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PRIMARY TREATMENT
INTRODUCTION
Primary treatment is intended to physically remove settle-
able solids and most of the discrete suspended and floating
solids from the municipal wastewater stream preparatory to
secondary treatment. In addition, primary treatment removes a
limited portion of the soluble constituents.
In primary treatment, the wastewater influent is divided
into three output pathways: primary effluent, primary sludge
(including grit, screenings, and precipitated matter), and
aerosols. Effluent from primary treatment can be directly
discharged (until 1977), discharged after disinfection (again
until 1977), or treated by a secondary process. Primary sludge
is normally subject to additional processing. At some ocean
coastal sites, however, the sludge is discharged without further
treatment. Aerosols are rarely a problem, due to the absence
of excessive turbulence.
The information reviewed during this study is tabulated in
Table 12. Most research conducted to date concerns the removal
by primary treatment of water quality parameter constituents.
It is only in recent years that researchers have examined the
effect of primary treatment on various public health impairing
contami nants.
WATER QUALITY PARAMETERS
For several decades, extensive work has been reported con-
cerning general contaminant removal efficiencies for primary
treatment. Removal varies widely, depending upon the physical
and chemical characteristics of the wastewater, the proportion
of settleable solids, concentrations of the solids, and deten-
tion time. Mi tchel 1 (922) reported the general performance effi-
ciencies that could be expected for typical primary treatment
(Table 13). Removals achieved during a three-year study of
an operational primary treatment system are shown in Table 13.
78
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TABLE 12. LITERATURE REVIEWED PERTAINING
TO PRIMARY WASTEWATER TREATMENT
Contaminant Reference Number
Water Quality Parameters
Ammonia 922
BOD 393, 622, 745, 922, 1404, 1435, 1547
COD 483, 622, 896, 922, 1435
Cyanides 922
Oil and grease 483, 810, 922
Phosphates 896
Suspended solids 393, 483, 622, 745, 896, 922, 1435, 1547
Total organic 483
carbon
Other (general) 531, 622
Elemental Contaminants
Arsenic 922
Cadmium 228, 443, 922, 1063
Chromium 228, 896, 922
Copper 228, 443, 896, 922, 1063
Iron 228, 896
Lead 228, 922, 1063
Manganese 228
Mercury 228, 922
Nickel 228, 922, 1063
Selenium 1114
Zinc 228, 896, 922, 1063
79
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TABLE 12 (continued)
Contaminant Reference Number
Biological Contaminants
Bacteria 79, 161, 1256
Coliforms 161, 483, 568, 717, 896, 1256, 1282
Coxsackie virus 161
(A & B)
Escherichia coli 568, 896
Streptococci 568
Hepatitis virus 1261
Mycobacterium 161, 428
Parasitic worms 161, 420, 428
Pol io vi rus 97, 161
Protozoa 161, 428
Salmonella 161, 420, 428, 568, 1261
Shigella 161, 1261
Vibrio cholerae 161
Virus 79, 92, 95, 96, 97, 100, 101, 161, 382,
428, 468, 1009, 1256
Other (general) 161, 1261
80
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TABLE 13. PRIMARY SETTLING TANK PERFORMANCE (922)
Parameter
COD
BOD5
Suspended Solids
Oil and Grease
Ammonia Nitrogen
Primary
Influent
(mg/£)
539
269
279
72
34
Primary
Effluent
(mg/£)
315
165
103
28
20
Percent
Removal
42
39
64
61
41
When used as a coagulant during primary treatment, lime is
most effective in reducing certain water quality parameter con-
stituents. When lime addition of 350 mg/£ was followed by air
flotation, Mennell et al . (896) reported the following removals:
turbidity, 98.5 percent; suspended solids, 95 percent; COD, 60
percent; and total phosphorus, 99 percent. Total nitrogen
removal varied between 10 and 20 percent. Lower lime dosages
provided proportionally lower removal percentages. The practice
of dosing primary clarifiers with chemical coagulants will
probably increase, as municipalities attempt to cost effectively
meet federal and state water quality standards.
ELEMENTAL CONTAMINANTS
Recent interest in elemental contaminants, particularly
trace metals, has prompted investigation into the partitioning
of these contaminants in the wastewater treatment stream.
Primary treatment receives elemental contaminants in a variety
of forms, e.g., soluble, insoluble, and complexed. The con-
centrations of each form vary intrinsically as a complex
function of such factors as influent metal concentration, pH,
and ligand concentration.
Mitchell (922) reported removal efficiencies for primary
settling over a three-year period at the Hyperion treatment
plant, Los Angeles, California,as shown in Table 14.
TABLE 14. PRIMARY TREATMENT REMOVAL OF METAL ELEMENTS (922)
Copper
Zinc
Nickel
Lead
Arsenic
Cadmium
Chromi urn
Primary
Influent(mg/£)
0.39
0.66
0.30
Q.03
0.015
0.01
0.55
Primary
Effluent(mg/£)
0.25
0.42
0.24
0.07
0.017
0.02
0.37
Percent
Removal
36
36
20
32
81
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No explanation was offered to account for the anomaly of
increased lead, arsenic, and cadmium concentrations.
Chen and Lockwood (228), also working with the Hyperion treatment
plant, discussed the partitioning of trace metals with particu-
lates as a function of particle size. It was reported that in
primary effluent, more than 70 percent of the total trace metals
content is associated with particulates as opposed to the solu-
ble ionic form. However, only 10 to 20 percent of the Ni, Pb,
or Mn was associated with the particulate fraction. Similar
concentrations of metals were found on the larger (44 ym) and
the smaller (0.2 ym) particles. However, particles as large as
44 ym will settle about 200 times as rapidly as 3-ym particles.
More efficient removals of elemental contaminants could be
expected by the use of either increased wastewater detention
time, or chemical precipitants (e.g., lime) for particle coagu-
lation. Trace metal removals reported (896) at a lime dose of
388 mg/£ approached 100 percent for chromium and copper, 97
percent for iron, and 94 percent for zinc. Molybdenum was not
effectively removed by this treatment.
BIOLOGICAL CONTAMINANTS
Primary sedimentation usually removes less than 50 percent
of coliform and pathogenic bacteria from sewage and is rela-
tively ineffective in removing viruses and protozoa. Literature
concerning the removal of water-borne pathogens by primary
treatment processes reports a varying degree of efficiency,
depending in part on the type of pathogen studied. Table 15
(161, 428) highlights the results of Bryan's investigation of
pathogen survival during primary treatment.
In their literature review, Foster and Englebrecht (428)
reported isolation of salmonella from six of seven different
primary effluent samples. The raw sludge also contained members
of this genus, with 19 of 20 samples tested as positive for
salmonella organisms. Tubercle bacilli were reduced about 50
percent in the wastewater stream during sedimentation. It was
concluded that bacterial pathogens are ineffectively removed
from wastewater by primary settling; furthermore, the process
produced a sludge that, without further treatment, constitutes
a health hazard.
Amoebic cysts and parasitic worm ova are also ineffectively
removed by primary treatment, due to their low specific densities
and resulting buoyancy. Ascaris ova are an exception: Foster
and Engelbrecht (428) reported 100 percent settlement of these
ova into the sludge within 15 min.
Viruses, because of their size (,02 to .3 ym), are rarely
removed by sedimentation, except for those that are associated
with wastewater solids. The nature of the surface chemistry of
82
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TABLE 15. SURVIVAL OF PATHOGENS
DURING PRIMARY TREATMENT (161, 428)
Pathogen
Salmonella typhi
Salmonella spp.
Streptococcus faecal is
Mycobacterium
Enteroviruses
Polio viruses
Coxsackie viruses
Endamoeba histolytica
Ascaris ova
Trichuris trichiura
Taenia saginata
% Removal
>50
0-15
<50
48-57
no reduction
no reduction
<50
0-50
0-100
>50
0-50
83
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viral units suggests that adsorption depends strongly on the
chemical environment, would be expected to vary according to
changes in input water chemistry, and would possibly be affected
by chemical additions.
The removal of viruses by primary settling has been both
researched and reviewed extensively by Berg (92, 95, 97, 100).
Berg described a project (95) in which only one to two-thirds
of the viral particles had settled out in one day, although 75
percent of the suspended solids had settled. In this review,
Berg discussed several additional studies on viral removal by
primary treatment; all failed to mention detention time, and
more importantly, the levels of virus in the incoming sewage
were not related to those in the effluent.
Although primary settling alone will not effectively reduce
the pathogen content of wastewater, dosing primary settling tanks
with chemical coagulants does show some promise in this regard.
Chemical precipitation, when used during primary treatment, is
capable of removing as much as 99.99 percent of the virus sus-
pended in water, effected through the formation of a coagulant-
cation-virus complex. Elevated pH levels attained during lime
treatment also result in substantial reductions in viral numbers
(468). Lime coagulation during primary treatment brings remark-
able reductions of coliform density as well. A 99.9 percent
coliform reduction was measured at a lime dose of 450 mg/£ (896).
84
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SECONDARY TREATMENT: ACTIVATED SLUDGE
INTRODUCTION
The activated sludge process involves the growth of
microorganisms in a reactor. This effects partial biological
degradation of organic compounds in wastewater to simpler
organic compounds, carbon dioxide, water, microorganisms, and
energy (393). The basic process requires two equipment compo-
nents: aeration tanks and clarifiers. Active biological sludge
is separated from the effluent in a clarifier and recycled to an
aeration tank.
Activated sludge, the most popular wastewater secondary
treatment process, has been extensively studied, as indicated
by Table 16 . Most research has focused on water quality
parameters such as BOD, COD, and suspended solids. The data
are usually presented as percent removal, with removal effi-
ciency determined by difference in influent and effluent con-
centrations. Removal of a specific contaminant can be
accomplished by separation into the sludge or by degradation
through biological activity. Aerosol generation from the
aeration tank is also a possible contaminant pathway.
In view of possible health effects, the difference between
separation and degradation can be significant. If the treatment
process merely partitions a particular contaminant into the
sludge or air, it remains available for migration back to man.
In contrast, biological degradation can terminate the contami-
nant pathway or transform the potentially harmful substance into
a nontoxic form. The separation and degradation components of
the removal process are often not distinguished in the activated
sludge literature.
WATER QUALITY PARAMETERS
Past research on activated sludge processes has concen-
trated on water quality parameters, with primary emphasis on
BOD, COD, and suspended solids. Because of the tremendous
volume of literature associated with BOD and suspended solids as
indicators of activity, and the absence of direct health effects
from these pollutants, this report placed greater emphasis on
literature dealing with chemical and biological contaminants of
more direct public health concern.
85
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TABLE 16. LITERATURE REVIEWED PERTAINING
TO ACTIVATED SLUDGE
Contaminant Reference Number
Water Quality Parameters
Ammonia 4, 10, 59, 64, 113, 196, 277, 351, 352,
364, 385, 454, 614, 618, 799, 922, 1115,
1333, 1351
BOD 3, 10, 113, 146, 196, 209, 276, 352, 364,
560, 614, 623, 745, 799, 814, 864, 875,922,
1003, 1084, 1240, 1337, 1360, 1435, 1493
COD 196, 277, 364, 560, 601, 623, 668, 799,922,
1084, 1158, 1333, 1493
Chlorides 114, 819, 899, 1062
- Cyanides 623, 824, 922, 1062
Fluorides 1062
Nitrates 10, 59, 64, 113, 122, 352, 364, 375, 447,
454, 1351
Nitrites 10, 122, 352, 454, 1351, 1516
Oil and grease 810, 922, 1062, 1516
Phosphates 10, 13, 62, 63, 64, 113, 114, 196, 277,
352, 364, 375, 410, 454, 510, 513, 555,
601, 614, 763, 785, 814, 899, 922, 1213,
1230, 1337, 1341, 1349
Suspended solids 3, 10, 113, 146, 196, 227, 352, 560, 623,
668, 745, 922, 1084, 1435, 1516
Total dissolved 196, 276, 352, 500, 899
solids
Total organic 10, 113, 114, 352, 615, 1158, 1333, 1516
carbon
Other (general) 385, 391, 393, 531, 602, 622, 1310, 1333
Biological Contaminants
Aluminum 513, 814, 1004
86
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TABLE 16 (continued)
Contaminant Reference Number
Arsenic 1062
Barium 1062
Boron 352, 899, 1062
Cadmium 227, 228, 230, 922, 982, 992, 1004, 1062,
1063, 1323
Chromium 69, 71, 227, 228, 623, 922, 940, 969,
982, 1062, 1323
Cobalt 353, 982
Copper 69, 71, 227, 228, 230, 623, 875, 922,
982, 1004, 1062, 1063, 1323
Iron 227, 228, 353, 982, 1004, 1062, 1323
Lead 227, 228, 230, 922, 982, 1004, 1062,
1063, 1323
Manganese 227, 228, 410, 982, 1062, 1323
Mercury 227, 228, 471, 982, 992, 1004, 1062
Molybdenum 1323
Nickel 69, 71, 227, 230, 623, 922, 982, 1323
Seleni urn 1062
Zinc 69, 71, 227, 228, 922, 992, 1004, 1062,
1063
Other (general) 1062, 1323
Pesticides
Aldrin 353
DDT 1493
Synthetic/Organic 81fi 1(lcn
f\ i • J. *-J -> U » I "T _/ \J
Contaminants
87
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TABLE 16 (continued)
Contaminants Reference Number
Biological Contaminants
Bacteria 79, 161, 694, 1107
Cl ostrich'urn welchi 61 5
Coliforms 113, 568, 615, 983, 1084
Coxsackie virus 97, 161, 890
(A & B)
Escherichia col i 568
Fecal streptococci 568, 615, 1084
Mycobacterium 428, 568, 615
Parasitic worms «61, 428
Polio virus 97, 99, 161, 839, 840, 890
Protozoa 428
Salmonella 161, 197, 428, 568, 615, 717
Shigella 161 , 568, 615
Vibrio cholerae 161
Virus 79, 92, 95, 96, 100, 161, 352, 380, 382,
400, 428, 468, 492, 900, 1010, 1510
Other (general) 161, 531, 622, 1493
-------
The various activated sludge processes are all able to
remove over 90 percent of the soluble BOD found in wastewater.
Mitchell (922) recorded data on the removals achieved with
activated sludge processes of these and other water quality
contaminants during his study of the Los Angeles Hyperion
Treatment Plant as shown in Table 17.
TABLE 17 . ACTIVATED SLUDGE TREATMENT POLLUTANT
REMOVALS, LOS ANGELES, CA (922)
COD
BOD5
Suspended Solids
Oil and Grease
Phenol s
Ammonia nitrogen
Phosphorus
Cyanide
Treatment
Inf 1 uent
(mg/£)
315
165
103
28
0.09
20
10.1
0.30
Treatment
Effluent
(mg/£)
31
9
9
0.5
0.009
9.6
3.3
0.13
Percent
Removal
90
95
91
98
90
52
67
57
As can be seen from this table, relatively high removals of
most water quality contaminants can be attained in a practical
application over an extended period of time. These removal
efficiencies are supported by other researchers and reviewers,
including Noland and Birkbeck (1003), Huang et al. (602), Rickert
and Hunter (1158), Lindstedt and Bennett (799), and Besik (114).
ELEMENTAL CONTAMINANTS
Although the activated sludge process efficiently removes
biodegradable organic materials, only limited removal of soluble
elemental contaminants from the wastewater stream can be
achieved. The removal of elemental contaminants is governed by
two basic mechanisms: (1) the precipitation of metal hydroxides;
and (2) the adsorption of elemental contaminants by the activated
sludge floe. In either case, the elemental contaminants removed
will be contained in the sludge.
When suspended solids removals were in the 90 to 95 percent
range, 90 percent of the aluminum, iron, mercury, lead, and zinc
settled readily with the biofloc, according to Nomura and Young
(1004). Chromium (VI) and nickel median removals of 77 percent
and 50 percent, respectively, were recorded under the same
conditions. Morgan (969) stated that the removal percentages
for chromium could vary, depending upon the treatment process
used. Chromium exists in sewer systems in Cr (III) and Cr (VI);
concentrations depend upon pH. Cr (III) is readily adsorbed on
89
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particles or precipitated as Cr(OH)3(S). Chromium entering as
Cr (VI) experiences a strongly reducing environment (little or
no dissolved 0?) in sewers and treatment plants, and is thus
reduced to Cr (III) and either precipitated or adsorbed. Aera-
tion used in activated sludge or stabilization processes can
cause the resolubilization by oxidation of trivalent to hexava-
lent chromium, with resulting effluent water degradation.
The association of trace metals with suspended solids during
the activated sludge process was investigated by Chen and
Hendricks (227) and Chen and Lockwood (228) at the Hyperion
Their work confirms that many trace metals are
suspended solids, although the concentration of
particles does not appear to depend significantly
Rather, the removal of trace metals from the
Treatment Plant
associated with
trace metals on
on particle size
waste stream by
extent upon the
activated sludge processes depends to a great
adsorptive capability of the activated floes.
Mitchell (922) has recorded elemental removal efficiencies
for the Hyperion Plant over a three-year period, as shown in
Table 18 .
TABLE 18 . REMOVALS OF TRACE METALS
BY ACTIVATED SLUDGE PROCESSES,
LOS ANGELES, CA (922)
Element
Copper
Zinc
Silver
Nickel
Lead
Arsenic
Cadmium
Chromium
Inf1uent
(mg/l)
0.25
0.42
0.019
0.24
0.07
0.017
0.02
0.37
Effluent
(mg/l)
0.
0.
0.
0,
0,
0,
0,
08
23
012
15
08
013
013
0.013
Percent
Removal
68
46
37
38
24
35
96
These figures can be compared with the removal percentages as
shown in Table 19 (influent metal concentrations averaged less
than 1 mg/1). Clearly, the activated sludge process can reduce
but will not eliminate, trace metal concentrations in the muni-
cipal wastewater stream.
90
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TABLE 19 . PERCENT REMOVALS OF TRACE METALS BY
THE ACTIVATED SLUDGE PROCESS (1323)
Average
Element Percent Removal
Cadmium 56
Chromium 36
Copper 47
Iron 46
Lead 36
Manganese 16
Molybdenum 15
Nickel 20
Silver 48
Zinc 56
SYNTHETIC/ORGANIC CONTAMINANTS
Malaney et al . (836), in a study of the removal of possible
carcinogenic organic compounds by activated sludge, concluded
that no significant reduction was accomplished within normal
detention times at the three treatment plants studied. The
following Table 20 lists the possible carcinogens included in
the analysis.
Recent work by Wachinski et al. (1439) suggests that herbi-
cide detoxification can be achieved with a pure oxygen-activated
sludge treatment system that was determined to be both economical
and ecologically safe. A proprietary strain of mutant micro-
organisms, PHENOBAC (developed by the Worne Biochemical Corp.),
was utilized that was able to degrade halogenated phenols. Even
with relatively high herbicide concentrations (1380 mg/£),
degradation of as much as 73 percent was accomplished after a
16-day aeration period using optimum proportions of required
nutrients, microflora, and oxygen. According to the authors,
this figure represents a conservative estimate of possible
reductions, since testing was conducted at 18°C, while the
optimum growth temperature for PHENOBAC is close to 30°C.
BIOLOGICAL CONTAMINANTS
Activated sludge followed by secondary sedimentation can
remove over 90 percent of coliform or pathogenic bacteria that
remain after primary sedimentation; other biological pathogens
are removed to varying degrees. Nonetheless, even with 90
percent removal, appreciable amounts of pathogens remain present
in the effluent.
91
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TABLE 20. POSSIBLE CARCINOGENS
INCLUDED IN THE ANALYSIS (836)
2,3 - Butylene oxide
B - Propiolactone
Thiourea
Ethycarbamate
2 - Thiouracil
4 - Ethoxyphenylurea
B e n z i d i n e
4,4' - Dihydroxy-a,b-diethylsti1bene
2 - Naphthylamine
4,4' - Bis (dimethyl ami no) benzopheuone
p-Phenylazophenol
p-Phenylazoaniline
9,10 - Dimethylanthracene
1,2 - Benzanthracene
7 - Methyl-1,2-benzanthracene
9,10 - Dimethyl-1,2-benzathracene
1,2,5,6 - Dibenzanthracene
3/4 - Benzpyrene
1,2,4,5 - Dibenzpyrene
20 - Methylcholanthrene
2 - Nitrofluorene
2 - Fluoreneamino
N-2 - Fluorenylacetamide
7,9 - Dimethylbenz (c) acridine
7,10 - Dimethylbenz (c) acridine
Dibenz (a,h) acridine
Dibenz (a,j) acridine
92
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Pathogens can either be removed by adsorption onto the
sludge floes or destroyed by the predatory activity of the
zoogleal component. A review of the literature (531, 622)
reveals discussion of general wastewater removal rates with
little differentiation between removals and the biocidal prop-
erties of activated sludge.
Foster and Engelbrecht (428) provided a review of pathogen
removal by activated sludge processes. Conclusions of this
review are summarized in Table 21 .
TABLE 21 . REMOVAL OF PATHOGENS BY
THE ACTIVATED SLUDGE PROCESS (428)
Pathogen Percent Removal
Salmonella 96 to 99
Mycoba'cterium Slight to 87
Amoebic cysts No apparent removal
Helminth ova No apparent removal
Virus 76 to 99
Ova of intestinal parasites are apparently unaffected by
the activated sludge process; in fact, the literature indicates
that activated sludge-mixed liquor provides an excellent hatch-
ing medium for eggs.
A review by Hunter and Kotalik (615) provided additional
pathogen removal data, as summarized in Table 22 .
TABLE 22 . PERCENT REMOVALS OF BIOLOGICAL PATHOGENS BY
THE ACTIVATED SLUDGE PROCESS (615)
Pathogen Percent Removal
Coliform 90 to 99
Fecal streptococci 84 to 94
Shigella 90 to 99
Salmonella 70
Pseudomonas aergglnosa 99
Clostridlum perfringlrTs 90 to 99
MycobacteTTum tuberculosis 66 to 88
A 11st of the species of protozoans, nematodes, and fungi that
have been found 1n activated sludge effluent was also presented
by the authors. Species recorded Include:
93
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Protozoa -
Amoeba sp.
Euplotes patel1 a
Loxophyl1qm he! us
Oi komonas sp^
Pelodini urn reni forme
Phyllomitus anylophagus
Trlgonomonas compressar
Vortice11 a campanula
Epi sty!i s pii ciati1s
Nematodes -
Rhabditidae
Diplogasteridae
Dorylaimidae
Monochidae
Alternaria
Aspergillus
Aureobasi dium
Candida
Cryptococcus
F u s a r i u m
Geotrichum
Hansenula
Kloeckera
Mucor
P e n i c i 11 i u m
Rhodotorula
Saccharomyces
Torulopsis
Tri chodsrma
Trichosporon
The removal of viral
recently become the topic
viral removal of up to 90
activated sludge process.
contaminants by activated sludge has
of considerable research. In general
percent has been observed after the
However, large variations in removal
have been reported, probably because sampling was not temporally
coordinated (468). Destruction by sewage microflora and virus
adsorption to floe during the process are believed to be the
main factors governing viral removal. Table 23 reports typical
viral removals that can be expected from activated sludge
treatment (161).
TAB
Pat
LE 23 .
hogen
V
IRAL
REMOVAL
B
Y ACTIVATED S
Percent Remov
LU
al
DG
E
TREATMENT
(161)
Enteroviruses
Polio viruses
Coxsackie viruses
ECHO viruses
0 to 90 percent
0 to 90 percent
0 to 50 percent
no apparent removal
Malina et al. (839) concluded from their research that
viral inactivation by activated sludge is independent of the
hydraulic detention time. Polio virus adsorption to sludge is
almost immediate; the adsorbed virus particles are inactivated
according to first order kinetics with a half-life in the range
of 4 to 5 hr. Activated sludge utilizes aeration for optimum
dispersion of the flocculant masses which, along with gases
produced during microbial respiration, may entrain bacterial
and viral pathogens in aerosols. The aerosols released are in
the 5-ym diameter range, small enough to permit lung penetration
of a substantial proportion of the particles.
94
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SECONDARY TREATMENT: TRICKLING FILTER
INTRODUCTION
Trickling filters have been widely used for secondary bio-
logical treatment of municipal wastewater, and substantial
literature is available on this porcess, as indicated on Table
24 .
The trickling filter system generally consists of a tank
open on both top and bottom. The tank is filled with a rock or
plastic filter media having a high surface area to allow attach-
ment of zoogleal slimes and void fraction for movement and dif-
fusion of 'oxygen. Contaminant removal is accomplished through
adsorption at the surface of the biological slimes covering the
filter media. Following adsorption, the organics are utilized
by the slimes for growth and energy. The trickling filter is
followed by clarification to remove biological solids periodi-
cally flushed from the filter.
Trickling filter influent is usually from a primary treat-
ment system. System outputs include effluent, sludge, and pos-
sible aerosols.
The literature generally refers to percent removal, with
no distinction made between separation and degradation or des-
truction. As in the case of other secondary processes, the
literature primarily addresses the general and biological con-
taminants and is sparse in the areas of elemental, synthetic,
and biocidal contaminants.
WATER QUALITY PARAMETERS
The removal of BOD and suspended solids by trickling fil-
ters is reported to be from 65 to 95 percent, averaging about
85 percent (622, 1323). The efficiency of trickling filtration
decreases as temperatures fall below 2QOC. Imhoff et al . (622)
reported that a reduction of temperature from 20° to 10°C
results in an efficiency loss' of about 40 percent. Nickerson
et al. (996) found that chemical addition ahead of primary
clarifiers increases overall BOD and suspended solids removals
in trickling filters. Lager and Smith (745) reported that no
significant removal of total nitrogen or phosphorus occurred
during the conventional trickling filter process. In low-
rate filters, ammonia and nitrogenous organic compounds are
95
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TABLE 24. LITERATURE REVIEWED PERTAINING
TO TRICKLING FILTERS
Contaminant Reference Number
Water Quality Parameters
Ammonia 5, 41, 349, 745, 891, 1403, 1484
BOD 60, 241, 622, 745, 814, 907, 996, 1013,
1143, 1323, 1360, 1403, 1546
Chlorides 907, 1484
COD 241, 491, 891, 907, 1485
Nitrates 4, 5, 349, 745, 891, 1484
Nitrites 349, 891, 1484
Phosphates 70, 633, 745, 814, 891, 1013, 1484
Suspended solids 498, 622, 745, 996, 1013, 1323, 1403, 1546
Total organic 60, 241, 615
carbon
Other (general) 391, 393, 531, 622
Elemental Contaminants
Aluminum 814
Boron 1484
Cadmium 1323
Chromium 69, 1143, 1323
Copper 69, 1143, 1323
Germanium 1411
Iron 1323, 1484
Lead 1323, 1484
Manganese 1323, 1484
Molybdenum 1323
96
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TABLE 24 (continued)
Contaminant Reference Number
Nickel 69, 876, 1143, 1323
Zinc 69, 1143, 1323
Synthetic/Organic 241, 615
Contaminants
Biological Contaminants
Bacteria 79, 142, 161, 400, 486
Coliforms 486, 568, 983, 1278
Coxsackie virus 161
(A & B)
Escherichia coli 568
Fecal streptococci 1278
Mycobacterium 428
Parasitic worms 161, 428, 615
Polio vi rus 161
Protozoa 428
Salmonella 161, 428, 717, 1278
Shigella 161
Vibrio cholerae 161, 717
Virus 79, 95, 96, 97, 100, 161, 380, 429, 492,
1278
Other (general) 161, 486, 622
97
-------
usually oxidized to yield high proportions of nitrates and some
nitrites in the effluent; high-rate trickling filter effluents
are low in nitrates and nitrites due to limited system oxidation
Barth et al. (70) reported total phosphorous removals of up to
75 percent with direct dosing of aluminate to a trickling filter
ELEMENTAL CONTAMINANTS
Removal of elemental contaminants by trickling filters is
not well documented. A summary of the literature on metal
removals as compiled by the State of California Water Resources
Board is shown in Table 25.
TABLE 25. TRICKLING FILTER PROCESS REMOVAL
OF TRACE METAL CONTAMINANTS (1323)
Average
Element Percent Removal
Cadmium 5
Chromium 19
Copper 47
Iron 46
Lead 36
Manganese 16
Molybdenum 15
Nickel 20
Silver 48
Zinc 56
Trace metal removals by trickling filters are substantially
lower than those achieved with the activated sludge process be-
cause there is less formation and sedimentation of trace metal
complexes.
BIOLOGICAL CONTAMINANTS
Trickling filters do not effectively remove many biological
pathogens. Table 26 illustrates reported removal efficiencies.
Organisms are adsorbed into the zoogleal slime but due to
similar surface charges and morphology, biocidal effects are
variable (622).
98
-------
TABLE 26. REMOVAL OF PATHOGENS BY
TRICKLING FILTERS (428)
Pathogen Group
Efficiency
Salmonel 1 a
Mycobacterium
Amoebic Cysts
Helminth Ova
Virus
88
66
11
62
0
to
to
to
to
to
99
99
99
76
84
.9
.9
Foster and Engelbrecht (428) observed that trick-
ling filters are capable of reducing paratyphoid organisms by
84 to 99 percent. A review by Hunter and Kotalik showed 99.7
percent removal ofSchistosoma mansoni ova. The authors also
concluded that trickling filter effluents can contribute a
major portion of the free living nematode population found in
receiving waters.
Improperly operated low-rate trickling filters can provide
an excellent breeding area for insects, especially filter flies
(Psychoda) and springtails. Trickling filters cannot be depen-
ded upon to produce significant or consistent viral reductions.
Foster and Engelbrecht (428) reported removals ranging from 0
to 84 percent. Berg (97) speculated that even when viruses are
adsorbed, they may eventually be replaced by other substances
and leach out of the filter slime as a result of an equilibrium
effect.
99
-------
SECONDARY TREATMENT: AERATED LAGOONS
INTRODUCTION
Aerated lagoons are ponds in which mechanical aeration
is used to increase the rate at which oxygen is made avail-
able to facilitate biological stabilization. The aeration
also provides mixing for suspension of microbial floe.
The biological process does not include algae, and organic
stablization depends on the mixed liquor that develops within
the pond. Literature surveyed concerning aerated lagoons is
1isted in Table 27.
WATER QUALITY PARAMETERS
BOD removal by aerated lagoons is a function of aeration
period, temperature, and the nature of the wastewater. The
aeration of a typical domestic wastewater for five days at 20°C
provides about 85 percent BOD reduction; lowering the temperature
to 10°C reduces the efficiency to approximately 65 percent (531).
BIOLOGICAL CONTAMINANTS
A discussion of the literature by Parker (1052) revealed
that coliform reductions in the range of 80 to 99 percent can be
achieved with optimum detention time. This is supported by the
experiments of Carpenter et al. (198), who reported that coli-
form organisms are efficiently removed by the use of aerated
lagoons. Klock (717) stated that the coliform survival rate
in lagoons is a function of the oxidation-reduction potential
and temperature.
Berg (95) discussed the removal of viruses by stabilization
ponds, concluding that virus removal can be expected to be
erratic.
100
-------
TABLE 27. LITERATURE REVIEWED PERTAINING
TO AERATED LAGOONS
Contaminant Reference Number
Water Quality Parameters
Ammonia 454
BOD 91 , 484, 531, 651, 784, 1404
COD 91, 266, 484
Nitrates 454
Nitrites 454
Phosphates 328, 784
Suspended solids 484, 745
Other (general) 393, 531, 622
Biological Contaminants
Bacteria 198, 717
Coliforms 198, 568, 717, 1052
Escherichia coli 1052
Fecal streptococci 568, 1052
Salmonella 568
Virus 95, 198, 382
101
-------
SECONDARY TREATMENT: PONDING
INTRODUCTION
An oxidation or facultative pond is generally a shallow
earthen basin designed to promote a symbiotic existence between
algae and bacteria (745). Algal photosynthesis and surface
reaction maintain aerobic conditions in the photic region, while
anaerobic bacteria flourish in the aphotic zone. Ponds are
normally operated in series and are sometimes used for
"polishing" effluent from conventional secondary processes.
Influent to a ponding system may be raw sanitary waste,
primary effluent, or secondary effluent. Pond effluent can
enter the environment by direct discharge or by seepage to the
groundwater. Literature reviewed concerning ponding is listed
in Table 28. As can be seen from this review, only a limited
amount of research has examined the removal of contaminants by
the ponding process.
WATER QUALITY PARAMETERS
Oxidation pond removal efficiencies for suspended solids
and BOD can vary widely and may even reach negative values
(745). Removal ranges of 60 to 50 percent have been reported
for suspended solids, and of 70 to 10 percent for BODg. This
variation occurs because most influent BOD is converted into
suspended algal mass. This mass exerts a BOD demand and provides
suspended solids that may be carried into the effluent.
Bacterial decomposition and algal growth are both retarded
by reduced temperatures, reducing removal efficiency of the
ponding process (531).
SYNTHETIC/ORGANIC CONTAMINANTS
The removal of trisodium nitri1otriacetate (NTA) by ponding
has been investigated by Klein (714). He found that after a
two-month acclimation period, steady-state removal was in excess
of 90 percent, with influent concentrations in the range of
30 mg/£.
102
-------
TABLE 28. LITERATURE REVIEWED PERTAINING TO PONDING
Contaminant Reference Number
Water Quality Parameters
BOD 326, 531, 745
COD 1484
Chlorides 427
Fluorides 427
Nitrates 226, 326, 375, 446, 1432
Phosphates 326, 375, 426, 446, 1484, 1500
Suspended solids 393, 745
Other (general) 393, 531, 745
Synthetic/Organic 714
Contami nants
Biological Contaminants
Bacteria 842, 1278
Coliforms 849, 850, 1278
Escherichia coli 850, 1048
Fecal streptococci 849, 850, 1278
Salmonel1 a 669
Virus 95, 96, 97, 1278
103
-------
BIOLOGICAL CONTAMINANTS
Ponding preceded by adequate secondary treatment provides
excellent bacteria removal. Kampelmacher and Jansen (669) found
that removal of salmonella by oxidation ponds was not Inferior
to removal achieved by conventional treatment plants. Species
of the coliform group, although reduced by ponding, are not
effectively eliminated according to Parhad and Rao (1048).
Slanetz et al. (1278), however, reported that if two ponds were
operated in a series at temperatures of 17° to 26 C, the die-off
rate of coliform, fecal coliforms, and fecal streptococci ranged
from 95 to 99 percent. During winter when temperatures were in
the 1° to IOC range, the die-off rate was 46 times lower. Berg
(97) states that virus removal by ponding is erratic, ranging
from 0 to 96 percent; virus recovery decreased as the effluent
passed through a series of maturation lagoons.
104
-------
TERTIARY TREATMENT: CHEMICAL TREATMENT
INTRODUCTION
The purpose of chemical treatment is to coagulate sus-
pended solids and precipitate phosphate and various trace
metals. Chemical coagulation of secondary effluents may
be accomplished by the addition of lime, alum, polymers, or
iron salts, and involves three operations: (1) injection
and rapid mixing of the coagulants to neutralize the pre-
dominantly negative charges on suspended matter; (2) gentle
stirring to promote agglomeration of the coagulated particles
into large, settleable floe; and (3) sedimentation to provide
gravity separation of the flocculated material from the waste
water. The settled material is transferred to a sludge hand-
ling system. As indicated by Table 29, a great deal of infor-
mation is available concerning the removal of various public
health impairing contaminants by chemical treatment processes.
WATER QUALITY PARAMETERS
Culp and Shuckrow (278) investigated chemical treatment of
raw wastewater with lime and found that removals of 95 to 98
percent phosphorus and 99 percent suspended solids can be
achieved with chemical clarification followed by carbon adsorp-
tion. The treatment of municipal wastewater with alum precipi-
tation as studied by Shuckrow et al. (1254) resulted in
removal efficiencies of 85 percent for COD and 83 percent for
total organic carbon.
The removal of BOD, suspended solids, and phosphorus as
reviewed by Lager and Smith (745) is summarized in Table 30 .
Removals from secondary effluents of the magnitudes listed
obviously provide a high quality effluent.
105
-------
TABLE 29 . LITERATURE REVIEWED PERTAINING TO CHEMICAL TREATMENT
Contaminant Reference Number
Water Quality Parameters
Ammonia 43, 120, 277, 284, 390, 601, 614, 885,
891, 1321 , 1510
BOD 119, 124, 277, 278, 284, 334, 498, 614,
745, 794, 799, 813, 814, 878, 885, 996,
1012, 1013, 1215, 1337, 1388, 1393, 1402,
1467, 1510
Chlorides 885
COD 119, 120, 124, 249, 277, 278, 284, 329,
498, 885, 1254
Cyanides 107, 922, 993
Fluorides 410, 1321
Nitrates 119, 120, 124, 249, 277, 278, 284, 329,
498, 885
Nitrites 284, 390, 891, 1085, 1321, 1510
Phosphates 278, 284, 290, 295, 326, 328, 375, 410,
423, 479, 513, 601, 614, 650, 711, 743,
745, 763, 794,,799, 814, 865, 876, 885,
891, 1012, 1013, 1036, 1039, 1213, 1215,
1265, 1311, 1321, 1337, 1341, 1393, 1402,
1466, 1500, 1510, 1547, 1552
Suspended solids 38, 108, 119, 120, 249, 278, 330, 498,
601, 701, 745, 799, 813, 896, 996, 1012,
1013, 1215, 1254, 1338, 1389, 1393, 1402,
1485, 1510
Total dissolved 277, 1215, 1321
sol ids
Total organic 119, 120, 124, 284, 1254, 1467
carbon
Other (general) 385, 391, 393, 531, 622
106
-------
TABLE 29 (continued)
Contami nant Reference Number
Elemental Contaminants
Aluminum 334, 814, 1036, 1383
Antimony 38
Arsenic 38, 855, 922, 1062, 1274, 1323, 1383
Barium 38, 855, 1062, 1323, 1383
Boron 1383
Cadmium 38, 39, 107, 802, 855, 922, 1103, 1323,
1383, 1504, 1505, 1506
Chromium 38, 39, 204, 802, 855, 1323, 1385, 1504,
1505, 1506
Cobalt 1383
Copper 38, 39, 107, 204, 855, 922, 1323, 1383,
1504, 1505, 1506
Iron 38, 334, 763, 1323, 1383, 1504, 1506
Lead 855, 922, 1323, 1383, 1411, 1504, 1506
Manganese 38, 334, 410, 855, 1323, 1383, 1504,
1505, 1506
Mercury 38, 775, 811, 855, 922, 1077, 1323,
1353, 1383, 1504, 1505, i506
Molybdenum 38, 1323
Nickel 38, 855, 922, 1323, 1383, 1504, 1505
Selenium 802, 1323, 1383
Uranium 38, 1323
Zinc 38, 107, 855, 922, 1323, 1383, 1504,
1505, 1506
Other (general) 38, 760, 799, 1323, 1506
107
-------
TABLE 29 (continued)
Contaminant Reference Number
Synthetic/Organic 6, 1496
Contaminants
Biological Contaminants
Adeno virus 1522
Bacteria 79, 331, 335, 670, 799, 830, 891
Coliforms 101, 284, 469, 799, 896, 1393
Coxsackie virus 97, 1522
(A & B)
ECHO virus 1522
Escherichia coli 880, 1183, 1382
Fecal streptococci 799
Hepatitis virus 469, 1522
Parasitic worms 830
Polio virus 103, 159, 223, 499, 837, 1293, 1313,
1382, 1510, 1522
Protozoa 830
Salmonella 670
Virus 79, 92, 96, 97, 159, 219, 220, 245, 246,
259, 283, 284, 331, 380, 381, 468, 848,
1009, 1057, 1071, 1243, 1302, 1312, 1313,
1510, 1511
108
-------
TABLE 30. REMOVALS ACHIEVED BY CHEMICAL
CLARIFICATION (745)
Chemical BOD Suspended Solids
Removal Removal
(Percent) (Percent)
Lime pH 11.5 80 90
Ferric Chloride 80 95
170 mg/£ dose
Ferric Chloride 75
80-100 mq/l dose
Phosphate removal by chemical precipitation (lime) has
received considerable attention in the literature in recent
years. The research on phosphate removal in general indicates
that lime clarification usually provides removal efficiencies
greater than 90 percent. This is supported by the work of
Davis (295), Sturm and Hatch (1341), Johnson (650), and
Bernhardt et al. (108) .
ELEMENTAL CONTAMINANTS
The precipitation of metal hydroxides from solution is
governed by the pH and the concentration of the metal ion in
solution. Since many of the trace metals form insoluble hydro-
xides near pH 11, lime coagulation results in a reduction of
these metal concentrations. Table 31 (1323) summarizes the
effects of lime coagulation on a number of heavy metals. Some
of the data were collected on industrial .metal wastes charac-
terized by metal ion concentrations a great deal higher than
would occur in any municipal plant influent. The data are
included here as examples of possible metal reductions, since
since such figures from chemical coagulation of municipal waste
waters are scarce.
As can be seen from these figures, arsenic, molybdenum,
and selenium had relatively poor removal rates,and the poten-
tial removal of mercury was estimated to be low. Only 11 per-
cent of hexavalent chromium was removed, although the trivalent
form was reduced more than 99.9 percent. Most other metals
tested were very effectively reduced at high pH. Lower remo-
vals of these same metals (usually less than 50 percent) can be
achieved with alum coagulation at near neutral pH values
(1323), a fact that illustrates the dependence of precipitation
on pH.
Gulledge and O'Connor (520) studied the removal of arsenic
(V) from tap water in jar tests using alum and ferric sulfate.
109
-------
TABLE 31 . REMOVAL OF ELEMENTAL CONTAMINANTS
BY LIME COAGULATION (1323)
Metal
Antimony*
Arsenic3
Barium9
Bi smuth3
Cadmium
Chromium (+6)
Chromium (+3)
Copper
Gold9
Iron
Leada
Manganese
Mercury3
Molybdenum
Concentration
Before Treatment
mg/i
23
--
Trace
0.0137
0.56
7,400
15
15,700
7
7
302
15
--
13
17
2.0
15
2.3
2.0
21.0
Trace
11
Concentration
After Treatment
mg/£
--
23
1.3 (sol)b
.0002 (sol)
0.00075
0.050
2.7
0.4
0.79
1
.05
Trace
0.6
<.001 (sol)
2.4
0.1
1.2C
<.001 (sol)b
0.5
<0.1
l.ic
0.05
Oxide Soluble
9
Percent
Removal
90
<10
0
Abt. 50
94.5
11
99.9 +
97
99.9 +
86
93
99 +
97
90 +
82
99 +
40
90+
97
96
45
95
<10
Abt. 10
18
110
-------
TABLE 31 (continued)
Metal
Nickel
Selenium
Silver
Teluri uma »d
Titanium3 >d
Urani ume
Zinc
Concentration
Before Treatment
mg/£
160
5
5
100
16
0.0123
0.0546
--
--
17
Concentration
After Treatment
mg/l
0.08
0.5
0.5
1.5
1.4
0.0103
0.0164
(<0.001?)
(<0.001?)
?
0.3
.007 (sol)
% Removal
99.9 +
90
90
99
91
16.2
97
( 90+)
( 90+)
?
98
90+
a The potential removal of these metals was estimated from
solubility data.
b Barium and lead reductions and solubilities are based
upon the carbonate.
These data were from experiments using iron and manganese
. in the organic form.
Titanium and telurium solubility and stability data made
the potential reduction estimate unsure.
Uranium forms complexes with carbonate ion. Quantitative
data were unavaiTable to allow determination of this
effect.
Ill
-------
In each case, increased coagulant dosage resulted in increased
arsenate removal. Dependence on pH was again seen in this
study. Under optimum conditions, removals of 85.8 percent with
alum and 96.8 percent with ferrous sulfate were achieved.
Pilot plant studies of municipal wastewater containing 5
mg/l arsenic cited by Patterson (1062) suggest that chemical
treatment can provide efficient removal of this element.
Ferric sulfate at 45 mg/£ Fe and pH 6.0 removed 90 percent of
the arsenic; lime at 600 mg/£ and pH 11.5 removed 73 percent.
In similar studies cited by Patterson, barium removals of 97
percent were obtained when municipal wastewater dosed with 5
mg/£ barium was treated with 45 mg/£ Fe at pH 6.0. Lime at
600 mg/£ and pH 11.5 resulted in 80 percent removal. The re-
moval of cadmium from waters by sorption onto hydrous oxides of
solid metals such as manganese and iron was investigated by
Posselt and Weber (1103). They concluded that sorptive uptake
of cadmium on such materials would constitute a method easily
adaptable to present treatment technology.
BIOLOGICAL CONTAMINANTS
Chemical treatment can be used to reduce or remove many
biological pathogens present in municipal wastewater. Lindstedt
and Bennett (799) evaluated the effectiveness of lime clarifi-
cation in reducing bacterial concentrations, finding that
treatment effectiveness increases with increasing chemical
dosage and pH. At a lime dosage of 400 mg/l , fecal coliform,
fecal streptococcus, and total coliform concentrations could be
reduced by two orders of magnitude. It was also found that
about 90 percent removal of bacteria can be achieved through
alum clarification over a broad range of alum dosage.
Jar tests employing the f2 bacteriophage virus, lake
water, and a variety of chemical coagulants and polyelectrolyte
coagulant aids were conducted by York and Drewry (1522). As
shown in Table 32 , aluminum sulfate (alum), ferric chloride,
ferric sulfate, ferrous sulfate, and polyelectrolyte B were
found to give maximum virus removals greater than 90 percent at
optimum dosage.
112
-------
TABLE 32 . COMPARISON OF THE EFFECTIVENESS OF
THE COAGULANTS TESTED (1522)
Coagulants-
Coagulant Aids
A12(S04)3
FeCl3
Fe2(S04)3 x H20
FeS04 and Ca(OH)2
Al 2( 50^)3 and
N52OAT 2U3
Polyelectrolyte A
Al2(S04)3 and
polyelectrolyte B
Polyelectrolyte B
A12(S04)3 and
polyelectrolyte B
Al2(S04)3 and
polyelectrolyte C
A12(S04)3 and
polyelectrolyte E
A12(S04)3 and
polyelectrolyte F
^12(504)3 and
polyelectrolyte D
Dose
mg/t
25
50
50
36
30
23
2.0
18
1.0
2.0
18
0.7
18
0.4
18
0.1
18
0.1
18
1.0
Maximum
Virus
Removal
percent
99.9
99.4
92.0
93.5
98.6
76
99.2
99.6
99.8
99.3
99.3
99.6
99.4
Berg et al. (103) experimentally mixed polio virus I and secon-
dary effluent in containers, added lime, and stirred the solu-
tion for 15 min to allow formation of floe particles. Settling
to 75 min. The removals obtained with varying
are shown in Table 33 . Large coagulant doses
effecting virus removals of up to 99.9 percent.
After further investigation, the authors concluded that signi-
ficant destruction of viruses can be attributed to the high
pH occurring with high lime concentrations (in the range of 400
to 500 mg/t).
followed for 60
dosages of lime
were capable of
113
-------
TABLE 33 . REMOVAL OF POLIO VIRUS I FROM SECONDARY
EFFLUENT BY FLOCCULATION WITH Ca(OH)2 (103)
Ca(OH)2
Concen-
tration
mg/£
200
300
400
500
500
Initial Virus
Concen-
tration
pfu/£
33,333
51,480
55,000
33,333
33,333
pH of
Treated
Effluent
9.30
10.21
11.30
11.03
11.01
Surviving Virus
Concen-
tration
pfu/£
2,200
15,912
1,940
505
47
Virus
Removal
percent
92.3
69.1
96.5
98.5
99.86
Chaudhuri and Engelbrecht (219) used water devoid of
extraneous organic matter in their laboratory investigation of
virus removal with alum. Using the experimentally determined
optimum pH and dosage, 98.0 percent removal of bacteriophage
T4 and 99.9 percent removal of bacteriophage MS2 were obtain-
able. However, the addition of organic matter in the form of
albumin or treated wastewater lowered these efficiencies. For
example, only 95.7 percent removal of bacteriophage T4 was ob-
tained after the addition of 200 ml/I of settled wastewater.
Further experiments demonstrated no inactivation of the virus
particles that were removed in the settled floe. However,
Brunner and Sproul (159) demonstrated 60 percent permanent Inac-
tivation in the case of polio virus I removed from solution
with aluminum phosphate precipitates. Their studies of polio
virus I and bacteriophage T2 removal showed that under optimum
conditions, removals can reach 98 and 94 percent, respectively,
with aluminum and calcium precipitation. Actual removals are
related to pH and chemical dosage.
Chemical treatment (high pH) holds considerable promise
as a means of effectively inactivating or destroying pathogenic
organisms contained in wastewater. By itself, chemical treat-
ment cannot be relied upon to produce a pathogen-free effluent;
used in conjunction with disinfection, however, it can help
ensure that such an effluent is achieved.
114
-------
TERTIARY TREATMENT: FILTRATION
INTRODUCTION
Inability of gravity sedimentation in secondary clarifiers
to remove small particles (and associated public health impair-
ing contaminants) is a limitation of BOD and suspended solids
removal by conventional wastewater treatment. Filtration as a
tertiary process upgrades treatment performance by removing a
portion of the unsettled suspended solids from secondary efflu-
ents. In addition, filtration often precedes other tertiary
processes such as adsorption and ion exchange since the pre-
sence of suspended solids interferes with the operation of
these processes. Reviewed literature on filtration is shown in
Table 34.
Filtration of wastewater to reduce the suspended solids
concentration is accomplished by passage through a bed of gran-
ular particles. Single, dual, or mixed media beds may be used,
composed of anthracite coal, granite, sand, and/or gravel
(531). Suspended solids are removed by a variety of mecha-
nisms: straining, impingement, settling, and adhesion. The
treatment efficiency of the process is influenced by:
• The concentration and characteristics of the wastewater
solids (particle-size distribution, surface character-
istics, organic versus inorganic, etc.)
• The characteristics of the filter media and filtering
aids used (particle-size distribution, surface charac-
teristics, etc.)
• The design and operation of the filter.
Since wastewater flow rate and solids content are variable, and
processes upstream of filtration may vary in performance, the
efficiency of filtration may also be expected to vary. For
this reason, values presented in the following discussion
should be considered as merely indicative of the range of
achievable removals.
WATER QUALITY PARAMETERS
In general, the best effluent quality achievable by
plain filtration of secondary effluent is about 5 to 10 mg/fc
for suspended solids and BOD. The suspended solids content of
115
-------
TABLE 34. LITERATURE REVIEWED PERTAINING TO FILTRATION
Contaminant Reference Number
Water Quality Parameters
Ammonia 43, 548, 885, 1323, 1546
BOD 119, 314, 697, 771, 885, 1319,1323,
1393, 1546
COD 119, 771, 885, 1319, 1323
Chlorides 114, 885, 1062, 1319, 1367
Cyanides 1062
Fluorides 1062
Nitrates 384, 885, 1319, 1367
Oil and grease 1062
Phosphates 108, 119, 314, 659, 885, 1323, 1393
Suspended solids 39, 108, 454, 531, 659, 771, 1323, 1367,
1393, 1452, 1546
Total dissolved 1062
solids
Total organic 114, 119, 1323
carbon
Other (general) 385, 531, 622
Elemental Contaminants
Arsenic 1062, 1244
Barium 1062
Boron 1062
Cadmium 38, 39, 802, 1062, 1063, 1559
Chromium 38, 39, 802, 1062, 1559
Copper 38, 39, 697, 1062, 1063, 1319, 1559
Iron 38. 1062. 1319, 1559
116
-------
TABLE 34 (continued)
Contaminant Reference Number
Lead 1062, 1063, 1559
Manganese 38, 635, 1062, 1319, 1559
Mercury 1062
Nickel 38, 1062, 1063
Selenium 38, 802, 1062
Zinc 38, 697, 1062, 1063, 1319, 1559
Other 38, 1062
Synthetic/Organic 1062, 1496
Contaminants
Biological Contaminants
Bacteria 161, 331
Coliforms 101, 469, 608, 617
Coxsackie virus 95, 161
(A & B)
ECHO virus 1182
Hepatitis virus 469
Parasitic worms 161, 1469
Polio virus 103, 153, 161, 223, 1168, 1182, 1293
Salmonella 161
Shigella 161
Vibrio cholerae 161, 424
Virus 25, 95, 96, 152, 154, 161, 261, 331,
454, 468, 492, 608, 1009, 1240, 1312
Other (general) 153, 161
117
-------
secondary effluent was reduced to 5 mg/s, with both rapid sand
and mixed media filters, employed respectively at a treatment
and a pilot plant. Complete removal, however, could not be
effected. If further reduction is desired, chemical coagula-
tion must precede filtration (454, 531).
