3.0
2.0
0.3
0.2
0.2
2.0
10.0

a. On  fat basis

b. Edible portion
                              37

-------
field containing 8.5 ppm PCBs in soil  showed 1.16 ppm PCBs (l/7th of that in
the soil), and rhubarb grown in the same soil  had 0.25 ppm PCBs (l/34th of
that in the soil).  The Bloomington sludge was much more heavily contaminated
with PCBs than the sludge used by Lawrence and Tosine (73), and was spread on
land at 25 tons per acre which was about three times the maximum application
rate recommended (15,74).  In order to protect the public health FDA has
recommended to EPA that sludges should not contain more than 10 ppm PCBs on
dry weight basis for the application of sludge to agricultural  lands (Table
14) (66,75), and EPA adopted this value in its regulations (76).  However,
municipalities without a significant source of PCBs would be expected to have
less than 10 ppm PCBs in their sludges.  In a  survey of sixteen American
cities (14), only two cities, Chicago Illinois, and Schenectady, New York, had
PCBs levels over 10 ppm in sludge.  Bloomington, Indiana, is an example where
very high levels of PCBs were found in sludge  - 300 ppm (15).  This is because
of direct discharge of PCBs waste by Westinghouse Electric Corporation into
the city sewerage system which is then concentrated in the sludge.  The levels
in Schenectady, New York, are high because of  the location of two General
Electric plants which use large amounts of PCBs in the manufacture of
electrical capacitors.

(c)  Uptake by Animals:  Cattle and other animals ingest soil as well as
plants while grazing.  Chemical contaminants,  especially metals, pesticides,
and PCBs, may build up in selected tissue of such animals when sewage sludge
is used on land and pastures (6,67,77,78).  Although wastewater effluent may
present a lesser problem, those from highly contaminated sources may result
in the buildup of contaminants in the surface  layer of soil similar to that
observed with sludges.

    Some efforts have been made to utilize sewage sludge as an animal feed
supplement because of its nutritive value. Sewage sludge subjected to gamma
radiation at a dosage of 1 mega-rad or more to eliminate  the risk from
pathogens and parasites was used as cattle feed supplement and the tissue
accumulation of heavy metals (77) and pesticide residues (77,78) was studied
by Smith et al.  Pesticide residues were determined in adipose tissue from
kidneys.  They found that feed consumption was decreased but there was no
evidence of toxicity or impaired reproduction.  Five of the pesticide
residues were significantly elevated by the diet containing 20% sewage sludge.
Subsequent feeding on a conventional finishing diet reduced these levels, but
not to the levels of the control animals (Table 15).

    In the Bloomington, Indiana, incident of contamination of wastewater and
sludge by PCBs described in an earlier section (15), PCBs were found in
ground beef from cattle which grazed on contaminated lands.  The cattle of
a farmer, whose pasture had been flooded by a  creek which had been contam-
inated by PCBs, suffered weight loss and one calf was born without pupils in
its eyes.  The milk fat of another farmer's cow who grazed on sludge-treated
pasture was found to contain 5 ppm PCBs - twice the FDA's 2.5 ppm tolerance
level.  FDA has currently lowered the tolerance level in milk fat to 1.5 ppm,
because data developed since 1973 show that PCBs are more toxic than
previously believed to be (Table 13) (63,64).
                                     38

-------
           TABLE 14.  FDA RECOMMENDATIONS TO EPA ON THE LAND
          	APPLICATION OF SLUDGE (66,75,76)	
a.  Sludges should not contain more than 20 ppm cadmium, 1000 ppm lead or 10
    ppm PCBs on the dry basis.

b.  In support of the limits proposed by the W 124/NC 118 Committees of Land
    Grant Colleges, the maximum total which should ever be added to an
    average soil  (cation exchange capacity of 5-15) is 9 Ibs/acre of cadmium
    and 900 Ibs/acre of lead.

c.  Crops which are customarily eaten raw should not be planted within three
    years after the last sludge application.

d.  Crops such as green beans, beets, etc. which may contaminate other foods
    in the kitchen before cooking should not be grown in sludge-treated land
    unless the sludge gives a negative test for pathogens.

e.  Because sewage can be regarded as filth, food physically contaminated
    with sludge can be considered adulterated even though there is no direct
    health hazard.  Sludge should not be applied directly to growing or
    mature crops where sludge particles may remain in or on the food.