Two studies at a pilot facility and a major treatment
plant (1323) indicated that essentially complete suspended
solids removal was accomplished when filtration was preceded
by chemical treatment of secondary effluent. Chemical clar-
ifier effluent contained 0.7 mg/n total phosphorus; after
filtration, this phosphorus content was reduced to 0.1 mg/fc.
At the pilot facility, the filter effluent contained 17.6 mg/£
COD, 9 mg/i total organic carbon (TOC) , and no detectable
phosphorus, compared with filter influent concentrations of
18.1 mg/£ COD, 8.6 mg/s, TOC, and 0.4 mg/i phosphorus.
When chemically treated secondary effluent was applied to
rapid-sand filters, generally 20 to 60 percent of applied BOD
was removed, 30 to 70 percent of phosphate, and 40 to 80 per-
cent of the suspended solids (1393). These values were ob-
tained using a variety of influent concentrations and chemical
dosages. The results of 30 days continuous operation of a
pilot plant practicing filtration preceded by chemical treat-
ment of secondary effluent are summarized in Table 35 (1323).
TABLE 35. RESULTS OF ONTARIO, CANADA, PILOT PLANT
STUDY INVOLVING FILTRATION PRECEDED BY
CHEMICAL TREATMENT OF SECONDARY EFFLUENT (1323)
Qua!i ty Parameter
Raw
Wastewater
Secondary
Effluent
Filter
Effluent
Total Organic Carbon
110-165
14-28
4.5-7.5
BOD5 (mg/l)
P04 (as P04)
Total Nitrogen N
Ammonia N
Suspended Solids
230-400
9-21
27-51
17-29
148-268
5-14
1.3-3.5
25-37
21-29
13-37
2.0-3.0
0.4-1.0
20-35
18-29
3-12
Results of a pilot, plant study at Cleveland, Ohio - where
chemical coagulation and settling of raw wastewater was
118
-------
followed by filtration and granular carbon adsorption - were
reviewed by Gulp and Shuckrow (278). On the basis of the data
provided, removals attributable to chemical treatment and fil-
tration can be calculated to be 66 percent of the applied BOD
and 77 percent of the applied COD. A second pilot plant study
reviewed by the authors involved the same treatment scheme.
Removals at this plant due to combined chemical treatment and
filtration can be inferred to range from 77 to 84 percent.
While studying soil filtration, de Vries (3K) applied
primary effluent to a sand filter and obtained BOD and phos-
phate removals of nearly 100 percent. Phosphate removals were
attri buted
grains
100
to the natural coatings of
Fe203
and
A1203
-on sand
ELEMENTAL CONTAMINANTS
After chemical treatment, filtration to remove residual
particulate matter may provide some additional removal of ele-
mental contaminants. Elemental contaminant removals achieved
by filtration depend primarily upon the extent of suspended
solids removals, with which the various trace elements are
associated. Table 36 , compiled from the literature by Argo
and Gulp (38) gives results for sand filtration of some
municipal and industrial wastes.
TABLE 36 . HEAVY METAL REMOVAL BY SAND FILTRATION
FOLLOWING LIME COAGULATION (38)
Metal
Cd
Cr+6
Cr+3
Cu
Fe
Mn
Ni
Se
Concentration
Before Filt.
0
0
2
0
0
Trace to
.00075 mg/l
.0503
.7
.79
-
_
_
.08
.0103
Concentrati on
After Treat. pH
0
0
0
0
0
1
0
1
0
0
0
.00070
.049
.63
.32
.5
.1
.2 Organic
.1
.1 Organic
.1
.5
.00932
8.
7.
7.
8.
9.
10.
10.
10.
10.
8.
9.
11
1
6
6
7
5
8
5
8
5
7
5
% Removal
By Filt.
95
6
2
77
59
9
.6
.6
.5
.5
119
-------
TABLE 36 (continued)
Metal
Ag
Zn
Concentration
Before Hit.
0.00164
0.97
Concentration
After Treat.
0.00145
0.23
2.5
£H
11
8.7
9.5
% Remova
By Filt.
11.6
76.3
1
Patterson (1062) cites evidence from pilot plant studies that
little or no additional removal of arsenic was afforded by fil-
tration of chemically treated municipal wastewater.
BIOLOGICAL CONTAMINANTS
Several investigations have been reported concerning the
removal of viruses by sand filtration. It has been shown that
insignificant virus removal is achieved by rapid filtration
through clean sand (25, 95). However, virus removal efficiency
will be increased by impregnation of the filter medium with
coagulated floe, the presence of organic matter trapped in the
sand, chemical flocculation prior to filtration, or a decrease
in the filtration rate. The addition of iron salts prior to
filtration has resulted in significantly higher coliform reduc-
tions, as discussed by Hunter et al. (617). Similarly,
Robeck et al. (1168) noted that if a low dose of alum was fed to
a rapid coal and sand filter just ahead of filtration, more
than 98 percent of polio virus Type I could be removed. If the
dosage was increased and conventional flocculators and settling
were used, removal was increased to over 99 percent. The
authors also noted a general trend toward better removal of
polio virus I with slower filtration rates although their data
were often erratic. At slow sand filter rates (0.6 to 1.2
£/min/m2), removal ranged from 50 percent to about 98 percent.
At rapid filtration rates (38 to 76 £/min/m2), virus removals
ranged from about 10 to 70 percent. Similarly, research exam-
ined by Berg (95) showed that filtration through sand at 7.5 I/
min/m2 removed 99 percent of the coxsackie virus A5 while fil-
tration at 75 £/min/m2 removed only about 10 percent of the
virus .
Brown et al. (153) reported 70 to 90 percent removals of
low concentrations of either bacteriophage T2 or polio virus
Type I by filtration through uncoated diatomaceous earth.
However, no significant virus removals by uncoated diatomaceous
earth were achieved in a laboratory study by Amirhor and
Engelbrecht (25). With polyelectrolyte-coated filter media,
removals greater than 99 percent were consistently achieved (25)
120
-------
In laboratory tests by Berg et al . (103), from 82 to
greater than 99.8 percent of polio virus I was removed from
chemically treated effluent by rapid sand filtration. The
results of these tests are given in Table 37 .
TABLE 37 . REMOVAL OF POLIO VIRUS I FROM
Ca(OH)2 FLOCCULATED EFFLUENT BY RAPID
SAND FILTRATION
AS MEASURED BY MEMBRANE FILTER RECOVERY OF VIRUS
(103)
Test No.
Virus Concentration pfu/£
Before Sand
Fi1tration t
After Sand
Fi1tration
Virus Removal
percent
1
2
3
4
5
2,200
15,912
1,940
505
47
397
750
<4
12
2.8
82.0
95.3
>99.8
97.5
94.0
* Filtration rate 2.25 gpm/sq ft through 8 in of sand.
t Virus concentration in flocculated effluent just prior to
sand filtration.
Laboratory experiments on the removal of nematodes by
rapid sand filtration were conducted by Wei et al . (1469).
Removal efficiency was about 96 percent when all the nematodes
in the influent were dead or nonmotile. However, most motile
nematodes were able to penetrate the filter bed.
Sand
cysts and
Bryan (161)
ded.
filtration may also provide some removal of amoebic
ascaris eggs, according to a literature survey by
He did not indicate the levels of removal affor-
121
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TERTIARY TREATMENT: ADSORPTION
INTRODUCTION
Adsorption refers to the removal from water or wastewater
streams of dissolved contaminants by their attraction to and
accumulation on the surface of an adsorbent substance. Activa-
ted carbon is the most widely used adsorbent in municipal
wastewater treatment to remove trace organics. Adsorption
using activated carbon is utilized as a tertiary treatment
step, usually following sand or multimedia filtration.
Carbon adsorption systems generally utilize granular or
powdered activated carbon packed in a column or forming a fil-
ter bed through which wastewater is passed. Three consecutive
steps occur in the adsorption of wastewater contaminants by
activated carbon: (1) the film diffusion phenomenon, or the
transport of the adsorbate through a surface film surrounding
the activated carbon; (2) the diffusion of the adsorbate within
the pores of the activated carbon; and (3) adsorption on the
interior surfaces of the activated carbon.
Carbon adsorption of contaminants has been the topic of
many research projects as shown in the literature surveyed for
this report, tabulated in Table 38.
WATER QUALITY PARAMETERS
Adsorption is most effective for removing refractory and
other organics from wastewater. This is especially important
when effluents of exceptional quality are required (e.g., for
groundwater recharge or other reuse applications). Adsorption
can be used either as a polishing step or as the major treat-
ment process (1467). Rizzo and Schade (1165) and Zanitsch and
Morand (1554) reported that carbon columns alone were capable
of about 85 percent removal of BOD from wastewaters entering
the columns. Bishop et al. (119, 123) and Zanitsch and Morand
(1554) reported 75 to 80 percent TOC removals under the same
conditions. Weber et al . (1467) found that a treatment system
composed of primary settling, ferric chloride coagulation, and
carbon adsorption could remove up to 97 percent of the influent
BOD.
There is some disagreement among researchers regarding the
ability of activated carbon to remove nitrogen species from
122
-------
TABLE 38. LITERATURE REVIEWED PERTAINING TO ADSORPTION
Contami nant Reference Number
Water Quality Parameters
Ammonia 113, 119, 120, 196, 885
BOD 113, 119, 120, 156, 170, 196, 278, 315,
326, 498, 522, 745, 885, 1165, 1467, 1554
COD 119, 120, 156, 196, 278, 329, 498, 668,
885, 1165, 1547
Chlorides 114, 885, 1026, 1289
Nitrates 113, 119, 120, 326, 1467
Oil and grease 480
Phosphates 24, 113, 114, 119, 120, 196, 326, 448,
885, 1467
Suspended solids 39, 113, 119, 120, 170, 196, 278, 326,
498, 668, 745, 1165, 1442
Total dissolved 196, 454, 1547
solids
Total organic 113, 114, 119, 120, 123, 315, 522, 1086,
carbon 1165, 1262, 1467S 1554
Other (general) 531, 622
Elemental Contaminants
Aluminum 1383
Arsenic 855, 1383
Barium 855, 1383
Boron 1140, 1383
Cadmium 38, 39, 619, 753, 760, 855, 1383
Chromium 38, 39, 603, 619, 753, 760, 855, 1169,
1383
Cobalt 753, 1383
123
-------
TABLE 38 (continued)
Contaminant Reference Number
Copper 39, 620, 855, 1383
Iron 620, 753, 1383
Lead 753, 855, 1383
Manganese 753, 855, 1873
Mercury 753, 811, 855
Nickel 753, 855, 1383
Selenium 38, 1062, 1383
Zinc 620, 855, 1383
Other (general) 38, 760
Biocidal Contaminants
Chlorinated 762, 1221
hydrocarbons
Dieldrin 523
Herbicides 514, 516, 1221
Other (general) 523, 628, 762, 1323
Synthetic/Organic 123, 315, 454, 480, 523, 628, 651, 762,
Contaminants 862, 1153, 1290, 1323, 1465, 1496
Biological Contaminants
Bacteria 283
Coliforms 113
Escherichia coli 263
Polio virus 223, 466, 467, 1293, 1313
Virus 246, 263, 468, 492, 1010, 1312, 1313
124
-------
wastewaters. Bishop et al . (119) reported that carbon adsorp-
tion had little effect on nitrogen concentrations. On the
other hand, Weber et al. (1467) found that their primary set-
tling ferric chloride coagulation, carbon adsorption system re-
moved 95 percent of the influent nitrate; the reduction was
attributed partly to biological populations growing in the col-
umns .
Weber et al. (1467) reported that their pilot system also
removed 90 percent of the phosphate in the influent wastewater.
However, much of the research on phosphate adsorption has been
concerned with adsorbents other than carbon. Gangoli and
Thodos (448) reported that both Fl Alumina and fly ash were
capable of removing up to 99 percent of influent phosphate
levels. Ames and Dean (24) demonstrated that an alumina column
could treat up to 400 column volumes before reaching the 10
percent phosphorus breakthrough level.
Since color is contributed largely by organic compounds in
water, high color removal levels with adsorption should be pos-
sible. Zanitsch and Morand (1554) demonstrated 90 percent
color removal. They also noted an 86 percent suspended solids
removal, presumably by filtration.
ELEMENTAL CONTAMINANTS
Not a great deal of literature is available on the removal
of elemental contaminants by carbon adsorption. Such systems
are not specifically designed to remove ionic elemental con-
taminants, but some elementals are incidentally removed. When
the metallic contaminants are in an organometal1ic complex,
carbon adsorption columns can remove specific species. Litera-
ture from several sources (619, 760) reveals that high removals
(95 percent) of cadmium and hexavalent chromium by carbon ad-
sorption are possible. Huang and Wu (603) found that the effi-
ciency of chromium removal increases with decreasing chromium
concentration. While the mechanism of removal is not well
understood, Roersma et al. (1169) were able to describe the
reduction of Cr+6 to Cr+3. The Cr+6 is adsorbed within the
pores of the activated carbon which, in turn, is slowly oxi-
dized to C02> reducing the chromium ion.
Activated carbon treatment of a secondary-treated munici-
pal wastewater was found to reduce selenium from 9.32 to 5.85
ppb in a study cited by Patterson (1062). This represents a 37
percent removal efficiency. Patterson cited a second study in
which the selenium removal efficiencies of several advanced
wastewater treatment processes were determined in the treatment
of secondary effluent containing 2.3 ppb selenium. While sand
filtration alone reduced the effluent concentration by 9.5 per-
cent, sand filtration followed by activated carbon treatment
125
-------
provided a cumulative removal of 43.2 percent of the selenium
from the secondary effluent.
Logsden and Symons (811) researched the removal of mercury
by carbon adsorption and found that powdered carbon, in a jar
test, would adsorb both inorganic and methyl forms in excess of
70 percent.
BIOCIDAL CONTAMINANTS
Carbon adsorption is widely applied to remove organic or
metal-organic biocides. The removal of insecticides and pesti-
cides has been reviewed by Hager and Flentje (523). Dieldrin,
lindane, parathion, and 2, 4, 5-T ester were reduced below the
detectable limit of 0.01 ppb with influent concentrations of
3.6 to 11.4 ppb. Influent concentrations of 3, 5 dinitro-o-
cresol of 30 to 180 ppb were reduced to less than 1 ppb by
carbon adsorption. It was concluded that granular carbo.n beds
will provide a margin of safety for treatment of water contain-
ing varying insecticide or pesticide residues.
Activated carbon removals of several pesticides and PCB's
are well illustrated by results of laboratory studies cited by
the California State Water Resources Control Board (1323), as
shown in Table 39 . A variety of pesticides were experimentally
added to distilled water and passed through carbon filters to
test removal efficiencies. Schwarz (1221) investigated the ad-
sorption of isoprophyl N-(3-chlorophenyl) carbamate (CIPC) onto
activated carbon, concluding that powdered activated carbon
readily adsorbs CIPC from aqueous solution. The adsorption of
CIPC on activated carbon was independent of the pH in the range
of 5 to 9.
Grover and Smith (516) studied adsorption onto activated
carbon of the acid and dimethyl amine forms of 2, 4-D, and
dicambamate. A strong adsorption effect was noted on both the
acidic and salt forms of the compounds. This effect was expec-
ted to increase at low pH values.
On the basis of the literature which has been reviewed, it
can be concluded that activated carbon adsorption is effective
in the removal of some biocidal contaminants; however, further
investigation of this process will be useful.
SYNTHETIC/ORGANIC CONTAMINANTS
As was mentioned earlier, activated carbon and many syn-
thetic compounds are effective at removing organic contaminants
from aqueous solutions, particularly organics of low water solu-
bility. In general, carbon adsorption following secondary treat-
ment is capable of producing an effluent with from 1 to 7 mg/£
of organic carbon (123, 454).
126
-------
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127
-------
Bishop et al . (123) found that carbon adsorption was least
effective in removing highly polar, highly soluble organic
species. DeWalle and Chian (315) found that removal was a
function, at least in part, of the molecular weight of the
synthetic organic contaminant: low (<100) and high (>50,000)
molecular weight compounds are poorly adsorbed. The major
fraction removed by adsorption falls into a 100 to 10,000 mole-
cular weight range.
Studies of the adsorption of 93 petrochemicals by Giusti
et al. (480) confirmed the results of Bishop et al. (123) and
DeWalle and Chian (315): adsorption is largely a function of
molecular weight, polarity, solubility, and branching. Func-
tion was seen to have a substantial effect in conjunction with
solubility and polarity. The relative amenabilities to car-
bon adsorption of straight chain molecules of fewer than four
carbon atoms were as follows: aldehydes >esters >ketones
>alcohols >glycols. For larger molecules, the alcohols moved
ahead of the esters.
Much of the research done on the adsorption of synthetic
organic compounds from wastewater has been concerned with
determining mechanisms of adsorption and optimum removal con-
ditions. The only general removal efficiency studies available
report removals in terms of total organic carbon with little or
no effort made to differentiate the organic compounds involved.
Based on these results, adsorption can reduce the levels of
synthetic organic compounds in a typical domestic wastewater by
75 to 85 percent. If a particular type or types of organic
compounds predominate in a wastewater, these removals must be
adjusted to reflect the effect of compound character on the
adsorption process.
BIOLOGICAL CONTAMINANTS
With the exception of enteroviruses, no information was
found on the adsorption of biological contaminants, although
incidental removal of other organisms would be expected by
filtering action. Adsorption brings about simple removal of
viruses from wastewater rather than inactivation or destruction
(263, 468). Consequently, viable viruses could be reintroduced
to wastewater should desorption of viruses adsorbed to activa-
ted carbon occur.
Columns of granular activated carbon removed between 18
and 40 percent of Type I polio virus from secondary effluent
in studies by Sproul et al. (1313). This research and research
by Gerba et al . (467) using Type I polio virus indicate that
adsorption is inversely related to the concentration of organic
matter in the wastewater. The organics and the virus compete
128
-------
for adsorption sites; consequently, desorption of virus can
occur as adsorption of organic matter continues, or if the
concentration of organics is increased. Several authors have
thus concluded that the process is not dependable for producing
virus-free effluents (246, 468, 1313).
The level of removal actually attained is closely related
to the type of treatment that precedes adsorption. For example,
reducing the concentration of soluble organics in wastewater
by lime coagulation increased polio-virus removal in studies by
Gerba et al. (466, 467). In addition, the degree of virus ad-
sorption from lime-treated wastewater exceeded that from fil-
tered wastewater. These investigations also showed that polio-
virus removal from wastewater effluents is greatly improved by
maintaining a pH value in the range of 3.5 to 4.5. It was
found that virus adsorbed at low pH could become desorbed by a
rise in pH.
129
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TERTIARY TREATMENT: ION EXCHANGE
INTRODUCTION
The process of selective ion exchange has long been util-
ized in the treatment of industrial process waters and in domes-
tic water supply softening. Ion exchange resins (1142) are
classified by the charge of the exchangeable ion. Thus, resins
may be either catonic or anionic. General purpose resins will
selectively exchange both cations and anions. The operational
features of the ion exchange process are well developed and
reliable. Such systems offer a reliable method of removing
inorganic contaminants from the wastewater stream.
As can be seen by an examination of Table 40 , very little
information is currently available on removals of contaminants
from municipal wastewater by use of ion exchange techniques.
The process has not been economically feasible for treatment of
municipal wastewater. Several research programs focusing on
the application of ion exchange to municipal wastewater treat-
ment are presently under way. The most promising future appli-
cation appears to be for ammonia or nitrate removals.
WATER QUALITY PARAMETERS
Eliassen and Tchobanoglous (374, 375) conducted a review
of the literature. They found that removals of phosphorus and
nitrogen by tertiary wastewater treatment incorporating ion
exchange can reach 90 percent. The actual removal efficiency
was seen to depend upon the type of preceding treatment. Evans
(397) investigated the removal of nitrate by ion exchange, con-
cluding that the strong acid/weak base ion exchange process is
well suited for this purpose. With the exception of these few
studies of phosphorus and nitrate, most research performed to
date has focused on ammonium removal, since specific exchange
resins are not available for either the phosphorus or nitrate
ions. However, some zeolite exchange resins do have unusual
selectivity for the ammonium ion. This fact has encouraged
research activity.
On the basis of both pilot and laboratory scale investiga-
tions, it appears that effluent ammonia concentrations of less
than 1 mg/£ can be expected with ion exchange (730, 885). In
a pilot plant study, Mercer et al. (898) used zeolite columns to
test secondary effluent containing 10-19 mg/£ ammonia. Greater
130
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TABLE 40 . LITERATURE REVIEWED PERTAINING TO ION EXCHANGE
Contaminant Reference Number
Water Quality Parameters
Ammonia 4, 120, 165, 196, 277, 374, 454, 730,
885, 898, 1085, 1142, 1501
BOD 119, 120, 196, 277, 487, 885
COD 119, 120, 196, 277, 376, 885, 1547
Chlorides 376, 885
Nitrates 4, 120, 165, 374, 375, 397, 1142, 1501
Nitrites 165, 374, 1501
Phosphates 119, 120, 196, 277, 374, 375, 376, 379,
397, 463, 885
Suspended solids 4, 119, 120, 196
Total dissolved 196, 224, 277, 454, 1547
sol ids
Total organic 119, 120
carbon
Other (general) 531, 622
Elemental Contaminants
Arsenic 520, 1062, 1244
Boron 1140
Cadmium 753, 802, 1062
Chromium 753, 802, 1062, 1157, 1169
Cobalt 753
Iron 753
Lead 753
Manganese 753
Mercury 753, 802, 912, 1062
131
-------
TABLE 40 (continued)
Contaminant Reference Number
Elemental Contaminants
Nickel 753
Selenium 802
Other (general) 760, 1062
Synthetic/Organic 515, 1153
Contaminants
than 99 percent removal of ammonia was achieved. Similarly, 99.7
percent of the ammonia in activated carbon effluent was removed
by a zeolite in laboratory scale experiments by McKendrick et
al . (885).
The Environmental Protection Agency (1085) reviewed pilot
plant studies involving the use of clinoptilolite - a naturally
occurring zeolite - for wastewater treatment. Ammonia removals
ranged from 93 to 97 percent.
It should be noted that the ion exchange process using a
zeolite such as clinoptilolite does not result in the produc-
tion of a sludge containing the removed ammonia. Rather, the
spent zeolite is regenerated with a lime slurry, which is sub-
sequently air stripped, discharging ammonia to the atmosphere.
ELEMENTAL CONTAMINANTS
Ion exchange techniques have been principally applied for
the removal of elemental contaminants from industrial waste
streams (1062). Few studies have dealt with the application of
ion exchange techniques to municipal wastewaters for elemental
contaminant removal. Lindstedtet al. (S02) investigated trace
metal removal and concluded that a cation-anion exchange se-
quence was effective in reducing the concentrations of cadmium,
chromium, and selenium in secondary effluent. Removal effi-
ciencies are summarized in Table 41 .
132
-------
TABLE 41. TRACE METAL REMOVALS BY ION EXCHANGE (802)
Percent Removal After Given Process
Cation Cation-Anion
Trace Metal Exchange Exchange
Cadmium
Chromium
Selenium
99
5
1
99.9
96
99.7
Shen (1244) studied the removal of arsenic from drinking
water by ion exchange, concluding that the process does not
effect adequate removals. Using a variety of input levels, he
was able to achieve arsenic reduction of only 21 percent.
BIOCIDAL CONTAMINANTS
Biocidal contaminant removal through ion exchange has also
received little attention in the literature. In the only study
located, Grover (515) stated that trifluralin, triallate,
diallate, and nonionic herbicides were readily adsorbed on
both cationic and anionic exchange resins, with somewhat more
adsorption occurring on the cationic than on the anionic form.
133
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TERTIARY TREATMENT: NITROGEN REMOVAL PROCESSES
INTRODUCTION
Interim primary drinking water standards established by the
EPA set a nitrate limit of 10 mg/£ in the nitrogen form. Nitro-
gen concentrations in raw municipal wastewaters generally exceed
this value, ranging from 15 to 50 mg/a. Unless facilities are
specifically designed to remove nitrogen, much of it will remain
essentially unaffected, passing through the varying stages of
treatment to ultimately enter the environment. Moreover, reuse
of wastewater treatment plant effluents for direct groundwater
recharge, indirect groundwater recharge through land application,
or indirect reuse as a potable water supply is on the increase.
Such reuse policies make effective nitrogen removal an important
aspect of any wastewater treatment scheme.
In raw municipal wastewater, nitrogen is primarily found in
the form of both soluble and particulate organic nitrogen and as
ammonium ions. Conventional primary and secondary treatment
transforms some of this organic nitrogen into ammonium ions.
Part of the ammonium ion is oxidized to nitrate, and about 15 to
30 percent of the total nitrogen is removed.
Tertiary treatment processes designed to remove wastewater
constituents other than nitrogen often remove some nitrogen
compounds as well. However, removal is often restricted to
particulate forms, and overall efficiency is generally low. Two
tertiary processes particularly designed to remove nitrogen have
been developed: nitrification-denitrification and ammonia
stripping. Tertiary nitrification-denitrification usually
involves two stages. Nitrification occurs in an initial stage,
during which ammonium ions are oxidized to nitrite and nitrate
ions by nitrifying bacteria. These nitrite and nitrate ions are
in turn reduced to nitrogen gas which simply escapes from the
system.
Ammonia stripping is effective only in removing ammonia
nitrogen from municipal wastewater and has no effect on organic
nitrogen, nitric--. ,,r nitrate. Several ammonia stripping plants
are in operation in '.he U.S. (Lake Tahoe, California, Orange
County, California). !>'Jt the process has been found to be
expensive. A nupi>ey r> f te'.nn-ical problems remain to be solved
as well (885),
134
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Nitrification and den i t r i f i cation are biological reactions
which occur naturally during several conventional treatment
processes such as activated sludge treatments, aerobic lagooning,
and anaerobic digestion. The activated sludge process, in
particular, can be closely controlled to promote nitrogen removal.
Such treatment processes are not principally designed to remove
nitrogen, and both nitrification and denitrification occur only
as secondary reactions. For ease of reference, however, all
literature reviewed on the general topic of nitrogen removal has
been tabulated on Table 42 , including tertiary processes
specifically designed for this purpose.
WATER QUALITY PARAMETERS
There is general agreement that a system incorporating
secondary biological treatment and tertiary nitrification-
denitrification should achieve 80 to 95 percent total nitrogen
removal at design flows (531,1001). The nitrification process
alone removes only 5 to 10 percent of the total nitrogen entering
the process, while oxidizing up to 98 percent of the ammonia
nitrogen present to nitrate (458).
Average nitrogen data from systems incorporating nitrifica-
tion-denitrification processes recorded by an EPA Technology
Transfer Publication (458) are presented in Table 43 . Based
on this report, the predicted effluent quality from a nitrogen-
deni trif ication system will be 1.0 nig/2. organic nitrogen, 0.5
mg/£ ammonia nitrogen, 0.5 mg/£ nitrate nitrogen, and 2.0 mg/z
total nitrogen.
Nitrification is in itself an oxygen-demanding process and
therefore reduces the total oxygen demand (TOD) in the waste-
water effluent. Conventional biological or physico-chemical
treatment obtaining up to 90 percent BOD reduction will only
partially reduce the TOD of treated wastewater. For instance,
such treatment will only reduce an influent TOD of 490 mg/a to
an effluent TOD of over 100 mg/£. Nitrification will reduce the
TOD of this effluent to less than 40 mg/£ (458).
Since the denitrification step involves the oxidation of
carbonaceous material, a reduction in biochemical oxygen demand
and total organic carbon can also be expected, in addition to
the effective reduction of TOD.
Nitrogen removal by ammonia stripping was studied by
O'Farrell et al. (1016), who reported a 90 percent removal of
ammonia from a non-nitrified, lime-clarified secondary effluent
at pH 11.5. During a warm weather study performed at Lake
Tahoe, stripping produced a 96 percent removal of ammonia
nitrogen at pH 11.5 and using 400 cu ft of air per gallon of
wastewater (531). Any arbitrary percentage removal can be
achieved with this type of system within available engineering
capabilities, although higher removals mean higher costs.
135
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TABLE 42.
LITERATURE REVIEWED PERTAINING TO
NITROGEN REMOVAL
Contaminant
Water Quality Parameters
Ammoni a
BOD
Chlorides
Nitrates
Phosphates
Suspended
solids
Reference Number
4, 5, 8, 81, 121, 236, 374, 390, 458,
531, 643, 869, 885, 986, 1001, 1016,
1085, 1106, 1142, 1282, 1333, 1351,
1482, 1501, 1546
81 , 458, 646
819
4, 5, 81 , 374, 375, 390, 458, 489,
490, 642, 643, 646, 869, 986, 1001,
1085, 1106, 1142, 1282, 1350, 1351 ,
1501
374
81 , 646, 1350
TABLE 43. EFFLUENT NITROGEN CONCENTRATIONS IN
TREATMENT SYSTEMS INCORPORATING NITRIFICATION - DENITRIFICATION
(458)
Average Effluent Nitrogen, mg/£
Type and Process Sequence Organic-N NH^-N NO^-N NO^-N °N
Lime treatment of raw sewage, 1.1 0.3 0.5 0.0 1.9
nitrification,
denitrification
Primary treatment,
high rate activated
sludge, nitrification,
denitrification,
filtration
Primary treatment,
roughing filters,
nitrification,
denitrification,
filtration
0.8
0.8
0.0
0.9
0.7
0.6
0.0 1.5
0.0 2.3
136
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DISINFECTION: CHLORINATION
INTRODUCTION
Until recently, chlorination was considered virtually an
unmixed blessing as a cheap, effective method to destroy bac-
teria and viruses. It is now recognized, however, that chlori-
nation of wastewater may create chlorinated compounds harmful
to the environment and to human health. The extent of this
potential hazard has not yet been determined; new and existing
wastewater treatment plants continue to utilize chlorine for
disinfection. The primary purpose of municipal wastewater
chlorination is the destruction of pathogenic microorganisms.
This is reflected in the literature reviewed, shown in Table 44.
WATER QUALITY PARAMETERS
Zaloum and Murphy (1553) concluded that chlorination of
treated wastewater effluents does not reduce BOD, COD, and
total organic carbon. Susag (1346), however, found BOD reduc-
tions by chlorination of up to 2 mg/a of chlorine were added.
These values are somewhat misleading, in that BOD reduction
was due both to oxidation of the organic material and to the
formation of chlorinated organics resistant to bacterial action.
When chlorine is added to a wastewater containing ammonia
nitrogen, ammonia reacts with the hypochlorous acid formed to
produce chloramines. Further addition of chlorine converts the
chloramines to nitrogen gas. The reaction is influenced by pH,
temperature, contact time, and initial chlorine-to-ammonia
ratio. If sufficient chlorine is added, 95 to 99 percent of
the ammonia will be converted to nitrogen gas with no signifi-
cant formation of nitrous oxide. The quantity of chlorine
required was found to be 10 parts by weight of chlorine to 1
part of ammonia nitrogen when treating raw sewage. This ratio
decreased to 9:1 for secondary effluents, and 8:1 for lime-
clarified and filtered secondary effluent (1346).
ELEMENTAL CONTAMINANTS
Little information is available on the minimal removal by
chlorination of elemental contaminants. Andelman (27) studied
the effects of chlorination on barium, copper, and nickel. The
treatment effected a 34 percent reduction in barium, a 5 percent
reduction in nickel, and had no effect upon copper. Kokoropoulos
137
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TABLE 44 . LITERATURE REVIEWED PERTAINING TO CHLORINATION
Contaminant Reference Number
Water Quality Parameters
Ammonia 43, 76, 114, 120,127,727, 728, 1085,
1116, 1288, 1555
BOD 120, 321, 593, 1046, 1084, 1215, 1346,
1553
COD 120, 1084, 1091, 1346, 1553
Chlorides 684
Cyanides 65, 1046
Nitrates 120, 684, 1085, 1322
Nitrites 727, 728, 1085
Phosphates 120, 684
Suspended solids 120, 1084, 1215
Total dissolved 1215
solids
Total organic 120, 1553
carbon
Others (general) 385, 391, 531, 727, 728, 884, 1468
Elemental Contaminants
Barium 27
Boron 1367
Copper 27
Iron 727, 1046
Manganese 727, 728, 1181
Mercury 1046, 1499
Nickel 27, 728
138
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TABLE 44 (continued)
Contaminant Reference Number
Synthetic/Organic 5, 84, 158, 191, 482, 657, 971, 1130,
Contaminants 1250, 1287, 1332, 1450, 1555
Biological Contaminants
Adeno virus 95
Bacteria 8, 79, 161, 210, 213, 283, 292, 321, 395,
615, 651, 830, 1304
Coliforms 161, 164, 292, 321, 395, 383, 395, 483,
612, 615, 727, 728, 937, 1084, 1304,
1312, 1389, 1393, 1458, 1489, 1490
Coxsackie virus 95, 257, 380, 615, 890, 1206
(A & B)
ECHO virus 380, 615, 1260
Escherichia coli 141, 375, 383, 428, 615, 1206, 1414, 1430
Fecal streptococci 292, 395, 612, 1084
Hepatitis virus 615
Mycobacterium 428, 615
Parasitic worms 161, 615, 1188, 1304
Polio virus 161, 223, 380, 615, 817, 820, 1206, 1260,
1293, 1425
Protozoa 161, 383, 428, 1335
Salmonella 161, 292, 395, 428, 1083
Shigella 161
Vibrio cholerae 161
Virus 79, 92, 95, 96, 100, 101, 127, 161, 210,
213, 280, 281, 283, 352, 382, 383, 395,
454, 492, 615, 651, 739, 745, 816, 817,
900, 970, 1009, 1083, 1095, 1243, 1259,
1260, 1304, 1366, 1434
Other (general) 161, 588
139
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(727) reported hypochlorous acid reacted with soluble iron (II)
and manganese (II) to form precipitates.
SYNTHETIC/ORGANIC CONTAMINANTS
No research was found to address removal or destruction
effects of chlorination on any of the synthetic/organic contami-
nants. However, considerable interest has recently developed
concerning the production of chlorine-containing organic com-
pounds by chlorination. The reactions of chlorine with organic
compounds in water are diverse, including oxidation, substitu-
tion, addition, and free radical reactions. Chlorination may
produce several different chlorinated products from a single
organic pollutant molecule. Some of these compounds have been
identified as toxic to aquatic life by Snoeyink (1287), Brungs
(158) , and others.
Jolley (657) evaluated chlorine-containing organic consti-
tuents in chlorinated effluents and found that stable chlorine-
containing compounds were present after effluents had been
chlorinated to a 1 to 2 mg/£ chlorine residual. These compounds
are identified in Table 45.
TABLE 45. IDENTIFICATION OF CHLORINE CONTAINING
CONSTITUENTS IN CHLORINATED EFFLUENTS (657)
5 - Chlorouracil 5 - Chlorouridlne
8 - Chlorocaffeine 6 - Chioroguanine
8 - Chloroxanthine 2 - Chlorobenzoic acid
5 - Chlorosalicylic acid 4 - Chloromandelic acid
2 - Chlorophenol 4 - Chlorophenylacetic
acid
4 - Chlorobenzoic acid 4 - Chlorophenol
3 - Chlorobenzoic acid 3 - Chlororesorcinol
3 - Chloro-4-hydroxybenzoic acid
4 - Chloro-3-methylphenol
A similar project was conducted by Glaze and Henderson
(482). The chlorinated organics identified in this study are
listed in Table 46.
Shimizuetal. (1250) stated that halogenated nucleic acid bases
are incorporated into the nucleic acid. Also, the incorporation
of 5-deoxybromouridine in DNA and 5-fluorouraci1 into RNA are
known to cause mutations. No work has been completed to deter-
mine how nucleic acids react with chlorine or the resulting
mutations.
140
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TABLE 46. CHLORINATED OR6ANICS IN
WASTEWATER EFFLUENT (482)
Chloroform
Dichlorobutane 3-chl
Chlorocyclohexane (-18)
0-di chlorobenzene
P-dichlorobenzene
Pentachloroacetone
Trichlorobenzine
Chiorocumene
N-methyl-tri chloroani1i ne
Trichlorophenol
Chloro-a-methyl benzyl alcohol
Di chloromethoxytoluene
Trichloromethylstyrene
Dichloro-a-methyl benzyl alcohol
Dichloro-bis (ethoxy) benzene
Dichloro-a-methyl benzyl alcohol
Trichloro-a-methyl benzyl alcohol
Trichloro-a-methyl benzyl alcohol
Tetrachloroethylstyrene
Tetrachloromethoxytoluene
Dichloroani1ine derivative
Dichloroani1ine derivative
Trichlorophthalate derivative
Tetrachlorophthalate derivative
Dibromochloromethane
3-chloro-2-methylbut-l-ene
Chloroalkyl acetate
Tetrachloroacetone
Chloroethylbenzene
Hexachloroacetone
Dichloroethyl benzene
Dichlorotoluene
Trichloroethyl benzene
Tri ch1oro-N-methylan 1 sole
Tetrachlorophenol
Trichlorocumeme
Trichlorodimethoxybenzene
Dichloroacetate derivative
141
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BIOLOGICAL CONTAMINANTS
The effectiveness of chlorination as a disinfection process
has long been recognized. All researchers are in agreement that
the effectiveness of disinfection by chlorine is influenced by
time and chlorine concentration and also by: (1) whether the
chlorine residual is free or combined; (2) effectiveness of
mixing; (3) whether or not particulates are present; (4) pH;
(5) temperature; and (6) the concentration, condition, and nature
of the organisms. Keeping these limitations in mind, an idea
of the relative resistances of organisms to disinfection by
chlorine can be seen in Table 47.
TABLE 47. EFFECT OF CHLORINATION ON VARIOUS ORGANISMS (615)
Group
Virus
Bacteria
Nematodes
Organism
Infectious
hepatitis
Coxsackie
Coxsackie
Echo
Poliovirus I
Coliphage B
Theiler Phage
M. tuberculosis
E. coli
Col iforms
Total Count
Di pi ogaster
Cheilobus
Chlorine
Residual
(mg/£)
1
15
5
1.0
1.95
0.53
0.03
0.03
1-5
2
1
0.14
0.03
1-1.2
some
2.5-3
15-45
Time
min.
30
30
2.5
3
6.5
14
10
10
120
30
30
3
10
15
15
120
1
Efficiency
Survived
Inactivated
Survived
99.6% Inactivated
Survived
Survived
20% Survival
Inactivated
99% Kill
99% Kill
Destroyed
99.9% Kill
52% Kill
99% Kill
98-99% Kill
Survived and
Mobi le
Others
S. mansom
Vo v a and
mi racidia)
S. japonicum
(ova and
m i r a c i d i a)
0.2-0.6
0.2-0.6
30
30
Killed
Killed
Eliassen and Tchobanoglous (375) found that 2 to 6 mg/£ of
chlorine applied for 20 min would effect a 99.99 percent kill
of the total coliforms, fecal coliforms, and fecal streptococci
present in wastewater influent.
142
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The effect of chlorination on entamoebic cysts was investi-
gated by Stringer and Kruse (1335). It was concluded that the
hypochlorous acid (HOC1) form of free available chlorine was
the most rapidly acting cysticide compared with other halogen
species. Entamoeba histolytica cysts and tapeworm eggs with-
stand the ch1 ori nation treatment generally applied to waste
treatment effluent (161). Rudolfs et al. (1188) reported the
development of active embryos from a majority of ascaris eggs
in contact with 5,000 ppm chlorine solutions for 30 min.
Davis and Keen (292) conducted a research project on the
ability of municipal wastewater bacteria to survive chlorination
and reestablish populations after discharge. Fecal coliform,
fecal streptococci, and total coliform enumeration was performed
with further differentiation into lactose nonfermenters within
and outside the family Enterobacteriaceae. It was determined
that the vast majority of the wastewater bacterial species that
reestablished their populations within 21 days following chlori-
nation were lactose nonfermenters not included in the Entero-
bacteriaceae. Many of these bacteria could be pathogenic under
the appropriate conditions and may constitute a threat to public
health in receiving waters designated for contact recreation.
Virus inactivation is one of the more difficult tasks of
chlorination, but as in any disinfection process, required kills
can be achieved by lengthening the time or increasing the con-
centration (615). A study of the inactivation of viruses in
wastewaters by chlorination was performed by Lothrup and Sproul
(817). It was ascertained that:
t High-level inactivation of viruses can be obtained in
treated and untreated domestic wastewaters. Present
chlorination practices (1 mg/£ of residual), however,
are inadequate for a high level of virus inactivation.
• A combined chlorine residual of 28 mg/£ was required
to produce a 99.99 percent inactivation of the T2
bacteriophage in settled raw wastewater after a 30-min
contact time.
• A combined chlorine residual of 40 mg/£ was required to
provide a 99.99 percent destruction of the Type I
polio virus in settled wastewater after a 30-min contact
time.
t Free chlorine residuals of 0.2 to 0.4 mg/£ , after 30
min, produced a complete inactivation of the polio virus
and T2 phage in the secondary effluent.
143
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• In experimental runs with synthesized storm-water over-
flow samples, a 100 percent inactivation of the Type I
polio virus was obtained by providing a free chlorine
resi dual .
• The T2 bacteriophage was much less sensitive to combined
chlorine residuals than is the coliform organism and
somewhat more sensitive than the polio virus to combined
chlori ne residuals .
A similar research project investigating the inactivation
of enteroviruses by chlorination was conducted by Shuval et al .
(1260). The following conclusions were obtained:
t The strain of ECHO virus used was sensitive to the com-
bined chlorine in the sewage, with reductions of 99 per-
cent in 30 min and 99.93 percent in 6 hr using 3.6 mg/£
of chlorine. No virus was recovered in the sample tested
after 4 hr contact with 7 mg/£ of chlorine dosage or
after 2.5 hr with 11 mg/l of applied chlorine. Inacti-
vation was shown to be a function of time and chlorine
concentration under the test conditions.
• The strain of polio virus Type I used was much less sen-
sitive to the combined chlorine, showing only 50 and 90
percent reductions in 6 hr using 4 and 11 mg/£ chlorine
dosage respectively.
• Coliform reductions obtained followed known patterns,
with a standard of less than 100 coliforms/100 mi being
obtained in 80 percent of the samples after 2 hr of
contact with a chlorine dose of about 8 mg/£.
• Although the inactivation of the ECHO virus strain was
comparable to that obtained with coliform organisms,
this study indicates that the coliform index in chlori-
nated sewage may not give a true picture of the degree
of inactivation obtained with the more resistant strains
of enterovirus such as polio virus Type 1.
The minimum concentration of chlorine required for complete
inactivation of the Sabin oral poliovaccine Type I virus strain
was examined by Varma et al. (1425). Various exposure periods
with pH 5.2 at 20°F were studied: a concentration of 22 mg/£ for
5 min of exposure time, 19 mg/£ for 15 min, 19 mg/l for 30 min,
17 mg/£ for 45 min, and 14 mg/£ for 60 min. Nonetheless, on
the basis of the literature surveyed, it is evident that chlori-
nation per se does not provide conclusive proof of disinfection.
Boardman and Sproul (127) described the protection afforded
viruses associated in particulate matter. Surface adsorption
144
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gave no viral protection. When viruses are embedded within
particles, the disinfecting molecules must diffuse through the
particle matrix before reaching the virus and initiating any
inactivation. Chemical diffusion is a slow process; as a con-
sequence, virtually all the embedded viruses are prtected from
disinfection.
145
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DISINFECTION: OZONATION
INTRODUCTION
Ozone, an allotropic form of oxygen, is a powerful oxidizing
agent for the disinfection of wastewater. Ozone is used in over
100 municipalities in Europe for disinfection of drinking water.
Certain chemical features make ozone treatment a particularly
attractive method of water purification:
t It is a powerful oxidant which reacts rapidly with most
organic compounds and microorganisms in wastewater.
• It does not impart taste and odor to potable water.
• It is produced from oxygen in air by means of electric
energy.
On the negative side, the cost of ozonation is not presently
competitive with chlorine disinfection. Moreover, long-term
residual disinfection capabilities are lacking, and the insta-
bility of ozone generally necessitates its generation on site
(1429).
The principal ozone decomposition products in aqueous
solution are molecular oxygen and the highly reactive free
radicals OH, H02, H0,+. Very little is known about the sig-
nificance of th'e free radical intermediates on the germicide!
properties of ozone solutions. The same free radicals are pro-
duced by irradiation of water, and it has been reported that
H02 and OH. radicals contribute significantly to the killing of
bacteria by this process.
As seen in Table 48, a considerable amount of information is
available on the destruction of various pathogens by ozonation,
however little information was found on the effect of ozone
upon other contaminants.
WATER QUALITY PARAMETERS
Because of its strong oxidizing character, ozone is very
reactive toward the organic compounds which make up the BOD,
COD, and total organic carbon. Under ideal conditions the
reactions would result in almost complete oxidation and only
carbon dioxide as a reaction product. In practice, ozonation results
146
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TABLE 48. LITERATURE REVIEWED PERTAINING TO OZONATION
Contami nant
Water Quality Parameters
Ammonia
BOD
COD
Nitrates
Nitrites
Phosphates
Suspended solids
Total organic
carbon
Others (general )
Elemental Contaminants
Adeno virus
Bacteria
Clos tridi urn
botulinium
ECHO virus
Escherichia coli
Fecal streptococci
Parasitic worms
Polio virus
Salmonel1 a
Virus
Other (general)
Reference Number
8, 470, 651, 709, 1166
320, 321, 709, 868, 970, 985
236, 320, 470, 707, 985, 1231
470, 651, 985, 1166
470, 651, 709, 1166
985
470
985, 1262
394
437, 438
95, 213
8, 72, 213, 320, 321, 469, 542, 707,
709, 1178
1429
1429
72, 95, 686, 687, 707, 1429
72, 707
897, 1429
213, 223, 686, 687, 835
707
95, 96, 97, 213, 280, 320, 492, 816,
818, 1069, 1070
686
147
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in only partial oxidation and produces simpler organic molecules.
Both Ghan and Nebel reported COD removals of Less than 40
percent. Morris found that the apparent BOD of a wastewater can
increase after ozonation as a result of refractory organic
molecules being oxidized to simpler, biodegradable compounds.
If the ozone is applied after other treatment processes (as is
normal), the increase in organic nutrient molecules can lead
to the growth in the distribution system of algae, slime
bacteria, and the possible regrowth of any pathogens not des-
troyed during treatment.
Ozone is effective at decreasing concentrations of organic
suspended solids and organic nitrogen through oxidation.
Ozonation can assist in suspended solids removal through froth
flotation mechanisms induced through the process. Ozone will
also oxidize ni-trites to nitrates, but will not react with
ammonia (651). There is little evidence to date that ozonation
will produce any toxic or carcinogenic oxidation by-products as
will chlorination.
ELEMENTAL CONTAMINANTS
Furgason and Day (438) studied the feasibility of
ozonation for iron and manganese removal from raw water with
relatively high input concentrations. The study demonstrated
that ozone effectively oxidized the iron and manganese to
an insoluble form which could be filtered from the water.
Complete oxidation of the minerals required a reaction time
of 30 sec. Filtration studies indicated a relatively fine
medium was required to remove the oxide precipitate.
BIOLOGICAL CONTAMINANTS
The use of ozone as a wastewater disinfectant was reviewed
by Venosa (1429). It was concluded that with 0.1 mg/2- of active
chlorine, 4 hr would be required to kill 6 x 104 E. coli cells
in water, whereas with 0.1 mg/a of ozone only 5 sec would be
necessary. When the temperature was raised from 22°C to 37°C,
the ozone inactivation time decreased from 5 sec to 0.5 sec.
These investigations revealed that the contact time with ozone
necessary for 99 percent destruction of E. coli was only one-
seventh that observed with the same concentration of hypochlo-
rous acid. The death rate for spores of Bacillus species was
about 300 times greater with ozone than with chlorine.
In the same study, Venosa also described bacteriological
studies performed on secondary effluent from an extended aera-
tion pilot plant in the Metropolitan Sewer District of Louisville,
Kentucky. Using an average applied ozone dosage of 15.2 mg/£
for an average contact time of 22 min, fecal coliform reductions
of greater than 99 percent were achieved, resulting in a mean
148
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fecal coliform concentration of 103 cells/100 ma , a mean
total coliform concentration of 500 cells/100 ma , and a mean
fecal streptococci concentration of 8 cells/100 m£ in the
final effluent. Laboratory results with raw sewage indicated
that ozone could be successfully used to sterilize sewage
containing Bacillus anthracis, influenza virus, and B. subti1 is
morph. globibii, and to inactivate toxins of Clostri dium
botuli num. Ozone consumption was 100 to 200 mg/£ for 30 min.
Finally, Venosa found ozone to be many times more effective
than chlorine in inactivating poliomyelitis virus. Identical
dilutions of the same strain and pool of virus, when exposed
to 0.5 to 1.0 mg/a of chlorine and 0.05 to 0.45 mg/Ji of ozone,
were devitalized within 1.5 to 2 hr by chlorine, while only
2 min of exposure were required with ozone.
Majumdar et al. (835) also studied the inactivation of
polio virus by ozonation and concluded that the inactivation
is not complete. Results are summarized in Table 49.
TABLE 49. SURVIVAL OF POLIO VIRUS IN
OZONATION CONTINUOUS FLOW STUDIES (835)
Ozone Residence Average
Type of Concentration Time Survival
Wastewater (mg/£) (min) (percent)
Primary
wastewater 0.84 8.0 1.820
1.47 2.0 0.016
4.44 1.0 0.006
Secondary
wastewater 0.79 8.0 2.055
1.77 2.0 0.013
5.05 1.0 0.006
Pavoni and Tittlebaum (1069) recently studied ozone
disinfection of viruses in the Fort Southworth Pilot Plant
of the Metropolitan Sewer District in Louisville. Using
F2 bacteriophage as the model virus, they demonstrated virtually
100 percent inactivation efficiency in the secondary effluent
after a contact time of 5 min at a ozone dosage of approximately
15 mg/x, and a residual of 0.015 mg/£ . Of particular interest
was the observation that the rate of inactivation was greater
for F2 bacteriophages than bacteria. In addition, the following
conclusions were reached:
1. F2 virus concentrations were shown to be unaffected
by the flow or mixing of the ozone reactor.
149
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2. F2 virus was inactivated with virtually 100 percent
efficiency after a contact time of 5. min at a total
ozone dosage of approximately 15 mg/£ and a residual
of 0.015 mg/a .
3- E. coli bacteria and F2 virus were inactivated with
virtually 100 percent efficiency after a contact time
of less than 15 sec in the absence of ozone-demanding
material.
4. An extremely small number of viral particles was
observed in effluent studies.
5. Oxidation by ozone appears to be the mechanism of
kill for bacterial cells and viral particles. Ozone
is theorized to act as a general oxidant causing
cell lysis and the release of soluble COD.
Mercado-Burgos et al. (897) examined the effect of ozone
on Schistosoma ova, concluding that the process was ineffective
150
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SLUDGE TREATMENT AND DISPOSAL SYSTEMS
THICKENING AND DEWATERING
INTRODUCTION
Sludge is the most notable by-product of the wastewater
treatment plant. Disposal of sludge materials is a problem
comparable in magnitude and importance to that of wastewater
treatment. Because of the high water content of sludge, any
reduction in volume through dewatering or thickening, of these
by-products marks a significant step towards an improved solu-
tion of the disposal problem. Processes available for sludge
volume reduction include:
• Gravity sludge thickeners
• Air flotation sludge thickeners
• Centrifugal sludge thickeners
• Vacuum fi1ters
• Drying lagoons
• Pressure filtration
Sludge dewatering by land methods (e.g., lagooning) has
been the accepted practice for many years. However, attention
has recently focused on the use of other techniques available
for dewaterina. Increased land costs together, with stringent
land, air, and water pollution standards have made sludge
dewatering an economically attractive process since it sig-
nificantly reduces the volume of sludge requiring disposal.
Literature concerning sludge thickening and dewatering
processes, as reviewed in Table 50 , is rarely pertinent to
discussions of adverse health effects of sludge-contained
contaminants. In general, this literature deals mainly with
engineering design and operation parameters and the relative
efficiency of dewatering processes, with only slight coverage
of partitioning, degradation, or concentration of either
general, elemental, or biological contaminants.
Coagulants are used for improved dewatering characteris-
tics and have been indicated as possible factors providing
viral inactivation or removal (246). Kampelmacher and Jansen
(670) reported reduction of bacteria in sludge through vacuum
filtration and chemical conditioning by ferric chloride,
151
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TABLE 50 . LITERATURE REVIEWED PERTAINING TO
SLUDGE THICKENING AND DEWATERING
Contamlnant Reference Number
Water Quality Parameters
Ammonia 925, 1080
BOD 16, 201, 334, 1435
COD 16, 334
Chlorides 1080
Nitrates 334
Phosphates 546, 1080
Suspended 16, 201, 229, 438, 518, 546, 864, 1008,
solids 1015, 1054, 1058, 1080, 1123, 1308, 1368,
1369, 1435
Others (general) 16, 201, 334, 401, 518, 531, 546, 551,
552, 622, 638, 639, 764, 1008, 1015,
105J, 1054, 1055, 1058, 1123, 1308, 1369,
1397
Elemental Contaminants
Aluminum 246, 1080
Boron 1080
Cadmium . 229, 1080
Chromium 229, 1080
Copper 229, 635, 1080
Iron 229, 1080
Lead 1080
Manganese 229, 1080
Mercury 635
Nickel 635, 1080
152
-------
TABLE 50 (continued)
Contami nant Reference Number
Zinc 229, 635, 1080
Other (general) 229
Biological Contaminants
Bacteria 670
Coliforms 401 , 568
Coxsackie virus 1053
(A & B)
Escherichia coli 568
Salmonella 244, 670
Virus 246
ferrous sulfate, and lime. Two separate analyses of Dutch
treatment plants showed a marked reduction (from two to
four orders of magnitude) of aerobic bacteria and entero-
bacteriaceae.
Peterson et al. (1080) studied the chemical properties of
waste activated sludge after vacuum filtration; his results,
presented in Table 51, provide a representative picture of
the constituents found in thickened and dewatered sludge.
153
-------
TABLE 51 . CHEMICAL PROPERTIES OF
VACUUM FILTERED WASTE ACTIVATED SLUDGE* (1080)
Analyses % of Dry Wt Basis
Total Nitrogen 6.37
Ammonia Nitrogen Trace
Phosphorus 2.49
Zinc
Boron 0.002-0.04
Iron 5.32
Manganese 0.012
Aluminum
Cadmium 0.028
Chloride
Chromium 0.362
Copper 0.11
Nickel 0.034
Lead 0.141
* Waste activated sludge; ferric chloride addition;
vacuum filtered; heat dried
154
-------
ANAEROBIC DIGESTION
INTRODUCTION
Sludge digestion converts bulky, odorous, raw wastewater
sludge to a relatively stable material that can be readily de-
watered Tfid disposed without excess obnoxious odors. Bacterial
digestion is a two-stage process effecting the decomposition
of organic and/or inorganic material in the absence of free
oxygen. The first stage is accomplished by facultative
bacteria, which break down large organic compounds and con-
vert them to simpler organic acids. Acid-splitting, methane-
forming, anaerobic bacteria complete the second step, con-
verting the organic acids to methane and carbon dioxide.
These strict anaerobes have a relatively slow growth rate
and are highly sensitive to environmental conditions of
temperature, pH, and anaerobiosis.
Health-related problems traceable to anaerobic digestion
would be dependent upon the final sludge solids disposal scheme,
since the dewatering liquor circulates inaclosed loop system
within the treatment plant. Pertinent literature reviewed con-
cerning this subject is indicated in Table 52.
WATER QUALITY PARAMETERS
Sekikawa et al. (1230) investigated the solubi1ization of
certain water quality parameters under anaerobic conditions.
A period of marked increase in dissolved phosphate concentra-
tion and BOD value was noted during the initial stage of
digestion. In the ensuing stage, these values decrease. The
maximum amount of phosphorus released equaled approximately
50 percent of the total phosphorus contained in the sludge.
These temporary increases were attributed to autolysis, or
microbial destruction, of sludge organisms. Table 53 shows
typical anaerobic digester content characteristics during the
study.
ELEMENTAL CONTAMINANTS
Anaerobically digested sludge characteristically contains high
concentrations of elemental contaminants. Sludge volume is
reduced during digestion, with a corresponding increase in
metal concentrations. The extent to which these metals inhibit
the digestion process, however, has in the past received more
attention than any ultimate effect on human health.
155
-------
TABLE 52 . LITERATURE REVIEWED PERTAINING
TO ANAEROBIC DIGESTION
Contaminant Reference Number
Water Quality Parameters
Ammonia 580, 584, 690, 864, 1080, 1190
BOD 205, 1080, 1230
COD 1080
Chlorides 1080
Nitrates 580, 584, 1195
Nitrites 112, 584
Phosphates 513, 580, 584, 623, 690, 736, 838, 1035,
1036, 1080, 1195, 1228, 1230, 1267
Suspended 497, 838, 1035, 1054, 1055, 1080, 1128,
solids 1230
Others (general) 531, 551, 552, 622, 690, 1035, 1053,
1123, 1230
Elemental Contaminants
Aluminum 513, 690, 1035, 1036, 1080, 1228
Barium 690
Boron 690, 1180, 1195
Cadmium 228, 580, 584, 690, 853, 975, 1063, 1080,
1195, 1400
Chromium 71, 228, 580, 584, 623, 690, 853, 1080,
1195, 1400
Cobalt 1195, 1400
Copper 71, 228, 584, 623, 690, 761, 853, 975,
1063, 1080, 1195, 1400, 1411
Iron 112, 228, 580, 690, 761, 975, 1080, 1228,
1267
156
-------
TABLE 52 (continued)
Contami nant Reference Number
Lead 228, 580, 584, 690, 853, 1063, 1080,
1195, 1400
Manganese 112, 228, 580, 584, 623, 690, 1080, 1195,
1400
Mercury 228, 690, 803, 1195
Nickel 71, 228, 584, 623, 690, 761, 1063, 1080,
1195, 1400
Zinc 71, 112, 228, 401, 584, 623, 690, 761,
853, 975, 1063, 1080, 1195, 1228, 1400
Other (general ) 1228
Biocidal Contaminants
DDT 14, 15
Synthetic/Organic
Contaminants 714
Biological Contaminants
Bacteria 161, 580, 935, 1123
Coliforms 568, 580, 582, 935
Coxsackie virus 95, 112, 161, 428, 1053
(A & B)
ECHO virus 112
Escherichia coli 568, 1080, 1123
Mycobacteriurn 428
Parasitic worms 161, 428, 791
Polio virus 112, 161, 428
Protozoa 428, 1080
Salmonella 95, 161, 428, 717, 1080, 1123
Shigella 161
157
-------
TABLE 52 (continued)
Contaminant Reference Number
Vibrio cholerae 161
Virus 95, 96, 112, 161, 428, 580, 908, 1209,
1476
Other (general ) 161
TABLE 53 . SLUDGE CHARACTERISTICS (1230)
Parameter Concentration
Sludge volume index (%) 25.0
Total suspended solids (mg/£) 2,784
Volatile suspended solids (mg/£) 1,920
Ash (mg/£) 864
Total nitrogen (mg/£) 282
Total phosphorus (mg/£) 60
as Phosphate 183.5
BOD (mg/£) 1,465
Table 54 presents the concentration range of various
constituents including elemental contaminants found in
anaerobically digested liquid sludge from 35 Wisconsin munici-
palities, recorded by Keeney et al. (690). Table 55 shows
the average metal concentrations reported by Salotto et al.
(1195). The authors thought the geometric mean would be the
best measure of central tendency. The spread associated with
the geometric mean was greater for certain metals such as
cadmium, chromium, and manganese, indicating that these
metals -- not ordinarily found in domestic wastewater -- may
occasionally be introduced (probably from industrial sources)
in relatively high concentrations.
A laboratory investigation of mercury distribution in an
anaerobic digester was reported by Lingle and Hermann (803).
Data indicate that during experimentation, more than 96 percent
of the mercury from phenyl mercuric chloride and mercuric
chloride remained in the sludge solids. It is suggested that
the biological methylation of mercury may have been inhibited
by the presence of sulfides in the digester sludge. The
158
-------
TABLE 54 . CONSTITUENT CONCENTRATIONS IN
ANAEROBICALLY DIGESTED SLUDGE (690)
Concentration
Constituent Range*
Total nitrogen (moist) 3.4-9.5
Total nitrogen (dried) 2.4-3.1
Ammonia nitrogen (moist) 0.8-4.1
Ammonia nitrogen (dried) 0.02-0.26
Organic Carbon 25.7-38.5
Phosphorus 2.7-6.1
Aluminum 0.36-1.2
Iron 0.8-7.8
Cadmium/Zinc 0.15-33
Zinc 490-12,220
Copper 140-10,000
Nickel 15-1,700
Cadmium 5-400
Lead 40-4,600
Chromium 50-32,000
Silver 0.6-31
Boron 150-750
Manganese 180-1 ,130
Barium 530-1 ,340
Strontium 52-7,810
* Range for the first 9 constituents is given in percent
of solids and in mg/kg for the last 11 constituents.
159
-------
TABLE 55. AVERAGE CONCENTRATIONS OF METALS IN DIGESTED SLUDGE (1195)*
Arithmetic
Metal
Silver
Boron
Cadmium
Calcium
Chromium
Cobalt
Copper
Mercury
Manganese
Nickel
Lead
Strontium
Zinc
Mean
250
430
75
36,500
1,860
350
1,590
10
1,300
680
2,750
520
4,210
Std. Dev.
(+ and -)
230
310
104
23,800
1,920
220
1,670
18
2,290
620
2,350
670
3,800
Geometries
Mean
190
380
43
31,100
1,050
290
1,270
6.5
475
530
2,210
290
2,900
Std. Dev.
(f and x)
1.99
1.58
2.47
1.77
3.22
1.88
1.95
2.34
3.67
1.88
1.82
2.70
2.40
Median
5%
Value
100
350
31
30,000
1,100
<100
1,230
6.6
380
410
830
175
1,780
* (All figures mg/kg dry sludge basis)
160
-------
sulfide content of the sludge (228 mg/£) may have precipitated
the mercury, thus making it unavailable for biological methyla-
t i o n .
The use of sulfide as a detoxicant for other heavy metals
has also been suggested, with the metal ions being precipitated
out as metallic sulfides (552).
BIOLOGICAL CONTAMINANTS
The anaerobic digestion process effectively degrades
proteins and other organic materials. Many studies have been
made of the destruction or inactivation of viruses and bacteria
Hinesly et al. (580) reported the incidence of fecal coliforms
to be approximately 10^ cells/m£ of digested sludge. The
number of fecal coliforms in liquid digested sludge gradually
decreases with increased digester retention time, as shown in
Table 56.
SI
udge
Total
SI
udge
LI
TABLE
QUID D
56. NUMBER OF
IGESTED SLUDGE
sampl es
si
s
udge
uperna
tant
0
4x1
3x1
FECAL COLI
AS A FUNCTI
0
0
4
3
Day
19
7x1
2x1
FORMS
ON OF
s
O3
O1
PER m*
TIME (
32
2xl02
0
OF
580)
A study of the destruction of various species of bacteria
by anaerobic digestion was performed for the EPA (1123).
Results of the study (presented in Table 57 ) indicate that
certain organisms were not entirely eliminated by digestion.
This was corroborated in a review by Foster and Engelbrecht
(428). The authors reported that destruction of S_. typhpsa
was 83 to 99.7 percent after 12 hr in batch digestion studies,
A 31 percent survival of mycobacteriurn species was noted after
digestion of more than 35 days. Tubercle bacilli were able
to survive from 6.5 months up to 2 years after digestion,
even though 90 percent of the organisms were destroyed during
treatment,
Viral inactivation by anaerobic digestion is accomplished
far more rapidly than bacteria destruction. The mechanism
of infectivity loss or inactivation has not been determined,
although the linearity of inactivation curves suggests that
a single mechanism predominates (112).
161
-------
Anaerobically digested sludge seeded with a swine entero-
virus (EPCO-1) was fed to germ-free piglets in experiments
performed by Meyer et al. (908). Indications of piglet
infection were found after four but not five days of digestion,
Based on the data provided, an inactivation rate of 91 percent
per day can be estimated.
The inactivation of polio virus I, coxsackie virus A-9,
coxsackie virus B-4, and ECHO virus II was studied by
Bertucci et al . (112). According to this study, viral inac-
tivation appeared to follow a first order reaction pattern.
Significant differences were noted among the inactivation
rates of the virus tested.
TABLE 57. BACTERIAL DESTRUCTION BY ANAEROBIC DIGESTION
(1123)
Bacteria
Endamoeba
hystolytica
Salmonella
typhosa
Tubercle
bacilli
Digestion Period
(days)
12
20
35
Destruction
%
<100
92
85
Remarks
Greatly reduced pop-
ulations at 68°F
85% reduction in 6
days detention
Digestion cannot be
relied upon for com-
plete destruction
Escherichia
coli
49
<100
Greatly reduced pop-
ulations at 99°F,
about the same re-
duction in 14 days
at 72°F
162
-------
AEROBIC DIGESTION
INTRODUCTION
Aerobic digestion is another method used to stabilize the
organic fraction of wastewater treatment plant sludge. Avail-
able literature is listed on Table 58. To date, this pro-
cess has only been employed at small wastewater treatment
plants or where polishing of excess waste-activated sludge is
necessary. Widespread application of aerobic digestion is
limited by the long solids retention time and consequential
high oxygenation costs required by the process.
Aerobic digestion is a biological process during which
oxidation is completed in two phases: (1) direct oxidation
of any biodegradable matter by microorganisms; and (2) oxi-
dation of microbial cellular material by endogenous respira-
tion. After input waste organics are completely oxidized,
the sludge mass is further reduced by endogenous metabolic
activity.
Advantages of aerobic digestion include: (1) a volatile
solids reduction comparable to that obtained by anaerobic
digestion; (2) a humus-like digested sludge that has no dis-
agreeable odor; (3) a relatively low BOD concentration in the
supernatant; (4) a sludge that is easily dewatered; and
(5) a relatively problem-free operation (531, 552, 622).
However, the process has certain disadvantages: power costs
to supply the required oxygen are high, and pH values as low
as 4.5 may result due to the absence of methane gas production.
Such extreme pH values inhibit nitrate formation and result
in the release of large amounts of soluble phosphorus (552).
163
-------
TABLE 58. LITERATURE REVIEWED
PERTAINING TO AEROBIC DIGESTION
Contaminant Reference Number
Water Quality Parameters
Ammonia 327
BOD 531, 552, 622, 1053
COD 456
Nitrates 327, 1281
Phosphates 552, 1230
Suspended 456, 531, 552, 622, 1053
solids
Other (qeneral) 531, 551, 552, 691, 1053, 1123
Elemental Contaminants
Chromium 71
Copper 71
Nickel 71
Zinc 71
Biological Contaminants
Bacteria 1281
Coliforms 568
Escherichia 568
coli
Virus 1281
164
-------
THERMAL PROCESSES
INTRODUCTION
Thermal processes, whether conventional heat treatment or
incineration, use increased temperature to achieve either
pasteurization or oxidation of organic material. Literature
concerning these processes is shown in Table 59. Reports on
heat treatment mainly cover the Inactivation of biological
contaminants; those on incineration more frequently address the
subject of elemental contaminants.
Heat treatment is a well known method of destroying patho-
genic organisms (1123). This wet air oxidation process is based
on the principle that any substance capable of burning can be
oxidized in the presence of liquid water at temperatures between
250°F and 700°F. The process can operate on difficult-to-dewater
waste liquors and sludges with extremely low solids concentra-
tion. In general, given the proper temperature, pressure,
reaction time, and sufficient compressed air or oxygen, any
degree of oxidation desired can be accomplished, nameless
oxidation of organics can be achieved at relatively low tempera-
tures of 300°F to 400°F with this technique, compared with the
1,500°F to 2,700°F necessary for conventional incineration. Air
pollution is minimized since oxidation takes place in water at
low temperatures, and no fly ash, dust, sulfur dioxide, or
nitrogen oxide by-products are formed (1123).
Incineration has been a popular sludge treatment and
disposal method for over 20 yr. Proper treatment of sludge
prior to its introduction into the incinerator unit is the key
to successful Incineration. Pretreatment may include sludge
thickening, a macerating or disintegrating system, and/or a
dewaterlng device (1123).
The air emission products of sludge combustion are essen-
tially steam, carbon dioxide, small amounts of particulate
emissions, and oxide of sulfur (1017). Such by-products could
pose problems for human health and environmental quality.
Table 60 summarizes particulate, NOX, sulfur dioxide, and
visible emissions from four incineration sites. As shown, NOX
emissions are most significant.
165
-------
TABLE 59 . LITERATURE REVIEWED PERTAINING
TO THERMAL PROCESSES
Contami nant Reference Number
Water Quality Parameters
Ar.n.ionia 1236
BOD 864, 1435
COD 222
Nitrates 528, 788, 1281
Phosphates 507, 1354
Suspended solids 126, 1435
Other (general) 7, 88, 393, 531, 551, 552, 642, 864,
1017, 1123, 1354
Elemental Contaminants
Aluminum 507
Boron 75
Cadmium 662, 926, 1017
Chromium 436, 746, 1017
Copper 401, 746, 1017
Iron 507, 1017
Lead 662, 746, 1017
Manganese 746
Mercury 401, 926, 1017, 1077
Nickel 401, 1040
Zinc 401, 436, 1040
Biocidal Contaminants
Chlorinated
hydrocarbons 401
166
-------
TABLE 59 (continued)
Contaminant Reference Number
DDT 401
D i e1d r i n 401
Synthetic/Organic 567
Contaminants
Biological Contaminants
Bacteria 1325
Coliforms 401
Escherichia coli 1123, 1325
Mycobacterium 1123, 1325
Parasitic worms 791, 1325
Protozoa 1325
Salmonella 1123, 1325
Virus 1123, 1281, 1325
Other (general) 1123, 1281, 1325
167
-------
TABLE 60. EXHAUST EMISSIONS FROM SLUDGE INCINERATION (1017)
Emissions
Minimum
Maximum
% Carbon Dioxide -
Vol. % (dry basis)
% Excess Air (test point)
Sulfur Dioxide (ppm)
NOX (ppm)
Hydrochloric acid (ppm)
Particulate - filter (GR/SCFD)
Particulate - total (GR/SCFD)
Sludge feed to furnace
(Ib DS/hr)
Stack flow rate (SCFM)
2.2
366.0
1.97
11.47
.621
.0127
.0170
221.8
1 ,170
10.2
51.0
14.26
271.63
11.9
.0766
.0859
1 ,710.0
10,290
ELEMENTAL CONTAMINANTS
Wastewater sludges contain metals that could be hazardous
if discharged to the atmosphere during sludge incineration. The
effect of incineration on such metals will be influenced by the
forms in which the metals are found in sludge. For example, if
cadmium is present in the sludge in solution as cadmium
chloride, it will volatilize during incineration. If present
as a precipitated hydroxide, however, cadmium will probably
decompose to the oxide, but will not volatilize at the tempera-
tures of incineration. It is believed that most hazardous
metals, with the exception of mercury, will not appear dispro-
portionately in stack gases because of volatilization, but will
instead be converted to oxides and appear as particulates either
in the fly or bottom ash.
High temperatures during incineration decompose mercury
compounds to volatile mercuric oxide or metallic mercury. Tests
conducted on five incinerators equipped with scrubbers showed
an average emission factor of 1.65 g of mercury emitted to the
atmosphere per metric ton of dry sludge incinerated.
Table 61 (1017) presents concentrations of metals in the
input sludge and the bottom ash for three plants. Any discrep-
ancy in concentration would indicate volatilization of the metal
in either the fly ash or vapor.
The chemical content of ash from multiple hearth incinera-
tors reported by Olaxsey (1017) is shown in Table 62 .
168
-------
TABLE 61 . METAL TO FIXED SOLID RATIO
THREE INCINERATORS (1017)
(mg/g)
FROM
Plant A
Plant B
Plant C
Element
Sludge Ash
Sludge Ash Sludge Ash
Cadmium
Chromium
Copper
Iron
Lead
Magnesium
0.37
2.0
2.6
18.0
5.8
9.0
0.20
0.3
1.3
8.9
0.7
n.d.
n.d.
2.9
2.5
12.0
7.0
20.0
0.58
0.5
1.7
11.0
0.85
n.d.
0.31
0.7
1.6
50.0
2.0
6.0
0.22
0.6
1.6
43.0
1 .0
n.d.
TABLE 62. CHEMICAL CONTENT OF
SLUDGE INCINERATION ASH (1017)
Content
Silica (Si02)
Alumina (Alp03)
Iron Oxide (Fe203)
Magnesium Oxide (MgO)
Total Calcium (CaO)
Available Calcium
Phosphorus Pentoxide
Loss of Ignition
Percent of Total
25-30
10-13
9-10
2-2.8
30-37
1-2
7-10
0.5-1.0
Chemical analysis of wastewater sludge ashes was also
performed by Gray and Penessis (507). In general, the ashes
were composed of predominantly silt-sized particles. All the
ashes showed a pH in the range of 10.7 to 12.8 and were not
appreciably soluble in water. The soluble salt content and
conductivity of the ash leachates was almost exclusively com-
posed of dissolved calcium and magnesium. Contrary to results
on the two preceding tables, the amount of soluble iron,
potassium, and phosphate was negligible, with the leachate
containing between 0 and 0.5 mg/100 g of air-dried ash.
BIOLOGICAL PATHOGENS
Table 63 shows the effect of various pasteurization
temperatures and times on the survival of typical pathogenic
organisms found in sludge.
169
-------
TABLE 63. EFFECT OF TIME AND TEMPERATURE ON THE
SURVIVAL OF TYPICAL PATHOGENS FOUND IN SLUDGE* (1123)
Temperature C
Organism 50 55 60 65 70
-- minutes --
Cysts of Entamoeba histolytica 5
Eggs of ascaris 1umbricoides 60 7
Brucella abortus 60 3
Corynebacterium diphtheria 45 4
Salmonella typhosa 30 4
Escherichiacoli 60 5
Micrococcus pyrogene var.
aursus 20
Mycobacteriurn tuberculosis
var. promixis 20
Viruses 25
*Pathogens completely eliminated at indicated time and
temperature.
170
-------
ENVIRONMENTAL PATHWAYS
FRESH SURFACE WATER
INTRODUCTION
Direct discharge of treated wastewater to fresh surface
water is the most popular method of wastewater disposal and
potentially the most significant pathway of wastewater contami-
nants through the biosphere. In addition, relatively minor
quantities of wastewater contaminants may indirectly reach fresh
surface waters through runoff or percolation from land disposal
of wastewater effluents and sludges. This section of the report
discusses current knowledge about the fate of various contami-
nants in fresh-water systems.
Surface waters receive contaminants from treated municipal
wastewaters (as previously stated) and from other significant
sources such as agricultural runoff, storm-water discharges,
mine drainage, and atmospheric fallout. Most of the literature
pertinent to the behavior of various contaminants in fresh-water
systems - listed in Table 64 - does not differentiate contami-
nants by source. This, however, does not affect the validity of
the literature research.
Much of the material contained in this chapter was derived
from the following references: 304, 403, 464, 636, 1126, 1266,
and 1339.
WATER QUALITY PARAMETERS
General water quality parameters in surface waters are not
of direct public health concern, although they often degrade the
quality of the aquatic habitat. For example, phosphorus concen-
trations resulting from sewage disposal contributes to luxuriant
growths of certain algae, such as Anabaena, Nodularia, or NostoC'
all of which produce toxins that can be harmful to humans (1331,
1472). However, the tastes and odor also associated with such
water degradation would generally make the water unpotable long
before the concentration of toxins reached levels harmful to
public health.
Suspended solids in wastewater can carry adsorbed viral and
other biological contaminants (1476). Trace metals occur in
higher concentrations when associated with suspended matter than
when they are in a dissolved state (227), a phenomenon that will
be discussed more fully in the following section on elemental
171
-------
TABLE 64. LITERATURE REVIEWED PERTAINING TO
WASTEWATER TREATMENT PLANT EFFLUENT
DISPOSAL TO FRESH-WATER SYSTEMS
Contaminant
Water Quality Parameters
Reference Number
Ammonia
BOD
COD
Chlorides
Cyani des
Fluorides
Ni trates
Ni tri tes
Oil and grease
Phosphates
46, 47, 54, 133, 138, 221, 364, 418, 454,
757, 829, 920, 1002, 1125, 1156, 1239, 1306,
1407, 1436, 1453
46, 133, 354, 364, 533, 757, 882, 1064,
1283, 1306, 1392, 1405, 1470
46, 108, 133, 418, 1156, 1283,1306, 1470, 1475
46, 47, 54, 133, 500, 1018, 1156, 1177,
1306, 1405, 1470
1306, 1436
54, 133
9, 46, 47, 138, 151, 190, 221, 364, 411,
443, 454, 500, 533, 572, 600, 663, 757,
793, 829, 883, 1000, 1002, 1027, 1076,
1125, 1156, 1239, 1306, 1331, 1407, 1453
46, 133, 138, 221, 454, 663, 757, 793,
829, 920, 1125, 1156, 1239, 1407
757, 1306, 1497
46, 47, 54, 133, 138, 190, 221, 364, 418,
454, 533, 555, 600, 663, 757, 784, 829,
882, 883, 1156, 1306, 1314, 1331, 1407,
1436, 1448, 1472
Suspended solids 47, 227, 354, 454, 757, 920, 1006, 1125,
1171, 1306, 1470, 1476
Total dissolved
solids
Total organic
carbon
364, 418, 454, 757, 1125, 1177, 1306
133, 1125, 1167, 1264, 1283, 1306
Other (general) 304, 336, 385, 403, 464, 757, 805, 1125,
1126, 1156, 1253, 1258, 1266, 1286, 1370
172
-------
TABLE 64. (continued)
Contaminant
Elemental Contaminants
Aluminum
Reference Number
Antimony
Arsenic
Barium
Beryl 1ium
Boron
Cadmi urn
Chromium
Cobalt
Copper
Germanium
Iron
28, 634, 636, 968, 1082, 1093, 1121,
1125, 1266, 1339, 1380, 1407, 1453
303, 636, 777, 1093, 1121, 1266, 1306,
1339, 1380, 1453
303, 360, 409, 418, 520, 636, 1093,
1121, 1138, 1266, 1306, 1339, 1380,
1453
23, 418, 636, 968, 1093, 1121, 1266,
1339, 1380, 1453
418, 636, 1093, 1121, 1266, 1339, 1380,
1453
28, 133, 418, 636, 757, 1093, 1113, 1121,
1266, 1339, 1380, 1453
77, 117, 151, 175, 190, 263, 303, 360,
418, 433, 441, 462, 524, 629, 636, 724,
740, 757, 859, 1075, 1082, 1093, 1121,
1124, 1125, 1171, 1195, 1266, 1306, 1355,
1380, 1407, 1433, 1453, 1523, 1526, 1538
151, 263, 365, 418, 473, 629, 777, 859,
1082, 1093, 1121, 1125, 1128, 1306, 1380,
1407, 1433, 1436, 1526, 1538
303, 445, 473, 600, 634, 636, 740, 782,
859, 968, 1056, 1074, 1075, 1082, 1093,
1121, 1125, 1266, 1339, 1380, 1456, 1538
28, 77, 151, 190, 206, 418, 433, 445, 451,
473, 504, 505, 629, 634, 740, 777, 782,
859, 968, 1044, 1074, 1075, 1082, 1093,
1121, 1125, 1171, 1266, 1339, 1355, 1407,
1433, 1453, 1454, 1543, 1562
532, 636, 1093, 1121, 1266, 1339, 1453
28, 263, 306, 438, 473, 528, 634, 636,
782, 852, 854, 968, 1074, 1075, 1093,
1121, 1125, 1266, 1339, 1355, 1371, 1380,
1407, 1562
173
-------
TABLE 64. (continued)
Contaminant Reference Number
Lead 117, 151, 190, 204, 206, 360, 418, 441, 445,
462, 511, 524, 629, 634, 636, 724, 740, 757,
777, 782, 859, 912, 968, 1018, 1060, 1074,
1075, 1082, 1088, 1093, 1121, 1171, 1174,
1306, 1339, 1355, 1380, 1391, 1433, 1453,
1508, 1544, 1562
Manganese 28, 190, 206, 263, 306, 418, 445, 462, 473,
600, 636, 645, 844, 1074, 1075, 1121, 1171,
1266, 1306, 1339, 1355, 1380, 1433, 1453,
1523, 1538, 1544
Mercury 12, 37, 40, 78, 110, 117, 151, 269, 303,
418, 455, 462, 512, 524, 591, 607, 630,
634, 636, 726, 741, 752, 757, 760, 777, 809,
861, 968, 988, 1082, 1089, 1093, 1121, 1125,
1266, 1306, 1339, 1355, 1359, 1378, 1379,,
1380, 1407, 1433, 1446, 1453, 1526, 1543, 1562
Molybdenum 303, 636, 1093, 1121, 1266, 1339, 1380, 1453
Nickel 28, 263, 418, 436, 445, 473, 629, 636, 782,
859, 968, 1074, 1093, 1121, 1125, 1171, 1266,
1306, 1355, 1380, 1407, 1453, 1544
Selenium 418, 636, 1093, 1114, 1121, 1266, 1306, 1339,
1380, 1453
Thorium 636, 1093, 1266, 1339, 1380, 1453
Tin 636, 1082, 1093, 1266, 1339, 1453, 1380
Uranium 636, 1093, 1121, 1266, 1339, 1380, 1453
Zinc 21, 77, 151, 190, 263, 303, 418, 441, 445,
504, 505, 524, 629, 636, 724, 740, 782, 844,
859, 968, 1074, 1075, 1082, 1093, 1121, 1125,
1171, 1266, 1306, 1319, 1339, 1355, 1380,
1407, 1433, 1453, 1523, 1538, 1544, 1562
Other (general) 133, 228, 636, 1211, 1339, 1380, 1454, 1508
Biocidal Contaminants
Aldrin 139, 304, 373, 403, 783, 846, 1150, 1237, 1418
174
-------
TABLE 64. (continued)
Contaminants
Arsenated 1237
hydrocarbons
Chlorinated 139, 275, 304, 324, 373, 387, 403,
hydrocarbons 418, 464, 501, 512, 577, 757, 759, 772,
778, 827, 846, 998, 999, 1022, 1023,
1049, 1068, 1125, 1132, 1170, 1220,
1237, 1532, 1543
ODD 373, 403, 429, 577, 757, 759, 846,
1022, 1225
DDE 139, 373, 403, 429, 464, 529, 577, 759,
846, 972, 1125, 1150
DDT 14, 139, 304, 325, 373, 403, 420, 429,
453, 464, 515, 577, 641, 706, 757, 759,
846, 902, 931, 972, 1022, 1023, 1125,
1150, 1170, 1180, 1220, 1306, 1418, 1532
Dieldrin 373, 403, 429, 846, 972, 1125, 1550,
1237, 1306, 1418, 1470
Endrin 373, 403, 464, 846, 1150, 1418
Herbicides 597, 627, 1125, 1220, 1488, 1551
Organophosphorus 304, 306, 373, 418, 451, 501, 566, 846,
pesticides 1196, 1245, 1550
Soil sterilants 73
Other (general) 291, 304, 418, 478, 600, 641, 827, 846,
846, 1049, 1090, 1225, 1550, 1454, 1512
Synthetic/Organic 58, 149, 166, 275, 587, 770, 808, 856,
Contaminants 879, 998, 999, 1029, 1126, 1323, 1331,
1340, 1420, 1460, 1558
Biological Contaminants
Adeno virus 757, 1509
Bacteria 74, 140, 197, 231, 243, 296, 304, 418,
434, 521, 588, 596, 656, 676, 678, 786,
815, 938, 1131, 1202, 1306, 1370, 1399
Clostridium 1131
botulinium
Clostridium welchi 1131
175
-------
TABLE 64. (continued)
Contaminants Reference Number
Coliforms 46, 133, 140, 147, 187, 188, 197, 248,
299, 307, 354, 418, 457, 596, 612, 655,
656, 663, 757, 938, 1064, 1131, 1202,
1263, 1268, 1275, 1283, 1366, 1436,
1458, 1475, 1509, 1518
Coxsackie virus 11, 588, 757, 1366, 1509
(A+B)
ECHO virus 11 , 588, 757, 1366
Escherichia coli 147, 180, 588, 655, 1275
Fecal
streptococci 140, 147, 180, 197, 307, 457, 458, 612,
656, 1131 , 1202, 1263, 1283
Hepatitis virus 163, 257, 380, 492, 890, 1366, 1509
Leptospirosis 380
Polio virus 11, 85, 492, 750, 1209, 1366, 1509
Protozoa 655
Salmonella 30, 85, 231, 248, 307, 457, 588, 671,
1283
Shigella 30, 85, 588, 1449
Staphylococcus 1131
aureus
Vibrio cholerae 74, 1331
Virus 46, 94, 99, 111, 133, 246, 251, 257,
380, 454, 468, 564, 588, 678, 750, 757,
815, 826, 877, 890, 938, 1182, 1207,
1237, 1240, 1283, 1331 , 1366, 1434,
1443, 1478
Yeasts 596
Other (general) 180, 250, 433, 786, 1225, 1370
176
-------
contaminants. Suspended matter and dissolved organics from
wastewater can affect the natural biological community which,
in turn, affects the nitrogen interconversions and nitrate con-
centrations.
The nitrogen-containing compounds (ammonia, nitrite, and
nitrate) are theoretically hazardous because of nitrate's
association with methemoglobinemia. Ammonia and nitrite nitrogen
can be readily converted into nitrate by chemical or biological
reactions. There are, however, no reported cases of detrimental
public health effects resulting from nitrates in surface waters.
This is because the dilution and natural processes occurring in
surface waters prevent nitrate concentrations from reaching
health impairing levels. There are, however, several reported
cases of groundwater nitrate contamination rising to dangerous
levels. These cases are discussed in the land/groundwater
section of this report.
ELEMENTAL CONTAMINANTS
The behavior of elemental contaminants in fresh-water
systems is very complex. Generally, elemental contaminant
transport mechanisms can be divided into either (1) elements in
solution, or (2) elements associated with inorganic or biologi-
cal particulates. Each of these mechanisms can be broken down
still farther. Dissolved elements may occur as unassociated
ions or as inorganic or organic complexes. Elemental contaminant/
inorganic particulate associations include coulombic attraction,
as in conventional adsorption; ionic bonding, as in ion exchange;
precipitated or coprecipitated metal coating; or incorporation
into particulate crystalline lattices. Elemental contaminant/
biological particulate associations include surface adsorption,
ingested particulation, and biochemical incorporation into the
organism. The particular transport mechanism that will predomi-
nate in a given water system depends, in part, on the geohy-
drologic environment, mineralogy/petrology of the river or lake
bed, pH, temperature, dissolved organic or oxygen content,
biological activity, elemental type and source, and nonelemental
chemical composition of the water.
This variety of factors does much to explain the seeming
discrepancies in the work of different researchers attempting
to establish elemental distributions in fresh-water systems.
For instance, Gibbs (473), in his examination of the Yukon and
Amazon Rivers, concluded that precipitated metal coating and
crystalline incorporation accounted for approximately 90 percent
of the transported iron, nickel, copper, chromium, cobalt, and
manganese (Table 65 ). Perhac (1074), on the other hand, in
his analysis of two Tennessee streams, concluded that 95 percent
of the total stream content of cadmium, cobalt, copper, nickel,
lead, and zinc was in the dissolved state (Table 66). Assuming
that there was no gross experimental error, widely differing
environmental factors must have prevailed.
177
-------
TABLE 65 . PERCENTAGES OF THE TOTAL AMOUNTS OF
IRON, NICKEL, COBALT, CHROMIUM, COPPER, AND MANGANESE
TRANSPORTED BY FIVE MECHANISMS IN THE
YUKON AND AMAZON RIVERS (473)
Mechanism
In solution and
organic complexes
Adsorbed
Precipitated and
copreci pita ted
In organic solids
In crystalline
sediments
In solution and
organic complexes
Adsorbed
Precipitated and
copreci pi tated
In organic solids
Iron Nickel
Amazon River
0:7 2.7
0.02 2.7
47.2 44.1
6.5 12.7
45.5 37.7
Yukon River
0.05 2.2
0.01 3.1
40.6 47.8
11.0 16.0
Cobalt
1.6
8.0
27.3
19.3
43.9
1.7
4.7
29.2
12.9
Chromium
10.4
3.5
2.9
7.6
75.6
12.6
2.3
7.2
13.2
Copper
6.9
4.9
8.1
5.8
74.3
3.3
2.3
3.8
3.3
Manganese
17.3
0.7
50
4.7
27.2
10.1
0.5
45.7
6.6
In crystalline
sediments 48.2 31.0 51.4 64.5 87.3 37.1
178
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TABLE 66. HEAVY METAL DISTRIBUTION IN STREAMS (1074)
Average percentage of element occurring in specified form
Dissolved Coarse
Solid Participate Colloid
Cadmium 92.9 5.1 2.0
Cobalt 91.8 7.8 0.4
Copper 93.2 5.4 1.4
Iron 19.6 77.0 3.3
Lead 90.8 8.0 1.2
Manganese 23.4 74.6 2.0
Nickel 93.2 6.3 0.5
Zinc 77.8 21.8 0.4
179
-------
The complexity of the chef.iistry, biology, and physics
involved in water behavior of elements precludes a detailed dis-
cussion. Instead, a brief discussion is presented of the more
important aspects.of the behavior of elements in water, followed
by a detailed examination of a few sample elements (mercury,
arsenic, lead, cadmium, copper, iron) to demonstrate the princi-
ples involved.
Dissolved elements may occur as unassociated ions or as
inorganic or organic complexes. Of the major elements under
discussion in this report, only barium appears to any great
extent as the unassociated cation; barium ions do not hydrolyze
and form only weak complexes. However, several of the elements
occur as unassociated anions: antimony, arsenic, boron, chromium,
molybdenum, and selenium generally occur in fresh-water systems
as the-oxo anion. This is largely because the major sources of
these elements, including wastewater, are rich in the anionic
forms, and because the cationic forms are easily oxidized to the
oxo anion in aquatic systems.
The majority of the dissolved elements normally exist as
inorganic or organic complexes. Table 67 lists the more common
ligands and the conditions and elements normally associated
with them. In relatively pure water, aquo (1^0) or hydroxo
(OH") complexes are formed. At pH levels above neutral, many of
the metal-hydroxo complexes are converted to metal hydroxides or
oxides, which will precipitate out of solution or behave as
colloids.
The other inorganic ligands responsible for keeping metals
in solution in natural waters include carbonate, halides
(notably chloride and fluoride), sulfur species (SH~, sulfate,
and sulfite), and nitrogen species (ammonia, nitrate, and
nitrite). Most of the complexes formed from these ligands are
thermodynamically unstable and appear as transition states
between the free metal ion and a precipitate. The complexes,
however, serve to keep the metals in solution for a time, and
play a role in dissolving otherwise insoluble metals from
precipitates or crystalline lattices.
Of somewhat more importance in terms of complex stability
are the multidentate organic ligands. One of the reasons for
the lack of inorganic complex stability is that most of the
inorganic ligands are monodentate, i.e., there is one ligand for
each metal ion coordination site. Organic ligands are multi-
dentate, i.e., a given ligand can usually bond to two or more
of a given ion's coordination sites. A multidentate complex
(chelate) is more stable than a corresponding complex with
monodentate ligands; thus, a chelate complex is apt to keep a
metal ion in solution far longer than will an inorganic complex.
Normally, this is not a problem; in relatively unpolluted fresh
water the organic content is low, but in highly polluted water
180
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TABLE 67. (continued)
Footnotes
5
The solubility falls markedly in the presence of this ligand
at above pH due to precipitation of a carbonate or similar
basic compound.
Coordination occurs only at pH above 7 due to ligand insta-
bility, etc.
Coordination occurs only at pH above 8-9.
pPrecipitation almost always occurs. If nothing is marked,
there is no coordination of this metal by this ligand in
natural waters.
aWater will only coordinate if no other stronger ligand is
present. In some cases, there is an equilibrium.
Bromide and iodide resemble chloride except that they both
precipitate silver, whereas silver chloride is fairly
soluble due to AgCl?-ions at high chloride concentrations.
Iodide also precipitates copper and gold.
cTwo valent iron in absence of air only.
If ammonia is absent, a complex may be formed.
eBicarbonate usually forms carbonate complexes, but metals
so marked have a soluble bicarbonate which is water co-
ordinated. Be and Tl have soluble water coordinated car-
bonates, and Ag has both sparingly soluble water coordi-
nated carbonate and hydroxide.
182
-------
unusually high soluble metal concentrations may result. Further-
more, there is evidence that some synthetic organic ligands,
such as may be found in wastewater, form stronger complexes than
do natural organic ligands (782). It has been demonstrated that
one synthetic ligand, nitri1otriacetate (a proposed substitute
for phosphates in detergents), is capable of dissolving signifi- •
cant quantities of precipitated lead out of bottom sediments
(511, 1562).
The tendency for a given metal ion and ligand to form
complexes depends on solution pH, concentration of the metal
and ligand, concentrations of other metals and ligands in
solution, equilibrium constants, redox conditions, and so forth.
No two elemental contaminants behave exactly alike, and even
different oxidation states of the same element may exhibit
widely varying solution chemistry. Moreover, natural water
systems are seldom in an equilibrium condition before, much less
after, wastewater addition. This constantly changing system
makes concise pathways almost impossible to construct. In
general, low pH, an oxidizing environment, and the presence of
a variety of ligands enhance solution tendencies. This is signi-
ficant from a public health standpoint, because soluble element
species are much more readily available for human contact than
are precipitates or particulate elements.
Elemental contaminant/inorganic particulate interactions
typically account for the bulk of the nondissolved element, fraction
These interactions include coulombic or ionic attraction,
precipitated or coprecipitated coating, or lattice incorporation.
Coulombic attraction, or adsorption, is the least important
transport mechanism except in the case of colloidal particulates,
such as microparticulate iron or manganese hydroxides, which
carry a weak negative charge and attract elemental cations.
Larger particulates do not possess a strong enough charge to
make coulombic attraction important.
Ionic attraction, or ion exchange, is somewhat more impor-
tant. In this process, the heavy metals (Mn, Fe, Co, Ni , Cu,
Zn, Mo, Cd, etc.) replace alkali and alkali earth cations (K,
Na, Li, Mg, Ca) attached to crystalline lattices by ionic bonds.
These ionic bonds will hold unless (1) the element is displaced
by another element forming a stronger ionic bond, (2) a ligand
forming a coordination bond stronger than the ionic bond breaks
the ionic bond, or (3) an excess of alkali earth cations is
available to force the equilibrium back to its original state.
According to Gibbs (473), lattice incorporation is generally
insignificant as a transport or removal mechanism of dissolved
wastewater elemental contaminants. It is a slow process that
takes place in the sediments and has a more significant impact
on the elemental composition of the sediments. The lattice-
incorporated elemental burden of a water system is primari lyfrom
weathered rock, sand, and clay.
183
-------
Precipitated and coprecipitated metal coatings account for
most of the non-native participate element content of a water
system. Under favorable pH-EH conditions, metal precipitates
will form. The initially small precipitate particles will tend
to agglomerate or adhere to any available surface. In addition,
cations held to participates by coulombic or ionic bonds can
form covalent bonds with anionic components of the particulate,
if solution redox potentials change. In either case, the
particulates are left with a coating of metal precipitates.
This coating ultimately settles out of solution with the partic-
ulate, removing the elements from possible ready human
contact unless they are redissolved by a change in redox
conditions, a strong ligand, or some other agent strong enough
to attach the precipitate. These coatings may account for the
bulk of the inorganic particulate element burden of waste-
waters .
Elemental contaminants incorporated with biological particu-
lates constitute the remainder of the particulate elemental
burden of a water body or wastewater. This incorporation may
take the form of surface adsorption, inorganic particulate
ingestion, or biochemical incorporation into an organism's
tissues. Obviously, the role played by biological transport is
highly dependent on the 'ype and quantity of organisms present.
Surface adsorption is usually associated with microorganisms.
Particulate ingestion is associated with those organisms that
have internal digestive organs (e.g., fish, crustaceans, worms,
etc.); ingested particulates are usually eliminated within a
short time, but the elements associated with them may be bio-
chemically incorporated into the organism's tissues. From a
public health standpoint, soluble and biochemically incorporated
elemental contaminants are the most important, for it is by
these routes that potentially hazardous elements reach man.
Biochemical incorporation involves both essential trace element
concentration (e.g., cobalt in vitamin B-12) and reaction of an
element with cellular chemicals (e.g., the reaction of mercury
with sulfur-containing amino acids in proteins). Both plants
and animals are involved and, thus, the concentration of a
given element may move up the food chain. The incorporation
is reversible; once the organism in its environment is removed
from contact with the element, the latter can gradually be
excreted .
No two elements behave exactly alike; furthermore, the
number of factors available that can affect transport mechanisms
makes the possibilities nearly endless. There are similarities,
however, that make the use of examples illustrative and useful;
mercury, arsenic, iron, cadmium, copper, and lead will bi used
to provide detailed descriptions of the general pathways
disucssed above.
184
-------
Mercury from wastewater enters a water system primarily as
the metal or divalent cation. Although of limited solubility,
it can reach concentrations of 100 ppb in aerated water (455).
Metallic mercury alone is soluble up to 25 ppb and will hydrolize
to soluble Hg (OH)2 in oxygenated systems, increasing the overall
solubility and water content. Despite these solubility figures,
mercury concentrations seldom exceed 5 ppb (Table 68 } except
in polluted water.
Inorganic and biological adsorption, absorption, and pr'e-
cipitation serve to keep the concentrations of dissolved mercury
much lower than the theoretical maximum. In general, the bulk
of the mercury in a given water system is in the sediments;
Table 69 gives a summary of some of the factors affecting
mercury incorporation in the sediments. In reducing sediments,
mercury i.s tied up as the sulfide, although if the system be-
comes sufficiently alkaline, HgSp may be released into solution.
Should the sediments become aerobic, the sulfide will be oxi-
dized to sulfate, and the mercury will be released.
All soluble mercury species except mercuric sulfide can be
absorbed by bacteria. Once the mercury is in the bacteria, a
series of transformations - possibly via a detoxification
mechanism - convert the incorporated mercury into mono- and
dimethyl mercury, both soluble at low concentrations and readily
released into solution. The methyl mercury compounds are much
more 1 ipid-preferring than the inorganic forms and are quickly
absorbed by living tissues. As a rule, mercury concentrations
tend to increase in organisms up the food chain, so that the
highest concer.trat ions are found in fish. This is partly due to
absorption of methyl mercury from the water and partly from
ingestion of plants or smaller organisms containing methyl
mercury. When the organisms die, the mercury returns to the
sediments, where most of the bacterial methylation occurs.
Table 70 lists some sample sediment and plankton/algae mercury
concentrations in Lake Erie.
Arsenic, selenium, and antimony are chemically similar and
exhibit analogous environmental behavior. Arsenic has been
studied far more than either selenium or antimony. The following
discussion of arsenic is largely applicable to selenium and
antimony as we!1.
Arsenic has an unusually complex chemistry in aquatic
systems: oxidation-reduction, ligand exchange, precipitation,
adsorption, and biomethylation reactions all take place.
Arsenic species can be removed from water via surface adsorption
and coprecipitation with metal ions; both arsenate (As04~3) and
arsenite (As03~3) have a high affinity for hydrous iron oxides
and readily coprecipitate with or adsorb onto them. Signifi-
cantly, iron ores are always enriched with arsenic (409).
Aluminum hydroxide and clays are adsorb arsenate species,
although to a lesser degree.
185
-------
TABLE 68 . SELECTED CONCENTRATIONS OF
MERCURY IN NATURAL WATERS (455)
Source and Location Mercury (ppb)
River water, European USSR 0.4-2.8
River water, Armenia 1-3
Saale River, Germany 0.035-0.145
River water, Italy 0.01-0.05
River water, near mercury deposits, Italy up to 136
Colorado River, Arizona <0.1
Ohio River, II1inois 0.1
Mississippi River, Kentucky <0.1
Missouri River, Montana <0.1
Missouri River, St. Louis, Missouri 2.8
Kansas River, Topeka, Kansas 3.5
Hudson River, New York 0.1
Lake Champlain, New York <0.1
Maumee River, Antwerp, Ohio 6.0
Delaware River, New York <0.1
186
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187
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TABLE 70. MERCURY CONTENT OF SEDIMENTS AND PLANKTON/ALGAE SAMPLES
COLLECTED FROM LAKE ERIE (1089)
Station
No.
01
02
03
04
05
06
07
08
09
10
11
12
13
14
15
16
Approximate
Location 5
Buffalo River
Cattaraugus Creek
Barcelona
Ashtabula
Fairport
Cleveland
Toledo
Detroit River
Mid. Bass Island
Port Crewe
Port Stanley
Long Point
Long Point Bay
Port Mai tl and
Mid-Lake
Black Rock Channel
Mercury content in yg/g*
Sediments** Plankton/Algae
2.0 31.2
1.2 25.1
0.6 2.8
4.6 7.4
1.5 12.8
12.0 33.5
10.4 20.5
4.5 26.1
1.5 20.1
0.5 12.4
1.5 12.0
7.0 14.7
1.0 23.7
1.8 15.4
1.5 0.6
12.4 27.8
**
In terms of the equivalent dry wt of the sample.
Sediment samples from 3 to 30 cm below the water-sediment interface.