f.  Commercial compost and bagged fertilizer products derived from sludges
    should be labeled properly to minimize contamination of crops in the
    human food chain which may result from their use.
                                     39

-------
     TABLE  15.  SOME PESTICIDE RESIDUES IN ADIPOSE TISSUE OF CATTLE
                      FED IRRADIATED SLUDGE*  (77,78)
                        (ppb, Fresh Weight Basis)

Treatment
qroup

Controls

X ± a
Fed diet
containing
20% sludge
for 68 days
X ± a
Fed diet
containing
20% sludge
for 68 days
followed by
conventional
diet for an
additional
56 days
X ± a
Irradiated
dried sludge
i
p.p'-DDE
20
20
30
23 ± 6
120

100
90
103 ± 15


60
20

60



47 ± 23

40

Dieldrin
20
<20
<20
<20
80

50
50
60 ± 17


50
<20

30



33 ± 15

36

Oxychlordane
0
0
0
0
70

50
120
80 ± 26


30
0

30



20 ± 17

0

TNC
0
<10
<10
<10
80

70
70
73 ± 6


20
0

20



13 ± 12

0

Aroclor 1254
0
500
500
333 ± 289
380

960
980
1107 ± 237


600
500

670



590 ± 85

1440
a.   Adapted from G.  S.  Smith et al. (77).
                                    40

-------
    The accidental  feed contamination of dairy cows in Michigan by poly-
brominated biphenyls (PBBs) illustrates what may happen when excessive
quantities of toxic organic chemicals are ingested by animals.   PBB levels
of 110-2480 ppm were found in body fat of the animals while levels of 44-900
ppm were found in milk fat.  The animals had the following symptoms:  loss of
appetite, eye watering, weight loss, increased frequency of urination, de-
creased milk production, matting and loss of hair, abscesses, hematornas,
abnormal hoof growth, embryo resorption, abortions, stillbirths, deaths
shortly after deliveries, delayed deliveries, etc. (79,80).

(d)  Uptake by Humans:  Although there is no direct evidence of human health
hazards from the uptake via food chain of the organic chemicals in waste-
water and sludge used in land application, some information is  available
from two incidents of accidental food contamination by PCBs in  Japan and
PBBs in Michigan.

      (i)  Food Contamination by PCBs in Japan:  Sporadic outbreaks of a
           peculiar skin disease characterized by acneiform eruptions and
           pigmentation of the skin and nails were reported in  Japan in 1968.
           The disease was found to be associated with the consumption of a
           particular batch of one brand of rice oil.  The disease was
           called Yusho (rice oil disease).  The cause of Yusho was traced to
           a specific batch of rice oil shipped by one company.  The oil was
           found to contain approximately 2000 ppm of Kanechlor KC400, a
           commercial preparation of PCB containing 48% chlorine.   The
           latency period between ingestion of the oil and onset of clinical
           symptoms was generally 5-6 months.  Elevated serum triglycerides,
           increased urinary 17-ketosteroid excretion and respiratory dis-
           tress are some of the physiological abnormalities that were ob-
           served in Yusho patients  (81).  Occupational exposure of PCBs had
           previously been linked to chloracne and hepatic dysfunction.

     (ii)  PBB Episode in Michigan:  The accidental contamination of Michigan
           dairy farm animal feed by the polybrominated biphenyl (PBB) com-
           pound Fire Master BP-6 in 1973-1974 was followed by illness and
           death of many cattle which  had consumed the PBB-containing feed.
           Widespread human exposure resulted from consumption of contaminated
           milk, eggs, meat, and poultry.  In response to concerns regarding
           reports of the appearance of adverse health effects among Michigan
           dairy farmers exposed to  PBB and the possible association of such
           symptoms to their PBB exposure, Anderson et al. (82) conducted
           comprehensive clinical and  laboratory examinations of PBB-exposed
           Michigan farmers.  A comparable group of Wisconsin farm families
           who were not exposed to PBB were used as controls.  The symptoms
           noted were neurological (marked tiredness, fatigue, sleepiness,
           weakness, poor memory, loss of appetite); musculoskeletal
           (arthritis-like symptoms);  and gastrointestinal (abdominal pain,
           diarrhea and weight  loss).   In most of the participants in the
           survey, the symptoms represented a distinct change from their
           previous health pattern.  Statistical analysis revealed that the
           Michigan group  had significantly higher prevalence of the above
                                     41

-------
            mentioned  symptoms.   No  clear  relationsnip  can  be  established  be-
            tween serum PBB  level  and  the  presence  of any of the  symptoms
            noted.   The existing  difference  could not be explained without
            considering an etiologic role  for  exposure  to PBBs.