188
-------
Microbial transformations of arsenic, while demonstrable
in the laboratory, have not been positively identified in
natural water systems. The two most commonly postulated trans-
formations are oxidation of arsenite and methylation. Methyla-
tion is important because it could be a means by which sediment
arsenic is recycled back into the water system; natural aquatic
methylation has not been demonstrated.
Soluble iron entering a water system in wastewater will
usually be either ferrous (Fe II) or complexed ferric (Fe III)
iron. The former is much more soluble than the latter (which
has a stronger tendency to form complexes), although neither
tends to remain in solution long. In the surface layers of
most natural waters, pH levels and oxygen conditions are such
that Fe (II) is readily oxidized to Fe (III), which just as
readily hydrolyzes to insoluble hydrous ferric oxide (FeOOH).
Hydroxide has a much stronger affinity for ferric iron than do
basic organic or inorganic ligands.
Hydrous ferric oxide tends to form microcrystalline preci-
pitates of a colloidal nature, so that it is almost impossible
to analytically distinguish between soluble and colloidal iron.
Consequently, the two forms of iron are usually reported together
as soluble iron. Although hydroxide supersedes other an ionic
ligands, frequent incorporation of coordinating anions into
ferric oxide precipitates enhances colloidal stability and
further blurs the distinction between the colloid and soluble
ferric complexes.
Cadmium readily precipitates as the hydroxide or carbonate
and consequently is not normally found in high concentrations
in surface waters. In fact, several researchers (360, 968) have
noted that high soluble cadmium concentrations are invariably
associated with polluted water that receives a steady cadmium
source, such as industrial wastewater.
Cadmium (II) readily hydrolyzes and forms transitory
inorganic complexes, such as chloride complexes that have a
limited affinity for hydrous iron and manganese oxides, and
organic particulates. The organic affinity probably indicates
a reaction between the cadmium and sulfur-containing compounds.
Cadmium forms the insoluble hydroxide at pH levels of 7
and above; it forms the insoluble carbonate under oxidizing
conditions, particularly in soft waters where cadmium does not
have to compete with calcium and magnesium for the carbonate
an ion. Once cadmium has precipitated and settled into the
sediments, it is not readily removed. Consequently, if cadmium
additions are reduced, a water body will tend to purify itself
of soluble cadmium.
Copper, and to a lesser extent nickel, occupy an unusual
position in water chemistry and biology because they are both
189
-------
nutrients and toxins. This has a pronounced effect on their
water chemistry. Copper contained in wastewater may be either
soluble or particulate; neither form predominates as a rule.
Copper adsorbs readily onto clay and organic particulates.
Copper also forms several very stable complexes. In pure water,
while the aquo complex may predominate, the carbonate, chloride,
and amine inorganic complexes are much more stable.
Ultimately, the stability soluble of copper can be
attributed to organic complexes, since copper forms coordination
complexes with virtually every conceivable organic ligand.
These complexes are very stable thermodynamically and are also
resistant to microbial attack, a mechanism responsible for the
destruction of most organic complexes. Copper is a bacterial
toxin and, if released from its complex by microbial attack,
simply kills the offending bacteria and forms a new complex (968).
Copper is removed from solution via precipitation or
biological incorporation. Since the most common precipitate is
the carbonate, most sediment copper is in the carbonate form
(263, 968). An essential trace nutrient, copper is readily
incorporated into aquatic plants and animals.
The main soluble species of lead in wastewater are the
lead (II) cation and the hydrolyzed complex Pb (OH)3~ . Lead
forms a variety of stable complexes as well; researchers (777)
have identified both PbOH+ and Pb(C03)2~2 in natural water
systems. Lead complexes easily with a variety of organic
chelates,. forming very stable complexes. Some of these com-
plexes are more stable than the precipitated lead in the sedi-
ments; therefore, they will actually dissolve otherwise in-
soluble lead. A case in point is nitrilotriacetate, which
can solubilize lead from lead carbonate precipitates (511).
Low water organic content generally prevents solution lead
concentrations from exceeding a few parts per billion. In most
water systems, lead introduced with wastewater readily forms
insoluble Pb(OH)2 and PbCC^, which will precipitate and adsorb
onto suspended particulates. Ionic lead is not so strongly
adsorbed, although it does have some affinity for clays.
Hydrous iron oxides strongly sorb ionic lead at neutral
to slightly acidic pH levels. Some ionic or complexed lead
adsorbs onto or is chelated with the surface mucilage of algae,
and microorganisms immobilize substantial quantities of inorganic
lead, presumably on or in all membranes (1391). As a result of
all of these adsorption/precipitation mechanisms, most of the
water lead burden is associated with particulate matter, and
most of the lead entering a normal water system ultimately
finds its way into the sediment.
190
-------
Natural water bodies normally contain very low dissolved
concentrations of the more harmful elemental contaminants.
Unless wastewater additions are voluminous and repeated, natural
water chemistry can purify the water of soluble species fairly
well. However, there is a buildup of these elementals in the
sediments. This means that if the local water chemistry should
change significantly, the elements can still be released to
solution. Natural water purification mechanisms can only change
the wastewater elemental problem from a real to a potential
hazard; they cannot solve the problem of elemental contamination.
BIOCIDAL CONTAMINANTS
The single most important source of biocidal contaminants
in fresh-water bodies is surface runoff, followed by aerial
fallout and industrial waste discharge from plants manufacturing
biocides. In general, municipal wastewater will have detectable
quantities of biocides only if it contains biocide manufacturing
wastes. Cleanup and disposal by households, farmers, gardeners,
etc., contribute minimally to the overall wastewater burden.
In this discussion, biocides will include chlorinates,
hydrocarbons, organophosphates, carbamates, and ionic bio-
cides (Table 71 ) .
Biocides can be transported or removed from a system by
microbial or chemical degradation, photodegradation, sediment
or humic matter, adsorption, volatilization, and biological
uptake. All of these mechanisms are in turn affected by pH,
temperature, salt or organic content, and bioproductivity. One
mechanism that has not been studied to any great degree -
especially in fresh water - is aerosolization. This mechanism
will be discussed in greater detail in the marine water section
of this chapter, as its importance in fresh-water systems is
limited mainly to the larger lakes. Briefly, however, aerosoli-
zation occurs through the action of wind and waves on floatables.
Aerosols and particulates can be released to the air and trans-
ported great distances by the wind; biocides can concentrate in
floatables via dissolution in surface oil, adsorption on floating
matter, or flotation (caused by low specific gravity and insolu-
bility), thus becoming amenable to the aerosolization process.
As mentioned above, this is not an important transport mechanism
in most fresh-water systems.
Various transport mechanisms affect the biocide classes
differently. This is demonstrated in Table 72 , which compares
the persistence of selected chlorinated hydrocarbons, organo-
phosphates, and carbamates in river water Because of these
differences, the biocide classes will be discussed seoarately.
191
-------
TABLE 71 . BIOCIDE TYPES AND EXAMPLES
Chlorinated Hydrocarbons
DDT (ODD, DDE)
Methoxychlor
Endrin
D i e 1 d r i n
Aldrin
Toxaphene
Llndane
Chlordane
Heptachlor
Organophosphates
Parathion
Malathlon
Dlmethoate
Methyl parathlon
Phorate
Demeton
Ethlon
Dlsulfaton
Carbamates
Carbaryl
S e v i n
Baygon
Pyrolan
D i m e t i 1 a n
Ionic BiPC ides
Diquat
Paraquat
Chlormequat
Morfaunquat
Phosphon
Hyami ne
2,4-D
2,4, 5-T
Dalapon
Silvex
Dichlobenil
192
-------
TABLE 72. PERSISTENCE OF COMPOUNDS IN RIVER WATER (846)
Compound
Organochlorine compounds
BHC
Heptachlor
Adlrin
Heptachlor epoxide
Telodrin
Endosulfan
Dieldrin
DDE
DDT
ODD
Chlordane (tech.)
Endrin
Organophosphorus compounds
Parathion
Methyl parathion
Malathion
Ethion
Trithion
Fenthlon
Dimethoate
Merphos
Merphos recov. as
Azodrin
Original compound found, percent
0-time
2 wk
4wk
~8wk
Def
Carbamate compounds
Sevin
Zectran
Matacil
Mesurol
Baygon
Monuron
Fenuron
100
100
100
100
100
100
100
100
100
100
100
100
100
25
100
100
25
30
100
100
100
100
90
100
100
0
80
100
10
5
100
100
100
100
85
100
100
0
40
100
0
0
100
100
100
100
85
100
100
0
20
100
0
0
100
100
100
100
85
100
100
80
100
100
90
100
100
0
100
100
50
25
25
90
25
50
100
0
50
100
30
10
10
75
10
10
85
0
30
100
<5
0
0
50
0
0
75
0
10
100
0
0
0
50
0
0
50
0
<5
100
90
100
100
90
100
80
80
5
15
60
0
50
40
60
0
0
10
0
30
30
20
0
0
0
0
10
20
0
0
0
0
0
5
0
0
193
-------
The chlorinated hydrocarbon pesticides are all insoluble
in water, with the exception of lindane, which is sparingly
soluble to iO ppm (403)- They are generally resistant to
microbial and chemical degradation, as evidenced by their
estimated environmental half-lives, shown in Table 73 .
TABLE 73 . ESTIMATED PESTICIDE HALF-LIVES (403)
Pesticide HalJr-LifgJ,j jr^s
Lindane 2
Chlordane 8
Toxaphene 11
Heptachlor 2 to 4
DDT 10 to 20
Endrin (Dieldrin) 8 to 10
These pesticides are somewhat more susceptible to photo-
degradation, although the degradation products are often as
toxic as the parent compound, regardless of the type of
degradation, DDT is decomposed chemically to ODD and DDE and
photochemically to PCB's (304, 1170); aldrin is photooxidized
to the more toxic dieldrin (304); and methoxychlor is degraded
to methoxychlor DDE (1049). Surface oil slicks tend to concen-
trate chlorinated hydrocarbons and thus make them more available
for photochemical degradation (304).
Chlorinated hydrocarbons in general readily adsorb onto
fungi, algae, and floe-forming bacteria (783, 1049), and thus
tend to concentrate in biological communities. When ingested
by higher organisms, they accumulate in lipid tissues; conse-
quently, there is a tendency for chlorinated hydrocarbons to
concentrate up the food chain.
Chlorinated hydrocarbon insecticides differ in chemical
structure, but they all exhibit affinity for organic sediments
and resistance to microbial attack. As a result, there is
accumulation in bottom sediment. Research on Lake Michigan
demonstrates this, as shown in Table 74 . Routh (1180) showed
that DDT, with its affinity for fine particulate clay sediments,
concentrated up to 20 times normal background levels, from 10
to 200 ppb. This affinity for organic matter and particulates
leads to high sediment DDT concentrations. Table 75 shows DDT
concentrations in stream sediments over a period of time.
Adsorption of DDT on algae can be 10 to 100 times greater than
adsorption on clay (706). Moreover, DDT seems to have an
inhibitory effect on sediment bacteria (14).
There has been little research on other chlorinated hydro-
carbons, much of it limited to an evaluation of environmental
194
-------
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195
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TABLE 75. DDT CONCENTRATIONS IN STREAM SEDIMENTS (515)
Years after DDT
one (ppm)
application muds
0 .83
(.04-1.6)
1 1 .08
(.25-1.9)
2
3 .21
(.12-.30)
4 .21
(.16-.25)
5 .59
(.07-1.9)
6 .06
7 .21
(.11-.31)
8 .13
9 .03
(.02-.04)
10 .07
(0-.16)
Never sprayed .006
(0-.02)
Two sprays .43
(.17-.77)
Three sprays .35
(.17-.6)
196
-------
levels. Table 76 gives the results of one such survey for
d i e 1 d r i n.
TABLE 76 . DIELDRIN IN RIVER BOTTOM SILTS (972)
Source Dieldrin (ppb)
Iowa River 8.8
Des Moines River 35
East Nishnabotna River 21
West Nishnabotna River 16
Upper Iowa River <1
Johnson County Creek 170
Other researchers have found that the highest reported
concentrations of several pesticides in major U.S. river basins
from 1958 to 1965 were as follows: dieldrin, 0.100 vg/l; endrin,
0.116 vg/l; and DDT, 0.148 yg/£. Dieldrin was the most widely
found pesticide (1470).
The organophosphorus biocides are more soluble than the
chlorinated hydrocarbons. These solubilities range from 1 ppm
for ethion to 20,000 ppm for dimethoate; most fall in the 25 to
150 ppm range (403). The organophosphorus biocides are also
more amenable to both microbial and chemical degradation. Even
parathion, the most chemically resistant of the organophosphates,
will degrade via ester linkage hydrolysis in a few months under
normal conditions. The degradation takes place in just a few
weeks in polluted water with a high bacteria count (501). Yu
and Sanborn's (1550) experimental evaluation of parathion in a
model ecosystem yielded a calculated half-life of 15 to 16 days.
In a similar study, guthion yielded a half-life of one month at
pH levels less than 9 and a half-life of less than one week at
more alkaline pH's.
Interestingly, the degradation of organophosphates can be
inhibited by the presence of other synthetic organic chemicals.
Experiments were conducted with two detergent surfactants -
alkyl benzene sulfonate (ABS) and linear alkyl benzene sulfonate
(LAS). These experiments demonstrated increased persistence
for several organophosphate insecticides, especially parathion
and diazinon (304). As a result, highly polluted water may
exhibit accumulations or half-lives far beyond the normal for
organophosphates, which, as a rule, neither persist nor accumu-
late in the environment, but are removed entirely within a few
months.
Carbamate biocides are moderately soluble, ranging from 7
ppm for terbutol to 250 ppm for propham and averaging around 100
ppm (403). In general, they decompose easily and show little
197
-------
tendency toward adsorption on suspended material, but hydrolyze
readily. The hydrolysis is particularly pH dependent, virtually
ceasing below pH 5 (403) and increasing as the pH and tempera-
ture rise. High salt content affects the hydrolysis rate
inversely, slowing the rate as the salt concentration increases
(403). Carbamates photodecompose readily - increasingly so,
as the pH rises - and can be rapidly biodegraded under normal
circumstances (1170). Carbamates are not, then, persistent
in. normal water systems, lasting only a few days to a few weeks,
but remain as a stable compound in acidic waters (403).
Ionic biocides are a broad class embracing a variety of
chemical types and uses. They are all considered soluble in
water, with solubilities ranging from 100 to more than 1,000,000
ppm. Ionic biocides that are marginally soluble in pure water
have increased solubilities in natural waters high in humic
acid salts (403). With few exceptions, these biocides do not
accumulate or persist and, consequently, are seldom found in
high concentrations.
Ionic biocides are, however, strongly adsorbed onto soil
particles, all types of clay, humic matter, and organisms - in
short, onto anything with a partial charge or an ion exchange
capability (403). They are generally resistant to chemical
attack but photodegrade readily, except when adsorbed onto
particulate matter (403). Ionic biocides respond differently to
microbial attack, but are absorbed by many organisms. As a
result, they tend to concentrate in organisms and up the food
chain. Research on TCDD, an ionic herbicide residue, demon-
strated that accumulation was directly related to water concen-
trations (0.05 to 1,330 ppb) and averaged between 400,000 and
2,000,000 times the water concentration (627).
SYNTHETIC/ORGANIC CONTAMINANTS
Recently, there has been a great interest in identifying
synthetic/organic trace compounds in water supplies drawn from
rivers and in other water bodies receiving treated wastewater.
Although studies have been made of the concentrations found
various water systems, neither the environmental
the potential health effects to man of these
been studied to any great extent.
i n
pathways nor
substances have
Over 100 synthetic/organic compounds have been identified
in various drinking water sources. Thirty-six compounds were
found in the lower Tennessee River (Table 77 ), while 66 were
identified and Quantified in Mississippi River water at New
Orleans (Tabl» ':? '' "able 79 lists the results of organic
analyses of s?ver*i -it he" domestic water supply sources.
The many d i f t e >~ ~ n t
make generalizations di
ivpes of compounds under discussion here
f;,.jli regarding their environmental
198
-------
TABLE 77. ORGANIC COMPOUNDS IDENTIFIED
UP TO 1975 IN LOWER TENNESSEE RIVER (1323)
COMPOUNDS
Acenaphthene
Allylbenzoate
Anthracene
Benzene
Biphenyl
Butylbenzene
5-Chloro~2-Methylbenzofuran
p-Cresol
Diallyl Adipate
Dibutyl Phthalate
Diphenylacetylene
1,1-Diphenylethene
2,6-Di-Tert-Butyl-4-Methylphenol
Ethylbenzene
Ethyl o~Phthalate
Ethylstyrene
Ethylene Dimethylacrylate
Fluoranthene
Fluorene
Hexachlorobenzene
Indene
o-Methoxybenzoic Acid
2-Methylanthracene
2-Methylbiphenyl
4-MethyIdiphenylacetylene
Methyl Indene (2 isomers)
1-Methylnaphthalene
Naphthalene
p-Nonylohenol
n-Octyl-o-Phthalate
Pyrene
Styrene
1,2-Tetradecanediol
Toluene
3,4,4-Trimethy1-2-Hexene
Xylene
199
-------
TABLE 78.
ORGANIC COMPOUND IDENTIFICATIONS
NEW ORLEANS AREA WATER SUPPLY STUDY
(856 )
1
2
3
4
5
6
7
8
9
10
Highest Measured Concentration
yg/1
Compound
Acetaldehyde
Acetone
Alkylbenzene-Cg isomer
Alkylbenzene-Cg isomer
Alkylbenzene-C2 isomer
Alkylbenzene-Cj isomer
Alkylbenzene-C3 isomer
Alky1benzene-C3 isomer
Atrazine *
(2-chloro-4-ethylamino-
6-isopropylamino-
s_-triazine)
Deethylatrazine
(2-chloro-4-amino-
6-isopropylamino-
s_-triazine)
Carrollton
Water Plant
D-VOA
D-VOA
0.05
0.33
0.11
0.01
0.04
0.02
5.0
0.51
Jefferson # 1
Water Plant
NE
NE
ND
ND
0.03
ND
0.05
ND
4.7
0.27
Jefferson # 2
Water Plant
NE
NE
ND
ND
ND
ND
0.02
ND
5.1
0.27
200
-------
TABLE 78. (continued)
Highest Measured Concentration
11
12
13
14
15
16
17
18
19
20
21
Compound
Benzyl butyl phthalate*
Bromodichloroethane
Bromoform *
Butanone
Carbon disulfide
Carbon tetrachloride
bis-2-Chloroethyl ether*
Chloroform *»a
bis-2-Chloroisopropyl
ether *
n-Decane *
Decane-branched isomer
Carrol.lton
Water Plant
0.64
D-VOA
0.57
D-VOA
D-VOA
D-VOA
0.07
113
0.18
0.04
0.03
Jefferson # 1
Water Plant
0.81
NE
ND
NE
NE
NE
0.16
NE
0.05
ND
ND
Jefferson # 2
Water Plant
0.73
NE
ND
NE
NE
NE
0.12
NE
0.03
ND
ND
201
-------
TABLE 78. (continued)
Highest"Measured Concentration
Compound
22
23
24
25
26
27
28
29
30
31
32
Di bromodi chl oroethane
isomer
Dibromochloromethane *
Dibutyl phthalate *
2,6-Di-t-butyl-£-
benzoquinone *
Dichlorobenzene isomer
T,2-Dichloroethane a
Dichloromethane
Dieldrin **
Diethyl phthalate *
Di(2-ethylhexyl) phthalate *
Dihexyl phthalate
Carroll ton
Water Plant
0.33
1.1
0.10
0.22
0.01
8
D-VOA
0.05
0.03
0.10
0.03
Jefferson # 1
Water Plant
ND
0.30
0.16
0.19
D-RE
NE
NE
0.07
0.03
0.31
ND
Jefferson s? 2
Water Plant
0.63
0.60
0.19
0.23
ND
NE
NE
0.05
0.01
0.06
ND
202
-------
TABLE 78. (continued)
Highest Measured Concentration
yg/1
33
34
35
36
37
38
39
40
41
42
43
Compound
Dihydrocarvone
Diisobutyl phthalate *
Dimethyl phthalate
Dioctyl adipate
Dipropyl phthalate *
n-Dodecane *
Endrin **
Ethanol
£-Ethyl toluene *
£-Ethyl toluene *
1, 2, 3, 4, 5, 7, 7-
Heptochloronorbornene *
Carroll ton
Water Plant
0.14
0.59
0.27
0.10
0.07
0.01
0.004
D-VOA
ND
0.02
0.06
Jefferson # 1
Water Plant
0.06
ND
0.13
ND
0.13
ND
NYE
NE
0.04
0.03
0.05
Jefferson ? 2
Water Plant
0.07
ND
0.18
ND
0.14
ND
NYE
NE
0.02
0.03
0.05
203
-------
TABLE 78. (continued)
Highest Measured Concentration
Compound
44
45
46
47
48
49
50
51
52
53
54
Heptachloronorbornene
isomer
Hexachloro-1 ,3-butadiene *
Hexachloroethane *
Isophorone *
Limonene *
Methanol
Methyl benzoate
3-Methylbutanal
2-Hethylpropenal
n-Nonane *
n-Pentadecane *
Carroll ton
Water Plant
0.06
0.16
4.4
1.5
0.03
D-VOA
ND
D-VOA
D-VOA
0.03
0.02
Jefferson # 1
Water Plant
0.04
0..27
0.19
2.2
ND
NE
D-RE
NE
NE
ND
ND
Jefferson # 2
Water Plant
0.04
0.21
0.16
2.9
ND
NE
ND
NE
NE
ND
ND
204
-------
TABLE 78. (continued)
Highest Measured Concentration
ng/1
Compound
55
56
57
58
59
60
61
62
63
64
65
66
Tetrachloroethane
isomer
Tetrachloroethylene
n-Tetradecane *
Toluene *
1 ,1 ,2-Trichloroethane *
1 ,1 ,2-Trichloroethylene
n-Tridecane *
Trimethyl-trioxo-
hexahydrotriazine
isorner
Triphenyl phosphate *
n-Undecane *
Undecane-branched isomer
Undecane-branched isomer
Carroll ton
Water Plant
0.11
D
0.02
0.08
0.35
D-VOA
0.01
0.07
0.12
0.02
0.04
0.06
Jefferson # 1
Water Plant
ND
0.5
ND
0.10
0.45
HE
ND
ND
ND
ND
ND
ND
Jefferson # 2
Water Plant
ND
0.41
ND
ND
0.41
NE
ND
ND
ND
ND
ND
ND
205
-------
TABLE 78. KEY TO SYMBOLS USED IN TABLE
KEY TO SYMBOLS USED IN TABLE
Symbols used in column headed Compound
* While all compounds listed in the table were identified by one or
more methods, those marked with this symbol gained added confirma-
tion by gas chromatography retention time match with an available
standard of the compound.
** Compounds marked with this symbol gained further confirmation by
gas chromatography retention time match with available standards on
each of three different columns, polar and non-polar.
a The quantitative values for these compounds were obtained on
Volatile Organics Analysis by comparison with standards of known
concentration at the Water Supply Research Laboratory. Compound 18
was detected but not quantified in Tetralin extracts of Carrollton
water at Southeast Environmental Laboratory, but not in Tetralin
extracts of Jefferson Mo. 1 or Jefferson No. 2. The latter labora-
tory did not detect compound 27.
Symbols used in columns headed Highest Concentration Measured.
D-VOA These compounds were detected by Volatile Organics
Analysis - Bellar Technique only. Quantitative values
have not yet been obtained. Ttvis -method was performed
only on the Carroll ton water at the Water Supply Research
Laboratory.
D-RE These compounds were detected only on XAD resin
extracts in the specific water for which this symbol
is used. Quantitative values were not obtained from
the resin extracts. The compound may have been detected
and quantified by another method in one or both of the
other waters examined.
D In the one instance v/here this symbol was used the
compound was detected by both the Water Supply Research
Laboratory and Southeast Environmental Research Laboratory
but not quantified by either laboratory.
NE This symbol means not examined. It is used
exclusively for some compounds reported by the Water
Supply Research Laboratory. This laboratory did not
obtain samples of water from Jefferson No. 1 or Jefferson
No. 2.
206
-------
TABLE 78. (continued)
ND This symbol means the compound was not detected in
that specific water by any of the methods employed.
NY£ Compound 39 was confirmed in Carroll ton water carbon
chloroform extracts shortly before preparation of this
report. Jefferson No. 1 and Jefferson No. 2 extracts
have not yet been re-examined specifically for compound 39.
207
-------
TABLE 79. MOLECULAR CONSTITUENTS IDENTIFIED
IN NATURAL WATER SAMPLES (1323)
Constituent
p-Cresol
Diethylene glycol
Ethylene glycol
Glycerine
Glyci ne
Manni tol
Methyl-a-D-glucopyranoside
Methyl-B-D-glucophranoside
Sucrose
Xylitol
Urea
Inosi tol
0-Methyl inosi tol
Linoleic Acid
Oleic Acid
Palmitic Acid
Stearic Acid
2,2' -Bipyridine
Sample*
3
5
5
1,2,3,4,5
1
5
4
4
1,5
5
1,2
1,2,3,4,5
1,2,3,4,5
1,5
1,5
1,5
1
4
Concentration
mg/l
7
1
20
1-20
2
2
30
3
2
1
4
0.5-1
0.3-10
1
1
0.4
0.5
4
*1 - Lake Marion, 2 - Fort Loudon Lake, 3 - Holston River,
4 - Mississippi River, 5 - Watts Bar Lake
208
-------
fate. For instance, acetone is infinitely soluble in water;
chloroform is soluble to about 8,200 mg/t; carbon tetrachloride
is soluble to about 800 mg/t; and n-decane is insoluble. The
specific gravity of toluene is less than that of water, while
the specific gravity of carbon disulfide is greater. Acetalde-
hyde is readily metabolized since it is a natural metabolic
intermediate, but branched alkyls are almost impervious to
microbial attack.
The differences in man-made synthetic/organic compounds
exceed the similarities, but in general, these compounds are
persistent and resist microbial degradation. Beyond that
generalization, research has been too limited to discuss
specific compounds in detail.
Polychlorinated biphenyls (PCB's) are the only class of
synthetic/organic contaminants that have been studied in detail.
They are virtually insoluble in water, which, combined with a
high specific gravity and volatility, serves to keep solution
PCB concentrations low. However, PCB's are strongly adsorbed
onto suspended particulate matter and transported through the
water system. Because of their heavy, insoluble character and
sediment affinity, they tend to accumulate in bottom sediments.
A comparison of selected water and sediment PCB concentrations
from across the United States is presented in Table 80 .
PCB's are fairly stable in fresh-water systems, resisting
hydrolysis and chemical degradation, and are not amenable to
photodegradation (998). Theoretically, they should readily
vaporize from solutions, but this is prevented by their tendency
to sink or strongly adsorb onto suspended matter. Only PCB's
that are associated with floatables or oil slicks appear to
vaporize to any great degree. The lower isomers (four or fewer
chlorine atoms) are somewhat responsive to biodegradation, but
the degradation products are frequently more toxic than the PCB
itself (998). The higher isomers resist microbial attack.
PCB's are thus quite persistent in water/sediment systems, and
lifetimes of years or even decades have been postulated (998).
The continued presence of PCB's makes it inevitable that
they will enter the food chain. As they tend to accumulate in
lipid tissues in higher plants and animals, it has been
estimated that PCB's will concentrate up the food chain to as
much as 10' times the water concentration (999).
BIOLOGICAL CONTAMINANTS
An important pathway for certain communicable disease
transmission to man is the consumption of contaminated water.
Direct disposal of wastewater is the principal contamination
route. Land disposal of wastewater and sludge is not an
important pathway, as pathogenic organisms have limited mobility
209
-------
TABLE 80. PCB CONCENTRATIONS IN
SELECTED WATER COURSES (275)
State
Alaska
Arkansas
Cal ifornia
Connecticut
Hawai i
Georgia
Mary! and
Mississippi
New Jersey
Oregon
Pennsylvania
South Carolina
Texas
Virginia
Washington
West Virginia
Concentration
Water
ug/£
ND
ND
0.1, 0.1
0.1-0.2
ND
0.1
ND
0.1
ND
0.2
--
0.1-3.0
0.1
ND
ND
Concentration
Sediment
yg/kg
ND
20-2,400
20-190
40
ND
10-1 ,300
10-1 ,200
50; 170
8-250
15; 140
10-50
30-200
7.9-290
5-80
ND
10
210
-------
in soil and seldom migrate far enough to contaminate water
supplies (588). However, in contrast to their restricted
mobility in soils, biological contaminants are readily dispersed
and transported by receiving waters. Consequently, there is a
high potential for direct public contact through drinking or
recreational use. Wastewater treatment has diminished this
threat by reducing the number of organisms in the wastewater.
This, combined with natural pathogen mortalities, has greatly
lessened the outbreak of water-borne diseases attributable to
public water supplies.
The environmental factors that influence the survival of
pathogens in fresh water are, in most cases, similar to those
that prevail in marine systems. These factors will be discussed
in greater detail in the marine water section of this chapter.
Briefly, however, the chief factors influencing survivabi1ity
are temperature, pH, sunlight, toxins, predators, and lack of
nutrition, which affect pathogens to different degrees. An
examination of Table 81 reveals that pathogens may survive for
long periods of time and travel great distances before destruc-
tion by environmental factors.
Pathogenic bacteria are best adapted to survival in the
human body or to conditions resembling those found in the body.
Consequently, natural water systems are a hostile environment.
However, cool water is generally more hospitable than warm water
because of the depressed metabolism of both the bacteria and
their predators. Predatory organisms, especially in slightly
polluted waters, are a major contributor to bacterial die-off.
For instance, Barua (74) noted that Vibrio cholerae survived
one to two weeks in clean water as opposed to one to two days in
water with a large bacterial population.
Pathogenic bacteria also suffer from a lack of proper
nutrition in clean waters; low nutrient levels prevent reproduc-
tion. Since die-off rates exceed growth rates, the overall
population will decline. Other factors affecting die-off are
ultraviolet radiation in sunlight, pH extremes, natural anti-
biotics, and chemical toxins.
In contrast to bacteria, viruses do not multiply in water
and, therefore, their number in a water body can never exceed
the number introduced into that body by waste disposal. Typi-
cally, viruses are much more resistant to external environmental
factors (chemical content, pH, temperature, time, etc.) and
survive longer than bacteria (257, 380). It was long suspected
that algae could inactivate viruses through some process because
of low virus concentrations in algae-rich waters. However, it
is now believed that the high pH and dissolved oxygen in the
vicinity of algal blooms are responsible for the inactivation.
211
-------
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212
-------
Virus inactivation in lake water is further enhanced by
the presence of proteolytic bacteria which degrade the
viral coat (564). Coxsackie is particularly susceptible to
proteolytic bacteria, while polio virus is generally resistant
except to Pseudomonas aeruginosa (564). Otherwise, the mechan-
isms of virus removal are obscure. Table 82 reports survival
times for various enteric viruses in fresh-water bodies.
Transport mechanisms for pathogens include physical current
motion, organism motility, adsorption, ingestion, and aerosoli-
zation. As most pathogens readily adsorb onto suspended matter,
sediment pathogen concentrations may greatly exceed water con-
centrations. Filter feeding organisms, such as fresh-water
shellfish, tend to concentrate pathogenic organisms. Conse-
quently, shellfish can be a major factor in the spreading of
certain communicable diseases.
213
-------
TABLE 82. SURVIVAL OF ENTERIC VIRUSES
IN WATER (11)
Temperature
Type of Water Virus
River water Coxsackie B-3
ECHO 5
Polio 1
Coxsackie B-3
ECHO 12
ECHO 7
Coxsackie A-9
Polio 2
Polio 3
ECHO 5
Coxsackie A-9
ECHO 12
Polio 1
Polio 1
ECHO 7
Polio 1
Polio 3
Polio 3
Coxsackie A-2
Coxsackie A-2
Coxsackie B-5
Coxsackie B
Impounded fresh Coxsackie B-3
water Polio 1
ECHO 7
ECHO 6
Coxsackie A-9
Polio 1
Coxsackie ?
ECHO 12
Polio ?
ECHO ?
ECHO ?
Polio ?
Polio ?
ECHO ?
4-6
75/3
7/0
7/1
7/1
19/3
15/3
10/3
75/3
30/3
60/3
20/3
33/3
19/3
60/3
26/3
27/3
50/3
67/3
-
-
-
18/2
7/1
7/1
22/3
5/3
6/3
27/3
18/3
14/3
21/3
23/3
21/3
52/3
52/3
42/3
15-16
(Range of
8/3
.5
-
.7
-
-
-
15/3
8/3
15/3
-
-
-
45/3
-
-
18/3
7/1
-
-
24/1
-
.7
.5
-
-
-
-
-
-
-
-
-
_
-
-
°C
20-25
Days)
2/3
3/3
3/3
3/3
5/3
7/3
8/3
8/3
8/3
8/3
8/3
12/3
13/3
16/3
16/3
20/3
-
.3 7/2.1
5/2
47/2
-
-
3/3
3/3
4/3
5/3
6/3
6/3
8/3
6/3
10/3
12/3
20/3
21/3
22/3
24/3
214
-------
SALINE WATER
INTRODUCTION
The ocean has traditionally been the depository for a
wide variety of civilization's wastes. Previously, the ocean
was considered an infinite sink that was not affected by
the waters discharged into it. Only recently has man
recognized that wastewater effluents and sludges can have
an adverse effect upon ocean waters.
Wastewater (treated and untreated) and wastewater sludges
are discharged directly to the ocean offshore through sub-
marine outfall pipelines. Beach outfalls are occasionally
used for wastewater discharge, although this usually results
in contamination of the beach. Sludges are also barged and
dumped into the open ocean.
The potential significance of a given discharge varies
with the characteristics of the discharge and of the receiving
waters. For example, discharges into a bay or estuary are
much less diluted than discharges into the open ocean. The
location of the outfall (e.g., on a shelf or near a submarine
canyon) strongly affects contaminant mobility. Seafood
obtained from open ocean areas is different from that harvested
from bays or estuaries. Shellfish, which are usually taken
from bays or estuaries, tend to concentrate contaminants to a
greater degree than does open ocean seafood. Furthermore,
the physico-chemical relationships affecting solubility and
mass transport of contaminants differ considerably for
estuaries and open ocean receiving waters.
Consequently, the fate of wastewater contaminants in
marine environments is highly site specific. For any given
site, an understanding of the potential pathways from the
effluent back to man requires knowledge of the dilution
achieved, discharge location hydraulics, chemical and physical
composition of both the effluent and receiving waters, com-
position and hydraulics of other contamination sources,
physical and chemical properties of the sediments and their
interactions with the water column, and an understanding of
the food web relationships. Food web relationships are per-
haps the most important element in terms of ultimate pathways
to man, and have received the most publicity in recent years.
Public health-impairing contaminants behave in somewhat
the same fashion in marine water as in fresh water. Therefore,
215
-------
concepts discussed extensively in the preceding fresh-water
section of this chapter will be mentioned only briefly here.
In general, wastewater contaminants in the ocean can return
to man via two pathways: ingestion of contaminated fish and
shellfish, or body contact and incidental ingestion associated
with marine aquatic sports.
Research concerning the disposal of sewage effluents and
sludges to marine water systems is abundant, as can be seen
in Table 83 . The volume of literature is somewhat deceptive,
however, in that most of these studies concentrate on one
aspect of a pollution problem in a specific area; comprehen-
sive generalizations are usually not possible. The most
nearly complete picture of the pathways and fates associated
with wastewater discharges comes from a study of the Southern
California coastal area by the Southern California Coastal
Water Research Project (SCCWRP), which began in 1969.
Figure 21 shows the study area, which encompasses approximately
400 m of coast and 20,000 km2 of water surface area. This
coastal area receives municipal wastewater, sludge, surface
runoff, and other discharges from a population of approxi-
mately 11 million people. The effluent volume from municipal
treatment systems alone is approximately one billion gpd, of
which 20 percent receives secondary treatment while 80 percent
receives only primary treatment (1544).
Because of the completeness of the research, much of the
following discussion relies heavily on the SCCWRP data.
However, this data is specific to the Southern California area,
which differs from other ocean areas; hence, the data must be
applied with caution.
WATER QUALITY PARAMETERS
Since saline water is not used for drinking water, there
are no potential direct health problems from marine water
quality parameters. However, as in fresh surface waters,
there are some indirect consequences from the introduction of
suspended solids and organic carbon into the marine environ-
ment. Trace metals, bacteria, viruses, and other hazardous
contaminants are often found in association with suspended
particulates. Researchers in Southern California have
determined that more than 90 percent of the possible pollutants
discharged through one sludge discharge pipeline are associated
with particulate matter (925).
Discharged organic matter can have a radical impact on
the local environment which, in turn, will affect the dis-
tribution, transport, and availability of other contaminants.
The oxidation of organic matter, particularly in bottom
sediments, severely depletes dissolved oxygen concentrations,
216
-------
TABLE 83 . LITERATURE REVIEWED
PERTAINING TO SALINE WATER
Contaminant Reference Number
Water Quality Parameters
Ammonia 61, 221, 264, 358, 829, 925, 1002, 1102,
1125, 1149, 1207, 1541
BOD 226, 338, 925, 979, 1002, 1102, 1207,
1268
COD 925, 1268
Chlorides 225, 1125
Fluorides 1451
Nitrates 61, 86, 221, 225, 264, 358, 829, 882,
883, 1002, 1125
Nitrites 61, 86, 221, 264, 358, 829, 1002, 1125
Oil and grease 61, 925, 1102, 1207, 1231
Phosphates 61, 86, 221, 264, 358, 829, 882, 883,
925, 1101 , 1102, 1207
Suspended 459, 499, 925, 1125, 1171, 1172, 1541
solids
Total dissolved 1125
sol ids
Total organic 225, 559, 720, 979, 1125, 1268
carbon
Other (general) 42, 226, 551, 552, 700, 828, 925, 1067,
1102, 1125, 1207, 1307, 1310, 1544
Elemental Contaminants
Aluminum 28, 436, 636, 720, 968, 1125, 1128, 1160,
1161, 1266, 1380, 1413, 1459
Antimony 303, 436, 636, 720, 1125, 1128, 1160,
1161, 1266, 1380, 1525
Arsenic 303, 636, 637, 720, 1128, 1160, 1161,
1207. 1266. 1339, 1380, 1525
217
-------
TABLE 83.(continued)
Contaminant Reference Number
Barium 28, 636, 968, 1128, 1160, 1161, 1266,
1339, 1380, 1459
Beryllium 636, 1128, 1161, 1266, 1339, 1380, 1459
Boron 28, 636, 1113, 1128, 1160, 1161, 1266,
1339, 1380, 1459, 1525
Cadmium 53, 75, 115, 157, 227, 303, 365, 441,
524, 558, 592, 636, 713, 720, 756, 828,
923, 925, 967, 968, 978, 1102, 1117,
1121, 1125, 1128, 1160, 1161, 1207, 1208,
1378, 1433, 1459, 1502, 1541, 1544, 1562
Chromium 53, 75, 157, 212, 227, 232, 365, 611,
632, 636, 700, 713, 720, 828, 923, 967,
969, 1102, 1121, 1125, 1128, 1137, 1160,
1207, 1208, 1266, 1306, 1307, 1380, 1433,
1459, 1528, 1541
Cobalt 75, 115, 157, 303, 365, 407, 445, 636,
713, 782, 828, 894, 923, 967, 968, 1044,
1102, 1117, 1121 , 1125, 1128, 1160, 1161 ,
1266, 1339, 1380, 1459, 1538, 1544
Copper 75, 115, 157, 227, 232, 305, 365, 407,
445, 611, 636, 713, 720, 782, 828, 844,
894, 923, 967, 968, 1044, 1066, 1102,
1121, 1125, 1128, 1137, 1159, 1160, 1161,
1171, 1207, 1208, 1259, 1266, 1339, 1380,
1433, 1459, 1538, 1541, 1543, 1544, 1562
Germanium 636, 1128, 1160, 1161, 1266, 1339, 1380
Iron 28, 75, 115, 227, 232, 365, 611, 636,
720, 782, 828, 844, 968, 1113, 1117,
1121, 1125, 1128, 1160, 1266, 1339, 1371,
1380, 1459, 1502, 1544, 1562
Lead 75, 115, 157, 227, 365, 407, 441, 462,
524, 558, 611, 636, 713, 720, 828, 923,
967, 968, 1060, 1066, 1102, 1117, 1121,
1128, 1161, 1171, 1207, 1208, 1266, 1307,
1339, 1363, 1380, 1433, 1459, 1544
218
-------
TABLE 83. (continued)
Contaminant Reference Number
Manganese 75, 227, 232, 365, 445, 611, 636, 713,
720, 828, 844, 923, 967, 1102, 1117, 1121,
1125, 1171 , 1433, 1459, 1502, 1538
Mercury 12, 37, 227, 303, 305, 365, 368, 452,
462, 524, 610, 620, 636, 637, 645, 654,
760, 780, 795, 809, 967, 968, 987, 988,
1102, 1125, 1128, 1145, 1160, 1161, 1207,
1208, 1266, 1295, 1339, 1380, 1413, 1433,
1502, 1503, 1526, 1527, 1543, 1544, 1562
Molybdenum 303, 636, 720, 828, 925, 1128, 1160, 1161,
1266, 1339, 1380, 1459
Nickel 75, 115, 232, 365, 445, 636, 713, 720,
782, 828, 923, 967, 968, 1102, 1117, 1121,
1125, 1128, 1160, 1161, 1171, 1207, 1208,
1266, 1339, 1380, 1459, 1541
Selenium 636, 1114, 1128, 1160, 1207, 1266, 1339,
1380, 1525
Thorium 636, 1128, 1160, 1161, 1266, 1339, 1380
Tin 636, 828, 923, 1128, 1160, 1161, 1266,
1339, 1380, 1459
Uranium 636, 1128, 1160, 1)61, 1266, 1339, 1380
Zinc 75, 115, 157, 175, 227, 232, 303, 305,
365, 407, 441, 445, 524, 592, 611, 636,
713, 720, 782, 828, 844, 923, 968, 1066,
1102, 1114, 1117, 1125, 1128, 1160, 1161,
1171, 1207, 1266, 1307, 1339, 1380, 1433,
1459, 1538, 1562
Other (general) 37, 42, 75, 157, 228, 636, 720, 893, 923,
967, 1161, 1207, 1307, 1339, 1380, 1454,
1460
Biocidal Contaminants
Aldrin 403, 1237, 1418
Arsenated 1237
hydrocarbons
219
-------
TABLE 83.(continued)
Contaminant Reference Number
Chlorinated 304, 324, 365, 605, 804, 827, 874, 893,
hydrocarbons 977, 998, 999, 1022, 1023, 1059, 1065,
1066, 1068, 1102, 1125, 1132, 1146, 1162,
1170, 1207, 1231, 1237, 1307, 1412, 1532,
1535, 1536, 1539, 1543
ODD 403, 1022, 1125
DDE 403, 977, 1125
DDT 17, 365, 403, 420, 605, 872, 874, 894,
977, 1022, 1023, 1059, 1125, 1170, 1207,
1307, 1418, 1532, 1535, 1536, 1539, 1542,
1543
Dieldrin 365, 605, 1125, 1155, 1237, 1418, 1536
Endrin 403, 1418
Herbicides 806, 1125, 1412
Organophosphorus 1196
pesticides
Soil sterilants 73
Other (general) 42, 130, 304, 478, 806, 827, 1049, 1102,
1125, 1407, 1454
Synthetic/Organic 42, 58, 149, 235, 300, 304, 318, 319,
Contaminants 365, 402, 653, 768, 770, 807, 808, 879,
893, 903, 1025, 1125, 1126, 1132, 1454,
1533, 1539, 1558, 1564
Biological Contaminants
Adeno virus 350
Bacteria 18, 44, 45, 74, 365, 569, 656, 674, 858,
929, 938, 987, 1047, 1200, 1202, 1307,
1345
Clostridium 858
we!chi
220
-------
TABLE 83.(continued)
Contaminant Reference Number
Coliforms 17, 18, 44, 61, 197, 253, 254, 304, 310,
311, 316, 338, 612, 613, 656, 674, 675,
677, 695, 705, 938, 973, 989, 1019, 1020,
1021, 1047, 1087, 1200, 1202, 1222, 1223,
1224, 1226, 1231, 1268, 1275, 1307, 1413
Coxsackie virus 11, 252, 564, 905
(A & B)
ECHO virus 252, 357, 905, 1515
Escherichia 929, 1275, 1306, 1307, 1443, 1515
col i
Fecal 197, 399, 612, 1202, 1275, 1307
streptococci
Listeria 989
monocytogens
Mycobacteriurn 1306
Parasitic worms 700
Polio virus 11, 252, 564, 905
Salmonella 1234, 1306, 1307
Shigella 1306
Staphylococcus 350, 1306, 1307
aureus
Vibrio cholerae 255, 1020, 1306, 1316
Virus 11, 251, 252, 255, 311, 365, 405, 465,
468, 695, 877, 905, 926, 938, 1273,
1306, 1307, 1316, 1317, 1515
Other (general) 250, 311, 433, 858, 1125
221
-------
35°N
34aN
33°N
32°N
DRAINAGE
DIVIDE
^
120eW
119°W
118°W
117"W
Figure 21,
The Southern California Bight. Outfall
systems are (1) Oxnard City, (2) Hyperion,
Los Angeles City, (3) Whites Point, Los
Angeles County, (4) Orange County, and
(5) San Diego City. (1544)
222
-------
leading to anaerobiosis and a reducing environment. In such
an environment most dissolved metals will precipitate as
sulfides. The presence of dissolved organics enriches the
local environment in nutrients and leads to increased
planktonic growth and overall biological activity. Fish and
crustacean populations may also increase. Since these regions
of high organic content may also be high in hazardous elemen-
tals and organics, the chances of these fish and crustaceans
becoming contaminated are higher than for normal ocean water
populations.
Another problem associated with water quality parameters
is floatable material. Floatables from wastewater generally
can be classified as oil and grease, and methylene blue active
substance (MBAS). Again, the hazard is not with these
materials but with associated contaminants. Bacteria have been
shown to concentrate in floatables (365). Although research
has been scanty, it is probable that viruses, heavy metals,
biocides, and synthetic organics will also concentrate in
floatable materials. These floatables can be carried along
the water surface to the shore by wind, current, and wave
activity. Once deposited along the beach, these contaminants
become readily accessible to both humans and insect/mammal
vectors. Wind and wave action can also agitate floatables
to the point where aerosol-type particulates are released.
These airborne particulates can likewise be high in hazardous
contami nants.
As in fresh water, the addition of nitrogen and phosphorus
species to marine water can result in biostimulation.
Natural seawater concentrations of phosphorus and nitrogen
range from 1 to 100 ppb and 10 to 700 ppb, respectively.
Discharges of nitrogen and phosphorus to open ocean waters
are seldom a problem, as the ocean can assimilate these
nutrients. Discharges into bays, however, can lead to
accumulations of nitrogen and phosphorus with subsequent
biostimulation. Copeland's study of St. Joseph Bay, Florida
(264), found phosphorus concentrations as high as 10 times the
normal and gross biostimulation as evidenced by massive algal
growths. These growths decreased the aesthetic appeal of the
affected water and drove away many food and sport fish.
Dissolved oxygen levels also decreased, and the bay exhibited
evidence of eutrophication.
ELEMENTAL CONTAMINANTS
Marine elemental chemistry is similar in many respects
to fresh-water elemental chemistry. The same physical and
chemical principles apply, but the marine system is somewhat
more complex. Descriptions of the principles of solution,
precipitation, adsorption, etc., given in the fresh-water
223
-------
section of this report will not be repeated. Whenever the
complexities of the marine system Introduce modifications 1n
principles already discussed, these will be mentioned. In
general, however, this discussion will be limited to a simple
description of some of the Important components of the marine
system and their Interactions, with little mention of the
underlying principles.
The concentrations of elemental contaminants entering the
marine system via sewage effluent or sludge vary widely depend-
ing on the source of the effluent or sludge (Table 84 ).
Recent research has shown that 50 to 90 percent of these
elemental contaminants are associated with the particulate
fraction of the discharge (558, 967). Analyses of sediments
around outfalls seem to indicate that this elemental/sewage
particulate association does not last long in seawater,
although the mechanism of release is not well understood.
Among the possible explanations are:
• Oxidation of element-containing organic
particulates with subsequent release of the
element
• Oxidation of particulate element sulfides
• Surface desorption caused by high dilution ratios
_2
t Complexation with inorganic ligands such as C£
• Complexation with organic ligands possibly
resulting from the oxidation, of organic particulates.
The behavior of the elemental contaminants after their
release from the sewage particulates is scarcely better under-
stood. Table 85 presents the average natural marine concen-
trations and principal dissolved species for several of these
elements. It should be noted that these principal species
were probably identified in open ocean waters; dissolved
elementals may take different forms in coastal waters.
Furthermore the chemistry of the sewage-rich ocean waters near
an outfall can be radically different from the chemistry of
the open ocean.
Sewage-borne elemental contaminants are concentrated and
generally associated with suspended matter. At sludge outfalls
reducing conditions that prevail may lead to the formation of
insoluble sulfide compounds. The organics in the sewage can
lead to a reducing or only moderately oxidizing environment
where many metals -- such as zinc, lead, cobalt, cadmium, and
copper -- form insoluble carbonate compounds. Chromium
224
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225
-------
TABLE 85 . CONCENTRATION OF SELECTED ELEMENTS
IN MARINE WATER (1128)
Element
Aluminum
Antimony
Arsenic
Barium
Beryl 1 ium
Boron
Cadmium
Chromium
Cobalt
Copper
Germanium
Iron
Lead
Manganese
Mercury
Molybdenum
Nickel
Sel eni urn
Thorium
Tin
Uraniurp
Zinc
Concentrati on
(VQ/t)
1
0.3
2.6
20
6 x 10"4
4.5 x 103
0.1
0.5
0.4
3
0.07
3
0.03
2
0.2
10
7
0.09
<5 x 10"4
0.8
3
10
Principal Dissolved
Species
Al(OH)^3~y) • (H90)n
y 2 ' n
HAsOl , H9AsO«
+ 9
8a z
B(OH)3, B(OH)4
Cd+2, cdOH+, CdCl+
0 +^
CrO^, Cr °
Co + 2
Cu+2, Cu(OH)2
Ge(OH)4
+ +2
PbCl3> PbCl , Pb *
Mn + 2
HgCl42, HgCl2
Mo042
Ni+2, NiOH+, NiCl+
SeO^2
Th(OH)4
U02(C03)34
Zn + 2
226
-------
which is predominantly trivalent in sewage (632), forms in-
soluble hydroxides and oxides.
Morel et al. (967) and Hendricks (558) indicated that
less than 10 percent of the particulate elements settle
in the immediate outfall area. Rather they are carried away
by current action, and the dilution and oxidation potential
are increased significantly. When thus spread and diluted,
many of the precipitates formed near the outfalls will
dissolve, e.g., sulfides will oxidize to soluble sulfates,
and carbonate compounds will dissolve due to the action of
competing ligands.
Once in solution in open water, dissolved elements
are subject to a wide variety of competing mechanisms that
determine whether a given elemental remains in solution or
is removed. In highly dilute, oxygenated seawater, most
elements are in solution as:
• Cations: Ba+2, C0+2, Cu+2, Ni+2
• Oxo anions: HAs04"2 , Cr04"2, Se04"2, Mo04~2
• Chloride complexes: CdCl+, PbClg", HgCl4"2, NiCl+
• Hydroxyl complexes: B(OH)3, B(OH)4§ Cu(OH)2
• Carbonate complexes: L^KO.,).," .