                Liver  function  tests (83)  (Table 16) showed that  the  Michigan
            group had  higher prevalence  of abnormal SGOT and SGPT.  A clear
            sex difference was  also  noted; Michigan men had a  higher  prevalence
            of abnormal SGPT and  LDH than  Michigan  women, and  a higher
            prevalence of abnormal SGOT  and  SGPT than Wisconsin men.   Michigan
            women did  not differ  from  Wisconsin women in prevalence of ab-
            normality  of any liver function  test.   The  authors did not ob-
            serve any  relationship between serum PBB  levels and  liver
            function tests but  they  tentatively ascribed the greater
            prevalence of abnormal SGPT  and  SGOT among  Michigan dairy farm
            residents  compared  to the  Wisconsin farm residents to the former
            group's  exposure to PBBs.

                Consumers who had purchased  farm products from both
            quarantined and  nonquarantined farms in Michigan were also
            surveyed by Lillis  et al.  (84).  The prevalence of liver  function
            abnormalities SGOT  and alkaline  phosphatase were similar  in
            farmers  from quarantined and nonquarantined farms. The prevalence
            of abnormal SGOT and  alkaline  phosphatase levels was  high in the
            subgroup of consumers of products  from  quarantined farms.

    These examples are  isolated cases of accidental contamination and as
such represent effects of acute exposure and may  not be representative of
potential contamination by organic chemicals of food chains from  land
application.  Nevertheless,  they  serve the purpose  of  providing  some  insight
into the effect of consuming these chemicals through food  chains  and  they may
be useful in setting standards.

    The Curene 442 (MOCA) contamination  incident mentioned  in  an  earlier
section illustrates how industry  can expose  general population to unknown
risks (23).   The residents  of the community  surrounding the Anderson  De-
velopment Company in Adrian, Michigan  have been exposed to  Curene 442 (MOCA),
a potential  human carcinogen, due to widespread contamination  of  roadside
soil   and air, and household dust (Table 4).  The contamination  is  so wide-
spread that Mr. Howard Tanner,  Director  of the Michigan Department  of Natural
Resources, in a press  release on  May 2,  1979,  stated  that  "Citizens  should
use precaution as our  analysis  thus  far  indicates there is  a concern  for direct
human contact with contaminated soils.  Possible sources of direct  human
contact could be in gardens, sandboxes,  and  playgrounds, in a  five-block
radius adjacent to the plant, which  is located at 1415  East  Michigan,  Adrian."

    The residents of this community  have consumed produce  grown  in  the house-
hold gardens.  However, laboratory analyses  by the  Michigan Department of
Agriculture showed that Curene  442 (MOCA)  was  not taken up  by  the plants that
were tested as mentioned before.   The  Michigan Department  of Public  Health
                                      42

-------
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has monitored the urine specimens of randomly selected persons living within
a five block radius of Anderson Development Company and found no evidence of
Curene 442 (MOCA) in urine of the study participants.   The long-term health
effects of exposure to Curene 442 (MOCA) on the residents of the community of
Adrian, Michigan are not known at present.   The Michigan Department of Natural
Resources and the Michigan Department of Public Health have formed a blue-
ribbon panel of experts from across the nation to assess the risk to the
public health of the type of exposure to Curene 442 (MOCA) in Adrian,
Michigan.
                                      44

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                                    45

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                                      46

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20.  Preliminary Report on Kepone levels Found in Environmental Samples
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25.  Weber, J. B.  Interaction of Organic Pesticides With Particulate Matter
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26.  Helig, C. S., D. C. Kearney, and M. Alexander.  'Behavior of Pesticides
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                                     47

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38.   Carter,  M. R.   The  Louisville  Incident.   In:   National Conference  on
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39.   Morse, D. L., J. R. Kominsky,  C.  L.  Wisseman   III, and P. J.  Landrigan.
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42.  Elia, V. J., C. S.  Clark, and  V.  A.  Majeti.   Evaluation of  Workers Ex-
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                                      48

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44.  Shuval,  H.  I., and B.  Fattal.   Epidemiological  Study of Wastewater
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47.  Murray,  C.   EPA Criticized for Chemical Wastes Handling.  Chem. and
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48.  RCRA in  Action.  In:   Rural  Solid Waste.  No.  6,  November/December
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49.  Clark,  C. S. et al.   Unpublished results.