Iron and manganese are major exceptions to the solubility
rules; both are more soluble in their lower valence states,
and as a result, are mobilized in reduced sediments and enter
solution as the divalent cations.
When divalent iron and manganese migrate to more highly
oxygenated waters, they oxidize to form insoluble hydrous
oxides that precipitate. These hydrous oxide particulates
have a high affinity for other ions and act somewhat as
scavengers. They are particularly effective at adsorbing
cobalt, nickel, cadmium, zinc, silver, selenium, and lead
but will also remove some chromium, copper, uranium, and
molybdenum.
If these hydrous iron and manganese oxides settle into
reducing sediments, the iron and manganese are again released
into solution. The accompanying ions, however, are usually
locked into the sediments as the extremely low solubility
carbonate or sulfide compound.
If these hydrous oxides settle into oxidizing sediments,
the adsorbed ions generally become incorporated into the
227
-------
precipitate. The iron and manganese oxides accrete to form
the ferro-manganese nodules that cover much of the ocean floor.
These nodules are invariably enriched in lead, cobalt, nickel,
zinc, cadmium, etc. A major exception to this behavior is
chromium, which is often carried with the hydrous oxides as
the Cr(III) oxide. The redox conditions around the iron/
manganese minerals are such, however, that the Cr(III) is
oxidized to the highly soluble Cr(VI), which is then released
back into solution. Most of the elementals, once they become
incorporated into the sediments, are effectively locked
away from further reaction with the seawater, barring bio-
logical activity or a major change in redox potential (Table
86 )•
Biological activity also plays an important role in the
transport of elemental contaminants. Biologically related
mechanisms take several forms: uptake and biomagnification
by organisms, biological transformation, sedimentation
associated with dead organisms or fecal matter, and complexes
with biologically related organic ligands.
Generally, elemental contaminants become a sociated with
marine organisms via one of several pathways. Some trace
metals (e.g., cobalt, iron, copper, zinc) can be incorporated
directly into metabolic pathways. Other trace metals
(notably mercury) exhibit 1ipid-preferential solubilities
whereby they concentrate in the fatty cells of small organisms,
the gill tissues of fish, or the digestive organs of filter
feeders. Metals can adsorb onto the surface of plankton
or can be transferred to higher marine organisms (and ul-
timately to terrestrial organisms and man) via ingestion of
contaminated food organisms. Two other pathways, bioaccumula-
tion and biomagnification, are discussed in more detail in
the "Pathways to Man" section of this report, under "Fish"
and "Shellfish."
Incorporated elemental contaminants can be returned to
the sediments in fecal material or in dead organisms. If
this occurs in a biologically active area, the elementals
can be ingested or sorbed by other organisms or simply re-
leased again to solution; otherwise they will probably be
incorporated into the sediments. Sediment elementals (whether
there by chemical or biological means) are subject to
ingestion by bottom feeders or transformation by sediment
bacteria. Biotransformation is probably an important trans-
port mechanism. For example, inorganic mercury and its
compounds, chemically immobile in sediments, are readily
absorbed by many bacteria. These bacteria, possibly via a
detoxification mechanism, convert the inorganic mercury to a
organomercurial. The organomercurial, usually methyl mercury,
is far more mobile than its inorganic counterpart. It is
228
-------
TABLE 86 . NATURAL TRACE METAL CONCENTRATIONS (MG/DRY KG)
AS REPORTED FOR SURFACE SEDIMENTS FROM SEVERAL
PARTS OF THE WORLD OCEAN (365)
Trace
Metal
Silver
Cadmium
Cobalt
Chromium
Copper
Iron
Mercury
Manganese
Nickel
Lead
Zinc
So.
Calif.8
1.0
0.4
7
46
16
2.5%
0.06
320
14
8
63
Other
Nearshore
2f
59
309
7h, 481
1-5%J>
0.04k
580f
15h, 551'
15h, 201
951'
Organic
Rich Cont. Pacific
Shelfb Basins0
4-195
4-93
18-129 82-686
0.4-5.5%
0.09-0.86
42-1,075
35-455
3-32
18-337
Manga-
nese d
Nodules
3,000
5,000
14%
19%
4,000
1,000
400
Outfall
Max.8
21
79
11
1,000
670
3.7%
4
380
45
490
2,400
Averages of natural values at the five major sewage outfalls in the
Bight. However, mercury value is estimated natural subsurface con-
centration in Santa Barbara Basin.
Organic-rich diatomaceous muds, S.W. Africa shelf.
c Sample No. 21-29, Pacific Ocean Basins.
Average composition of ferromanganese minerals from the Pacific Ocean.
6 Maximum surface sediment concentration measured off Palos Verdes
Peninsula sewage outfalls.
Caribbean sediment, Station 50.
9 Japanese Island sediments,
Gulf of Paria, Caribbean sediments.
Atlantic nearshore sediments.
Gulf of Paria, Caribbean sediments.
Washington Shelf, N.E. Pacific.
229
-------
easily released into the water column and is even more lipid
preferential than inorganic mercury. Only mercury sulfide
compounds and mercury bound to organic sulfhydryl groups are
relatively unaffected by bacteria. This type of behavior has
also been postulated, or demonstrated in the laboratory, for
arsenic, selenium, antimony, lead, cadmium, and other
elementals.
Organic ligands from decaying organisms or excretory pro-
ducts also may play a role in the solubility of many elements.
Examples are the copper-heme, iron-heme, and cobal t- vi tami n B-,~
complexes. All are natural complexes and are extremely
stable in marine environments. Several metals, such as mercury
and nickel, show a high affinity for organic ligands and
particulates. These element-organic ligand complexes will
stay in solution until the organic nqand decays, the complex
is ingested or sorbed, or the elements can form a more stable
compound.
The ocean as a whole is in a relatively steady state or
equilibrium condition, i.e., the rate of input of natural
materials roughly equals the rate of sedimentation. Conse-
quently, the concentrations of most elemental contaminants
in seawater are constant. Generally speaking, those elements
present in highest concentrations are the least reactive and
least likely to sediment. The converse is equally true.
Moreover, the elements considered hazardous to man are among
those present at extremely low concentrations. Therefore,
it is difficult to see how man's additions can have a serious
impact on the levels of these contaminants in seawater. Of
course, man has been adding these metals to seawater for
decades; but, as was just mentioned, these metals are among
the most reactive and most likely to precipitate. The
cations, an ions, and ligands most responsible for this pre-
cipitation are present in excess and are much more readily
replenished than are the more hazardous elements. Conse-
quently man's additions can be removed relatively rapidly
without seriously affecting marine equilibrium.
While this may sound comforting, it does not take into
account the fact that sludge and wastewater disposal occurs
in coastal waters where exchange with open ocean waters may
be limited. Ocean waters form an open, steady-state system;
coastal waters form a partially closed system that is subject
to varying inputs from the land. Thus coastal waters are
the most biologically active of the ocean's areas; conse-
quently, they a^e far more readily upset by wastewater addi-
tions than ;s t'*e o-.,ean as a whole.
It would u. i- e < ~: r ?", e 1 y useful to be able to describe the
relative impact d'ffcrent wastewater element concentrations
230
-------
would have on coastal equilibrium models. Unfortunately,
as discussed earlier in this section, there is a distinct
lack of uniformity among various coastal regions that makes
the task virtually impossible. Even the SCCWRP (the most
complete characterization of a specific region) does not
adequately address the problem of the diverse effects of
different wastewater levels. Suffice it to say that, in
general, wastewater disposal in coastal waters will increase
the concentrations of elements in the water, sediments, and
marine organisms.
BIOCIDAL CONTAMINANTS
The behavior of the biocidal contaminants in marine
water systems is largely the same as in fresh-water systems.
The mechanisms of microbial and chemical degradation, photo-
degradation, sediment and particulate adsorption, volatiliza-
tion, and biological uptake are physically the same. The most
important difference is the reduced solubility of many of the
biocides in the more highly ionic seawater. This will lead
either to increased sedimentation or increased concentration
in surface films, depending on the density of the particular
b i o c i d e .
Biocides in marine systems have not been studied as
extensively as biocides in fresh-water systems. Most of
the research on the former is concerned with uptake by or
effects on aquatic life. Little has been done to characterize
the physico-chemical transport and removal mechanisms active
in seawater. Furthermore, what research has been conducted
has been limited largely to DDT.
Table 87 lists the reported concentrations of DDT,
PCB, and dieldrin in selected effluents and sludges dis-
charged to the ocean off Southern California. These effluents
contain both domestic and industrial sewage and, in some
cases, are not treated beyond advanced primary treatment.
The chlorinated hydrocarbons are not metabolized to
any extent in seawater, polluted estuaries, or bottom sedi-
ments (1059). Rather the bottom sediments, particularly those
near the outfalls, act as a sink where these biocides may
persist for years and even decades (874).
Suspended or dissolved chlorinated hydrocarbons are
subject to uptake by algae. A number of researchers have
determined that algae are extremely efficient accumulators
of these biocides and thei*- residues (804, 1155, 1418). The
algae do not degrade the biocides but store them. The
biocides can be released if the algae are placed in clean
seawater. Otherwise, the algae retain the biocides until the
231
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algae are either eaten or die. in which case the biocides
will sediment with the decaying organic matter.
Chlorinated hydrocarbons in surface films are subject
to photodegradation, but even this may be more of a problem
than a solution. For instance, Rogers and Landreth (1170)
demonstrated that DDT could photodegrade to PCB's.
Although the sediments act as a sink for many biocides,
they do not permanently remove them from the environment.
On the contrary, contaminated sediments will act as a source
for the biocides long after major reductions have been made
in the dominant inputs. Bottom-feeding fish placed in an
otherwise clean environment (clean seawater with no biocide
inputs but with contaminated sediments) soon show significant
increases in tissue biocide content (1539). This problem
is limited largely to PCB's and the persistent chlorinated
hydrocarbons. Carbamates, organophosphates, and ionic
biocides all hydrolize rapidly in seawater, with half-lives
of hours or days, seldom exceeding a few weeks.
SYNTHETIC/ORGANIC CONTAMINANTS
Most of the research conducted to date on organic con-
taminants in the marine environment has been concerned with
PCB's and the petroleum hydrocarbons associated with oil
spills. Little has been done to determine the environmental
fate of the plethora of other synthetic organic compounds
released to the ocean. Because of the nonpotability of
seawater, little concern has been expressed regarding the
fate of the synthetic/organic compounds therein. The lipid
solubility of some of these compounds, however, suggests
that some research is in order, though the sheer number of
compounds may discourage meaningful research.
Polychlorinated biphenyls are one group of synthetic/
organic contaminants that has been studied in depth. PCB's
are highly insoluble in seawater, adsorb rapidly and strongly
onto suspended matter, and concentrate in surface oil slicks
or sediment. Adsorbed PCB's will ultimately diffuse into the
sediments, while those PCB's concentrated on the surface
photodegrade to lower isomers that hydrolize relatively
easily (1132).
The research on petroleum hydrocarbons is only partially
useful. Municipal wastewater ranks low among marine petroleum
hydrocarbon sources; natural seeps, oil spills, aerial fall-
out, industrial discharge, and deliberate dumping all con-
tribute more petroleum hydrocarbons to the sea. However, as
the behavior of many organic compounds in seawater is similar,
theoretical pathways can be suggested.
233
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In general, any organic compound that can occur naturally,
can be metabolized and effectively removed from solution.
Totally synthetic compounds may or may not be metabolized,
but those structurally similar to natural compounds are more
amenable to microbial attack than those with no natural analogs.
Increasing substitution, particularly with halogens, increases
resistance to biodegradation.
Most organic compounds are degradable via photolytic
oxidation or chemical attack. In some cases, e.g., plastics
or chlorinated hydrocarbons, half-lives of years are not
unusual. Most organic compounds, however, degrade more
quickly; half-lives of hours to perhaps a few weeks are more
common.
Chemical degradation may take the form of hydrolysis or
reaction with another chemical species in the water. Hydroly-
sis is a reaction with water and usually consists of adding
a hydroxyl group or breaking an ester-type linkage. The
number of chemical reactions possible are almost limitless.
Furthermore, there is no guarantee that reaction or hydroly-
sis products will be any less harmful or more biodegradable
than the parent compound. For instance, azo dyes are readily
attacked by hydrogen sulfide to give carcinogenic, non-
biodegradable benzidines (1126).
Photodegradation is limited to surface films, as
ultraviolet radiation will not penetrate beyond a few
centimeters. Consequently those organic compounds dissolved
in surface films, adsorbed onto floatables, or less dense than
water are most amenable to photolysis.
Again, in general, municipal effluents are not responsible
for most organic contaminants in the oceans. Furthermore,
most organics discharged in such effluents, if not degraded,
remain in the general vicinity of the outfall. Also, the
wide variety and small quantities of most organic contaminants
make it unlikely that any one will become a hazard in recrea-
tional waters or food organisms. Unfortunately this does not
take into account possible synergistic effects of contaminant
combinations nor the postulated zero threshhold value for
some carcinogens.
BIOLOGICAL CONTAMINANTS
Both untreated and partially treated wastewater and
sludge are carriers of a variety of pathogenic organisms.
Furthermore, since sewage destined for ocean disposal is
often given minimal treatment, pathogen concentrations in
effluents and sludges can be extremely high (44).
234
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There are five principal types of human pathogens, and
many of the disease-producing organisms therein can be trans-
mitted via water routes. The five types and some of the more
prevalent waterborne diseases are:
• Protozoa (amebiasis, balantidiasis)
• Nematodes (angiostrongyliasis )
• Platyhelminths (clonorchiasis)
t Viruses (viral hepatitis, viral meningitis,
viral respiratory diseases)
t Bacteria (coliform diarrhea, cholera, 1eptospirosis ,
salmonellosis, shigellosis, typhoid fever)
There has been little research on the behavior of
pathogenic protozoa, nematodes, and platyhelminths in marine
systems. They are not as prevalent in industrialized
societies nor generally as serious from a public health stand-
point. Furthermore, they are largely host specific with few
marine hosts and usually a problem only in fresh-water systems.
Bacteria and viruses are much better represented in the
literature. Both are virtually ubiquitous, and the diseases
they cause are more prevalent with more serious outbreaks.
A number of researchers have attempted to assess the fate of
these human pathogens in the marine environment. Unfortunately,
many of the studies have been done in the laboratory with
simulated seawater, and the results may not always be appli-
cable to real systems. At best, these laboratory studies can
only evaluate one or two factors, so the effects of factor
combinations and synergisms must remain largely a mystery.
Consequently, those factors primarily responsible for pathogen
die-off or transport in the sea have not been isolated
definitively. Table 88 presents reported marine survival
times for viruses and selected bacteria.
The greatest proportion of pathogenic bacteria in
municipal effluent is associated with particulate matter (44).
As a result, ordinary sedimentation accounts for the initial
removal of many bacteria. However, some bottom-feeding fish
and shellfish can accumulate bacteria (e.g., Clostridium
perfringens ) and provide favorable living condi ti bris ("8 58).
Consumption of raw or partially cooked seafood taken near
outfalls then becomes a problem.
Bacterial populations can increase near outfalls as
well. The relatively higher nutrient content of the water
near an outfall provides a much better growth media than does
normal seawater, with a resulting increase in bacterial
235
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TABLE 88 . BIOLOGICAL SURVIVAL' TIMES (DAYS)
IN MARINE ENVIRONMENTS
Vi ruses
Viruses
Viruses
Salmonel la
E. Coll
2-130
<28-130
15-88
>25
58-69
>25
> 4
75
Source
468
905
11
1307
1234
1307
929
1306
populations (1200, 1515). In general, though, normal seawater
Is considered bacterlostatlc, and d1e-offs rather than pop-
ulation Increases prevail in most of the ocean. These die-
offs are attributable to a variety of factors, including:
• Sensitivity of many bacteria to oceanic extremes
of pH and temperature (365, 674);
• Severe disruption of normal osmotic cell balance
due to marine salinities (365);
• Bacteriostatic effects of solar radiation on
any organisms near the surface (365);
• Bacterial predators flourishing near outfalls
(365, 929);
• Secretion by marine plankton of a fairly potent
antibiotic (44, 45); and
• Normal seawater nutrient levels that are too low
to support bacterial growth (345, 1200, 1515).
Consequently, bacterial die-off is generally rapid away
from the influence of the outfall, except for those bacteria
that may be ingested by fish or shellfish.
Bacterial populations will stay high in areas where
effluent discharges are continuous, particularly if there is
little current mixing. As a result, many bays and estuaries
can exhibit pathogen concentrations far beyond normal expecta-
tions, and recreational use of the water may become hazardous.
236
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Pathogenic bacteria tend to concentrate In surface films
and floatables. Aubert et al. (44) found concurrent coliform
concentrations of <1/100 ml in the water, 3 to 300/100 m£ in
surface films, and 3,500 to 21,000/particulate in floatables.
This raises the possibilities of aerosolization of bacteria
or surface transport of bacteria to recreational beach areas.
Viruses are far more resistant to seawater than are
bacteria. The relative time required for 90 percent inactiva-
tion of viruses in seawater has been estimated to be three to
six times that for coliform bacteria. Water temperature seems
to be the most important factor in virus inactivation; water
temperatures of 25°C and lower yield survival times in months
(252). Studies in warm waters, such as off Tel Aviv, have
shown 90 percent inactivation in less than 48 hr (365). Die-
off times are also largely virus specific, with several
studies showing that coxsackie survives best, followed by
ECHO virus and then polio virus (252, 905).
Although the viruses survive longer than do bacteria,
they do not have the tendency to increase in population as
do bacteria (1515). Viruses require living hosts to replicate
and are very host specific. Human viruses generally do not
reproduce in nonhuman hosts.
Viruses can, however, accumulate in marine organisms.
Fish and shellfish can ingest viruses and essentially store
them. Viruses survive quite well in a variety of shellfish
without harming their hosts (365, 905). Viruses can also com-
centrate on particulates and floatables with the same con-
sequences as for bacteria.
237
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LAND/GROUNDWATER
INTRODUCTION
Wastewater treatment sludges have traditionally been
disposed to land, and wastewater effluents are also increas-
ingly being disposed to land. Land disposal of sludges and
effluents, if improperly managed, can result in a potential
public health hazard. This hazard can be brought about
directly through surface contamination of food crops, or
indirectly through contamination of groundwater supplies,
consumption of livestock fed with contaminated crops, and
surface runoff affecting water supplies, aquatic life, or
bodies of water used for recreational activities. Aerosols
from spray application of effluents and/or direct vaporiza-
tion of volatile contaminants may also pose a direct or
indirect threat to human health. The major potential prob-
lem is the contamination of groundwater resources, which sup-
ply a significant percentage of domestic water consumption
in the United States.
Many variables affect the potential for a public health
hazard from land disposal. These include:
• The characteristics of the sludge or wastewater
di sposed
t The rate of waste application
• The hydrogeological characteristics of the disposal
site
• The method of disposal, e.g., crop irrigation, land
spreading, percolation ponds, sanitary landfill, etc.
• Proximity of public access
• Utilization of groundwater, crops, etc., potentially
affected
• Local climate.
The above listed variables are not mutually exclusive;
they interact in many ways to influence the rate and extent of
transport of contaminants from each source and to influence the
importance of each potential pathway. It is beyond the scope
of this report to delve deeply into the science of waste land
238
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application technology. This subject is being researched heavily
by the EPA and other agencies to establish guidelines for the
safe land disposal of effluents and sludges. This report will,
however, discuss the current knowledge about potential public
health problems.
Literature reviewed concerning wastewater and sludge
disposal to land (tabulated in Table 89) has centered on ground-
water elemental and biological contaminants, and water quality
parameters providing plant nutrients, such as nitrogen and
phosphorus forms. The increased use of wastewater application
to land has created a need for increased research into the
dynamics of wastewater contaminants in soil systems. It is
necessary to study the capabilities of these systems to destroy,
neutralize, remove, concentrate, or otherwise affect applied
wastewater contaminants.
A number of factors determine the degree to which ground-
water may be contaminated by wastewater or sludge that is
applied to land. Depth to the groundwater table and distance
to an extraction point affect residual levels of phosphorus,
bacteria, and other constituents for which removal appears to
be a function of travel distance. Soil characteristics, native
groundwater quality, assimilation capacity of the aquifer, and
method of waste application also determine groundwater degrada-
tion and consequent health problems (1214). Cation exchange
and adsorptive capacities important in the removal of metal ions
and viruses, and of trace organics and solids, respectively are
determined by soil composition. Porosity regulates infiltration
rates to some extent, affecting contaminant residence time in
surface layers. Residence time may, in turn, determine aerobic
or anaerobic conditions.
Total groundwater volume cannot necessarily be considered
an effective diluting agent. Uniform diffusion of recharged
water cannot be guaranteed, and water quality may vary consider-
ably both in area and in depth.
WATER QUALITY PARAMETERS
Research in this area has been principally concerned with
nitrogen and phosphorus forms entering groundwater as a result
of land application of wastewater and sludge. Removal of
suspended solids from wastewater effluent has also received
attenti on.
The problems and transformations associated with nitrogen
forms in soils are relatively well known. Organic nitrogen
and ammonia, when applied to soils under normal aerobic condi-
tions, are rapidly converted by nitrifying bacteria to nitrite
and nitrate. Both of these anionic forms move through soils in
239
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TABLE 89. LITERATURE REVIEWED PERTAINING
TO LAND/GROUNDWATER
Contaminant
Reference Number
Water Quality Parameters
Ammonia
BOD
COD
Chiorides
Fluorides
Ni trates
Ni tri tes
Phosphates
Suspended solids
Total dissolved
solids
Total organic
carbon
Other (general )
Elemental Contaminants
Aluminum
Arsenic
Boron
Cadmi urn
26, 47, 134, 218, 377, 479, 704, 705,
755, 1118, 1214, 1323, 1328, 1484
26, 134, 1140, 1215, 1233
26, 134, 1148, 1214, 1484
26, 47, 352, 1018, 1215, 1419, 1440,
1484
134, 1119, 1173
26, 47, 134, 218, 272, 377, 479, 690,
704, 705, 776, 798, 1118, 1119, 1167,
1214, 1233, 1323, 1328, 1419, 1440,
1484
47, 218, 479, 705, 798, 1118, 1119,
1284, 1432, 1484
47, 68, 134, 352, 595, 690, 755, 1214,
1299, 1419, 1484
47, 84, 134, 352, 415, 1140, 1214,
1215, 1233, 1388
26, 134, 352, 1215, 1304, 1323
134
106, 169, 393, 916
378, 634, 776, 1108, 1323
1323, 1419
134, 378, 736, 797, 1007, 1024,
1327, 1484
134, 401, 690, 776, 1323
240
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TABLE 89 (continued)
Contaminant
Reference Number
Chromium
Cobalt
Copper
Iron
Lead
Manganese
Mercury
Nickel
Selenium
Zinc
Other (general )
Biocidal Contaminants
Chlorinated
hydrocarbons
DDT
Dieldrin
Herbicides
Other (general)
Synthetic/Organic
Contaminants
Biological Contaminants
Bacteria
776, 1419
634, 776
134, 378, 401, 634, 690, 736, 776,
797, 1007, 1024, 1323, 1327, 1495
26, 47, 634, 736, 776, 782, 797, 939,
1007, 1024,.1214, 1285, 1323i 1327
39, 134, 634, 776, 782, 1323
378, 634, 736, 776, 782, 797, 1007,
1024, 1323, 1327
128, 134, 401
396, 401, 634, 690, 798, 1141, 1423
1323
134, 378, 634, 690, 736, 776, 797,
1007, 1024, 1323, 1327
634, 661, 690, 1173, 1284, 1440
401
401
401
1014, 1417, 1474
1173, 1323, 1326
934, 1384
428, 619, 860, 892, 1105, 1175, 1210,
1304, 1323, 1388, 1419
241
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TABLE 89. (continued)
Contaminant Reference Number
Conforms 47, 134, 155, 401, 776, 917, 1129,
1140, 1175, 1215, 1233, 1323, 1440,
1484
Coxsackie virus 322
(A&B)
Fecal 1210
streptococci
Parasitic worms 1323
Polio virus 322, 774
Protozoa 428, 1304, 1323
Salmonella 401, 1083, 1323, 1440
Virus 134, 322, 352, 428, 892, 1083, 1175,
1210, 1215, 1304, 1323, 1479, 1548
Other (general) 619, 776, 917
percolating water with little difficulty. Under anaerobic soil
conditions, on the other hand, the process of conversion to
nitrite and nitrate is inhibited. Ammonium ions and free
ammonia persist and are held near the soil surface by adsorption
onto soil particles, by cation exchange reactions, or by fixation
in clay lattices.
In an acidic environment, nitrite has been found to react
with secondary amines to produce nitrosamines. These compounds
have recently been labeled carcinogenic, teratogenic, and
mutagenic. The health hazards associated with nitrite and
other forms of nitrogen in drinking water and crops have been
delineated by the U.S. Department of Agriculture (1432).
The most definitive study of nitrogen removal by land
application of wastewater effluent was conducted by Bouwer, et al.
at Flushing Meadows, Arizona (134). They found that short flooding
periods (two days flooding followed by five days drying) did not
provide sufficient time to develop the anaerobic conditions for
nitrate denitrification. A longer flooding period of ten days
followed by two weeks of drying proved to be more favorable.
242
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With this schedule, oxygen in the soil was depleted during
flooding, causing nitrogen (in the ammonium form) to be adsorbed
by the clay and organic particles. Flooding was stopped before
the cation exchange complex in the soil was saturated with
ammonium. Upon drying, oxygen entered the soil, and ammonium was
nitrified under aerobic conditions to nitrate. Concurrently,
some of the nitrate formed was denitrified - in micro-anaerobic
pockets in the otherwise aerobic upper soil zone - to nitrogen
gas that escaped to the atmosphere. When flooding was resumed,
if the basins were immediately flooded to a depth above 1 ft,
the nitrates were quickly leached out of the top few feet of
the soil to groundwater. However, if initial flooding was
shallow (a few inches deep), the lower head allowed a low infil-
tration rate, a larger nitrate retention time in the micro-
biologically active soil zone, and further denitrification. At
these lower initial hydraulic loading rates, nitrogen removals
were as high as 80 percent. If high application rates were
consistently maintained, nitrogen removal was only 30 percent
with a peak nitrate surge to the groundwater after the start of
each new flooding cycle.
A study by Preul (1119) in 1966 provided the following
observations of the movement and conversion of nitrogen in soil
and the potential dangers of nitrate contamination:
1. Biological oxidation is the dominant mechanism
affecting ammonia nitrogen as it passes through
the soil. This action initially occurs at a high
rate and to a large extent within several feet of
the point of release of the septic tank effluent,
if soil conditions are well aerated.
2. Nitrate contamination of groundwaters is a serious
threat from shallow soil adsorption systems. High
concentrations of ammonia nitrogen in septic tank
effluents are quickly nitrified to high concentra-
tions of nitrate, which pollute the groundwater.
Dilution from groundwater or soil moisture and
possibly denitrification aid in the deterrence of
nitrate.
3. The effectiveness of adsorption in deterring the
travel of nitrogen is limited because of the
rapid conversion of ammonia to nitrate. Laboratory
experiments have shown that ammonium can be readily
removed in soil by adsorption but, under aerated
soil circumstances, nitrification of these ions
occurs before the flow can contact a sufficiently
effective volume of soil.
243
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Similarly, results of a study by Chapman et al. (218) have
shown that, in Texas, irrigation with a sewage effluent was a
potential source of nitrate pollution of the local groundwater.
The results indicated that nitrification of ammonia nitrogen
in the effluent is rapid and complete, taking place within the
top 3 ft of soil. It was concluded that substantial amounts
of nitrate would not be fixed by the soil and that, at a 3-in
per week application rate, appreciable amounts of high nitrate
water would percolate to the groundwater. Selective crop
production of grains and grasses having high nitrogen uptakes
(corn, bermuda grass, oats) was deemed the most effective method
of protecting the groundwater.
Short daily flooding schedu
efficient nitrification to nitra
reported data from test basins i
Rio Hondo spreading grounds near
basins, equipped to collect wate
received treated wastewaters on
period of flooding and a longer
ensured completely aerobic condi
almost all the nitrogen had been
at depths of 8 ft.
les evidently result in highly
te. McMichael and McKee (892)
n the Whittier Narrows and the
Los Angeles, California. These
r at 2-, 4-, 6-, and 8-ft depths,
a daily basis using a short
period of drying. This cycle
tions. Studies indicated that
converted to the nitrate form
Intermittent and continuous spreading of secondary effluent
at the aforementioned Hyperion Treatment Plant (1233) resulted
in the nitrogen transformations shown in Table 90 .
TABLE 90 . NITROGEN TRANSFORMATIONS RESULTING FROM
DIFFERENT SPREADING TECHNIQUES (1233)
I.
Under continuous
spreading:
Effluent applied
Organic-N Ammonia-N Nitrate-N
7.1-8.5 15.5-17.5 0.2- 0.8
II.
Percolate from 7-10 ft
below ground (mg/£)
Under intermittent
spreading:
Effluent applied
1.2-2.7
8.7-18.5 5.2-18.1
Organic-N Ammonia-N Nitrate-N
2.3-3.6 4.9-27.9 0.1-14.2
Percolate from 7-10 ft
below ground (mg/£)
1.1-2.1
0.0- 0.7 8.4-22.4
244
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As can be seen from this table, intermittent spreading
techniques maintained aerobic conditions in the soil, making
possible the oxidation of ammonia and organic nitrogen to nitrate.
Under continuous spreading, anaerobic conditions prevailed, and
ammonia was still present in significant concentrations at a
7- to 10-ft depth.
When a low-rate application system is used, the amount of
nitrogen applied to soil with sewage effluent is not much more
than can be removed by crops, according to Bouwer (133). A low-
rate system involving application to wheat at 2.5 and 5 cm/week
was cited. At the lower application rate, 92 percent of the
nitrogen in the wastewater was removed in the soil, while at the
5 cm/week rate, 60 percent was removed. On the other hand, when
animal waste slurries or other wastewater with a relatively high
nitrogen content are applied, the amount of nitrogen supplied
may far exceed that which can be utilized by crops. To obtain
significant nitrogen removal under these circumstances, Bouwer
suggests that the system be designed to stimulate denitrification
in the soil. He cites an instance where this was done by instal-
ling an artificial barrier to water movement at a depth of 2 m,
causing the formation of an anaerobic region. Ammonia and organic
nitrogen in applied wastewater were converted to nitrate in the
upper, aerobic region of the soil, which was then denitrified
in the lower, anaerobic zone. The system removed 96 to 99 percent
of the total nitrogen applied at rates of 1 to 2 cm/day.
A study (1233) conducted at the sewage farm in Arroyo Grande,
California, indicated the pulse like effect of intermittent
spreading on the nitrate level in the percolate. During weekly
flooding of the field with settled sewage effluent, the upper
foot of the soil adsorbed 2,840 Ib of organic and ammonia nitro-
gen/ac. As the fields drained and were exposed to oxygen, this
adsorbed nitrogen was rapidly converted to nitrate, resulting
in nitrate levels of 1,000 to 2,000 mq/t in the soil solution
of the top foot. Consequently, the subsurface drainage water
exhibited pulses of high nitrate concentration when flooding
began. After all the nitrate was leached from the topsoil by
the applied wastewater, the nitrate content of the drainage water
returned to a low level.
When the South Tahoe Public Utilities Department sprayed
treated sewage on forested hillsides in the fall of 1963,
nitrogen removals by the soil mantle were more than 65 percent.
The removals dropped to 26 percent in the winter when the ground
was frozen. Significant amounts of ammonium ion were present
in the upper 4 in of soil, but nitrate levels were low at all
depths. The removal of nitrogen was attributed to the denitrifi-
cation in the soil mantle under anaerobic conditions (1233).
245
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The California State Health Department (1233) reviewed
nitrogen removals and management at a number of well-injection
waste disposal/recharge systems. Results of a six-month study
on the injection of slow sand filter effluent are shown
in Table 91 .
TABLE 91 . NITROGEN TRANSFORMATION IN RECHARGE
AQUIFER. MG/l (1233)
Organic-N Ammonia-N Nitrite-N Nitrate-N
Natural water in
the aquifer .4-.5 .2 0.0 .4-4.8
Filter effluent
before injection 2.2 1.5 .01 21.3
Recharged water in
aquifer, 20 ft
from injection well 1.4 1.2 .21 18.2
Recharged water
mixture in aquifer,
500 ft from injec-
tion well .9 .8 .003 6.1
Analysi s
of nitrate in
tion, as well
nitrogen level
a distance of 500
of data in Table 91 indicated that the decay
the aquifer was due to some extent to denitrifica-
as dilution. Considering such decay, the nitrate
was expected to fall to 10 mg/l before traveling
ft in the aquifer. Further tests revealed an
anaerobic, microbiologically active zone in the aquifer in the
vicinity of the injection well. During the tests, nitrate was
largely removed by microbial denitrification within 150 ft of
the injection wel1.
In summary, data indicate that, under proper management
conditions, land application of wastewater effluent offers the
potential to efficiently remove nitrogen from wastewater and
protect groundwater from nitrate contamination. The most
successful programs stressed an appropriate flooding/drying
schedule to promote both aerobic nitrification and anaerobic
denitrification processes, in order to ultimately convert
ammonia nitrogen in the wastewater to nitrogen gas. However,
if not properly managed, a definite danger exists of polluting
groundwater resources with excess nitrates.
246
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A number of investigators have mentioned the possibility
of groundwater contamination by nitrogen forms from land
application of sludges (377, 690, 705). Yet few quantitative
studies were found. Walker (1440) concluded that trenching
was a viable method to dispose of sludge with minimal ground-
water contamination by nitrates. Results of his study showed
no increase in pollutants (with the exception of chlorides) in
groundwater monitoring wells for up to 19 months after sludge
entrenchment. There was evidence that nitrate pollution would
become a problem when sludge dried out and became aerobic. In
order to prevent excessive nitrogen from reaching groundwater,
it was recommended that the site be underdrained, and that the
drained water be used to irrigate surrounding cropland.
Five sites receiving applications of municipal sewage
sludge were examined by Prothero (1124). At all sites, the
ammonia nitrogen and total nitrogen concentrations of the
treated soils compared closely to the control soils at a depth
of 50 cm in the soil profile. The nitrate concentrations at
this depth were above those of the control soils and increased
with increasing application rate.
Brown (151) discussed sludge application to croplands.
He stated that serious nitrate pollution becomes a potential
problem only when the plant-available nitrogen application to
soils exceeds the sum of gaseous nitrogen losses (through
denitrification and volatilization) and the nitrogen require-
ments of the crop. He divided the nitrogen content of sludge
into the soluble ammonia fraction (which is immediately avail-
able for plant uptake) and the organic nitrogen fraction (which
must be converted to inorganic nitrogen by soil microorganisms
before it is available). The conversion of organic nitrogen
is estimated to occur at a rate of 10 percent the first year
that the sludge is applied and 5 percent per year in the
following years. The 90 percent of organic nitrogen that is
not converted the first year is incorporated into humus-like
substances. As this organic nitrogen accumulates in the soil,
the rate of sludge application must be decreased if the balance
is to be obtained between yearly inputs and losses of plant-
available nitrogen to and from the soil.
Brown cited a study which shows that the nitrate content
of drainage waters from a sludge disposal site will be excessive-
ly high if no restrictions are placed on the quantity of nitro-
genous material applied to the soil. When 10 in/yr of digested
sludge were applied to soil lysimeters, the drainage waters
contained up to 449 mg/i N.
247
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Since 1971, the Metropolitan Sanitary District of Greater
Chicago has been monitoring a digested sludge land application
site. A 1974 report (1556) states that increases in nitrite
and nitrate concentrations have not occurred in groundwater
observation wells 1n areas receiving the sludge, indicating
that chese constituents are not migrating into the aquifer.
Recent studies of land application of wastewater effluent
indicate that the soil system is highly efficient in removing
phosphates from wastewater. Phosphate removal is both a function
of soil composition and travel distance. In most soils, phos-
phorus not taken up by plants is immobilized due to the adsorp-
tion of phosphate onto the soil. Adsorption is followed by fix-
ation by iron and aluminum oxides if the soil is acid, or by
precipitation into various forms of calciurn- phosphate if the
soil is basic (133). These reaction products are sufficiently
insoluble, so that phosphorus is held in the upper few centime-
ters of most soils, and very little phosphorus moves into the
groundwater (798). However, in the case of acidic, sandy soils
with no iron or aluminum oxides, little phosphate is fixed. Thus,
it may be necessary to remove phosphorus from wastewater before
its application to such soils (133).
Hook et al. (595) Deported that under proper management,
most of the phosphorus n wastewater remains in the soil at the
disposal site or leaves as a nutrient in harvested crops. They
found that soils differed in their abilities to retain phosphorus
In a heavy-textured soil high in iron and aluminum oxides and
hydroxides (sesquioxides) , phosphorus from effluent irrigation
did not increase in the soil below a depth of 1 ft after 7 yr of
irrigation. In a light-textured soil with half as much sesqui-
oxides, phosphorus content increased to a depth of 3 ft after
6 yr of treatment.
Phosphorus removals at Flushing Meadows, Arizona, (134)
were found to be basically dependent upon the distance traveled
by the wastewater through the soil. The chief removal mechanism
was precipitation as calcium phosphate or magnesium ammonium
phosphate, since the soils tested contained little iron,
aluminum oxides, or other phosphate fixing materials. Under-
ground travel distances of 30 ft produced 50 percent reduction;
distances of several hundred feet were found to be sufficient
for 90 percent phosphorus removal. However, the capacity of
the soil to remove phosphorus decreased after the start of
the project, holding stable at approximately 50 percent removal.
The fact that soils gradually lose their capacity to adsorb
phosphates over long-term application is substantiated by
Barrow's detailed analysis of this phenomenon (68). He
concluded that previously applied phosphate had been converted
to a form that was occupying phosphate adsorption sites, thus
reducing the capacity of the soil to further adsorb phosphate.
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Continuing studies at Lake George, New York (47), have
shown that significant amounts of nitrates appear to reach
the waters tributary to the lake. However, the wastewater land
treatment system appears to remove essentially all phosphorus,
thus reducing the potential for algal bloom in the lake.
Dugan et al. (352), in their work on land disposal of
wastewater in Hawaii, noted that phosphorus removals of over
95 percent within a 5-ft depth of percolation were obtained
when secondary wastewater was applied to grassed areas.
Suspended solids are removed very effectively by land
application systems. In fact, one problem encountered in the
spreading of wastewater is that nearly all suspended solids
are filtered out in the top few inches of soil. This can cause
clogging of soil pores and reduction of infiltration rates.
There is no danger of groundwater contamination in applied
wastewater from suspended solids. Literature data on suspended
solids are not extensive, because experience has shown land
application to be capable of removing virturally all solids at
the surface. A study at Whittier Narrows, California (1233),
showed suspended solids removal, due to percolation, of 95
percent. At Flushing Meadows (134), the suspended solids concen-
tration of the percolate was essentially zero, even though the
solids in the wastewater applied reached 100 mg/l. Similar
findings were reported at Lake George (47), where virtually
all BOD and suspended solids were removed from percolated
effluent.
Results from a spray irrigation and runoff system used to
dispose of a cannery waste (87) showed that even with a runoff-
type system, suspended solids removals averaged 97 percent.
Dugan et al. (352) reported similar high suspended solids
removals with application of secondary effluent to Bermuda
grass in Hawaii.
ELEMENTAL CONTAMINANTS
Municipal wastewater and sludge contain small amounts of
nearly all metals. The degree to which a particular soil will
protect underlying groundwater through removal of contaminants
is primarily determined by the chemical and physical composition
of the soil. Removal can occur through such processes as precip-
itation of solid phases, ion exchange, and adsorption. These
processes are in turn controlled by soil pH, the oxidation/
reduction potential, clay content, the presence and type of
organic material, and the extent of soil saturation.
The general nature of reactions of sewage wastes with soil
is well known. With time, wastes applied to land are broken
down, and the dissolved constituents become part of the soil
solution. Released cations can exchange with those already
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on exchange sites in the soil. Metals as ions or in the
colloidal state can be adsorbed onto soil surfaces. When the
levels of ions in solution exceed the solubility of correspond-
ing solid phase compounds and minerals, those compounds can
precipitate. When the solubility of solid phase compounds and
minerals exceeds the levels of corresponding ions in solution,
the compounds can dissolve. Constituents are also ingested
by soil microorganisms and incorporated into soil organic matter.
Ions that are not removed by any of these processes but
that remain in the soil solution are available for uptake by
plant roots or leaching by water moving through the soil profile.
Lindsay (798) studied the composition of the soil solution,
concluding that it is controlled by the solubilities of solid
phases. Thus, precipitation and dissolution reactions determine
the activity of ions in solution, which in turn governs ion
exchange.
Lindsay (798) also recognized the importance of the forma-
tion of metal-organic complexes and chelates in increasing the
solubility and mobility of metals in soils. Brown (151) stressed
this point. He found that it is misleading to predict the
availability of metals in soils from their solubility in distilled
water. He cites evidence that plant uptake of metal ions could
not be predicted by the water solubility of the solid compounds.
This may be because the soil solution in the vicinity of roots,
unlike distilled water, is mildly acidic and contains organic
metal-complexing agents (798).
All of the trace elements for which water quality criteria
have been established may occur as either soluble or insoluble
metal-organic complexes (1323). Low molecular weight organic
molecules tend to increase the penetration of complexed metal
ions into the soil, while high molecular weight molecules and
their complexed ions may be filtered out by the soil (133).
The chemistry of the metal organic complexes is complex, and
present knowledge of organic forms of the elements is insuffi-
cient to generalize. Where concentrations of trace elements in
soil solutions are in excess of those predicted from inorganic
solubility product considerations, the element is thought to
occur in organic form. Because of this lack of knowledge, the
literature discusses mainly the chemistry of inorganic forms.
This is unfortunate, because most of the metal ions in waste-
water and sludge probably occur in complexed form.
Most metals are less mobile under aerobic and basic soil
conditions than they are under anaerobic and acid conditions
(133). The neutral water extract of soils contains less heavy
metals than acidified extracts of the same soils, indicating
the importance of the pH factor in influencing the mobility of
metals (1173). Lindsay (798) cites evidence that for zinc and
copper there is a 100-fold increase in ionic activity for each
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unit decrease in soil pH. Normally insoluble metals may
become mobilized in the event of a change in the characteristics
of percolating water, such that acidic or anaerobic conditions
occur.
The removal of metals by ion exchange or adsorption depends
upon the availability of exchange and adsorption sites in the
soil as well as on the factors (ionic activity and pH) just
discussed. Therefore, the clay content of the soil is important;
clay soils provide more exchange and adsorption capacity than
sands and gravels (1173). A correlation also exists between
the form in which the elements occur in solution and their
removal by exchange or adsorption. In general, elements that
occur in solution as anions or neutral molecules pass through
soils more readily than do elements that occur as cations.
Inorganic arsenic, selenium, and fluorine in aerated soils
occur as anions or neutral molecules. Although there are
exceptions (depending upon the chemistry of the system),
inorganic cadmium, copper, chromium, lead, mercury, silver, and
zinc most commonly occur in fresh waters and soil solutions in
the inorganic form as cations (1323).
Many conclusions in the literature lack substantiating
experimental data but are based on a knowledge of chemistry.
The use of sanitary sludge for land reclamation projects may
increase the toxic metal content of the soil. The work of
Lejcher and Kunkle (776) showed significant reductions in the
leachate of iron, aluminum, copper, manganese, and sulfate
combined with increases in cadmium, zinc, and chromium when
304 tons dry wt/ac were applied. In this experiment, the
resulting pH of the surface soils was 6.2, still low enough to
account for the mobilization of the metals. Higher application
rates or the utilization of sludges with higher buffering
capacities may help immobilize the metals that showed increases.
The work by Sopper et al. (1299) revealed similar results.
Bernard (106) considered metal concentrations in sludge
a prime deterrent to landfilling as a disposal method, but he
concluded that metals tend to concentrate in the upper soil
layer rather than leaching through the soil profile. Limited
monitoring by Lofy (ongoing research) at eight landfill sites
accepting wastewater sludge indicated that there was measurable
migration of certain metals to considerable distances from the
disposal area. Lead was particularly mobile. Preliminary
indications are that many metals, such as chromium, are strongly
attenuated by the majority of soils studied.
Prothero (1124) studied five sites where sludge is disposed
of on land. The heaviest application rate at a site was 500 dry
metric tons of sludge/ha. Water samples were collected from
wells in close proximity to the sludge disposal locations and
were analyzed for cadmium, chromium, manganese, nickel, and
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zinc. The trace element content of the applied sludge fell
within ranges generally reported for municipal sludges, except
for the chromium content of one sludge (17,700 ppm). Results
showed the cadmium, chromium, and nickel contents of the well
waters were generally undetectable while the copper, manganese,
and zinc concentrations did not exceed 0.3, 0.01, and 0.04 ppm,
respectively. There was an exceptionally high manganese content
(1.2 ppm) at one site, however, which was apparently due to
strong reducing conditions. The other well samples were below
maximum allowable drinking water concentrations set by the
Public Health Service for each metal.
Walker (1440) considered groundwater contamination by
heavy metals at a sludge entrenchment- site. For 19 months after
sludge was buried at 350 to 500 tons/ac dry sludge solids, no
metals were detected in groundwater observation wells.
Data from actual land application operations, which
included arsenic and selenium determinations, were not found.
Predictions of removal of these metals based on chemical
properties are also hindered by limited understanding of the
reactions involved.
Only one reference was located that provided experimental
data on cadmium in relation to wastewater applied to land.
At Flushing Meadows, Bouwer et al. (134) found that cadmium in
wastewater applied to land in shallow basins showed very little
change due to migration through the soil. The cadmium concen-
tration dropped only slightly from 7.7 yg/£ to 7.2 yg/£.
Aerobic conditions and alkaline pH prevailed in the soil studied.
A study (1323) by the California State Water Resources Control
Board (CSWRCB) reviewed available data on soil reduction of
cadmium in effluents, concluding that information is not
sufficiently detailed to allow adequate evaluation of cadmium
concentrations in water reaching groundwater basins. According
to the study, it must be demonstrated that a particular soil
is able to reduce the concentration of cadmium to a level that
is acceptable for drinking water. Otherwise, the study advised
against the use of wastewater effluents with concentrations
above this limit for groundwater recharge operations involving
percolation through soil.
Bouwer's work at Flushing Meadows (134) found that the
copper concentration of applied wastewater was reduced about
86 percent by passage through the soil. This removal occurred
rapidly, usually in the first 30 ft of downward flow.
f
Iron and manganese in we!1-oxidized soils are characterized
by the formation of highly insoluble oxides and hydroxides.
However, at low pH and under reducing conditions, these metals
can be solubilized and become mobile in the soil as Fe2+ and
Mn2+. Amramy (26) conducted a study of sewage lagoon effluent
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spreading on sand dunes. He found that after a subsurface
travel distance of 8 m, the concentration of iron in the waste-
water actually increased from 0.28 mg/£ to 0.57 mg/i. The
manganese concentration increased from 0.08 mg/i to 0.19 mg/i
after 25 ft of travel through sand. Wesner and Baier (1484)
found a similar phenomenon when tracing the underground move-
ment of wastewater after injection. Over a travel distance of
400 or 500 ft, the concentration of iron did not change.
Manganese concentrations, on the other hand, increased up to
300 percent in the first 100 ft of subsurface travel. Anaerobic
conditions, favoring formation of soluble manganese compounds,
are mentioned as the possible cause of the large increase.
These conditions are most likely caused by biological oxidation
depleting oxygen near the point of injection, thus causing the
reduction of manganese to soluble forms. However, after greater
travel distances and the return to aerobic conditions, the
manganese may revert to insoluble compounds and be removed from
the migrating water.
Ragone et al. (1129) reported on deep well recharge expe-
riments conducted in Nassau County, Long Island. Tertiary
effluent was recharged by a deep well into the Magothy aquifer,
the primary water supply source for Nassau County. As of
September 1972, 12 recharge tests had been run since the incep-
tion of the recharge program in September 1968. Although
the iron concentrations of reclaimed and native water averaged
0.44 mg/i and 0.24 mg/i, respectively, the iron concentration of
the mixed (native and reclaimed) water at times exceeded 3 mg/i .
The authors mentioned several sources that could account for
the increase in iron concentration, but the most probable source
was the pyrite native to the Magothy aquifer. During recharge,
the natural reducing condition in the aquifer was replaced by
a progressively more oxidizing environment. The initial
response to this change was the oxidation of pyrite, which
released Fe+z, $04-2, and H+ into solution. Eventually, ferric
hydroxide precipitated, and the Fe + 2 concentration decreased.
The exact oxidation mechanism apparently involved inorganic
and/or organic constituents in the reclaimed water, because
water from the public potable water supply system caused no
increase in iron concentration when injected into the aquifer.
The Flushing Meadows study by Bouwer et al. (134) contained'
data on the reduction of lead by soil infiltration. Bouwer found
that the wastewater concentration of lead decreased by 20 percent
after significant travel distance underground. Apparently, a
small portion of the lead was tied up rapidly (within 50 ft),
while the majority was unaffected by further travel. It should
be noted, however, that the soil examined in these experiments
was a sand with limited adsorption and exchange capacity for
many trace elements.
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Both mercury and zinc form insoluble compounds in soil,
lowering the activity of the ions in solution so that little
movement occurs. Mercury is particularly insoluble as phosphate,
carbonate, or sulfide. However, under low pH conditions, the
metals may become mobilized. They can also form soluble
complexes that affect their mobility under certain circumstances
(798). At Flushing Meadows (134), underground percolation
through 100 ft of sand produced 40 percent removal of mercury
and approximately 58 percent removal of zinc. Further travel
produced no further removal of mercury but reduced the zinc
concentration to about 20 percent of that in the applied waste-
water. The final concentrations of mercury and zinc were
.00014 mg/£ and .037 mg/£, respectively.
In conclusion, the information garnered in this study of
the literature is inadequate to define fully the chemical
behavior of elemental contaminants in the soil and their fate
as they percolate through the unsaturated zone. The CSWRCB
recommended, on the basis of its literature review (1323), that
wastes containing concentrations of certain metals above those
acceptable for drinking water supplies should not be applied to
land, unless it can be demonstrated that contamination of
groundwater does not occur.
BIOCIDAL CONTAMINANTS
Use of chemical pesticides in agriculture Generated many
studies of the potential harmful effects of these compounds
on land, crops, surface water, and groundwater. However, there
is little data available on biocides in municipal wastewater or
on the potential dangers of groundwater contamination through
land wastewater application operations. This lack of informa-
tion is understandable considering the minimal role that munici-
pal wastewater plays in transporting biocides to the land.
Biocides come in contact with the land through a number of
activities, primarily by direct application to the land for
pest control. Return irrigation water, and spills and wastes
from pesticide manufacturing operations also bring biocides in
contact with the land.
The reactions of pesticides with soil has received limited
attention in the literature. Volatilization, chemical degrada-
tion, and absorption by plant roots and seeds apparently remove
a small portion of pesticides reaching the soil. A more signi-
ficant process for pesticide removal may be microbiological
degradation. Although this process is very slow in some cases,
often taking several years, microbiological degradation accounts
for the breakdown of a remarkable variety of organic compounds.
Pesticides that are not removed from the soil column or broken
down by these processes may be available for leaching into
groundwaters.