50.  Old Landfill Site Poses Health Problems.  Chem. and Eng.  News, August
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51.  Zim. M.  H.   Allied Chemical's $20 - Million Ordeal With Kepone.
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53.  Womack,  B.   Carbon Tet Danger Debated at Hearing.   The Cincinnati Post,
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54.  Geraghty, J. J., and D. W. Miller.   Status of Groundwater Contamination
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58.   Multimediurn Management of Municipal  Sludge.   Vol.  IX,  National  Academy
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59.   Tu, C.  M.,  and J. R.  W.  Miles, Interactions Between Insecticides and
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                                      49

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60.  SCS  Engineers.   Health  Effects  Associated  With  Wastewater  Treatment and
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66.  Jelinek, C. F., and G.  L. Braude.  Management of Sludge  Use on Land.
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                                      50

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74.  Center for Disease Control.  Polychlorinated Biphenyl Exposure-Indiana.
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     Perspectives, 23:105-109, 1978.
                                      51

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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1. REPORT NO. 2.
EPA-600/ 1-80-025
4. TITLE AND SUBTITLE
Potential Health Effects from Persistent Organics in
Wastewater and Sludges Used for Land Application
7. AUTHOR(S)
Vimala A. Majeti and C. Scott Clark
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Department of Environmental Health
University of Cincinnati Medical Center
Cincinnati, Ohio 45267
12. SPONSORING AGENCY NAME AND ADDRESS
Health Effects Research Laboratory - Cinn, OH
Office of Research and Development
U.S. Environmental Protection Agency
Cincinnati, Ohio 45268
3. RECIPIENT'S ACCESSION NO.
5. REPORT DATE
May 1980
6. PERFORMING ORGANIZATION CODE
8. PERFORMING ORGANIZATION REPORT NO.
10. PROGRAM ELEMENT NO.
1BA607
11. CONTRACT/GRANT NO.
R-805445
13. TYPE OF REPORT AND PERIOD COVERED
Final Feb. 1978-Feb. 1980
14. SPONSORING AGENCY CODE
EPA/600/10
15. SUPPLEMENTARY NOTES
16. ABSTRACT

       The  potential  health problems  associated  with  the  presence  of persistent
  organic chemicals  in wastewater and sludge, when applied to agricultural lands,  are
  reviewed.   The  type and  amounts  of organic  chemicals present  in  wastewater  and
  sludge,  their  fate  on  land,  and  available  control measures  are discussed.    The
  potential  health effects of organic  chemicals on workers/populations  who come  in
  contact with them during wastewater treatment, transportation,  and/or application
  are considered.

       The  review  concludes that there  is not  sufficient  information at present  to
  assess the full  extent  of  long-term health risks  of  exposure to organics in  the
  wastewater  treatment plants or at  land application sites.  Recommendations  are made
  concerning  guidelines and further  research.  Further research  is recommended on  the
  uptake of  organic  chemicals by food crops.   Long-term follow-upis also recommended
  for populations  who have had acute short-term exposure  to  organic  chemicals from
  waste materials.
17.
KEY WORDS AND DOCUMENT ANALYSIS
a. DESCRIPTORS
Organic wastes, ground water, industrial,
industrial wastes, water quality, public
health, waste water, water, toxicity,
chemical removal
18. DISTRIBUTION STATEMENT
Release to the public
b.lDENTIFIERS/OPEN ENDED TERMS
Chemical monitoring,
municipal sludge,
industrial sludge,
hazardous wastes,
irrigation
19. SECURITY CLASS (This Report)'
Unclassified
20. SECURITY CLASS (This page)
Unclassified
c. COSATI Field/Group
68D
21. NO. OF PAGES
60
22. PRICE
EPA Form 2220-1 (Rev. 4-77)   PREVIOUS EDITION is OBSOLETE
                                            52
                                                                   US GOVERNMENT PRICING OfFICE I98G-6 57 - L46 / 5688

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