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Gerakis and Sficas (464) reviewed the literature on pesti-
cide degradation and leaching. They reported that the most
important factors involved in these two processes are soil
temperature and moisture, organic matter and clay content, soil
management practices, pH, and species and population density of
microorganisms present. The presence of organic matter and clay
in the soil appears to be positively correlated with adsorption
of pesticides onto soil particles.
Van Bladel and Moreale (1417) studied herbicide adsorption
onto clay minerals. They found that adsorption increased with
the polarizing power of the exchangeable cation, and concluded
that adsorption appears to be one of the most important factors
in reducing pesticide removal from soil layers by leaching.
Laboratory studies of land-applied sludge were conducted by
the University of Nebraska (1474) to determine degradation rates
in groundwater for selected herbicides. The study indicates that
herbicide degradation was much slower in groundwater than in soil.
O'Connor and Anderson (1014) analyzed factors affecting adsorption
of the herbicide 2,4, 5-T on four soils in the western United
States. The study found that organic matter contributed to
adsorption, while oxides of iron and aluminum did not.
Gerakis and Sficas (464) cite evidence that pesticides
differ in their mobilities in the same soil. One study showed
that (1) acidic compounds are relatively mobile, (2) phenyl
ureas and triazines are of intermediate to low mobility, and
(3) organochlorine compounds and organic cations are least
mobile. Further data that were reviewed supported the conclu-
sion that under normal agricultural practices and rainfall, it
is very unlikely that pesticides may be leached deeply enough
and in such quantities as to cause appreciable contamination
of groundwaters.
A California State Water Resources Control Board report
(1323) mentioned that pesticides are adsorbed by soil clays,
iron aluminum oxides, and especially by organic colloids, and
that they are susceptible to microbial decomposition. However,
the amount of biocides in average municipal wastewater and
sludges, was found to be so minimal that the spreading of
municipal waste on land offers extremely low potential for
groundwater biocide contamination.
SYNTHETIC/ORGANIC CONTAMINANTS
One of the most intensely debated questions regarding land
application for treatment and/or disposal of municipal wastes
concerns the problem of residual organic contaminants. Refrac-
tory organic compounds may survive conventional treatment
processes and penetrate through the soil to contaminate ground-
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water supplies. The controversy centers around the fate of
residual organlcs within the soil systems, including such issues
as the synerglstlc effects between organlcs and Inorganics or
other groundwater and soil constituents, or conversion of safe
organlcs to hazardous compounds 1n the soil. Despite this
controversy, no literature was found concerning groundwater
pollution by the synthetic/organic contaminants in municipal
wastes as a result of land application.
The absence of literature concerning the movement through
soil of synthetic/organic contaminants 1n applied sludge 1s
not surprising, since the specific organic makeup of sludge 1s
unknown. Some of the chemicals of concern (PCB's, polycyclic
aromatics, and other chlorinated hydrocarbons, etc.) have low
solubilities in water 1n comparison with vapor pressures. As
a result, there 1s a distinct possibility of vaporization when
sludges containing these chemicals are applied to the land surface
The California State Water Resources Control Board (1323)
cited a study carried out 1n Colorado that compared the nature
of the soluble organic material in the soil profiles under a
feedlot and under grassland with selected ground, well, and
river waters. It was concluded that the major portion of the
soluble materials in all the waters was polymeric. The soluble
organlcs under grassland were essentially the same as those
under the feedlot, although phenols were present in greater
abundance in the manure and surface soil of the feedlots. About
13 percent of the soluble material in the soil profiles was
carbohydrate (polysaccharides), and much of the remainder, based
on IR spectra and reductive degradation procedures, appeared to
be polymerized aromatic structures. This report by the CSWRCB
Interpreted these observations to indicate that the soluble
organlcs under wastewater-treated soils would be similar to
those under feedlot manure or grassland.
BIOLOGICAL CONTAMINANTS
Most available data suggest that virus, bacteria, and
other biological pathogens present in wastewater and sludge
are removed or Inactivated by percolation through soil.
The California State Water Resources Control Board study
(1323) provides a summary of the fate of viruses, bacteria,
protozoa, and parasitic worms in wastewaters applied to land.
The summary states that most of these pathogens prefer warm-
blooded animals as their habitat and do not flourish in the
soil environment. When introduced into soils, the pathogens
do not compete well with the vast number and variety of normal
soil inhabitants and are subject to attack by antagonistic soil
species. The time necessary for their ultimate destruction
varies, according to species and environmental conditions.
A compilation of pathogen survival data in the literature is
shown in Table 92 below.
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TABLE 92 . SURVIVAL OF PATHOGENS
IN SOILS (1323)
Ascari s 1 umbri coides ova
Endamoeba histolytica cysts
Salmonella species
Coliform group organisms
Q-fever organisms
Bruce!la abqrtus
Tuberculosis bacteria
Enteroviruses
2.5-7 years
8 days
6 hours
133 - 147 days
148 days
30 - 100 days
6 months
12 days
The most persistent pathogens in soils appear to be ova,
cysts, and spore-forming bacteria. The survival of enteric
viruses in soil has not been thoroughly studied. The dependence
of enteric viruses on specific host organisms for reproduction
suggests that they would not multiply and would not be expected
to survive for a long period of time, although survival may,
at times, be long enough to cause public health concern.
Two and a half years of continuous observation was conducted
of wastewater reclamation by 1andspreading in Lodi , California
(1175). It was found that the MPN of coliform group organisms,
which averaged 1.9 x 1Q8/100 ml in the wastewater, was consis-
tently reduced to less than 1/100 ml after 4 to 7 ft of soil travel.
The average percolation rate was 0.3 ft/day in coarse-textured
Hanford sandy loam. It was observed that the number of coliforms
penetrating 1 ft or more was essentially independent of the
coliform concentration of the wastewater.
At Whittier Narrows (892), percolation tests showed that
vertical percolation of wastewater through 4 to 7 ft of soil
is an effective method of removing bacteria of fecal origin,
despite heavy growth of coliforms of soil origin. The formation
of an organic-microbial slime layer at the water-soil interface
was found to increase the efficiency of the filtering action.
Lejcher and Kunkle (776) reported, with regard to biological
pathogens, that no fecal coliform bacteria were found in the
runoff from the sludge-treated plots (treated at a rate of
78 to 304 dry tons of sludge/ha) during the year immediately
following application. They concluded that it appeared unlikely'
that pathogens would survive in the runoff. Limited transfer
of microbial cells through the soil profile and rapid die-off
of the pathogens in the soil matrix suggested low-risk
conditions (619, 917).
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Research by Bernard (106) on the disposal of sewage sludge
to sanitary landfills concluded that pathogens tend to concen-
trate in the upper soil layer, rather than leaching through
the soil profile. In contrast, Lofy (ongoing research) found
that fecal coliform and fecal streptococcus are particularly
mobile and can travel considerable distances.
Results from studies at Flushing Meadows, Arizona (134)»
show that fecal coliform density was reduced significantly in
the first 2 or 3 ft of travel. Buuwer found that fecal coliform
density at a particular depth tended to decrease with increased
flooding time. The peak bacteria density invariably appeared
immediately after flooding was resumed. The concentration of
fecal coliforms was consistently decreased to less than 10/100 mi
after 100 ft, and to 0/100 ml after .300 ft of travel.
A project at Santee, California (1215), is famous for its
pioneering work in the reclamation of domestic sewage for
recreational lakes. Travel of secondary effluent through
1,500 ft of very coarse sand was sufficient to remove all fecal
coliforms. Sampling showed that most of the coliforms were
removed in the first 200 ft.
At Orange County, California (1484), tests conducted on
a well injection system showed coliform organisms 30 m from
the injection well, but none approximately 80 m from the well.
The results indicated that fecal conforms are more easily
removed by underground travel than other coliforms. Some of the
other coliforms may have been supported by nutrients 1n
the effluent.
Results of percolation tests at Lake George, New York
(1129), showed again that: percolation of applied secondary
effluent through 5 to 10 ft of soil in two different beds was
sufficient to remove essentially all coliform organisms.
Browning and Mankin (155) reported an unusual case of
disease outbreak due to contamination of groundwater well
supplies by land application of treated sewage. In Madera,
California, undisinfected secondary effluent was used to irrigate
a pasture located adjacent to a deep well drawing part of the
city water supply. The wastewater migrated through gopher holes,
filling a construction pit around the well, and eventually
flowed into the well itself.
On the basis of experience and results of full-scale,
long-term wastewater reclamation studies, the CSWRCB (1323)
concluded that, although soil is an excellent media for removing
bacteria, a small fraction of the fecal coliform bacteria there-
in may reach qroundwater reservoirs at hiqh percolation rates.
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Horizontal travel of viable fecal coliform bacteria in the
aquifer does not appear to occur to a significant degree. The
available data on horizontal travel, however, are inconclusive.
Further investigation of the transport and survival of pathogenic
bacteria in groundwater, therefore, is required.
Research shows that travel through soil removes significant
amounts of viruses, primarily through adsorption. Adsorption
is influenced by the pH and ionic strength of the soil solution.
The available information indicates that adsorption of virus
by soil is nearly complete at pH 7 or less, but decreases as
the pH value increases above 7. This is mainly because the
overall electric charge surrounding both the virus and soil
particles becomes increasingly negative as pH levels increase
and, therefore, mutual repulsion occurs (1323).
It also appears that increasing cationic strength of the
percolating water or soil solution increases virus removal. At
the pH values normally encountered in wastewater, viruses are
slightly negatively charged. The presence of calcium, magnesium,
sodium, aluminum, and other positive ions in the soil solution
decreases the potential for negatively charged soil and virus
particles to repel each other. This results in the formation
of soil-cation-virus bridges that immobilize virions (1323).
The ionic strength in percolating wastewater is usually
sufficient so that it does not limit adsorption. In circum-
stances where ionic strength is significantly decreased,
however, desorption of adsorbed viruses may occur. Organic
matter in wastewater can also compete with viruses for adsorp-
tion sites. In laboratory studies, when virus-adsorbed clay
particles were washed with distilled water, an essentially
complete desorption and reactivation of viruses took place.
In field conditions, other mechanisms in soil systems may
inactivate or destroy adsorbed viruses before they are subject
to desorption (1323). In addition to pH and ionic strength,
the clay and organic matter content of soil evidently influences
adsorption to some degree. In general, soils of higher clay
and/or organic matter content are more effective in adsorbing
viruses (1323).
Definitive work on virus interaction with soil was conducted
at Santee, California, where extensive studies showed that
percolation through several hundred feet of soil consistently
removed all virus from secondary effluent (1215).
Other studies also supported the conclusion that soil
effectively removes viruses. Viral analyses in Hawaii by Dugan
et al. (352) showed that test soils in 5-ft lysimeters were
completely effective in removing viruses. Brief tests at
Whittier Narrows, California (892), achieved complete removals
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of Sabin Type III polio-virus vaccine. Although 250 plaque-
forming units (PFU) of enteric viruses/^ were present in the
applied wastewater, no measurable concentrations were found below
2 ft in the percolate.
In 1974 at Flushing Meadows (134), virus analyses were
performed bimonthly to determine the fate of viruses in the
soil system. Secondary effluent was allowed to infiltrate into
six parallel horizontal basins consisting of 60 to 90 cm of
fine loamy sand underlain by several coarse sand and gravel
layers to a depth of 75 m, where a clay layer begins. Observa-
tion wells were installed in line across the basin area. No
viruses were detected in any of the wells at any time during
each flooding period. Gilbert et al. (475) stated that the
failure to detect viruses in the wells indicates that the virus
count was reduced by at least 99.99 percent within 3 to 9 m
of basin soil.
Romero (1175) reviewed the studies performed ^or the
Department of the Army on sands ranging in classification from
silty sand to coarse-granite alluvium. Results indicated that
the bacterophages Tl, T2, and 65 are more effectively retained
in the finer sands, particularly in those containing a relatively
high percentage of clay and silt. Virus removal was shown to
increase with decreasing particle size. The greatest percentage
of removal took place in the uppermost portion of the sand
columns tested." It was shown that for a well-sorted sand of
particle size averaging 0.12 mm, the removal efficiency in 2 ft
of penetration was 99.999 percent.
Young and Burbank (1548) described studies of virus removal ;'
in Hawaiian soils. In the laboratory, columns of various types
of Hawaiian soil were subjected intermittently to percolating
water with a known concentration of virus (coliphage T4B II mutant,
and polio virus Type II (Lansing) H8), simulating the action of
cesspool leaching. The effluent from each soil column was
analyzed for viral content. Coliphage T4 was applied to
slightly acid soils (pH 5-6) at a concentration of 2.5 x 10b/m£.
Percolation through 2.5 to 6 in of soil was 100 percent effec-
tive in retention of the virus. Slightly alkaline soil was
less effective, removing only 67 percent of applied coliphage
and 35 percent of applied polio virus in 15 in. Removal of
polio virus Type II was less complete; 6-in columns were able
to effect only 99.3 percent removal with an initial feed concen-
tration o.f 1.5 x 105 pfu/m£.
Wellings et al. (1479) found that virus can be isolated at
the 6.5-m level below a spray irrigation' field. Another study
by Wellings et al. (1477) measured virus migration through the
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ground from chlorinated packaged plant effluent applied to a
cypress dome. Both horizontal and vertical migration was
detected at distances of approximately 7 m for polio and
coxsackle viruses. Wells beyond that distance showed no virus.
The survival of virus within the dome was at least 28 days.
At Fort Devins, Massachusetts, where a land application
site has been 1n operation for over 30 years, Schaub et al.
(1210) studied the removal of bacteria from unchlorlnated
primary effluent applied to soil cells. Using tracer f2 bac-
terlophage and the enterovlruses polio virus I and EMC virus,
it was demonstrated that tracer bacteriophage penetrated Into
the groundwater along with the percolating wastewater. The
concentration 1n the groundwater stabilized at almost 50 percent
of the applied virus concentration. The tracer and entero-
vlruses were sporadically detected at horizontal distances up
to 600 ft from the application point.
Lance et al. (750) passed secondary sewage effluent con-
taining 3 x 104 pfu/m£ polio-virus Type I (LSc) through' 250 cm-
long columns packed with calcareous sand from an area 1n the
Salt River bed used for groundwater recharge of secondary sewage
effluent. Viruses were not detected in 1-ml samples extracted
from columns below the 160-cm level, but were detected 1n 5 of
43 IQQ-ml samples of the column drainage water. Most of the
viruses were adsorbed in the top 5 cm of soil. Virus removal
was not affected by the Infiltration rate, which varied between
15 and 55 cm/day. Flooding a column continuously for 27 days
did not saturate the top few centimeters of soil with viruses
and did not seem to affect virus movement. Flooding with
deionized water caused virus desorption from the soil and
increased virus movement through the columns. Drying the
soil for one day between applying the virus and flooding with
deionized water greatly reduced desorption, and drying for
five days totally prevented desorption. The investigators
concluded that large reductions (99.99 percent or more) of
virus are expected after passage of secondary effluent through
250 cm or more of calcareous sand, unless heavy rains fall with-
in one day after application of sewage.
261
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PATHWAYS TO MAN
AIR
INTRODUCTION
Health-impairing contaminants contained in wastewater are
most likely to return to man by way of surface or groundwater
migration; however, some contaminants may also be transmitted
through the atmosphere. Aerosolized particles ranging in size
from 1 to 40 microns are generated as an incidental by-product
of various wastewater treatment processes and may contain
health-impair ing contaminants that can be directly inhaled by
man. Glaser and Ledbetter (481) found that 40 percent of the
particles aerosolized during activated sludge treatment were
smaller than 10 microns-. Larger particles pose a minimal
hazard to respiratory systems but may be ingested; however,
aerosols of 10 microns or less will be captured in the upper
respiratory tract, transported through the pharynx, and will
enter the digestive tract.
Activated sludge, trickling filters, and spray irrigation
of wastewaters and liquid sludges are considered to be the
major potential sources of aerosols. In addition, vaporized
contaminants are emitted from sludge incinerators and furnaces
used for activated carbon regeneration.
Bubbles are produced in wastewater by natural biological
action or by mechanical aeration during activated sludge and
similar processes. These bubbles burst at the surface, eject-
ing contaminant-bearing water droplets into the air. When
wastewater is sprayed, as in land application, large numbers
of particles are released into the atmosphere. Aerosols con-
taining wastewater contaminants are also produced above bodies
of water into which wastewater effluent is released as a
result of wind spray, breaking waves, splashing rain, or
bursting bubbles.
Certain contaminants are floatable and tend to concen-
trate in a layer on the water surface. Particles that are
aerosolized from this layer may contain high concentrations
of these contaminants relative to their concentrations in the
bulk of the liquid. For example, Blanchard and Syzdik (125)
found the bacterial concentration of Serratia marcescens in
drops from bursting bubbles to be from 10 to 1000 times higher
than that of the tap water in which the bubbles formed. These
investigators suggested that DDT and several species or
organisms could be expected to concentrate in surface films
and be transferred to the atmosphere.
262
-------
Direct vaporization of certain contaminants also occurs.
For instance, low solubility contaminants such as pesticides,
polychlorinated biphenyls, or hydrocarbons have high evapora-
tion rates from water bodies to the atmosphere, according to
a paper cited by Mackay and Leinonen (827).
The viability of biological aerosols from sewage treatment
plants is affected by distance traveled, deposition, dispersion,
and hostile environmental conditions.
One study revealed the correlation between human respira-
tory difficulty and high concentrations of plankton in the
sea. This study has often been cited (125) as indicative of
the airborne, onshore movement of marine organisms. The
"blowback" of microorganisms rising to the surface from sub-
marine sewage outfalls may also have a significant, localized
impact on public health.
A considerable body of information has been developed in
medical literature pertaining to the movement of pathogenic
bacteria through air. In scientific literature topics studied
include atmospheric physics and dispersion modeling, aerosol
physics, liquid surface physics, dissolved air and froth
flotation technology, and other subjects indirectly related to
potential atmospheric pathways of contaminants from waste-
water treatment systems to man. Very little of this work,
however, deals directly with the subject of atmospheric path-
ways of contaminants from wastewater to man. Available
literature is listed in Table 93. Research in this area has
been principally concerned with the transport of biological
pa thogens .
ELEMENTAL CONTAMINANTS
For most elemental impurities, direct vaporization will
not occur. Few references were found in the literature re-
viewed that dealt directly with vaporization or aerosoliza-
tion from wastewater systems, although Haque and Freed (538)
included a discussion of the thermodynamics involved.
The atmospheric transport of mercury and dimethyl-mercury
has been studied and reviewed by Jernelov et al. (645), with
theoretical calculations performed by Baughman et al. (78).
On the basis of Baughman's calculations, it can be assumed
that the evaporative loss of these substances from aqueous
solutions may pose a problem under turbulent conditions.
Elemental mercury appears to be volatilized twice as rapidly as
the dimethyl form.
Soldano et al. (1295) measured organic and elemental
mercury concentrations in cities with central sewage facilities.
A broad range of mercury concentrations was detected in the
vicinity of treatment facilities. Numerous measurements were
in the range of 103 n g / m 3 , but values as low as 0.125 n g / m 3
263
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TABLE 93. LITERATURE REVIEWED PERTAINING
TO ATMOSPHERIC TRANSPORT
Contaminant Reference Number
Water Quality Parameters 481
Elemental Contaminants
Boron 1113
Mercury 78, 538, 645, 1295, 1302
Selenium 1114
Other (general ) 538
Biocidal Contaminants
Chlorinated 1532
hydrocarbons
DDT 553, 1472, 1551
Dieldrin 553, 1551
2,4D 553
Synthetic/Organic 1219, 1564
Contaminants
Biological Contaminants
Bacteria 79, 125, 238, 400, 481, 545, 568,
624, 649, 685, 765, 766, 792, 936,
983, 1069, 1073, 1099, 1100, 1234,
1302, 1304, 1463, 1560
Coliforms 2, 400, 568, 685, 983, 1099, 1100,
1234, 1304
Hepatitis virus 1151
Parasitic worms 1234
Protozoa 1234
Salmonella 568, 1234
Shigella 568, 1234
264
-------
TABLE 93 (continued)
Contaminant Reference Number
Virus 79, 238, 400, 649, 792, 1261, 1302,
1304
Other (general) 125, 238, 481, 568, 765, 766, 983,
1073, 1234
were also found. The atmospheric concentration of elemental
mercury fell off sharply with increasing distance from the
sewage plant, while the concentration of organic mercury rose
with increasing distance. The concentration maxima of organic
mercury at any particular plant was related to population size
of the area served. The authors concluded that sewage treat-
ment systems concentrate and re-emit elemental mercury after
some of it has been converted into the more volatile organic
forms by bacterial action.
BIOCIDAL CONTAMINANTS
Biocides tend to concentrate in the liquid surface and
aerosol fractions. However, the threat of adverse health
effects from aerosolized biocides contributed by sanitary waste
systems appears small in relation to that posed by other sources
of these contaminants. It is therefore not surprising that
only indirectly related research is available on the transport
of biocides from sanitary waste systems through the atmosphere.
Information on pesticides in rainfall and runoff is provided
by Weibel et al. (1472), and factors affecting the volatility
of DDT, dieldrin, and 2, 4-D from leaf and glass surfaces have
been examined by Hee et al. (553). Young and Heesen (1532)
conducted a study of the atmospheric transport of chlorinated
hydrocarbons to the waters of three southern California harbors.
They determined that atmospheric transport accounted for less
of the total concentrations of p,p'-DDT and PCB 1254 than
surface runoff.
SYNTHETIC/ORGANIC CONTAMINANTS
In general, insoluble or limited solubility organic
materials are concentrated at the air/water interface, in turn
producing a concentrated aerosol. The primary significance
of this surface concentration of organic materials and aerosols
lies in the effect that these materials may have on the sur-
vival of biological aerosols, Webb (1463) has conducted
265
-------
experiments showing enhanced survival of several species of
bacteria when amino acids, long chain protein degradates,
some sugars, and polyhydroxycyclohexanes were added to
bacterial suspensions before aerosolization. Hatch and
Wolochow (545) have also reviewed several aspects of this
problem, concluding that most of the organic compounds shown
to be the best protective agents for pathogen survival are
sugars or polyhydricalcohols.
BIOLOGICAL CONTAMINANTS
•A number of recent studies have examined the airborne
bacterial levels adjacent to treatment plant and land irriga-
tion sites. However, no correlation has yet been made between
specific atmospheric organism levels and the incidence of
disease (238). In their 1975 review of the literature,
Hickey and Reist (568) found only one survey that
had a direct bearing on increased disease rates associated
with occupational exposure to viable aerosols in wastewater
treatment operations. In this survey, the rate of pneumonia
incidence was identical for both water purification plant and
sewage plant workers, but the incidence of flu and colds was
higher among sewage workers by factors of 50 to 28 percent,
respectively.
The literature on airborne levels of micro-organisms is
difficult to interpret for several reasons. For instance,
sampling methods are not standardized, and a suitable indicator
organism is lacking. Also, there has been no research to
date suggesting that the traditional water quality indicator
organisms, the coliforms, provide a reliable indication of
pathogens present in aerosolized particles. In fact, the
half-life of airborne coliforms was found to be shorter than
that of the total bacteria in studies of the downwind disper-
sion of bacterial aerosols from activated sludge tanks performed
by Ledbetter and Randall (766). Pavoni and Tittlebaum (1069)
cited a study that found the survival rate of enterobacteriaceae
to be only 13 percent of that recorded for the total bacterial
aerosol emanating from an activated sludge unit. A second study
cited by Pavoni and Tittlebaum (1069) indicated that capsulated
organisms (klebsiella, aerobacter) are better able to survive
in the air than acapsulate organisms (escherichia) . The suit-
ability of coliforms and coliphages as animal virus indicators
was the subject of research by Fannin et al . (400). Evidence
collected from both trickling filter and activated sludge plants
showed coliforms to be far less stable than coliphages in the
airborne state. On the basis of this evidence, it was sug-
gested that coliphages may prove to be far more acceptable^
indicators of airborne animal viral contamination than coliforms
266
-------
Most research to date, however, has relied upon coliforms as pri-
mary indicator organisms to determine total bacterial concen-
trations. The bacterial concentrations at various distances
from treatment units, which are reported in the literature by
a number of investigators, are given in Table 94. This table
represents a sample of the available literature on activated
sludge and trickling filter plants.
The Adams and Spendlove paper (2) is unique in that it
reports recovery of airborne coliforms as far as 0.8 mi down-
wind from a large trickling filter plant. In contrast,
Hickey and Reist (568) cited one study in which no Escherichia
coli was found beyond 100 ft, and a second study that reported
no observable effects at greater than 150 ft downwind from a
trickling filter. Napolitano and Rowe (983) offer data show-
ing duplicate samples with coliform concentrations that differ
by as much as two orders of magnitude.
Relatively few investigations involved the recovery of
actual pathogens. According to research reviewed by Hickey
and Reist (568), of the total bacteria recovered near aeration
tanks, 10.5 percent were klebsiella, aerobacter or proteus
organisms. Despite repeated long-term sampling, neither the
shigella nor salmonella bacteria were recovered near the tanks,
a finding that was expected considering the small numbers of
these genera found in wastewater. Airborne Stapjry_J_o_coc_c_us aureus
hemolytic streptococcus, mycobarerium, and a cTcf-'fa s fTa c fl 1 i w e r e
also isolated.
A study conducted by Fanniri et al. (400) evaluated animal
virus concentrations. No animal viruses were found in aerosol
emissions from activated sludge and trickling filter plants
with sewage containing about 100 plaque-forming units (pfu)/-£.
Airborne coliphage viruses and coliform bacteria were re- -
covered at average levels of .23 to .3/m3 and 210 colonies/m ,
respectively. As shown in Table 94, the average coliphage
concentration decreased with distance from the source, but
only the coliforms showed a statistically significant decrease.
Fannin et al. compared the ratio of airborne coliphages to
coliphages found in sewage w'th the level of animal viruses in
sewage and calculated that, the expected concentration of
airborne animal viruses is 6.2-6.5 x 10~5/rn3 (Most Probable
Number).
In summary, the literature indicates that activated
sludge and trickling filter units emit potentially hazardous
bacterial aerosols and low levels of airborne animal viruses.
The concentrations of viable organisms generally decrease
rapidly with distance from the source, the rate of decrease
depending on such variables as wind speed, relative humidity,
solar radiation, air temperature, and obstructing vegetation.
267
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Poon (1099, 1100) used Escherichia coli to investigate the
effects of different factors on the viability of airborne
bacteria and to determine the mechanism involved in bacterial
destruction. His studies indicate that the destruction in-
creased in direct proportion to dryness of air and increased
exponentially as temperature increased. Sodium chloride in
bacterial aerosols affected the destruction by retarding water
evaporation from within cells. Webb (1463) concurred that
water evaporation is responsible for the destruction of
bacterial aerosols in his study of Serratia marcescens,
Escherichia coli. Staphylococcus albus. and Bacillis subtil is.
Both Poon and Webb conducted their research under labora-
tory conditions. Results of field studies have not always
proved as consistent. The expected correlation between the
number of colonies recovered downwind from activated sludge
tanks and air temperature was not substantiated by Ledbetter
and Randall (766). Higher rates of bacterial recovery were
found to occur when wind speed or relative humidity was high.
Data from these tests also revealed that the rate of bacterial
die-off was characterized by two distinct phases: an extremely
short and rapid initial die-off followed by stabilization, and
a very slow die-off rate for the more resistant organisms.
A study cited by Hickey and Reist (568) indicates that
the downwind travel distance of the viable aerosol from waste-
water sprays increases as both relative humidity and wind
speed increase, but will decrease with increasing ultraviolet
radiation. It was estimated that coliform organisms may
remain viable as far as 400 m downwind from the source under
conditions of darkness, 100 percent relative humidity, and
wind speed of 7 m/sec.
In recent years, spray irrigation has become popular for
municipal wastewater and liquid sludges. Consequently, some
studies have been made of the problem of biological aerosols
generated by spray irrigation. Coliform bacteria were found in
the air 350 m downwind from wastewater spray sprinklers by
Katzenelson and Teltch (685). Their research program consisted
of air sampling performed at various distances downwind from
the line of irrigation. Bacterial colonies suspected to be
of salmonella species were examined. Only one salmonella
bacterium was found during the sampling, at a distance of
60 m. Salmonellae are relatively rare in wastewater, so this
result was not surprising. However, the detection of even
one pathogenic salmonella in the air was felt by the authors
to have important public health implications. The authors
also calculated, on the basis of their findings and normal
breathing volume, that an individual working at a distance of
100 m from a wastewater sprinkler would inhale about 36
coliform bacteria every 10 min.
271
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Sorber et al. (1302) calculated the health hazards
posed by viral and bacterial aerosols released in spray irriga-
tion of wastewater. Calculations were derived from a model
developed to ascertain the effects of varying degrees of
treatment and meteorological conditions on virus viability.
On the basis of this model, the authors determined that within
10 min, up to 20 infectious units of airborne virus could be
inhaled by an individual working 200 m downwind from the
irrigation site. The 200-m distance provided no definitive
safeguard, as significant numbers of enteri-c viruses were
were estimated to survive beyond this point. Increased
temperature, lower relative humidity, and sunlight reduced
the viability of such pathogenic microorganisms; however,
neither meteorological conditions or aerosol dilution by
diffus ion were judged to provide reliable pathogen reductions.
The authors suggest instead that removals be effected either
by treating wastewater before disposal or by allowing an
adequate buffer zone around the spray irrigation site. An
800-m buffer zone would provide a reduction of two orders of
magnitude in airborne virus concentration. Removal or destruc-
tion of wastewater-contained microorganisms by filtration or
disinfection prior to spray application - which would achieve
reductions of up to three orders of magnitude - was judged
to be a more certain method of reducing the aerosol hazard.
A recent project reported by Shuval et al . (1261) demonstra-
ted that spray irrigation of unchlorinated wastewater may in fact
have severe Implications for public health. The incidence ot
enteric communicable diseases at 77 agricultural settlements
practicing spray irrigation of wastewater was significantly
higher than at 130 kibbutzim studied, where no form of waste-
water irrigation was practiced. In the communities using
wastewater for crop irrigation, the incidence of shigellosis,
salmonel1osis, typhoid fever, and infectious hepatitis was two
to four times higher than in the control communities. Sig-
nificantly, no difference in the outbreak of disease caused by
enteric virus was noted between test and control communities
during the winter months, when no irrigation occurred. It
was concluded that effective viral and bacterial disinfection
is required if spray irrigation or land disposal of wastewater
takes place near residential areas.
Research evidence indicates that biological pathogens
are present in wastewater aerosols and that these pathogens
may be inhaled by man with serious consequences to human
health. However, precise information on the minimum dose
of these organisms required to produce human infection is not
yet available. This problem is one that ought to receive
increasing attention as wastewater reuse for irrigation becomes
more widespread.
272
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DRINKING WATER
CHEMICAL COAGULATION/FLOCCULATION FOLLOWED BY SOLIDS SEPARATION
Introduction
Chemical coagulation and flocculation, followed by clari-
fication oMr filtration, is common water treatment practice for
the treatment of surface waters. The primary purpose is to
remove suspended and colloidal solids.
The overall process takes place in three distinct phases.
Coagulation involves destabi1ization of the colloids by rapid
mixing of the chemical coagulant with the water in some type
of agitated rapid mix tank. Retention time in rapid mixing
is very brief, on the order of a few minutes. Flocculation
follows in which the wastewater is gently stirred with paddles,
allowing the particles to collide and aggregate into larger
floes. Depending on temperature, concentration of the solids,
and the type and dosage of coagulant, flocculation requires from
15 minutes to one hour. Clarification and/or filtration
usually follows, to provide solids separation.
Commercially available flocculator-clarifier units (often
called solids contact units) combine all three operations in
a single compartmented tank. In a typical design, coagulant
is fed and mixed with the wastewater at the influent pipe;
flocculation occurs in a central cone-shaped skirt where a high
floe concentration is maintained. Flow passing under the skirt
passes up through a solids blanket and out over surface weirs.
These units are particularly advantageous for lime softening of
hard water, since the precipitated solids help seed the floe,
growing larger crystals of precipitate to provide a thicker
waste sludge. Recently, flocculator-clarifiershave been receiv-
ing wider application in the chemical treatment of industrial
wastes and surface water supplies. The major advantages promot-
ing their use are reduced space requirements and less costly
installation. However, the unitized nature of construction
generally results in a sacrifice of operating flexibility.
The primary substances used as coagulants are described
below:
1. Aluminum sulfate + calcium carbonate
A12(S04)3 + 3 Ca(HC03)2 = 3 CaS04 + 2 A1(OH)3 + 6 C02
273
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2. Aluminum sulfate + sodium aluminate:
6NaA10o -t- AT,(SO,). . 18 H50 + 8A1(OH), + 3Na0SOA +
6H20 ^443 i 6 24
3. Aluminum chloride (used under exceptional circumstances
only):
2 A1C13 + 3 Ca(HC03)2 = 2 A1(OH)3 + 3 CAC12 + 6 C02
4. Aluminum sulfate + hydrated lime:
A12(S04)3 + 3 Ca(OH)2 = 3 CaS04 + 2 A1(OH)3
5. Ferric sulfate:
Fe2(S04)3 + 3 Ca(HC03)2 = 2 Fe(OH)3 + 3 CaS04 + 6 C02
6. Ferric sulfate + hydrated lime:
Fe2(SO)3 + 3 Ca(OH)2 = 2 Fe(OH)3 + 3 CaS04
7. Ferrous sulfate:
FeS04 + Ca(HC03)2 = Fe(.OH)2 + CaS04 + 2 C02
8. Ferrous sulfate + hydrated lime:
FeS04 + Ca(OH)2 = Fe(OH)2 + CaS04
9. Ferrous sulfate + chlorine
2 FeSOA + 3 Ca(HCOo)0 + C10 = 2 Fe(OH), + 2 CaSOA +
CaCl2 -f 6 C02 J L *•
The most commonly used coagulant is A12(S04)3 . 18 H20,
which is known as filter alum. The amount of hydrolysis which
occurs when filter alum is introduced to the water is a function
of the pH of the water, with optimum efficiency achieved at a
pH of 7 to 8 (1062).
Exjstjng Literature and Research Presently Under Way
Because chemical coagulation and clarification is
probably the most popular water treatment technique, there
exists a substantial volume of information on this technology.
Table 95 summarizes the available literature located during the
study. As shown in the table, most research work has been
performed on the elemental group of contaminants as many of
the metals are most efficiently removed by chemical precipita-
tion. Substantial study of turbidity removal and virus in-
activation/removal have also been conducted. With the current
focus on synthetic/organic and biocidal contaminants in water
supplies and their potential carcinogenic effects with long-
term ingestion, a surge in research in these areas is anticipated
274
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TABLE 95. LITERATURE REVIEWED PERTAINING TO CHEMICAL
COAGULATION AND CLARIFICATION
Contaminants Reference Number
Water Quality Parameters
Asbestos 1637, 1638
COD 1243
Color 1243, 1620, 1645
Hardness 1607
Suspended solids 1595
Turbidity 1243, 1588, 1606, 1610, 1619, 1620, 1623,
1665
Elemental Contaminants
Antimony 1662
Arsenic 520, 531, 1244, 1590, 1596, 1610, 1643,
1655, 1669
Barium 1062, 1590, -1643,-1671
Cadmium 1590, 1610
Chromium 1610
Cobalt 1653, 1654, 1662
Iron 1605, 1610
Manganese 1605, 1610
Mercury 811, 1062, 1610
Molybdenum 1662
Nickel 1662
Selenium 1062, 1610
Vanadium
275
-------
TABLE 95 (continued)
Contaminants Reference Number
Biocidal Contaminants '
DDT 1662» 1664
Dieldrin 1662« 1664
Endrin 1652' 1654
Lindane 1664
Parathion 81
Synthetic/Organic Contaminants
PAH (Polynuclear
Aromatic Hydrocarbons) 1627
PCB 708
TTHM (total trihalo-
methanes) I676
Biological Contaminants
Bacteria 25, 103, 219, 380, 1168, 1243, 1382,
1510, 1600, 1601 , 1648, 1679
Virus 1168, 1600, 1601
276
-------
Water Quality Parameters
Asbestos has recently been implicated as a carcinogen of
potential danger to workers breathing the fiber in asbestos
manufacturing plants. Thus, it is feared that the incidence
of asbestos in drinking water supplies may also be a health
hazard.
Several studies have investigated the ability of chemical
coagulation followed by clarification and/or filtration to
remove asbestos from water intended for potable purposes.
Lawrence et al . (1638), examined the effectiveness of various
methods: straight filtration, diatomaceous earth filtration,
chemical coagulation and combinations. The most effective
method involved chemical coagulation with iron salts and poly-
electrolytes followed by filtration, which resulted in better
than 99.8 percent removal from water containing 12 x 10"
fibers/^ . The optimum ferric chloride dosage was found to
range from 6 to 8 mg/£ ; satisfactory floes were formed at all
test temperatures. Other reported removal efficiencies were
reported as follows:
% Asbestos Fiber
Treatment Removal
Ferric chloride, polyelectrolyte
coagulation and filtration 99.8
Graded sand filtration only 90
Diatomaceous earth filtration only 96.8
. Bentanite clay, polyelectrolyte
coagulation and filtration 99
As a continuation of the above effort, Lawrence and
Zimmermann (1637)studied the optimization of alum and polyelectro
lyte coagulation for asbestos removal. Optimum removals were
obtained with alum concentrations of 30 to 50 mg/t and poly-
electrolyte values of 0.3 to 0.6 mg/a . Asbestos removals^of
over 99.9 percent were achieved. Rapid coagulation and direct
filtration was also evaluated and the performance found to be
comparable to conventional treatment employing flocculation and
sedimentation. In addition, a survey of turbidities and fiber
concentrations for several municipal water supplies indicated
no correlation between these two parameters.
Shelton and Drewry (.1243) eval uated the effectiveness of
various coagulants in the removal of COD from a raw surface
water supply. Results are summarized in Table 96..
277
-------
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278
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They concluded that aluminum sulfate was the most effective
coagulant for COD removal. Cationic polyelectrolyte additions
were ineffective while anionic aids gave better results.
Color is caused by humus, tannins, weeks, algae, soluble
wastes, and to a certain extent, metals (1676) In itself, color
is not a health hazard; however, it signals the presence of dis-
solved organics and metals that may be of some health concern.
The above researchers evaluated color removal in the same inves-
tigation (1243). Ferric chloride was found to perform erratically
at differing dosages. Excellent removals were achieved at a
dosage of 35 mg/Ji, but at dosages around 50 mg/x,, color was
significantly increased. A study by Mangravlte et. al (1645)
showed that removal of humic acid (one source of color in water
supplies) by microf1otation produced the same high percentage of
removals as the conventional coagulation/sedimentation technique,
but at a rate of 5 to 13 times faster. Fulton and Bryant (1620)
investigated the use of alum with 18 coagulant aids for color
removal. Optimum alum dosages ranged from 20 to 25 mg/a and
successfully lowered the color concentration to below five stan-
dard units. The use of iron salts, oxidation, adsorption, or
polymers alone could not achieve this level of removal.
Hardness removal (CaH and MgH ions predominantly) via time-
soda precipitative softening is a common practice at many water
treatment facilities. Soft water has generally been considered
beneficial in that it reduces the usage of soap and detergents,
tastes better, and reduces scaling and precipitation in pipes
and water heaters. However, some recent studies, summarized by
Cooper (1607)have discovered an apparent inverse relationship
between hardness and heart disease; i.e., people drinking soft
water showed a higher incidence of heart disease than those using
hard water supplies. In light of these results, the overall
benefit of the softening process may have to be reevaluated.
Suspended solids removal from water supplies by coated
and uncoated diatomite filter was evaluated by Burns et al . (1595)
They found that special polyelectrolyte coatings were useful
for a final polishing filter process, but that these aids were
not as effective as conventional filter aids where large amounts
of suspended solids had to be removed.
Turbidity is a uniformly measured water quality parameter
specifying the visual clarity of the water. Turbidity is caused
by clay and other colloidal matter which in themselves are of
no health concern. However, heavy metals, virus, and bacteria
may be adsorbed onto the clay particles, and the removal of
turbidity can be of importance in regards to potential long-term
health effects. Because of its popularity as a quality test,
many studies of turbidity removal have been performed as
summarized below. Robinson (1665) compared the effectiveness of
279
-------
alum versus polyelectrolytes for removal of turbidity from muddy
surface water. Figure 22 summarizes the performance he reports.
Figure 22.The effectiveness of a small
amount of N 607 polymer relative to
Alum for raw water with a turbidity of
1-250 Otu
Fulton and Bryant (1620) 1nvestigated turbidity removal at
a pilot plant treating water from the Croton watershed of New
York City. They found that although alum coagulation (with
coagulant aids) could produce water below the 1.0 TU Federal
Standard, the American Waterworks Association (AWWA) goal of
0.1 TU could not be achieved without further treatment.
Middlebrook et al . (1588) studied the optimum values for opera-
tional variables in turbidity removal (alum dosage, flocculation
time, and paddle speed).
The following conclusions were drawn from this research:
1. The most significant independent variable was the
paddle speed followed by flocculation time and alum
dosage.
2. All variables and their first order interactions were
significant at the 1 percent level.
3. The optimum alum dosage was 25 mg/jj, for the conditions
under which the study was performed.
280
-------
4. The optimum paddle speed ranges between 40 and 50
rpm.
5. The optimum flocculation time was approximately 30
min.
6. This study revealed that the significant interactions
between the independent variables (alum dosage, floc-
culation time, and paddle speed) can be utilized in more
efficient water treatment. For example, a higher
percentage removal of turbidity can be obtained by
using low alum dosage and increasing the flocculation
time and/or paddle speed. On the other hand, high
alum dosages and reduced flocculation times and/or paddle
speeds can be utilized.
7. The study shows the importance of the following equip-
ment and methods in the removal of turbidity in water
treatment plants:
a. Variable speed flocculator paddles.
b. Multiple flocculation basins that can be used in
series or parallel operation.
c. The use of jar tests to determine the optimum alum
dosage continuously during the operation of water
treatment plants.
Gruninger et al.(1623) compared the performance of ferric
chloride versus alum as the primary coagulant and found that
the combination of 8 mg/a FeCL-i + 4 mg/£ bentonite clay + 0.25
mg/5, polymer provided comparable performance to the system with
alum and clay; there was approximately 95-98 percent turbidity
removal .
Reference 1610summarizes the performance of various treat-
ment technologies in removing turbidity. These results are -
• Plain sedimentation: 50 to 95 percent, depending
totally on the settling characteristics of solids
• Coagulation with sedimentation: 80 to 99 percent
• Rapid sand filtration: 80 to 99 percent with influent
turbidity of 10 JTU or less
• Slow sand filtration: 80 to 99 percent with influent
turbidity of 10 JTU or less
• Diatomite filtration: 80 to 99 percent with influent
turbidity of less than 10 JTU.
281
-------
Shelton and Drewry (1243) analyzed the effectiveness of
different cationic, nonionic, and anionic polyelectrolytes in
reducing turbidity. Table 96, presented earlier, displays their
results. Aluminum sulfate with anionic coagulant aids was found
to be the most effective, achieving 99+ percent removal at a
10 mg/£ dosage. Frissora (1619) evaluated the performance of
rapid multimedia filtration alone on turbidity removal and
achieved removals of 96 to 99.7 percent at high loading rates of
4 to 16 gpm/ft2. Conley (1606) al so studied rapid filtration
preceded by chemical coagulation and settling, for turbidity
removal at a number of water treatment plants around the country
Table 97 summarizes the results of his study; removals ranged
from 80 to 97 percent and averaged 94 percent.
EJemental Contaminants
Many elemental contaminants are readily removed by chemical
coagulation and subsequent solids separation steps (settling or
filtration). As some of the elemental contaminants are being
more closely reviewed for possible long-term health effects, the
importance of chemical coagulation as a removal process becomes
more pronounced.
TABLE 97. TYPICAL THREE-MEDIA HIGH-RATE FILTRATION PLANT PERFORMANCE
Location
Regina, Sask.
Siler City, N.C.
Pasadena, Tex. (industrial)
Corvallis, Ore.
Ocaquan, Va.
Samoa, Ca. (industrial)
Fort Lauderdale, Fla.
Knoxville, Tenn.
Albany, Ore.
Longview, Tex.
Paris, Tex.
Newport, Ore.
Norristown, Pa.
Springfield, Mo.
Winnetka, 111.
Stanton, Del .
Turbidity
Applied Filtered
JTU JTU
0.5
1
3
3
1
10
1
1
2
4
10
3
6
1.5
2
2
0.1
0.2
0.5
0.2
0.1
0.5
0.1
0.2
0.2
0.2
0.3
0.2
0.3
0.2
0.3
0.2
Filter
Rate
gpm/ft2*
4
5
6
3
4
5
4
5t
5
3
3
4
4
4k
5
4
Filter
Runs
hr
30
30
40
50
48
18
80
60
20
48
50
20
45
24
15
30
Backwash
Water
percent
2
2
1
1
1
2
1
1
2
2
2
3
1
1
2
3
* Typical summer peak daily flow rate. Hourly peaks
are generally in the range of 4-6 gmp/sq ft.
t Under test. Some filters are out of service so
that rate could be increased on remaining filters.
282
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Arsenic is one element being closely watched in water sup-
plies as it has a relatively high toxicity, accumulates in the
body, and has been associated with the occurrence of cancer (1590).
Some 1,056 cases of black-foot disease and skin cancer have been
reported in the southwest part of Taiwan. According to statis-
tical data, there is a close relationship between these diseases
and' the high arsenic content (0.6 to 1.0 mg/£) in deep-well water
used for drinking (1669). Since there is no other available
water in the area, some practical and economical method to remove
the arsenic compounds was urgently needed. To satisfy this need,
Sher, (1144) performed a lengthy analysis of treatability tests
to evaluate the arsenic removal capability of coagulation/settling/
filtration processes. Initial coagulant tests showed ferric chlo-
ride to be the best chemical, achieving 92 percent As removal at
a 30 mg/£ dosage. Subsequent testing, however, showed that these
removals could be improved by preoxidation before coagulation.
Adding 20 mg/£ of chlorine and then coagulating with 50 mg/£ of
ferric chloride provided the best results, achieving 98.7 percent
As removal.
Gulledge and 0'Connor (520)showed that As removal was
affected by pH and doses of suitable coagulants. Arsenic
adsorption onto ferric hydroxide exceeded adsorption onto
aluminum hydroxide. For both coagulants, increased dosages
(up to 50 mg/£) resulted in increased removal. A significant
decrease in arsenic removal was seen at pH over 8.0.
Logsdon et al . (1643) studied arsenate removal by precipi-
tation with ferric sulfate and alum, in pilot plant tests.
For initial arsenic concentrations of 0.3 mg/£, ferric sulfate
treatment yielded 91 to 94 percent removal. Dual media
filtration achieved an additional 5 to 7 percent removal for
overall removals of 98 to 99 percent and effluent levels of
0.003 to 0.006 mg/£ arsenic. Alum treatment was less effective,
yielding 75 to 79 percent removal without filtration and 85 to
92 percent removal with filtration (531) Arsenite removals
of only 10 to 25 percent were achieved by alum, and 40 to 60
percent by ferric chloride. However, when chlorination preceded
coagulant addition, removals equivalent to those reported for
arsenate were observed (531). Chlorine apparently oxidized the
arsenite to arsenate. For ferric sulfate precipitation, treat-
ment efficiency remained constant from pH 5.5 to 8.5. Above
this pH, efficiency declined. With alum, optional precipi-
tation pH was at 7.0, with slight reduction in efficiency at
pH below 7.0, and rapid drop-off in removal efficiency at pH
above 7.0. Similar pH effects for arsenate treatment by iron
and aluminum salts have been observed in another study (1655).
Calmon (1596) found that cold lime-soda precipitation with
filtration was capable of removing 96.4 percent of the arsenic,
whereas ferric sulfate removed less than 50 percent.
283
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The toxicity of antimony is similar to arsenic, although
less acute. Very little research has been conducted related
to Sb, as other metals appear to be of more importance from
a health-effects standpoint. Lime coagulation has been shown to
provide Sb removals of better than 90 percent from wastewater
effluent (1662). Similar removals may be possible in water
supply treatment, but no data were found.
Barium is a toxin that acts as a muscle stimulant. As
such, it strongly affects the heart muscles and causes high
blood pressure and nerve blockage (1590). Barium removal -
only for wastewater treatment - was reported by several re-
searchers. Sigworth- and Smith (1671) found during pilot waste-
water plant tests that lime coagulation and settling was an
effective method, resulting in a 99 percent Ba removal. Dosage
rates were 45 mg/£ FeCl3, 260 mg/£ lime plus 20 mg/£ FeCl3 for
the low lime test, and 600 mg/£ lime for the high lime run.
Logsdon (1643)found improved removals with the lime softening
process. Treatment efficiency was pH dependent, increasing
to a maximum of 98 percent at pH 10.5, and dropping off at
higher pH values. Barium is not appreciably removed by ferric
or alum coagulation.
Cadmium has a high toxic potential, accumulates in various
organs of the body, and is a causative factor in high blood
pressure (1610). Only minute traces of cadmium are found in
natural waters. However, several industries discharge cadmium
in their wastewaters, including metallurgical alloying,
ceramics manufacture, electroplating, inorganic pigments,
textile printing, chemical industries, and acid mine drainage.
Very little data are available regarding the use of coagulation
for Cd removal at water treatment plants. The Summary Reference
(1610) lists removal s at 50 to 90 percent with coagulation followed
by filtration. Unpublished data developed by EPA indicates
that lime softening and ferric sulphate coagulation above pH 8
achieves Cd removals of over 98 percent.
Chromium in the hexavalent form is highly toxic to man
and has been shown to be carcinogenic to man when inhaled.
Volkert and Associates, in a study for EPA (1610) summarized
that coagulation and sedimentation with filtration is capable
of removing 50 to 90 percent of the insoluble chromium (Cr)
forms present in water supplies.
The hexavalent form is much more difficult to remove with
typical water treatment coagulants than is the trivalent form.
It is desirable, therefore, to reduce the chromium present
to trivalent prior to treatment. Laboratory studies by EPA
(unpublished) indicate that trivalent chromium is removed at
284
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better than 95 percent levels by ferric sulphate up to pH
9.5, removed at 90 percent levels by alum up to pH 8.5, and
removed at 98 percent level by lime softening at pH from 10
to 11.5. Hexavalent chromium, however, is not effectively
removed by any of these coagulants. Cobalt (Co) concentration
in potable water sources seldom reaches levels that require
special consideration. Cobalt is currently best treated by
lime coagulation, although as much as 2 mg/£ may be left in
the effluent (1662). Ni 1 sson (1654) found that lime coagulation
was capable of achieving 88 percent removal of cobalt. Another
study (1653)found that cobalt precipitation could be enhanced
by the addition of chitosan or a chelate as a polishing agent.
An EPA study (1662) concluded that similar precipitation techni-
ques are also applicable to molybdenum (Mo), nickel (Ni), and
vanadium (V) removal.
Iron and manganese, often found together, are important
constituents of potable water supplies because they can import
unwanted aesthetic qualities. From a health standpoint, how-
ever, iron and manganese do not pose any significant threat
1n the concentrations normally found in surface and ground-
water supplies. Therefore, removal of these constituents will
not be discussed In any depth here. Effective removal can be
provided by aeration or more commonly, by chemical precipitation,
sedimentation, and filtration (1605).
Recent attention has been focused on the contamination of
water supplies by organic and inorganic mercury (Hg) by
industrial discharges. Fortunately, recent rests by the EPA of
273 water supplies across the country showed very low mercury
levels in nearly all of them. Even so, the performance of
conventional water treatment technologies and new techniques for
removing Hg from water is of interest. Logsdon and Symons (811)
investigated the efficiency of conventional water treatment
processes in removing Hg. Bench scale studies of chemical
coagulation and settling yielded the following conclusions:
1. Mercury removal during coagulation was related
mainly to adsorption of mercury onto the
turbidity-causing agents in the water.
2. In raw waters with low turbidity, ferric sulfate
was more effective than alum for removal of
inorganic mercury. Removals ranged from 40 to
60 percent over a turbidity range of 2 to 100
JTU's.
3. Removal by coagulation or adsorption onto turbidity-
causing agents was less for methyl mercury than
for inorganic mercury.
285
-------
4. Inorganic mercury removal by softening was most
effective in the pH range of 10.7 to 11.4 and
is thought to be related to adsorption onto
magnesium hydroxide floe.
5. Methyl mercury was not removed by softening.
The authors concluded by stating that as long as environ-
mental levels of mercury in raw water remain low (near drink-
ing water standards), extremely high removals will not be
required, and conventional technology should be sufficient.
Molybdenum can occur naturally in drinking water supplies
at concentrations up to 20 yg/£ due to weathering of minerals.
It can also be found in water as a result of waste discharges
from industries related to the manufacture of glassware,
ceramics, printing inks, electrical equipment, and certain
steel alloys. Virtually no data relative to molybdenum removal
from water supplies are available, because molybdenum is not
currently seen as a primary health hazard.
Nickel occurs naturally at concentrations up to 0.072 mg/£
with an average concentration of about 0.005 mg/£. Wastewater
discharges from industries associated with nickel-plating,
nickel alloying, storage battery manufacturing, organic hydro-
genation, and the manufacture of nickel-chrome resistance wire
can contribute to the presence of nickel in water sources (43).
In large doses, Ni can be harmful; however, in this country,
natural concentrations are low, and lime coagulation appears to
be successful in removing large percentages of Ni from waste-
water. No literature pertinent to Ni removal by water treatment
facilities was found.
Alum and ferric sulfate coagulation and lime softening
are only moderately effective for selenite (Se+4) removal,
and are largely ineffective for selenate (Se+6) removal (1643).
Studies with ferric sulfate (30 mg/£) at a pH of 5.5 yielded
removals of 85 percent from river water containing 0.03 mg$e + %.
Removals decreased as the pH increased. The maximum achievable
Se+4 removal with alum (100 mg/£, pH 6.9) was 32 percent. A
maximum removal of 45 percent was obtained with lime softening.
No conventional method achieved greater than 10 percent removal
of Se+6.
No data were located relative to vanadium removal from
water supplies. In wastewater treatment, however, very good
vanadium removals were achieved via coagulation with iron or
aluminum salts or chitosan polymers (1662).
286
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Biocidal Contaminants
Recently, there has been increased awareness of the
potential health hazards of biocidals. Limited data, however,
are available in the literature regarding the removal of
these constituents from water supplies by chemical coagulation
Robeck et al. (1664) studied the effects of various water treat-
ment processes on pesticides. Their results, in regards to
pesticide removal via chemical coagulation (alum) and filtra-
tion, are shown in Table 98 below.
TABLE 98. PERCENTAGE OF PESTICIDE REMOVED BY
CONVENTIONAL WATER TREATMENT
Coagulation and Filtration
Pesticide Load - ppb
1 5 10 25
Lindane <10 <10 <10
Dieldrin 55 55 55
DDT 98 97
Parathion 20
2, 4, 5-T ester 63
Endrin 35 35
* Total hardness as CaCOs reduced from 260 to 33 ppm
and pH increased from 7.6 to 10.4.
As can be seen, DDT was readily removed, whereas lindane,
parathion, and endrin were not. Dieldrin and 2, 4, 5-T ester
are removed at slightly better than 50 percent. Softening
with lime and soda ash and with an iron salt as a coagulant
did not improve on the removals obtained with alum coagulation
alone.
Another study (1640)evaluated the effect of KMn04 as an
oxidant and precipitating agent. It was found that KMn04 was
not significantly effective in removing lindane, but was
capable of removing over 80 percent of the heptachlor present
in under 5 hours. Removals of DDT were less than 20 percent
in 48 hours, and endrin was totally unaffected by the process.
287
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Synthetic/Organic Contaminants
In recent years, concern has been expressed over the
possible occurrence of certain carcinogenic compounds 1n
drinking water (World Health Organization, 1964). A group
of compounds which has received particular attention 1s the
polynuclear (polycyclic) aromatic hydrocarbons (PAH), some .
of which are potent carcinogens under certain conditions. It
1s, however, far from certain that these compounds are signi-
ficant when present 1n the trace amounts found 1n drinking
water. Clearly, further research 1s needed into both the
levels and health effects of PAH in the environment (1627).
Harrison et al. conclude (1627): "The reliability of much
of the Information concerning the removal of PAH by conven-
tional water treatment processes is open to considerable doubt.
Field experiments have frequently ignored retention times
within the works, and hence been rendered unreliable at the
sampling stage. Laboratory studies have commonly used unreal-
istic high concentrations of PAH, and the high removals achieved
may be largely explained often by the low solubility of the
PAH themselves. Further analytical work is required in this
field, and fundamental studies of the chemical changes that
occur upon chlorinatlon of these compounds at low concentrations
are necessary. Increasing water reuse makes the need for this
type of Information particularly acute."
After the EPA disclosed Its findings of organic chemicals
in New Orleans' water, 1t was decided to conduct another,
more Inclusive study at specific sites across the U.S. In
this study, Symons et al. (1676) found that precipitative softening
at water treatment plants increased the concentration of tri-
halomethane in the product water from an average of 0.49 ym/£
(80 locations) to 0.84 ym/£ (17 plants with softening). This
Indicates that chlorlnation at a higher pH will produce higher
concentrations of trihalomethanes.
Klnoshita and Sunada (708) performed an experiment
on the removal of PCB by chemical coagulation. Bentonite,
sodium carbonates, and aluminum sulfate were added to a solution
of 100 ppb PCB. After settling, the PCB concentration has been
reduced 90 percent, suggesting that conventional water treat-
ment by coagulation and settling or filtration provides a margin
of safety against the ingestion of PCB's in raw water supplies.
Biological Contaminants
The use of ulatcnite filtration with and without chemical
addition is capable of removing bacteria from water supplies,
Mclndoe (1648) n'!;rin.-r1 zed research in this area as follows:
288
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t Work by the U.S. Army Engineering Research and
Development Laboratories at Fort Belvoir, Virginia,
showed that a diatomite filter using a coarse grade
of filter aid was capable not only of 100 percent
removal of the entamoeba cysts, but also of partial
removal of other pathogenic organisms. Work done
at Rutgers University has shown that even the
coarsest grade of diatomite gave coliform removals
of greater than 50 percent for influent levels of
210 to 1300/100 m£. Finer grades gave "complete"
coliform removals of influent levels up to several
thousand per 100 ml.
• Work by S. L. Chang (1600, 1601) and J. V. Hunter
(617) with solutions of iron salts added to bacteria-
contaminated water has indicated a reaction takes
place between the iron ions and the protein sheath
of both bacterial and viral organisms. Subsequent
removal of the iron by the diatomite MgO process
has produced total count reductions on the order of
99 percent, with fecal strep and Escherichia coli
counts of zero.
• Waters so clarified would be expected to be readily
disinfected by usual practices.
Amirhor and Englebrecht (25) also analyzed the potential
use of uncoated and polyelectrolyte -aided diatomaceous earth DE
filtration for bacterial virus removal. They concluded that all
uncoated DE filtration was not effective for virus removal,
but that precoating of cationic polyelectrolyte greatly
improved removals. Certain variables such as pH, level and
concentration of polyelectrolyte coating, and virus concentra-
tion affected removals.
Wolf et al . (1510)conducted a large-scale pilot study of
virus removal by both lime and alum. They demonstrated that
virus removals from secondary effluents by alum coagulation-
sedimentation and coagulation-sedimentation-filtration pro-
cesses are essentially the same as described in the literature
using smaller-scale processes. Removals of bacterial virus
as high as 99.845 percent for coagulation-sedimentation and
99.985 percent for coagulation-sedimentation-filtration pro-
cesses were observed at an Al:P ratio of 7:1.
At a lower alum dose there was a marked decrease in virus
removals. At an A1:P ratio of 0.44:1, removals of only 46
percent of f£ coliphage and 63 percent of polio virus by the
coagulation-sedimentation process per se were observed.
289
-------
High lime treatment of secondary effluents achieved
very high degrees of virus removal, but the percentage has not
yet been quantified.
Englebrecht and Chaudhuri (219) conducted a study to extend
the knowledge in this field. Their conclusions follow:
1. Chemical coagulation and flocculation is an
effective process in removing viruses from
water. Removals in the range of 98.0 to 99.9
percent can be expected.
2. The presence of bivalent cations like calcium
and magnesium up to a concentration of 50 mg/£
each does not interfere with the efficiency of
the process.
3. The efficiency of virus removal is reduced when
the raw water contains organic matter.
4. Intelligent use of commercially available
cationic polyelectrolytes with or without
hydrolyzed metal ions may markedly increase
the efficiency of the coagulation and floccula-
tion process in removing virus.
5. Virus particles remain active in the settled
sludge following their removal from water by
coagulation and flocculation, and can be recovered
from the floe by various eluants. Therefore,
proper care should be taken in sludge disposal.
Thorup et al . (1382) conducted a study to determine the
effectiveness of polyelectrolytes used as coagulant aids
for the removal of virus from artificially seeded water. They
found that the cationic polyelectrolyte performed more
acceptably than the anionic and nonionic types and was benefi-
cial in aiding floe formation under conditions of poor coagula^
tion. However, the 80 to 94 percent removal achieved under
these circumstances was well below the 99+ percent usually
considered acceptable. In instances of adequate coagulation,
however, cationic polyelectrolytes did not increase virus re-
moval beyond the levels obtained with unaided Al2(S04)3 or
coagulation.
290
-------
Shelton and Drewry(1243) performed a literature search of
virus (f2 bacteriophage) removal via coagulation and, based
on the results, studied the effectiveness of different chemical
coagulants and polyelectrolytes for this purpose. Their
conclusions were:
1. Aluminum sulfate, ferric chloride, and ferric
sulfate are the most promising of the group
of primary coagulants tested, from the stand-
point of f2 bacteriophage removal, all produc-
ing greater than 99 percent removal. Aluminum
sulfate is considered to be the most effective
coagulant, whereas ferric chloride and ferric
sulfate are comparable and less effective.
2. The cationic polyelectrolyte tested is not
satisfactory as a primary coagulant because of
its poor floe formation and settling characteris-
tics. Virus removals with the cationic flocculant
were only moderate (92 percent).
3. Anionic, nonionic, and cationic polyelectrolytes
have only minor significance in virus removal.
It is noted, however, that the anionic coagulant
aids are useful in widening the effective dosage
range for good virus reduction. The nonionic
coagulant aids give moderately better results,
which are attributable to an ability to form more
dense and "sticky" floe. This improvement of virus
removal is indirect, because the nonionic poly-
electrolytes do not form a virus-ion complex with
the virus protein coat. The cationic coagulant aid
produces a moderate improvement in virus removal;
however, it is questionable if this improvement
would be economically justifiable for a full-
scale operation.
4. The use of sodium aluminate with aluminum sulfate
does cause a marked increase in virus removal,
to 99.9 percent overall. This increases however,
could be used only for "special-case" situations,
since the sodium aluminate dosage for optimum virus
removal is not compatible (by a factor of 3) with
turbidity and COD optimums.
Thayer and Sproul (1679)of the University of Maine did
extensive research concerning the effects of water softening
upon virus inactivation. Their primary objective was the
determination of the effect of chemical precipitation in water
291
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softening upon bacterial viruses. Inactivation of T2 virus
varied widely, with the best results, on the order of 99.999
percent inactivation, occurring when magnesium hydroxide was
the only precipitate formed. The standard excess lime-soda-
ash process also produced good results with about 99.45 per-
cent virus reduction.
Lime flocculation with rapid sand filtration, a long-used
standard water-treatment method, was investigated for its
virus-removal characteristics by Berg et al . (103) at the
Cincinnati Water Research Lab. Conclusions based on their
study using polio virus I (LSC nacuine) exclusively were that
(1) flocculation of secondary effluent yielded up to 99.86
percent removal of the virus, dependent upon the coagulant
dose and the pH level attained, and (2) the total removal by
lime flocculation and rapid sand filtration through an 8-in-
deep filter achieved a maximum of 99.997 percent.
The ASCE Journal of Sanitary Engineering published an
article in 1961 summarizing the virus work done up to that
time (380). Table 99 shows the results of this work. As
shown, the dosage of flocculant alone is not a measure of the
efficiency of the process.
Robeck et al. (1168)investigated the fate of human viruses
in rapid filtration processes with and without flocculation and
settling. They found that if low alum doses were fed just
ahead of the dual-media filter (operating at 6 or 2 gp
more than 98 percent of the virus was removed. When the alum
dose was increased and conventional flocculators and settling
added, removals were increased to over 99 percent. When turbid
water was treated, a floe breakthrough was usually accompanied
by an increase in virus penetration. Polyelectrolyte doses
as low as 0.05 mg/£ increased floe strength and helped to
prevent such breakthroughs.
The current state of knowledge indicates that chemical
flocculation, settling, and filtration are effective in remov-
ing virus from water. Removals of gg^percent have been reported
under proper operating conditions. However, more research is
still needed in the area to fully determine the most effective
doses of coagulants and coagulant aids, the physiochemical
effects of turbidity, pH, temperature, and colloidal charge,
and to develop optimal operating parameters.
292
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TABLE 99. REDUCTION OF HUMAN ENTERIC VIRUSES IN
WATER BY CHEMICAL FLOCCULATION
Flocculatlon Process
Virus
Polio
Polio
Infectious
hepatitis6
Coxsackie A5
Coxsackie A2
(purified)
Type of Water
Tap
Raw
River
Distilled
Spring
Ohio River
(16-255ppm
turbidity)
Stages
1
1
1
1
1
1
1
1
1
1
2
2
Coagulant
Added*
ppm
100
100
136
410
136-273
273-546
69
28-45
15
25
15
15*
25
25*
Floe Amount
or
Description
0.4-1.03
mi per 1
1.5-2.2
mi per 1
Good
Very good
Very good
Very good
Very good
Very good
Virus Removal
L1ttleb
Some0
Some to
s1gnificantd
Some
Little to some
Significant
Little to some
Some
95.7% at 25°C
95.9% at 5°C
98.6% at 25°C
99.8% at 25°C
99.6% at 5°C
99.9% at 25°C
Alum except where marked with an asterisk; asterisks
indicate ferric chloride.
bProbably less than 25%.
cProbably less than 50%.
dMore than 50%.
eGauze-strained fecal suspension in distilled water.
293
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Chang et al.(T601) performed comprehensive studies of the
dynamics of removal of bacterial virus by aluminum sulfate
flocculation. From their observations they concluded:
1. Flocculation by aluminum sulfate can remove high
percentages of virus, and within the zone of
f1occulation, higher doses produced greater
effi ciency.
2. The virus is concentrated in the floe sediment
and is not destroyed, but only temporarily
inactivated. It will become active again, if
dissociated from the aluminum.
3. Virus inactivation is believed to be the result
of the formation of an aluminum protein salt
in the virus.
Chang et al. performed another study (1600)evaluating the
efficiencies of alum and ferric chloride in removing coxsackie
and bacterial viruses. They analyzed the effects of coagulant
dosage, pH, and rate and method of stirring on virus removal.
A 40 mg/£ dose of A^CSO^s yielded an 86.3 percent removal of
coxsackie virus and a 93.5 percent removal of bacterial virus.
Under similar testing conditions, 20 and 40 mg/£ of FeCl3
facilitated 96.6 and 99.3, and 98.1 and 99.9 percent removal
of these viruses, respectively.
294
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DISINFECTION
Introduction
Disinfection refers to the inactivation or destruction of
pathogenic microorganisms. Disinfectants (chlorine, ozone,
ultraviolet and ionizing /adiation) also have secondary applica-
tions, particularly as oxidants for the removal of organic con-
taminants. Both applications are included in the literature
pertaining to the treatment of drinking water with disinfectants
(Table 100).
In the United States, the traditional disinfectant is
chlorine, which is usually applied to the water in gaseous form
as the last treatment step. The chlorine gas (Clo) reacts with
the water to form hypochlorous acid (HOC!), which dissociates
at pH values above 7 to form the hypochlorite ion (OCl") (651).
Occasionally hypochlorous acid, hypochlorite, or chlorine dioxide
(CI02) are used instead of chlorine gas.
After chlorine, the most popular disinfectant is ozone,
especially in Europe. Ozone (03) is an unstable gas and must be
generated at the site and used immediately. It is a powerful
oxidant. Both its germicidal and oxidizing properties seem to be
the result of the formation of several free radicals in water
(H02> OH, H03+), which will attack almost all organic compounds.
Ultraviolet and ionizing radiation have been used in pilot
plant and small industrial applications. Like ozone, they seem
to act by forming a series of free radicals in water, which can
attack organic bonds. Ultraviolet is incapable of acting at more
than a few centimeters depth, and both forms of radiation are
highly susceptible to interference from turbidity and suspended
matter. Ionizing radiation requires radioisotopes and the con-
comrnitant shielding and elaborate safety precautions.
All of the disinfectants have disadvantages that prevent
any of them from being universally applicable. For a given
situation the choice depends largely on the water quality, types
of microorganisms in the water, desirability of nondisinfection
applications, and cost.
295
-------
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296
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Water Quality Parameters
Although disinfectants are seldom specifically employed to
remove any of the water quality parameters, there are certain
chemical reactions that make the idea feasible. The reactions of
chlorine with ammonia are the best known. If allowed to go to
completion, the ammonia will be oxidized to nitrogen gas and will
thus be removed from the water. Ozone does not react with ammonia
(651). Ammonia is seldom an issue, since it is not a common con-
stituent of most water supplies.
The organics, as represented by BOD, COD, and total organic
carbon, in drinking water are susceptible to oxidation by disin-
fectants. However, reactions other than oxidation may produce
potentially hazardous compounds. For instance, Rook (1667) and
McClanahan (651) reported that chlorine reacted with humic and
sulvic substances, forming chlorinated organic compounds. These
chlorinated compounds are much more resistant than the precursor
compounds to both biodegradation and chemical oxidation. Con-
sequently they persist in a water supply that is not treated any
further than chlorination. Some of the chlorinated compounds
formed are suspected to have carcinogenic properties.
Ozone is even more reactive toward organic compounds than
is chlorine. With ozone, though, the reactions are almost exclu-
sively oxidation, with few if any hazardous compounds formed in
side reactions. The formation of ozonides and similar compounds
has been postulated, but there has been no evidence to data demon-
strating their formation during the ozonation of water. Morris
(1651) reported an increase in BOD after ozonation and attributed
it to the breakdown of nonbiodegradable organic molecules into
simple, degradable compounds.
Murphy (980) recently demonstrated that gamma radiation had
an oxidizing effect on organic compounds similar to that of ozone.
Ultraviolet radiation theoretically has a similar effect.
It should be noted that the use of chemical disinfectants
for oxidizing nonbiological contaminants interferes with the
primary disinfection role of these chemicals by consuming the
disinfectants. To achieve proper disinfection in high organic
waters, for instance, requires large increases in applied dosages.
Some water-borne disease outbreaks are attributed to improper dis-
infection of highly organic water supplies.
Elemental Contaminants
In general, the disinfectants have no effect on elemental
concentrations. Elements would have to be in a reduced state
before oxidizing disinfectants could have an impact. This is not
likely in most drinking water supplies. Exceptions are
297
-------
iron and manganese, which are more soluble in their lower oxida-
tion states. Morris (1651) reported that ozone readily oxidized
soluble iron and manganese to the insoluble oxides, which could
then be removed by sedimentation or filtration.
Trivalent chromium can be oxidized to the hexavalent form,
which is more toxic and difficult to remove with conventional
coagulation/filtration processes.
Biocidal Contaminants
Chlorinated hydrocarbon biocides are generally resistant
to chemical oxidations. Stone et al . (1662) reported that
chlorine was not a particularly effective oxidant for such bio-
cides. Ozone was more effective, but removal efficiencies
varied widely from 16 to 93 percent, depending on the type of
biocide, ozone concentration, and contact time (Table 101 ).
Stone et al. reported other ozone studies that yielded 50
percent removal of endrin, 75 percent removal of lindane, and
approximately 100 percent removal of dieldrin and alrin. They
also stated that ultraviolet radiation could completely elimi-
nate carbamate biocides, reduce aldrin by 45 percent, and reduce
endrin and dieldrin by 18 percent.
Buescher et al . (1594) studied the chemical oxidation of
chlorinated hydrocarbons in water. They included the following:
• Lindane concentrations in aqueous solutions were
readily decreased by ozonation and only partially
affected by potassium permanganate. Treatment with
chlorination, peroxides, and aeration had no measurable
effects.
• Aldrin in aqueous solutions was readily attacked by
chlorination, potassium permanganate, ozone and aera-
tion; peroxides had no measurable effects.
t Dieldrin concentrations in aqueouj solutions were
decreased by ozonation and aeration.
t Lindane and aldrin in aqueous solution were found to
be volatile. The degree of volatility may be an
indication of the susceptability of that pesticide to
chemical treatment.
• Lindane in the presence of other naturally occurring
trace organics found in river water was readily attacked
by ozonation, though aeration had only a minor effect.
298
-------
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299
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Synthetic/Organic Contaminants
As previously mentioned under "Water Quality Parameters,"
both chlorine and ozone readily react with dissolved organics.
However, synthetic organics are often more resistant to oxidation
than the natural organics. Rosenblatt (651) indicated that chlor-
ine reacted with many organics or give both chlorinated and oxida-
tion products, but that there was no reaction with many others
(Table 102). Ozone is an effective oxidant against the phenobics
and organic nitrogen compounds, but not against many of the sim-
pler organic molecules, such as ethanol. Harrison et al. (1627)
reported that chlorine was more effective than ozone against ben-
?o(a) pyrene.
Many of these synthetic organics, such as nitrobenzene, ben-
zo(a) pyrene, oniline, and ethyl benzene are reportedly carcino-
genic. While these chemicals are seldom found in drinking water
supplies at concentrations exceeding a few ppm, the postulated
no-threshold-dose character of many carcinogens makes even one
molecule a potential hazard. Note also that chlorine is suspected
of producing chlorinated organic compounds which may themselves be
carcinogenic.
Kinoshita and Sunada (708) investigated the effects of irra-
dation on PCB in water. They concluded that PCB in aqueous micro-
particulate colloidal solution is destroyed by ionizing irradation
(up to 95 percent), but that its resistance to radiation is far
greater than other chlorinated hydrocarbons used as penthachloro-
phenol or DDT, and other pesticides such as parathion. They also
found that the acute toxicity of the irradiated PCB solution was
far less than the nonirradiated solution for striped shrimps.
Biological Contaminants
The major application of disinfectants is against biological
contaminants. In this light, the disinfectants have been primar-
ily on their effectiveness in controlling biologicals (e.g., bac-
teria, viruses, protozoa, parasitic worms).
Chlorine is the traditional disinfectant in the United States.
It is effective to some extent against all types of pathogenic
organisms found in water. Bacterial kills of at least 99 percent
are considered normal (1662), and 4 to 5 log reductions are not
unusual. Both Sobsey (1291) and Long (815) reported virus reduc-
tions of up to 99.99 percent. Reference 257 summarized several
researches on virus destruction by chlorine as shown in Table 103.
Chlorine can be very effective against free-swimming protozoa and
parasitic worms. Chlorine has the further advantage of persistence;
given a sufficiently large dose, a low residual chlorine concentra-
tion will remain in the water after treatment, providing continued
300
-------
TABLE 102. PROBABLE REACTION PRODUCTS OF
CHLORINE AND SOME TYPICAL ORGANIC COMPOUNDS
FOUND IN POLLUTED WATER SUPPLIES (651)
Organic Compound
Probable Reaction Products
Alcohols
Methanol
Isopropanol
tert-Batanol
Ketones
Acetone
Benzene and Derivatives
Benzene
To!uene
Ethyl benzene
Benzoic acid
Phenol and Phenolics
Phenol
m-Cresol
Hydroqui none
Organic Nitrogen Compounds
Aniline
Dimethyl ami ne
Nitrobenzene
None
None
None
None
None
None
None
None
Moro-, di-, and trichlorophenols;
non-aromatic oxidation products
Mono-, di-, and trichlorocresols;
non-aromatic oxidation products
p-Benzoquinone, non-aromatic
oxidation products
Mono-, di-, and trichloroani1ines;
non-aromatic oxidation products
N-Chlorodimethylamine, oxidation
products
None
301
-------
TABLE 103. VIRICIDAL EFFICIENCY OF
FREE CHLORINE IN WATER (257)
Investigator
Chang et al.
Neefe et al.
Lensen et al.
Clarke and
Kabler
Weidenkopf
Kelly and
Sanderson
Virus
Part, purif.
Theiler's
virus in
tap water
Feces-borne
Inf. Hepat.
virus in
dist. water
Purif.
Polio II in
dist. and
lake water
Purif.
Coxsackie
A2 in
demand-free
water
Purif.
Polio I
(Ma honey)
in demand-
free water
Purif.
Polio I
(Ma honey)
in demand -
free water
Purif.
Polio III
(Saukett)
in demand-
free water
Temp.
°C
25-27
25-27
Room
19-25
3-6
3-6
3-6
3-6
3-6
3-6
27-29
27-29
27-29
27-29
27-29
0
0
0
0
0
0
0
25-28
25-28
25-28
25-28
Final
pH
6.5-7.0
6.5-7.0
6.7-6.8
7.4-7.9
6.9-7.1
6.8-7.1
6.9-7.1
8.8-9.0
8.8-9.0
8.8-9.0
6.9-7.1
6.9-7.1
8.8-9.0
8.8-9.0
8.8-9.0
6.0
6.0
7.0
7.0
8.5
8.5
8.5
7.0
9.0
7.0
9.0
Free Chlo-
rine
mg per a
4.0-6.0
4.0-6.0
3.25
1.0-1.5
0.58-0.62
1.9-2.2
3.8-4.2
1.9-2.0
3.7-4.3
7.4-8.3
0.16-0.18
0.44-0.58
0.10-0.18
0.27-0.32
0.92-1.0
0.39
0.80
0.23
0.53
0.53
1.95
5.00
0.21-0.30
0.21-0.30
0.11-0.20
0.11-0.20
Virus Destruction
98.6% in 10 min
99% in 5 min
30 min cont. time
protected all of 12
volunteers
10 min cont. time
protected all of 164
inoc. mice
99.6% in 10 min
99.6% in 4 min
99.6% in 2h min
99.6% in 24 min
99.6% in 9 min
99.6% in 5 min
99.6% in 4 min
99.6% in 3 min
99.6% in 10 min
99.6% in 7 min
99.6% in 3 min
99.6% in 3% min
99.6% in 1% min
99.6% in 8 min
99.6% in 4% min
99.6% in 16 min
99.6% in 7% min
99.6% in 3 min
99.9% in 3 min
99.9% in 8 min
99.9% in 2 min
99.9% in 16 min
302
-------
TABLE 103 (continued)
Investigator
Kelly
and
Sanderson
(cont1
Clarke
d)
et al.
Virus
Purif.
Coxsackie
B5 in
demand-free
water
Purif.
Adenovirus
3 in
demand-free
water
Temp.
°C
25-28
25-28
1-5
1-5
25
25
4
4
Final
PH
7.0
9.0
7.0
8.0
8.8-9.
6.9-7.
8.8-9.
6.9-7.
Free Chlo-
rine
mg per i
0
1
0
1
0.
0.
0.
0.
0.
0.
0.
0.
21-0.
21-0.
21-0.
21-0.
20
20
20
20
30
30
30
30
Virus Destruction
99.9%
99.9%
99.9%
99.9%
99.8%
99.8%
99.8%
99.8%
in
in
in
in
in
in
in
in
1 min
8 min
16 min
30 min
40 sec-50 sec
8 sec-16 sec
80 sec-100 sec
8 sec-10 sec
germicidal action. This prevents regrowth and protects against
accidental contamination during distribution.
Despite chlorine's usefulness, it does have some serious
disadvantages. Clarke et al. (240) and Sobsey (1291 ) reported
the isolation of viruses in chlorinated drinking water in Paris
(1 pfu/300*) and South Africa (1 pfu/loM- In view of the
fact that only one to two viruses of some types are sufficient
to cause infection, anything less than 100 percent inactivation
may be unacceptable. But with chlorine even the absence of
any living viruses still may not be acceptable. McClanahan
( 1646 ) reported that chlorine removes the protein coat of a
virus - thus rendering the virus technical ly nonviable - but
may leave the infectious nucleic acid core intact. Consequently,
a water supply free of any living viruses may still be infec-
tious .
Chlorine is also relatively ineffective against protozoa!
and helminthic cysts. These encysted organisms are very
resistant to oxidation by chlorine.
Ozone is equally as effective as chlorine against bacteria
and viruses and has a much faster reaction rate. Once the
proper "threshold" ozone dose is applied (usually less than
5 mg/£) , the bactericidal action is almost instantaneous. Tests
have shown ozone to be between 600 and 3.00Q times more rapid
than chlorine in its destruction of bacteria ( 1646 ). McClanahan
(651) was unable to recover viable nucleic acids from
ozonated water, suggesting that virus destruction was complete,
as opposed to the action of chlorine. Venosa ( 1429 ) reported
that protozoa! cysts resistant to chlorine were easily inactiva-
ted by ozone. Futhermore, the biocidal character of ozone is
not affected by pH, as is the biocida! character of chlorine.
303
-------
Ozone is not without problems ; however, ozone leaves no
residual. It has a fairly short half-life in water and rapidly
loses all disinfectant ability. Experience in Europe has
revealed few problems along these lines, but the added margin
of safety with chlorine has worked against the adoption of
ozone in the United States. The versatility of ozone and its
relatively greater disinfecting ability has led to the suggestion
that Initial ozonation could be followed by low-level chlorina-
tlon to provide a residual. However, little research has been
conducted along these lines.
Murphy (980) and Vajdic ( 1414) both reported that gamma
radiation was as good a disinfectant as chlorine against
bacteria and was somewhat better against the more chlorine-
resistant biologicals. Ultraviolet is a proven bactericide,
but research on other biocidal characteristics has been limited.
Nevertheless, any radiation treatment suffers from operational
difficulties, and, like ozone, provides no residuals.
The sanitation districts of Los Angeles County are in the
final stages of an extensive study for EPA and the California
State Water Resources EJoard. This study titled "The Pomona
Virus Study," has evaluated virus removals by various combina-
tions of tertiary treatment processes and followed by chlori-
nation or ozonation. Their conclusions in part are that the
majority of virus inactivation occurs during disinfection and
the main function of the preceeding tertiary unit processes
was that of removing substances (turbidity, organics, etc.)
which interfere with efficient disinfection. In virus seeding
experiments involving combined chlorine residuals of 5 mg/2,
average seed virus removals of 4.7 to 5.1 logs were achieved.
With 10 mg/£, of combined chlorine residuals ,5.? logs of virus
removal were achieved. In seeding experiments involving ozona-
tion, average log virus removals ranged from 5.1 to 5.4 logs.
304
-------
ADSORPTION ONTO ACTIVATED CARBON AND OTHER MATERIALS
Introduction
Activated carbon adsorption (or simply carbon adsorp-
tion) is employed to remove color, odor, taste, and refrac-
tory organic compounds from water. Many water treatment
plants presently pass their effluent through a carbon column
or fine-grain carbon bed to polish the final product.
Available data indicate that carbon adsorption is an effec-
tive method for removing synthetic and natural organic
contaminants, particularly chlorinated hydrocarbons and
organophosphorus pesticides, from plain water. Carbon adsorp-
tion may also be used to remove some metals. There is some
natural adsorption, but metal removal can be greatly enhanced
by the addition of an organic chelating agent prior to
passage through the carbon. The carbon will readily adsorb
the chelating agent, thereby also removing the complexed
metal.
The literature that has been reviewed on the effective-
ness of the adsorption process in potable water treatment is
summarized in Table 104. The major portion of the research
to date has involved tertiary wastewater treatment application,
although there has been substantial work also in the water
treatment field shown in Table 104. With the recent
concern over residual organics in U.S. water supplies, one
can anticipate increased activity in both pilot and full-
scale activated carbon systems for treating water supplies.
In addition to activated carbon, synthetic polymeric adsor-
bents have been extensively tested and show promise for
potable water treatment. They are not widely used in water
treatment plants but have been tested in pilot-scale instal-
lations. Some tests have indicated higher removal efficiencies
for synthetic adsorbents than for activated carbon for some
contaminants. Inorganic adsorbents, such as clays and
magnetite, are also capable of contaminant removal.
Water Quality Parameters
Activated carbon adsorption was used following chemical
coagulation and rapid sand filtration at the much-publicized
Windhoek, South Africa, water treatment plant. The influent
305
-------
TABLE 104. LITERATURE REVIEWED PERTAINING TO ADSORPTION
Contaminant Reference Number
Water Quality Parameters
Ammonia 1649, 1674
BOD 1660, 1674
COD 1660
Chlorides 1649, 1666, 1672
Nitrates 1649, 1674
Nitrites 1674
Oil and grease 620
Phosphates 1660
Sulfates 1674
Sulfides 1639
Suspended solids 1660
Taste and odors 620, 1593, 1610, 1624, 1626, 1639, 1649, 1661
Turbidity 1593, 1624, 1649
Elemental Contaminants
Arsenic 1062, 1652
Barium 1062
Cadmium 1652
Chromium 1062
Iron 1649
Lead 1652
Mercury 811, 1062, 1610, 1631, 1652, 1680,
1681
Selenium 1062
306
-------
TABLE 104 (continued)
Contaminant Reference Number
Silica 1604
Biocidal Contaminants
DDT 1610, 1617, 1662, 1664, 1672
DDE 1617
Aldrin 1610, 1617, 1662
Dieldrin 620, 1610, 1617, 1662, 1664
Endrin 1610, 1617, 1662, 1664
Carbamates 1618
Chlori nated
hydrocarbons 620, 1610, 1617, 1662, 1666, 1672
Organophos 1610, 1617, 1652, 1662
Herbicides 1610, 1652
Lindane 1664
Other (general) 499, 1221, 1610, 1664
Synthetic/Organic 499, 620, 708, 1062, 1610, 1624, 1627,
Contaminants 1649, 1650, 1652, 1662, 1672, 1674,
1676
Biological Contaminants
Polio Virus 1652
Virus 1652, 1657
307
-------
to this plant was treated wastev/ater which was subsequently
mixed with surface water for direct reuse. Stander and
Funke (1674) reported on the effluent quality through the
pilot plant. The concentration of ammonia nitrogen in the
effluent was lowered from 0.3 to 0.1 mg/i by passage through
an activated carbon filter. ABS and BOD were also signi-
ficantly reduced, 82 and 67 percent, respectively.
Table 105, from Medlar (1649), summarizes water quality
analysis data from several water treatment plants in New
England employing granular activated carbon filters. Two
of these plants (Amesbury and Scituate) use carbon for both
filtration and adsorption, while the remaining four use
carbon for adsorption only. At each plant, the carbon signi-
ficantly reduced ammonia levels, as between 33 and 100 percent
of the influent ammonia was removed.
Phillips and Shell (1660) presented a study of the
effectiveness of granular activated carbon and other general
contaminants in removing BOD. The study was conducted at a
pilot water plant treating wastewater effluent by chemical
coagulation, filtration, and passage through 16-ft carbon
columns. Data are presented in Table 106 BOD removal by
the carbon columns averaged 33 percent, while COD was
reduced 80 percent.
TABLE 106, ACTIVATED CARBON FILTRATION AT
COLORADO SPRINGS PILOT PLANT (1660)
BOD5
COD
SS
P04
ABS
Influent
(may
3
41
4
2
0.9
Effluent
'£)
2
8
3
1
0.03
Removal
m
33
80
25
50
97
Activated carbon is highly efficient for removing noncol-
loidal, soluble, aromatic-structured color sources. David Volkert
and Associates (1610) indicated that the carbon removal efficiency
for color-producing substances is 100 percent of methylene-blue
active substances. Table 106 shows that the color removal effi-
ciency of carbon filters in six water treatment plants was nearly
100 percent (1649). Activated carbon has also been used indus-
trially for decolorizing organic dye waste effluents. Recently,
the nonionic polymeric adsorbents, such as Amberlite XAD-7, have
been gaining popularity for this purpose (1672).
308
-------
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309
-------
While Table 105 and the operation at Windhoek (1674)
show that both organic and ammonia nitrogen were reduced by
carbon adsorption, they also show that oxides of nitrogen
(nitrate and nitrite) were not reduced.
Oils derived from natural, domestic, or industrial sources
may occasionally be found in wastewater effluents and in water
supplies. Hyndshaw (620) reported that petroleum products
are very quickly adsorbed from water by activated carbon.
He stated that for emergencies, such as gasoline or oil
spills, large quantities of powdered activated carbon will
remove the hydrocarbons.
Reduction of phosphates as P04 from 2 mg/£ in the carbon
filter influent to an effluent concentration of 1 mg/£ is shown
in Table 106 (166.0). Sulfate as S04 was not reduced from its
concentration of 220 mg/£ by carbon filtration at the Windhoek
plant. However, sulfides in the form of hydrogen sulfide,
and polysulfides that result from the reaction of chlorine
with hydrogen sulfide were removed from well water, according
to Lee (1639). The removal was indirectly evidenced by the
destruction of sulfide odor in the water supply and resulted
from a catalytic reaction with the carbon rather than from
adsorption.
Activated carbon is commonly used for removing tastes and
odors from water. Undesirable odors in water are caused by the
vapors from many chemicals, including halogens, sulfides, ammonia,
turpentine, phenols and cresols, picrates, and various hydrocar-
bons and unsaturated organic compounds, some of which have not
been identified. Tastes and odors are also caused by substances
produced by living microorganisms or decaying organic matter.
Some inorganic substances, such as metal ions in high concentra-
tions (especially iron) also impart taste and odor to water.
Removal of many tastes and odors with activated carbon approaches
100 percent. Successful taste and odor removal from a municipal
water supply by carbon bed filters was demonstrated in Buckingham
England (1624). The water was taken from a river that runs
through farmland and had an earthy taste that resisted chlorina-
tion; clarification and sand filtration; and experimentation with
ozone, permanganate, and chlorine. At Goleta, California, taste
and odor in the water supply were also eliminated by passage
through granular activated carbon beds (1624). Popalisky and
Pogge (1661) reported that powdered activated carbon was used
at a water plant treating Missouri River water to eliminate taste
and odor caused by microorganic compounds". The compounds and
their concentrations were not identified.
Hansen (1626) reported that installation of granular
carbon filters at Mount Clemens, Michigan, completely removed
310
-------
the septic and phenol tastes and odors that were present in the
Clinton River water supply during runoff periods. Granite City,
Illinois, reported a similar experience (1593). The dosage of
activated carbon required to remove taste and odor is influenced
by chlorine application. Generally, carbon should be applied
before chlorination (620).
Many pesticides and herbicides produce tastes and odors
when present only in very small concentrations in water.
Hyndshaw (620) used the beta isomer of benzene hexachloride
to illustrate the influence of a small concentration of a
biocide on the taste and odor quality of water. This substance,
when present in amounts as little as 17 ppb in odor-free water,
gives a threshold odor number (TON) of 8. (The threshold
number denotes the number of volumes of odor-free water
required to dilute the odor concentration to a point where
the odor is just barely perceptible.) Other organic pesticides
and their concentrations and subsequent effects upon taste
and odor are shown in Table 107 (620).
TABLE 107. ODOR IMPARTED TO ODOR-FREE WATER
BY PESTICIDES AND HERBICIDES (620)
Substance
Toxaphene
2,4 D (isoctyl)
2,2 D
D-D
Rothane
Chlordane
BHC
Concentration
ppm
0.84
2.0
92.5
0.0235
50.0
0.07
0.0175
Odor
TON
6
17
4
17
Nil
140
8
A simple study employing the threshold odor test gave
evidence of the reduction of these compounds by activated
carbon. The amount of activated carbon required to reduce the
odor of each compound to a palatable level is presented in
Table 108 (620).
311
-------
TABLE 108. ACTIVATED CARBON REQUIRED TO REDUCE
ODORS CAUSED BY PESTICIDES AND HERBICIDES
TO PALATABLE LEVELS (620)
Substance
Pa rat hi on
37 gamma BHC
Mai at hi on
2,4 D
DDT
Concentration
of substance
ppm
10
25
2
6
5
Odor
TON
50
70
50
50
70
Carbon
Dosage
ppm
20
15
20
40
4
Odor
after Carbon
TON
4
1.4
4
3
3
Significant reduction in turbidity and suspended solids con-
centration is also effected with activated carbon. The data in
Table 105 (1649) show that turbidity is reduced both at plants
where granular activated carbon is used for filtration and adsorp-
tion and where it is used for adsorption only. Passage of water
through 16-ft carbon columns effected 25 percent removal of sus-
pended solids at Colorado Springs (Table 106, 1660).
Turbidity removal is essentially complete at Nitro, West
Virginia, where activated carbon has replaced sand in the filters
(1624). Final effluent JTU's are typically less than 0.1. At
Granite City, Illinois, Blanck and Sulick (1593) report that sus-
pended solids removal by carbon filtration exceeds that achieved
with sand filters.
Elemental Contaminants
Although little data from municipal water purification appli-
cations are available, it appears that activated carbon can pro-
vide some removal of heavy metals. Direct adsorption provides
some removal, but efficiencies can be increased to nearly 100
percent by adding an organic chelating agent (1662). The carbon
removes the complex by adsorbing the organic agent, removing the
metal along with it.
Patterson (1062) cited evidence that filtration of water
containing 0.2 mg/l arsenic through a charcoal bed yielded an
effluent containing 0.06 mg/SL of arsenic, or 70 percent removal.
He cited another report of 40 percent reduction of arsenite by
activated carbon from an initial concentration of 0.5 mg/i to a
concentration of 0.3 mg/£. Morton and Sawyer (1652) tested heavy
metal adsorption during filtration through a granular bed of
attapulgite clay. Data are presented in Table 109 that show the
312
-------
amounts of metals remaining in the effluent after filtration of
various quantities of water at two different rates. The initial
solutions contained 1 mg/A of each metal. Arsenic was reduced
from 0.97 and 0.98 mg/i to 0.02 and 0.03 mg/i upon filtration
of 2.5 volumes of water per volume of bed.
TABLE 109. REMOVAL OF HEAVY METALS BY PERCOLATION WITH
GRANULAR LOW VOLATILE MATTER ATTAPULGITE CLAY (1652)
- !• . ii
Ratio o
Percola
Vol ume
0
2.
5.
1.0.
0
2.
5.
12.
f Volume
te to
Bed
Recoveries
in
Effluent
0.
5 0.
0 0.
8 0.
0.
5 0.
0 0.
6 0.
As
97 ppm
02
12 ppm
56 ppm
98
03
16
68
1
0
0
0
1
0
0
0
Cd
.00
.01
.01
.01
.00
.01
.01
.01
Pb
Slow
1 .
0.
0.
0.
Fast
1 .
0.
0.
0.
Rate*
06
01
01
01
Ratef
06
01
01
01
Hg
1 .
0.
0.
0.
1.
0.
0.
0.
n
004
016
116
11
010
072
152
* 960 gal/ton clay/hour.
+ 2,880 gal/ton clay/hour
In a study cited by Patterson (1244), carbon adsorption
did not improve barium removal efficiency over that achieved
with chemical coagulation and clarification. Patterson notes
that others have also found poor removal efficiency for barium.
Cadmium removal data are also presented in Table (1652).
Removal of 99 percent was achieved and was unaffected by the
changes in flow volume and rate.
Some success has been reported from pilot plant work on
chromate removal by activated carbon. Patterson (1062)
reported on a study of metal removal from municipal wastewater
plant effluent, in which initial hexavalent chromium levels
of 0.09 to 0.19 mg/l were reduced to 0.04 mg/t or less. The
average effluent concentration reported was 0.017 mg/£.
313
-------
Initial hexavalent chromium levels of 5 mg/l were reduced to
0.09 mg/£ following carbon adsorption. Patterson noted that
it appears that activated carbon may not be equally effec-
tive at higher chromate levels.
Table 105 reports removal of iron at six water treatment
plants by granular activated carbon filtration. Removal effi-
ciencies ranged from 99 percent to 36 percent(1649) .
Lead removal is shown in Table 109 for adsorption onto
attapulgite clay. Over 99 percent removal was achieved at
all flow volumes and rates tested.
Mercury adsorption has been studied extensively. In
Table 109 , it is shown that adsorption onto attapulgite clay
of over 99 percent was achieved after filtration of 2.5
volumes of water per volume of bed. Removals decreased to
86 percent removal as 12.6 volumes per volume of bed were
filtered. Logsdon and Symons (811) conducted jar tests
using powdered activated carbon, increasing carbon dosages
increased removal of both inorganic and organic (methyl)
mercury. Organic mercury removal was more efficient than inorganic
mercury removal for a given dosage of powdered activated
carbon at effluent concentrations less than 2 ppb. Residual
concentrations of 0.8 ppb of inorganic and 0.2 ppb of methyl
mercury were achieved. Further tests were performed in
which powdered carbon was added just before alum coagulation
to improve mercury removal. Removal by alum alone was about
40 percent, whereas removal with 65 mg/£ of activated carbon
plus 30 mg/i of alum was in excess of 70 percent with an ini-
tial mercury concentration of 9.3 ppb.
The capacity of granular activated carbon for removing
mercury from water was also evaluated by pumping mercury
solutions through columns (811). Average influent concentra-
tions ranged from 20 to 29 ppb. Mercury removals declined
as the number of bed volumes (based on gross void space) of
water treated increased. Columns with 3.5-min contact times
removed 80 percent of the inorganic mercury for up to 15,000
bed volumes of water and 80 percent of the methyl mercury for
up to 25,000 bed volumes treated. Evaluation of carbon column
performance at 80 percent removal indicated that as contact
time in the column increased, the amount of mercury adsorbed
by the carbon increased. Also, granular activated carbon
adsorbed more methyl mercury than it did inorganic mercury per
gram of adsorbent. This behavior was expected, since acti-
vated carbon has a high capacity to adsorb organics.
Thlem (1680)also conducted jar tests on mercury adsorp-
tion using powdered activated carbon. Solutions containing
10 ppb mercury were brought into equilibrium with various
carbon dosages. Less than 30 percent of the mercury was
314
-------
adsorbed at a carbon dosage of 10 mg/£ at pH 7. When 100
mg/£ of carbon was applied to the test solution, removal
approached 80 percent. Removal decreased with increasing
pH, with best removal occurring at pH 7. The addition of
chelating agents such as EDTA or tannic acid prior to contact
with the carbon increased adsorption. Concentrations of as
little as 0.02 mg/£ of EDTA or 1 mg/l of tannic acid increased
removals from 10 to 30 percent, depending upon the carbon
dosage that was applied and the pH of the system.
Patterson (1062) summarized the data on activated carbon
removal of mercury, saying that the highest percentage removals
(80 to 95 percent) are achieved with more concentrated mercury
solutions. However, lowest effluent mercury results from
treatment of less concentrated waters, although the relative
efficiency is less. Thus carbon treatment of initial mercury
below 1 ppb yields an efficiency of removal of less than
70 percent, but effluent mercury below 0.25 ppb. Carbon treat-
ment of initial mercury concentrations of 5 to 10 ppb yields
about 80 percent removal and effluent levels of below 2
ppb. Carbon treatment of initial mercury concentrations
between 10 and 100 ppb yields 90 percent or greater effi-
ciency.
Poor selenium removal from well water by activated carbon
has been reported in one case cited by Patterson (1062).
Removal was less than 4 percent. Poor or no reduction of
silica has also been shown by the data from six operating water
purification plants employing carbon sdsorption and filtra-
tion (1649).
Biocldal Contaminants
As with other synthetic-organic compounds, some of the
organic pesticides and herbicides that are resistant to removal
by conventional treatment techniques are effectively removed
by adsorption. David Volkert and Associates (1610).
cited evidence that over 99 percent of the following chlorinated
hydrocarbons can be adsorbed by activated carbon:
• DDT
• A1 d r i n
t D i e 1 d r i n
• Endrin
• Chlordane
• Heptaclor epoxide
315
-------
• Lindane
• Methoxychlor
• Toxaphene
Laboratory studies cited by Stone (1662)have shown that
the following reductions in chlorinated hydrocarbon concen-
trations can be achieved by contacting with appropriate
doses of activated carbon (Table 110):
TABLE 110. ACTIVATED CARBON REMOVALS OF CHLORINATED
HYDROCARBONS ACHIEVED IN LABORATORY EXPERIMENTS (1662)
Substance
Chlorinated
hydrocarbons
DDT
DDT
Aldrin
Aldrin
Aldrin
Dieldrin
Dieldrin
Dieldrin
Endrln
Endrln
Chlordane
Lindane
Lindane
Lindane
Initial
Concentration
6.3 ppb
5 ppm
5 ppm
6.6 ppb
5 ppm
-
-
0.5-10 ppb
4.4 ppb
5 ppm
0. 5-10 ppb
50 ppm
10 ppb
25 ppb
1 ppb
Treated
Concentration
0.04-0.11 ppb
-
-
-
-
-
-
0.25 ppb
-
-
0.25 ppb
-
1 ppb
-
0.05 ppb
Percent
Reduction
98-99
90
76
90
85
99
99
50-97
99
86
50-97
99
90
90
95
Activated carbon removals of several pesticides are well
Illustrated by results of laboratory studies cited by the
California State Water Resources Control Board (1323)
shown in Table 111.
TABLE HI. REMOVAL OF SPECIFIC TOXIC MATERIALS BY
CARBON ADSORPTION (1323)
Carbon Residual (ppb)
Dosage (ma/l) Aldrin Endrin Dieldrin DDJ ODD DDE Toxaphene
Control
1.0
2.0
2.5
5.0
48
—
26
- _
15
62
—
15
_ _
3.4
19
—
6.
—
2.
3
4
41
41
—
21
3.7
56
6.
- _
3.
9
7
38
34
—
29
12
1
1
55
47
80
- _
31
316
-------
TABLE
(continued)
Carbon Residual (ppb)
Dosage (mg/l) Aldn'n Endrin Dieldrin DDT ODD DDE Toxaphene
10
12
25
50
.0
.5
.0
.0
12
6.
4.
3
4
1.
—
0.
0.
5
56
22
1 .1
<1
— —
— —
2
—
0
0
.2
.45
.35
3.
1 .
0.
3
1
9
2.7
—
- _
—
Adsorption of the carbamate pesticides Sevin and Baygon
on granular activated carbon was investigated by El-Dib et al.
(1618). passage of a 5 mg/a solution of Baygon through carbon
columns effectei complete removal for up to 273 bed volumes
of water when a contact time of 3.76 min was allowed. In
the case of Sevin, 1,800 bed volumes were passed with complete
removal under the same conditions. Rapid breakthrough of
the pesticides into the effluent occurred, however, as the
contact times were decreased to 1 or 0.5 min.
According to reference 198 the available data on
organophosphorus pesticide removal indicates that the effi-
ciency of activated carbon ranges from 50 to over 99 percent.
Stone and Company (1662)cited laboratory-scale tests showing that Para-
thion was reduced from 10 to 2.5 mg/a using 20 mg/a powdered
carbon; and from 11.4 to 0.05 mg/a using dual granulated carbon
filters. Malathion was reduced in laboratory-scale tests
from 2 to 0.25 mg/a with 10 mg/a powdered carbon. Some data
on removal efficiencies of the organic herbicides were also
cited. They report that over 99 percent removal of 2,4-5-TP and
2,4-D is possible.
Robeck et al . (1168) surveyed the effectiveness of various
water treatment processes in pesticide removal. Table 112 sum-
marizes their results using carbon in both a slurry form and in
beds.
TABLE 112- SUMMARY OF CUMULATIVE PESTICIDE
REMOVAL AT 10-ppb LOAD
Process
Pesticide Removed - Percent
DDT
Lindane Parathion Dieldrin
2,4,5-T
Ester
Endrin
Carbon :
SI
Bed
1 urry
5 ppm
1 0 ppm
20 ppm
0.5 gpm/
cu ft > 99
30
55
80
> 99
> 99
> 99
> 99
> 99
75
85
92
> 99
80
90
95
> 99
84
90
94
>99
317
-------
In addition to activated carbon, other adsorbents such
as clays and synthetic polymeric adsorbents are capable of
removing biocidal contaminants. Morton and Sawyer(1652) studied
the adsorption of diazinon, an organophosphorus pesticide,
onto attapulgite clay. Coarse-ground, high-volatile matter
attapulgite was stirred with contaminated water in laboratory
experiments. At least 50 percent of the diazinon in a 0.1
mg/x, solution was removed by the clay in a 10 percent clay
suspension. An investigation of the use of the synthetic
polymer Amberlite XAD-4 for the removal of various pesticides
was cited by Stone and Company (1662) The pesticides examined included
-BHC, lindane, B-BHC, aldrin, and dieldrin in tap water at
initial concentrations of 1 ppb each. Consistent removals
of over 60 percent were reported.
Schwartz (1221)al so studied the adsorption of selected pesti-
cides on activated carbon and mineral surfaces. He found that
the clay minerals ilite, kaolinite, and montmori11onite
suspended in dilute pesticide solutions adsorbed very little
2,4-dichlorphenoxyacetic acid (2,4-D) or isopropyl N-(3-
chlorophenyl) carbamate (CIPC). Adsorption of CIPC from
aqueous solution with powdered activated carbon, however,
was extensive (90+ percent).
Syntheti c/Organi c Contaminants
Adsorption is commonly cited as a presently available
technology for removing particulate, colloidal, and soluble
organic contaminants from water. Many of the organics pre-
sent in water supplies - particularly the soluble and colloidal
organics - are of a refractory nature, i.e., they resist removal
by conventional methods. A number of these are potentially
toxic or carcinogenic and, as a result, their detection, iden-
tification, and treatment in water is receiving increasing
attention. These substances, even in small amounts, contri-
bute to taste and odor conditions and may pose a chronic
health hazard. As has been discussed, activated carbon is
widely applied for taste and odor removal; however, its
effectiveness for removing residual organics has just come
under study in recent years. The delay has been caused in
part by the lack of standard procedures for identifying and
classifying the vast assortment of organics that occurs in
trace quantities in water (499, 1650). The delay is also due
to the search for a gross organic parameter that can be used
as a measure of organics. The more common parameters used
include carbon chloroform extract, liquid extraction,
paper and gas chromatography, fluorescent spectroscopy, and
radi ation.
Traditionally, carbon life expectancy has been based on
the capability of the carbon to absorb tastes and odors.
But research has shown that the life expectancy of carbon
318
-------
to reduce carbon chloroform extract or organic compounds is
somewhat less than that to remove tastes and odors (1649).
Medlar (1649) suggested that monitoring carbon chloroform
extract (CCE) concentration in carbon filtered water would
provide a conservative estimate of filter performance, but noted
that the CCE test may not encompass all the compounds that
should be considered.
Carbon chloroform extract indicates the presence of stable
organic compounds in water. The extract has an operational
definition and is a mixture of organic compounds that can be
adsorbed onto activated carbon and then desorbed with organic
solvents under specific controls. Examples of substances mea-
sured with this method include substituted benzene compounds,
kerosene, polycyclic hydrocarbons, phenylether, and insec-
ticides. The efficiency of activated carbon in reducing CCE
depends upon several factors including water temperature, ini-
tial amount of contaminant, and the molecular weight of the
contaminant (1610). Percentage removals must therefore be deter-
mined by laboratory testing. Removals ranging from 50 to 99
percent were reported by David Volkert and Associates (1610).
The adsorption of polycyclic (polynuclear) aromatic
hydrocarbons (PAH) from water by activated carbon was dis-
cussed by Harrison et al. (1677). These compounds are poten-
tial carcinogens under certain conditions. Carbon adsorp-
tion has been shown to give 99 percent removal of PAH from
water filtered by prior seepage through river bank soil.
Bis-ethers are synthetic organic compounds that may
occur in water associated with industrial discharges. Stone
and Company (1662) cited laboratory tests of activated car-
bon treatment in which isopropyl ether concentrations were
reduced from 1,023 to 20 mg/£, butyl ether concentrations
from 197 mg/l to nil, and dichloroisopropyl ether concen-
trations from 1,008 mg/£ to nil.
The treatment of dilute phenolic industrial wastewater
was reviewed by Patterson (1062). Adsorption onto activated car-
bon has been employed to remove over 99 percent of the phenol
present in process waters with initial concentrations ranging
from 5,325 mg/£ to 0.12 mg/£. Final phenol concentrations
ranged from 0.25 mg/Jl for treatment of a concentrated solu-
tion to 0.001 rng/5, for treatment of weaker solutions.
Foaming agents such as linear alkyl benzene sulfonate in con-
centrations up to 5 mg/l can be removed by activated carbon with
90 to TOO percent efficiency according to evidence cited by David
Volkert and Associates (1610). Table 106 (1660), which presents
data on activated carbon filtration at the Colorado Springs
319
-------
pilot plant, shows 97 percent removal of alkyl benzene sul-
fonate (ABS). Stander and Funke (1674) reported reduction of
ABS from 4 to 0.7 mg/z at the WindhoeK pilot plant. Organic
acids are also reported to have been reduced from 1 to 0.4 mg/£.
Morton and Sawyer (~16~5~2) studied the adsorption of two
organic compounds - diethylstiIbestrol (DES), which is a hormone
fungi and aflatoxin, which is a natural toxin produced by fungi
onto attapulgite clay. Attapulgite is a magnesium aluminum
silcate clay that exhibits a high debree of adsorption for
low-weight organic molecules. Coarse-ground, high-volatile-
matter attapulgite was contacted with contaminated water in
laboratory experiments. DES at a concentration of 5 ppb was
decreased 68 and 76 percent by contacting with 1.1 and 10
percent (by weight) clay suspensions, while in a 50 ppb
solution the removals were 68 and 89 percent, respectively.
More than 98 percent of the aflatoxin at concentrations of
0.5 ppb and 5.0 ppb was removed by both 1.1 and 10 percent
clay suspensions. The results of column percolation studies
through granular low-volatile-matter clay are presented in
Table 113.
TABLE 113. REMOVAL OF ORGANICS BY PERCOLATION
UITH GRANULAR. LVM ATTAPULGITE
Volume rates percolate
to bed volume
Recoveries in Effluent
Slow rate* Fast ratef
50 ppb DES Solution
0
2.5
5.0
10.8
12.6
52 ppb
ND?
ND
ND
—
48 ppb
ND
1
__
2
2
5
10
0
5
,0
8
20 ppb Aflatoxin Solution
17 ppb
ND
ND
ND
12.6
17
ND
ND
ND
ppb
* 960 gal/ton clay/hour.
t 2,880 gal/ton clay/hour.
f ND = not detectable.
Stone and Company (1662) cited data concerning the treatment of
synthetic-organic polychl orinated biphenyls (PCB's) by adsorption
320
-------
onto clay minerals and Amberlite polymeric adsorbents.
In laboratory tests Amberlite XAD-4 removed up to 76 percent
of the PCB present in solutions. Several clay minerals demon-
strated PCB removal capability in laboratory tests: illite -
60 percent, montmoril1onite - 40 percent, and kaolinite -
40 percent. Kinoshita and Sunata (708) evaluated the' adsorp-
tion of PCB onto powdered activated carbon in a jar test
and found that the initial concentration of 100 ppb PCB was
reduced to 10 ppb in the product water.
The Amberlite adsorbents represent a new technology for
adsorbing organic molecules from water. They are used spe-
cifically for adsorbing aromatic and aliphatic compounds.
According to Simpson (1672) small molecules such as phenol
are effectively adsorbed by Amberlite XAD-4, while for a
larger molecule such as an alkylbenzene sulfonate, Amberlite
XAD-2 has a much higher adsorptive capacity. Phenol is a
model aromatic, low-molecular weight compound that is con-
sidered to be highly objectionable, as are some of the chlori-
nated phenol products. Using the XAD-4 adsorbent, up to 40
bed volumes of a 500 ppm water solution of phenol were treated
with less than 10 percent leakage at a flow rate of 0.5 gal/ft3/
min. At a higher flow rate of 2.0 gal/ft3/min, 20 bed volumes
were treated with less than 10 percent leakage. It was further
found that the adsorptive capacity was higher for chlorinated
phenols than for simple phenol. Simpson (1672) cited a labora-
tory study in which the removal efficiency of Amberlite XAD-2
for a list of organics at flow rates of 1.25 gpm/cu ft were
determined. The results are presented in Table 114. Non-
ionic compounds were removed with 100 percent efficiency while
ionized compounds were less effectively removed.
In the nationwide study of water supplies and water treat-
ment facilities by Symons et al . (1676), it was concluded that
both powdered and granular activated carbon treatment signi-
ficantly reduced the trace concentrations of total trihalo-
methane in the product water.
TABLE 114 . ADSORPTION OF ORGANIC COMPOUNDS ONTO
AMBERLITE XAD-2 POLYMERIC ADSORBENT (1672)
Retention
1. Aliphatics Influent Effluent Efficiency, %
a) alcohol: n hexanol 200 ppm 30 ppm 85
b) ester: ethyl butyrate 100 0 100
c) ketone: methylisobutyIketone 100 0 100
2. Aromatics
Benzene 100 0 100
Benzene sulfonic acid 3.0 2.1 31
321
-------
TABLE114- (continued)
2. Aromatics
Influent Effluent
Retention
Efficiency,
p-toluene sulfonic acid
Benzoic acid
Benzoic acid (pH 3.2)
Phenol
Phenol (Amber-lite XAD-7)
0-Cresol
2, 4-dimethyl phenol
p-nitrophenol
2-methyl phenol
4, 6-dinitro-2-aminophenol
Phenylenediamine
Aniline (Amber! ite XAD-7)
Naphthalene
2-hydroxy-3 naphthoic acid
9.0
1.0
1.0
0.4
0.4
0.3
0.4
0.2
0.3
0.4
0.9
4.0
0.05
0.6
6.9
0.8
0
0.22
0.06
0
0
0
0
0.22
0.02
0
0
0.37
23
23
100
45
86
100
100
100
100
43
98
100
100
39
Biological Contaminants
The limited efficiency of activated carbon in removing
viruses from wastewater was discussed in the advanced waste-
water treatment section of this report. Results show that
activated carbon is inefficient in removing viruses from
drinking water. Oza and Chaudhuri (1657) suggested that the
inefficiency may be due to the exclusion of viruses from the
micropores of activated carbon because of their size.
Coal adsorption of a bacterial virus was investigated,
and results indicated that coal may be a more effective
adsorbent than activated carbon. Morton and Sawyer (1652)
demonstrated that attapulgite clay also has the capacity to
adsorb polio virus from water. Aqueous virus-clay suspensions
were shaken for 1 min and then filtered. High-volatile-
matter clay completely removed virus infectiyity from a
20 percent clay suspension with an initial virus concentration
of 16 million infectious particles per mi. However, reducing
the contact time from 30 to 5 min or the clay concentration
from 20 to 5 percent resulted in incomplete removal.
322
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ION EXCHANGE
Introduction
Ion exchange has its greatest current application in
industrial and small-scale potable water supply operations. The
most common use of ion exchange is for removal of hardness
(calcium and magnesium cations) from municipal, industrial,
household, and laboratory water supplies. It is particularly
suited for desalting brackish water, pretreating water that must
be almost completely demi neral ized for industrial use, and
removing metals from industrial metal plating rinse wastewaters.
No one ion exchange resin is capable of removing all ionic
contaminants. Various resins, depending upon their chemical
nature, show preferential selectivity for specific ions.
Table 115 presents data on ion selectivity for various types of
exchange resins (1062).
_ TABLE 115. ION EXCHANGE RESINS SELECTIVITY (1062) _
_ Resin _ Resin Selectivity* _
Strong-acid cation Li+, H+, Na+, NH4+, K+, Rb+. Cs+,
(Sulfonic) Mg+2, Zn+2, Cu+2, Ca+2, Pb+2
Weak-acid cation Na+, K+, Mg+2, Ca+2,
(Carboxylic) Cu+2, H+
Strong-base anion F", OH-, H2P04-, HC03-, Cl", N02",
(Type I) HS03-, CN-, Br-, N03", HS04~, I"
Strong-base anion F", H2P04-, OH", HC03"
(Type II) C1-, N02~, HS03- , CN",
Br-, N03-, HS04~, I~
Weak-base anion F", Cl', Br", I", P04'3,
N03~, Cr04-2, S04-2, OH-
*Increasing selectivity left to right.
The more strongly a resin adsorbs a particular ion, the
more complete the ion removal. However, a high affinity
between a particular resin and a specific ion also means greater
difficulty in regenerating the resin; that is, it is more
323
-------
difficult to release the adsorbed ions to make the resin reuse-
able. As a result, regeneration of an effective resin is
seldom carried to completion, and the operational capacity of an
ion exchange resin may be redvced to 50 to 60 percent of theoret-
ical capacity.
Ion exchange processes are very sensitive to both clogging
and fouling. An ion exchange resin bed is a good filter;
therefore, suspended solids in water will clog the bed. Fouling
results when the resin adsorbs materials which, because of their
adsorption or absorption into the resin pores, cannot be removed
in the regeneration step. Fouling often results from the
irreversible sorption of high molecular weight organic acids.
The nonselective nature of most exchange resins is a
drawback when attempting to remove a low-level contaminant from
water. The simultaneous removal of other nontarget ions rapidly
increases the cost of using the process. More selective resins
are currently becoming available (1634).
In the past, application of ion exchange processes was
confined to the removal of ionic contaminants. Recently,
however, some ion exchangers have been developed that can remove
nonionic species, e.g., AlgOs, Feo03, HgSiOa, etc. Resinous
adsorbents are also available that are particularly suited for
removing organic compounds - including biocidal and synthetic/
organic contaminants - from water. While often used in conjunc-
tion with true ion exchange processes, the mechanism of organic
removal is actually adsorption; therefore, the resinous or
polymeric adsorbents (as they are called) are discussed in the
carbon adsorption section of this report. The literature
utilized during this review on the removal of various contami-
nants by 1on exchange methods is indicated in Table 116.
Water Quality Parameters
Reduction of total dissolved solids may be an Important
application of the ion exchange process when reclaimed waste-
water for potable reuse is the objective of treatment. High
total dissolved solids concentrations, from 500 to over 1,000
mg/£, are found in wastewaters. Approximately 300 mg/jz, of total
dissolved solids is generally considered the increment added
during one cycle of domestic use of a water supply. Ion
exchange treatment of water and wastewater for removal of
dissolved solids is most successful after prior treatment using
both conventional and advanced techniques has taken place. This
prevents clogging and fouling of the exchange resins.
Ion exchange is technically capable of producing a water
with only 0.055 micromhos (pmhos) of specific conductance. One
micromho will normally indicate a dissolved solids concentration
of 0.5 to 0.6 mg/ji. However, water of such purity is rarely
324
-------
TABLE 116. LITERATURE REVIEWED PERTAINING TO ION EXCHANGE
C_o._ntam1 nant Reference Number
Water Quality
Parameters
Ammonia 1062, 1598, 1659, 1661
Chlorides 1062, 1610, 1659, 1661
Color 1610
Cyanides 1062, 1610
Fluorides 1062, 1610
Hardness 1659
Nitrates 165, 1592, 1598, 1602, 1610, 1622, 1630
Phosphates 1592, 1602
Sodium 1602, 1610, 1659
Sulfates 1602, 1610, 1659
Total dissolved 1062, 1592, 1602, 1610
solids
Elemental Contaminants
Arsenic 1062, 1244, 1596
Barium 1062
Boron 1062
Cadmium 1062
Chromium 1062
Copper 1062, 1634
Iron 1062, 1589
Manganese 1062, 1589
Mercury 1062, 1634
Nickel 1062
325
-------
TABLE 116 (continued)
Contami nant Reference Number
Selenium 1062
Zinc 1062, 1634
required, and the costs to achieve such purity would be pro-
hibitive. Complete demineralization of municipal water supplies
is unwarranted and may even have adverse consequences, as the
body requires certain trace concentrations of many minerals.
The EPA and the LA County Sanitation Districts jointly
funded an advanced wastewater treatment facility in Pomona,
California. The results of the ongoing tests have been compre-
hensively reported by Parkhurst (1659) and Chen (1602). The ion
exchange system, which was proven to be of economic and technical
feasibility, effectively reduced the total dissolved solids by
90 percent. The treatment involved passage first through a
primary cation column and an anion column, then through a
secondary cation column and a secondary anion column. A series
of 80 complete operating cycles including exchange, backwashing,
and regeneration was completed at a 2.5-gpm flow rate. The
total dissolved solids concentrations of the feed and product
waters averaged 610 mg/£ and 72 mg/a, indicating an 89 percent
average reduction. A complete listing of the various consti-
tuents at successive stages of the demineralization sequence is
presented in Table 117 (1659).
All of the major anions and cations were removed to a
considerable degree except silica. Silica removal can be
accomplished, however, with highly basic anion resins
(1592). Calcium and magnesium, the cations responsible for water
hardness, are almost completely removed in the primary cation
exchanger; but only about half of the sodium, potassium, and
ammonium ions are removed in this column. The secondary cation
exchanger, however, efficiently removed the majority of the
remaining ions. Similarly, the primary anion exchanger removed
most of the sulfate ions, while the nitrate, chloride, and
orthophosphate ions were partially removed by both the primary
and secondary stages.
David Vol kert and Associates (1610) cited evidence
that the sodium and fluoride concentrations of water can be
reduced by 95 percent using ion exchange. It reported that
chloride, sulfate, and nitrate can be reduced by as much as 95
percent, depending on the degree to which the exchange resin can
be regenerated.
326
-------
TABLE 117. AVERAGE WATER QUALITY CHARACTERISTICS OF THE
ION EXCHANGE PILOT PLANT UNDER TYPICAL OPERATING CONDITIONS (1659)*
Calcium
Magnesium
Sodium
Potassium
Ammonia, as N
Sulfate
Nitrate, as N
Chloride
Orthophosphate,
as PQfl
Total alkalinity,
as CaCOo
pH
Conductivity
Silica, as Si02
Carbon
Column
Effluent
(feed)
53+
17
126
14
20
72
2.9
135
27
7.4
10
23
Primary
Cation
Effluent
2.0
0.59
61
7.3
9.6
72
2.8
132
27
2.7
9.7
Primary
An ion
Effluent
1.7
0.56
59
7.1
9.2
3.6
1.6
84
15
51
5.7
6.8
Secondary
Cation
Effluent
1.1
0.38
16
1.9
4.0
3.6
1.5
83
14
2.8
5.5
Secondary
Anion
Effluent
(product)
0.60
0.00
15
1.9
3.8
1.3
0.35
14
0.25
39
5.8
3.7
23
*Data taken from May 1968 through December 1968.
tAll constituents in mg/a except: (1) pH and (2) conductivity (ymhos/cm).
The application of ion exchange to nitrate reduction of
reclaimed wastewaters may be particularly important, as these
waters frequently may contain nitrate concentrations in excess
of the 10 mg/ii limit set by the U.S. Environmental Protection
Agency as an interim primary drinking water standard. The use
of ion exchange resins for the removal of ammonium and nitrate
ions has been discussed in the adsorption section of this report.
Few specific exchange resins are available for removal of the
nitrate ion from wastewater; ammonium ion removal with certain
specific ziolite resins can be quite effective. In wastewater
treatment, significant nitrogen removal may be effected by
removing ammonia with ion exchange; in water purification treat-
ment, nitrate is often the most significant form of nitrogen.
Strong nonspecific anion exchange resins have been applied to
the removal of nitrates from drinking water; but because the
resins are nonspecific, competition from sulfides, chlorides,
silicates, and phosphates limits the target removal of nitrates.
This problem of competing ion? may be significant when
considering potable reuse, since reclaimed wastewaters that are
high in nitrates are also likely tu be high in these anions.
The caking and clogging problems caused by iron, turbidity, and
colloidal matter are also significant. In other words, ion
327
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exchange technology for nitrate removal is still developing. A
successful application of the available technology has taken
place at Long Island, New York(1622, 1630). A few years ago, Long
Island communities began experiencing rising nitrate levels in
their drinking water supply source. Drinking water was obtained
from groundwater wells that had been contaminated with nitrates
from septic tanks and cesspools. An ion exchange process
originally developed to demineralize industrial process water
was adapted in a prototype ion exchange plant; it reduced the
nitrate content of several thousand gallons of the Long Island
water from 22 ppm to 0,5 ppm nitrate. A plant was then built
that successfully provided ion exchange treatment for the Long
Island well water under the constant flow and pressure require-
ments of a municipal water system. However, ,the well water was
of relatively low total dissolved solids, and it 1s uncertain
how this process would perform on waters of poorer quality.
A water quality parameter that is of Interest 1n potable
water treatment is color. According to David Volkert and
Associates (1610),1on exchange resins have been developed
that will completely remove color-causing organic dye wastes,
humates, and lignates.
Elemental Contaminants
Ion exchange techniques have been applied to the treatment
of industrial process water containing trace metals for several
years. Application of these techniques to drinking waters con-
taining trace concentrations of these metals is analogous. In
a review of the literature, David Volkert and Associates
(1610) found that several trace elements can be removed from
water to a level of 95 percent. Table 118 lists these elements
and gives the maximum concentrations that can be reduced to
1974 Standards and Guidelines in a single pass through an ion
exchange process (1610). Water containing concentrations of a
particular contaminant higher than the maximum listed in the
table can be either passed through a series of ion exchange
columns with different types of resins, or pretreated by a
method such as lime coagulation to precipitate the major amount
of the metal present.
Calmon(1596) noted that anion exchange treatment can be
used to remove residual arsenic after lime coagulation is used
to precipitate the major amount prerent. Both weak and strong-
base ion exchange resins appear effective in removing arsenate
and arsenite from drinking water (1062). Calmon (1596),
treating an arsenate water containing 68 mg/d arsenic at pH
6.95 with a weak-base anion exchange resin (lonac A-260),
reported 82 to 100 percent removal. Medium and strong-base
resins (lonac A-300, A-540, and A-55LJ) were less effective.
328
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TABLE 118. REMOVAL OF TRACE ELEMENTAL
CONTAMINANTS FROM WATER BY
ION EXCHANGE (1610)
Treatment Contaminant % Removal
Maximum*
Concentration
Ion
Exchange
Arsenic
Barium
Cadmium
Chromium
Copper
Cyanides
Lead
Iron
Manganese
Mercury
Selenium
Silver
Zinc
95
95
95
95
95
95
95
95
95
95
95
95
95
2.0 mg/
20.0
0.2
1 . 0 mg/
20.0
4.0
0.1
6.0
0.1
0.04
0.2
0.1
100
a
a
*Maximum concentration in raw water, which can be reduced to
1974 Standards and Guidelines in a single pass through process,
If raw water concentrations are higher, then combination or
duplication of processes or other processes must be considered
Again using the weak-base anion exchange resin (lonac A-260),
Shen (1244) treated synthetic water containing 106 mg/x, of
arsenic. Only 20.7 percent of the arsenic was removed. When
well waters with naturally high arsenic levels were treated,
essentially 100 percent removal was achieved. The disparity of
the results was not explained.
Bone char and activated alumina readily remove arsenic via
an ion exchange mechanism. Arsenic sorption on bone char
results in an irreversible change in the chemical structure of
the char. Consequently, exhausted bone char must be discarded;
it cannot be regenerated. Activated alumina is regenerable.
329
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Effective removal of barium by ion exchange has been
reported. Patterson (1062) cited a 98.5 percent reduction of
barium from 11.7 to 0.17 mg/a in a full-scale ion exchange
groundwater softening plant in which a general nonspecific water
softening resin was used.
According to Patterson (1062), ion exchange is a common
method for recovery of cadmium from industrial wastewaters, and
many exchange resins are available with high specificity for
the metal. To meet stringent effluent standards, some industries
are using ion exchange rather than cheaper but less effective
methods to treat chromate and chromic acid waters. With proper
pH adjustment, chromate is removed even in the presence of high
concentrations of sulfate and chl oride (1062). Reduction of
hexavalent chromium to 0.023 mg/2, in a metal finishing waste-
water has been reported (1062). Cation exchange can be applied
to remove trivalent chromium, and anion exchange can be employed
to remove chromate and dichromate (1062).
Ion exchange is capable of achieving very high levels of
copper removal. Reduction of 1.02 mg/£ copper to less than 0.03
mg/i has been reported. A selective ion exchange resin (Amber-
lite IR 120) reduced the copper concentration of an industrial
copper plating rinse solution from 45 mg/a to an undetectable
amount (1062). Koerts (1634) found that ion exchange can remove
copper and zinc from industrial waters to produce effluents
containing as little as 0.04 mg/2, of copper and 0.1 mg/x, of
zi nc.
Removal of several metals, such as iron, manganese, lead,
copper, and nickel can be accomplished with ion exchange, but
the processes involve low pH or anaerobic water streams, which
make them normally unsuitable for municipal water treatment.
This technology, however, may be expected to develop as more
attention is given to the application of ion exchange for the
purification of reclaimed municipal wastewaters.
Ion exchange treatment of inorganic mercury-bearing waters
appears to be capable of furnishing an effluent with 1 to 5 ppb
inorganic mercury. Table 119 from Patterson (1062) reviews the
experience with ion exchange treatment for inorganic mercury.
Effluent values in the ppb range are indicated. Preliminary
tests have indicated that cation and anion exchange resins in
series can remove 98 percent of both inorganic and organic
mercury forms. Akzo Chemie has developed a special resin for
mercury, which produces effluent levels below 5 ppb mercury
(1634).
330
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TABLE 119. ION EXCHANGE TREATMENT
FOR INORGANIC MERCURY (1062)
Resin Type
Mtylon-T
Anion*
Macroreticular
Anion*
Osaka IE*
Osaka MR*
ActiveX
Ajinomoto
Billingsfors
Treatment
pH
5-6
7
na
na
"acidic"
na
na
1.5
6.0
11.0
6.5
Mercury
Initial
5,000-25,000
850
10,000
470
3,000-10,000
100-150
10
60
87
1,800
35
Final
1
2.5
<10
30
100-150
2-5
<5
5
3
990
1
Additional
Treatment
« —
--
--
_-
Prefilter
Osaka IE Resin
__
—
—
—
--
Percent
Removal
100
99.7
100
94
98
98
50
92
97
45
97
*Mercury removed as mercuric chloride complex, HgCl
(x-2)
Patterson (1062) presented evidence that cation plus anion
exchange applied to secondary wastewater effluent can remove
selenium to a level of 99.7 percent. He also cited an example
of 85 percent removal of silver from an extremely dilute
secondary sewage effluent by cation exchange, and 91.7 percent
removal by combined cation-anion exchange.
Calmon (1598) discussed the use of ion-exchange for trace
heavy metal removal. As part of his paper, he listed the
specific resins that can be used to remove various heavy metals
These are as follows:
El ement
Arsenic (3+)
Beryl 1i urn
Bi smuth
Boron
Cesi urn
Cobalt
Copper
Germani urn
Gold
Polar Group
Fluorone
Phosphonic Diallyl phosphate
Pyrogallol
N-methyl glucamine, tris hydroxymethyl
ami no methane
Phenolic OH + Sulfonic groups
M-phenylene diamine, 8-hydroxvquino!ine
Phenolic OH + phosphonic groups,
8-hydroxy quincline
m-phenylene diamine
i m i n o d i a c e t i c acid
a 1g i n i c acid
Phoro; e
Pyridinium, thiourea
331
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Element Polar Group
Iron Alginic acid
m-phenylene diamine
hydroxamic acid
phosphonous
phorone
chlorophyl1
haemin deriv.
Lead Pyragallol, Phosphoric
Mercury Thiourea, thiol, iminodi acetic acid,
mercapto resins
Nickel Alginic acid, Dimethylglyoxime
Potassium Dipi cry!amine
Strontium Phosphorous
Titanium Chromotropic acid
Uranium Pyridinium, phosphorous ester
Viruses Metal cation proteins
Zinc Anthranilic
Zirconium Phosphate ester
He also discussed the various types of exchangers, dosages,
operating problems, etc., that can be anticipated for removal
of each metal.
Biocidal Contaminants
Ion exchange units are not specifically designed to remove
biocidal contaminants. However, some incidental removal of
these pesticides, insecticides, and herbicides may occur due to
adsorption on the resin material. This phenomenon will occur
until the adsorptive capacity of the resin is exhausted.
Synthetic/Organic Contaminants
Because many of the synthetic/organic contaminants have
chemical and physical properties that are similar to the
biocidal contaminants, the same considerations apply here as in
the biocidal section.
Biological Contaminants
Since the primary removal mechanism of ion exchange is
based on particle charge properties, any removal of the
biological contaminants will be incidental. Any removal that
does occur will probably be due to mechanical filtration.
332
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REVERSE OSMOSIS
Introduction
For readers unfamiliar with the osmotic membrane process,
one can picture these membranes as thin sheet filter materials.,
Initial Investigators thought that the membranes acted as
strainer-type materials with such small pore sizes that most
Ionic and biological molecules were too large to pass through.
Recent studies with electron microscopes have shown that
removals are controlled by molecular diffusion through the
membrane and that salts and other Impurities diffuse much more
slowly than water (1682). The differential pressure to provide
a driving force through the membrane 1s supplied by pumps. The
wastewater bleed of concentrated contaminants 1s continuous!
and its volume normally equals from 5 to 30 percent of the
volume of the process influent volume. Membrane fouling by
suspended solids, organic slimes, and precipitates 1s a problem
unless substantial pretreatment of the influent water is pro-
vided. Therefore, reverse osmosis 1s normally located as the
last unit process in the water treatment chain.
Very little actual operating data are available regarding
the use of reverse osmosis (RO) for treatment of municipal
water supplies, because the quality provided by reverse osmosis
systems has not as yet been required. Even in areas of high
TDS that could benefit from RO treatment, the cost of this
unit process has been prohibitive. There has, however, been
a substantial amount of research conducted on the use of RO
for polishing highly treated wastewaters. This research,
though, primarily focuses on the removal of selected contami-
nants from solution in laboratory and pilot scale projects.
Since these are similar in many respects to raw water supplies,
performance is often analogous to water treatment situations.
Reverse osmosis may become more important in the future
as both a tertiary wastewater and raw water supply treatment
process, because of its capability to remove a high percentage
of all types of general, elemental, and biological contaminants
as well as many synthetic/organic and biocidal constituents.
With the recent concern over even very small concentrations of
heavy metals, residual organics, and toxic compounds in water
supplies, RO with its 99 + percent removal efficiency may see
increased usage, albeit at a high cost.
333
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Aqueous solutions of two or more solutes reacting with a
membrane may give product flux and solute retentions that are
quite different from those predicted from the behavior of
solutions of the individual organics. This results from
interactions between solutes, their products, and the membrane.
One interesting result in this regard is that improved reten-
tions of solutes were observed when mixed in partially treated
wastewaters, thus increasing the attractiveness of wastewater
RO treatment for reuse (367). Improved retentions are thought
to be due to synergistic effects among the high molecular
weighted components.
Various types of membrane systems have been tested on a
variety of wastewater effluents from primary to highly
treated tertiary. Laboratory tests have also been conducted
on the removal of many synthetic/organic chemicals and bio-
cidal compounds. The RO process does not destroy any of the
input contaminants, but only separates them into two streams,
with the waste stream containing the rejected materials.
Depending upon the feed conditions and the desired objectives,
the product water volume can range up to 95 percent of the
total influent, with the remainder representing the discarded
flow. The characteristics of RO membranes can be controlled
within a wide range by controlling the manufacturing variables.
In general, as one improves the contaminant removal efficiencies,
the flux per unit area decreases. This type of trade-off
implies that the systems can be optimally designed to achieve
the desired objectives.
For this study, the literature reviewed was oriented
towards tertiary wastewater applications as well as laboratory
and pilot scale tests of osmotic membranes. The literature
excluded the extensive basic research on osmotic membranes
for other applications (e.g., industrial wastewater treatment).
The very extensive patent literature on the different types
of membranes, designs, and manufacturing processes was also
excluded. Table 120 provides a summary of the current literature
pertaining to the performance of reverse osmosis units.
Water Quality Parameters
RO systems are not commonly used specifically for general
contaminant removal (with the exception of TDS) , as these
constituents can be sufficiently removed by other less expen-
sive treatment units. However, there were quite a few references
that noted the performance of RO on general contaminant removal
from wastewaters as shown in Table 120. The performance of RO
systems in terms of percent removal is excellent (90 to 99+
percent) for all general contaminants except for low molecular
components of BOD, or COD, and N03.
334
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TABLE 120. LITERATURE REVIEWED PERTAINING TO REVERSE OSMOSIS
r"
Contaminant Reference Number
Water Quality Parameters
ABS 5.S4, 547, 901, 1591 , 1673
NH4 90, 1603, 1608, 1609, 1613, 1616, 1636, 1673
BOD 547, 1608
COD 901, 1323, 1603, 1608, 1609, 1613, 1616,
1636, 1673
Chlorides 901, 1603, 1608, 1609, 1629, 1673, 1684
CN 1629, 1684
Fluorides 1608, 1629, 1684
Hardness 547, 901, 1629
N03 263, 547, 584, 1608, 1613, 1629, 1673
P04 534, 547, 901, 1603, 1608, 1609, 1613, 1629,
1673
S04 901, 1603, 1608, 1609, 1629, 1673
IDS 901, 534, 547, 1603, 1608, 1609, 1613, 1636,
1673
Elemental Contaminants
Aluminum 1608, 1629
Arsenic 1610
Barium 1610
Boron 1608, 1610, 1629, 1684
Cadmium 1323, 1610, 1629
Chromium 1323, 1608, 1610, 1629, 1684
Copper 1323, 1610, 1629, 1684
Iron 901 , 1323. 1610. 1629. 1673
335
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TABLE 120. (continued)
Contaminant Reference Number
Lead 1323
Magnesium 901, 1603, 1608, 1609, 1629, 1670, 1673,
1684
Mercury 1610
Nickel 1323, 1684
Potassium 901, 1608, 1609, 1629, 1670, 1673
Selenium 1610
Silver 1323, 1610
Zinc 1323, 1610
Biocidal Contaminants
DDT 1591, 1604
ODD 1591, 1604
Aldrin 1604
Organophosphorus 1604
insecticide
Chlorinated 1604
hydrocarbons
Dieldrin 1604
Herbicides 1604
Lindane 1591, 1604
Pesticides 367, 1604
Biological Contaminants
Bacteria 1608, 1629
Virus 1608
Synthetic/Organic Contaminants
Misc. organics 534. 1591 . 1608. 1616 ..
336
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Several references discussed the removal of ABS from
solution. The presence of highly nonbiodegradable alkyl
benzene sulfonate (ABS) even in concentrations of only 1 mg/£
can produce undesirable frothing and foams although health
implications do not appear significant. Hauck and Sourirajan
(547) reported removals of 99* percent with a high feed con-
centration of 300 mg/£ . Merten and Bray (901) and an EPA
study (1673) both reported ABS rejection of about 98 percent
with a variety of membranes. Bennett et al. (46) tested RO
performance on a vast array of organics. They showed ABS
removals of 90 percent at a 14 gpd/ft2 flux.
Many studies were conducted that included ammonia removal
(see Table 120). Reported removals ranged from 60 to 97
percent. Since ammonia concentrations are not generally
of significance in water supplies and NH is readily oxidized
in treatment processes, further discussion is not necessary
here.
Hauck and Sourirajan (547) studied the performance of RO on
hard water and on wastewater. The average BOD removal from
secondary effluent was 85.8 and 80.8 percent at 1,000 and 500
psig, respectively. Reference 148 reported BOD secondary
effluent BOD rejections varying from 81 to 94 percent with a
cellulose acetate membrane.
COD removal is studied more frequently than BOD removal
in regard to RO performance, because many of the nonbiodegradable
constituents of COD can be effectively removed by RO. A review
of all nine references reporting on COD removal shows a removal
range of 90 to 99+ percent with an average of about 95 percent.
As a typical example, one of the larger scale pilot programs
performed at Hemet and Pomona, California (1323) found that
RO provided very good removals of trace organics. The COD of
secondary effluent was reduced from 39 mg/£ to 1 mg/£ at
Pomona, while activated carbon effluent COD was reduced from
11.4 mg/£ to 0.3-1.0 mg/£ . Similar removals were reported
from the RO pilot plant at Hemet. It was found that although
RO was capable of greatly reducing effluent COD concentrations,
the costs for full-scale operation are very high.
Chloride is readily removed by RO. Many studies have
evaluated this constituent with removals ranging from 85 to
97 percent (901, 1603, 1608, 1609, 1629, 1673,1684).
Two references included CN removal in research efforts
(1629, 1684). Hindin and Bennett (1629) found that CN removals
ranged from 79 to 85 percent at a flux of about 18 gpd/ft . A
summary report (1684) listed typical CN removal at about 90
percent.
337
-------
A study by Cruver (1608) reviewed RO performance in removing
various contaminants. It was found that fluoride removals
ranged from 88 to 98 percent using selective cellulose acetate
membranes. Hindin and Bennett (1629) and reference 1684 reported
similar results.
RO units are highly efficient at removing hardness (Ca"H"
and Mn"tf~) from water supplies. Hauck and Sourirajan (547)
summarized the effects of RO treatment of hard-water supplies
in five cities and formal removals ranging from 96 to 99.9
psig as CaCOs. Operating pressure was 1,000 psig with a 90
percent product recovery. Performance was directly related to
flux, with the higher removals achieved at lower flow rates.
Merten and Bray also reported removals at roughly 99 percent
for the more efficient membranes they analyzed.
The reviewed data indicates that nitrate nitrogen is one of
the most difficult compounds for RO processes to remove (1673).
Hauck and Sourirajan (547) reported N03-N removals ranging from
50 to 60 percent. Extensive pilot testing by the EPA at Pomona,
California, showed NQ3-N removals of 54 percent over the first
9,475 hours of operation (1603). The five other references
showed similar poor removals ranging from 51 to 86 percent and
averaging around 60 percent.
Both P04= and S04=, on the other hand, were very readily
removed by RO processes. All references reviewed showed
removals of 94 percent or better, some up to 99.9 percent.
The primary water treatment use of RO units is to reduce
the TDS concentrations of highly mineralized waters. One full-
scale example of this is the Orange County Water Districts
Water Factory 21 (1636)where 5mgd of highly treated effluent
is given RO treatment prior to recharge of potable aquifers.
Results from the operation to date show a 90 to 95 percent
TDS removal at 90 percent feed recovery. Results from other
references using various membranes, pressures, and fluxes
showed that average TDS removals were about 91 percent and
ranged from 89 to 99 percent. Removals can be controlled by
membrane selection and adjustment of flux. Studies of pilot
RO systems at Pomona (1603) showed TOC removals of 86 percent
when using primary effluent on the feed.
The major problem areas associated with general contaminant
removal are fouling, short membrane life, and associated
engineering problems. If the membrane life and flux rate prob-
lems are solved, the RO membrane technology may become applicable
to wastewater treatment where some sort of reuse is desirable
and salt content would restrict reuse. At present, the tubular
type membrane systems appear to be more applicable to sanitary
wastewaters due to the lower fouling and easier cleaning
338
-------
Inherent in this type of design. This advantage may not be as
significant in potable water treatment.
Elemental Contaminants
A good deal of available literature on RO membranes
deals with removal of elemental contaminants. RO systems can
be designed to remove almost any elemental contaminant existing
in either an ionic form or colloidal form in water. Generally,
multivalent ions (Fe+3, Cu++, Zn++, S07)are rejected more
effectively than monovalent ions (B+, NOo). As previously
mentioned, the percentage removal will depend upon the specific
membrane and manufacturing procedures. Most references provide
a lengthy list of contaminant removals. It would be redundant
to discuss each of them here. References 283, 1323, 1625 pro-
vide typical summaries of the performance of reverse osmosis
units in removing elemental contaminants. Results are shown
in Table 121. As shown, RO is generally very effective.
TABLE 121. REVERSE OSMOSIS REMOVAL OF
ELEMENTAL CONTAMINANTS (283. 1323, 1629)
Percent Removal (Single Pass)
Contaminant Reference 283 Reference 1.323 Reference 1629
Aluminum - - 97
Arsenic 90-95
Barium 90-95
Boron - - 50
Cadmium 90-98 66-98 68-70
Chromium 90-97 82-98 93-98
Fluorides 90-97 - 88^,98
Copper 90-97 99 82-96
Lead 90-99 99
Iron 90-99 94-99 95-98
Manganese 90-99
Mercury 90-97
Nickel - 98-99
Selenium 90-97
Silver 90-97 96
Zinc 90-99 97
339
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Bjocidal Contaminants
A few studies have been conducted on the removal of bio-
cidals by osmotic membranes (367, 1591, 1604). Excellent
removals were reported for a wide variety of pesticides,
insecticides, and herbicides including chlorinated hydrocarbons,
organophosphorus compounds, and halogenous cyclodienes.
However, a considerable amount of this removal can be attributed
to adsorption or absorption on the membrane itself. Since
these tests were for short time periods relative to commercial
application, the long-term rejection may be more complex and
may depend upon whether the contaminant is adsorped or absorbed
and upon the diffusion rates through the membrane.
With such a large percentage of the removal being related
to adsorption/absorption, it is clear that different types of
membrane materials will show significantly different results.
For example, cellulose acetate (CA) membranes show rather
poor performance on the more polar randox and atrazine, whereas
the less polar polythylenimine based membranes showed satis-
factory performance. Since the active surface on some types
of membranes is on the order of a few tenths of a micron, any
significant amount of absorption can change the membrane compo-
sition and possible rejection of other contaminants.
Reference 367 summarized some results of various studies
using cellulose acetate (CA) membranes for the removal of the
common pesticide 2, 4-D. Results varied widely from 57 to 99+
percent removal depending on influent concentrations, esterifi-
cation, and feed rate. Performance for removal of the insec-
ticide lindane was also sporadic, ranging from rather poor
removals up to 84 percent. DDT and ODD have a very low solu-
bility and tend toward micelle formation thus enhancing RO
performance. Reported DDT and ODD removals were 97 to 99
percent (367, 1610).
Chian et al . (1604) performed a detailed analysis of the
performance of RO units in removing biocidals. Two types of
membranes were evaluated, cellulose acetate (CA) and cross-
linked polyethylenimine (NS-100). With each membrane, rejection
of all types of pesticides (chlorinated hydrocarbons, organo-
phosphorous, and miscellaneous) was better than 99 percent.
Specifically, the following chlorinated pesticides were retained
at greater than 99 percent: aldrin, lindane, heptachlor, hepta-
chlor epoxide, DDE, DDT, and dieldrin.
Of the organophosphorus pesticides, diazinon was removed
at greater than 98 percent, and methylparathion, malathion,
and parathion at better than 99 percent. The lowest removals
were reported with the CA membrane on randox (72 percent) and
atrazine (84 percent). A significant portion of the pesticide
removed was adsorbed on the membrane itself: about 80 to 95
340
-------
percent for hydrocarbons, 30 to 50 percent fororganophosphorus
compounds, and 5 to 60 percent for the miscellaneous pesticides.
Bennett et al . (1591) reported on the removal of organic
refractories including some biocidals. They found that lindane
removal was 84 percent; DDT, 99+percent; and casein, 99 percent.
The literature data indicate that removal of biocidals is
highly variable, depending not only on contaminant concentra-
tions and membrane characteristics, but on synergistic effects
of other components in the water. In any case, RO provides a
high level of treatment for many of the common pesticides and
insecticides.
Synthetic/Organic Contaminants
The performance of RO membranes with respect to removal of
synthetic/organic contaminants is similar to that of many of
the biocides. In general, these contaminants can be adsorbed,
absorbed, rejected or transmitted by the membrane, with removals
depending on chemical species and membrane type. In general,
larger molecular weight compounds are readily rejected or
sorbed by the membrane, whereas low molecular weight compounds
(<100) are more likely to pass through.
Studies by Duvel and Helfgott (1616)have shown that
the cellulose acetate (CA) type membranes rejection of low
molecular wet organics depends upon the molecular weight and
molecular size (as determined by steric geometry, with the size
being more important) ; it also depends on the ability of the
molecule to form hydrogen bonds. The hydrogen bonding behavior
affects the solubility in the membrane surface and hence the
permeabi1i ty.
Studies by Hamoda et al. (534) have shown that high
flux membranes can be developed that have good rejections (90+
percent) of tested organic compounds such as sucrose, glutamic
acid, starch, sodium stearate, ABS, LAS, and beef extract.
Cruver (276) reviewed similar contaminant removals and listed
sucrose at 99.9 percent and glucose at 99.5 percent.
Bennett et al . (1591) performed a comprehensive study of
the removal of organic refractories by RO. Results showed
that the RO process is capable of producing a product water
that is extremely low in organic matter in aqueous solution or
dispersion, with the exception of t!iose organic compounds that,
when in solution or dispersion, have a lower vapor pressure
than water.
The classes of compounds that do not appear to be well
rejected and are present in wastewater effluents include com-
pounds such as methanol , ethanol , and phenol . No data were
341
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found on the low-molecular-weight, halogenated hydrocarbons
such as chloroform, bromoform, halogenated ethane, or ethylene
compounds; but, based on the present theoretical knowledge, one
would expect the removals to be poor.
B.i'o.logica.1 Contaminants
Due to the large size of biological contaminants - including
virus - relative to the effective pore size of RO membranes,
high reductions of these contaminants can be expected.
H Hindin and Bennett (1629)conducted microbiological studies
to determine the permeation through a porous cellulose acetate
membrane of microorganisms found in sewage effluent. Their
results showed that E. coli , A. aerogenes, coliphage 1-7 and
X-175, and S. narcesence were all removed 100 percent by the
RO unit, with the exception of one test in which a leak in
the membrane may have permitted permeation.
Reference 1662 states that bacterial removal efficiency
approximates 99+ percent when the membrane consists of material
that is safe from bacterial decay. Cruver (1608) reports that
several studies have shown that 99.9 percent removals of bac-
teria and virus can be attained.
However, even with these excellent removals, RO processes
are not used alone for disinfection because of the presence
of imperfections in the membranes. These systems are primarily
designed for TDS removal in which small leaks through the
membrane and at seal joints are generally inconsequential.
Nevertheless, these leaks could be significant when they reduce
the removal of virus and bacteria from 99.9999 to 98 percent.
To depend upon these systems for 100 percent biological con-
taminant removal would require continuous monitoring for
biologicals and a degree of quality control that would be
considered beyond the state of the art for field systems.
The present literature indicates that whereas removals
of biological contaminants with RO are very good, they are not
as high or as fail safe as other disinfection practices
(chlorination, ozonation). It should also be remembered that
RO is only a separation process, not a destruction unit, and
that the biological contaminants, once removed, will remain in
the waste solution.
342
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RECREATIONAL WATER
INTRODUCTION
Public health problems can arise if municipal wastewater
effluents are discharged directly into waters used for body
contact recreation. In addition, combined sewer overflows
as well as storm water runoff from urban areas and animal feed-
lots can add to the contamination of recreational waters. At
a few sites in the United States, land-applied wastewater is
being recovered for recreational use (boating, fishing,
swimming). Unless properly supervised, such reuse schemes may
also pose a hazard to public health (134, 1214).
Nearly all health problems associated with recreational
waters can be traced to the presence of pathogenic micro-
organisms of fecal origin. Human infection is most often the
result of direct body contact. As a consequence, recreational
water quality standards have been established that identify
the maximum allowable concentrations of coliform indicator
organisms. The adverse health effects of most other contam-
inants in recreational waters have received scant attention,
since few, if any, outbreaks of disease or infection have been
traced to other than biological pathogens. This fact is re-
flected in the available literature (Table 122).
BIOCIDAL CONTAMINANTS
Pesticides and herbicides found in recreational waters
are not considered to pose a significant public health
problem. The concentration or dosage of such biocides required
to constitute a health hazard is far in excess of water
solubility (1455). Four aspects of the problem were addressed:
• Identification of the acute and chronic levels of
pesticides toxicity in man;
• The amount of pesticides in the human diet;
• Pesticide concentrations in surface waters; and
• The epidemiology of pesticide exposure.
It was concluded that no significant hazard to public
health can be traced to pesticide contact during aquatic
recreation.
343
-------
TABLE 122. LITERATURE REVIEWED PERTAINING TO THE
CONTAMINATION OF RECREATIONAL WATERS FROM
MUNICIPAL WASTEWATER EFFLUENTS
Contaminant Reference Number
Water Quality Parameters
BOD 1342
Chlorides 899
Nitrates 1342
Phosphates 899, 1342
Total dissolved 899
sol ids
Elemental Contaminants
Boron 899
Biological Contaminants
Adeno virus 1455
Bacteria 434, 773, 1094
Conforms 178, 248, 434, 773, 1455
Coxsackie virus 1455
(A&B)
ECHO virus 1455
Fecal 178, 180, 457, 773, 1455
streptococci
Escherichla coli 180
Hepatitis virus 111
Polio virus 888, 1455
Salmonella 178, 248, 457, 1455
Shlgella 178
V1rui 178, 773, 888, 900, 1342
Other (general) 180. 279. 434. 1455
344
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BIOLOGICAL CONTAMINANTS
The following types of disease have been associated with
primary body contact during aquatic recreation: (1) eye, ear,
nose, and throat infections; (2) skin diseases; and (3)
gastrointestinal disorders. Enteric infection from recreational
water is of far less importance than infection from drinking
water, since only small amounts of water are usually consumed
during swimming. Nonetheless, cases of typhoid and other
intestinal diseases traceable to recreational contact have been
reported in the literature, and there is growing concern that
viral infections, particularly infectious hepatitis, may be
contracted by bathing in sewage-contaminated water (1455).
The magnitude of the health risk posed by bacteriological
or viral contamination is uncertain, even when the concentra-
tion of specific pathogens is known. When only the indicator
organism concentrations are known, the risk is even more
difficult to assess. This is because data are lacking from
disease outbreaks or epidemiological studies that establish a
clear correlation between individual cases of disease or the
rate of illness associated with the use of recreational waters,
and a given level of any one of the several potential indica-
tors of microbial water quality (831, 1422, 1455).
A number of case reports has linked outbreaks of viral
or bacterial disease to swimming in contaminated waters.
However, in most cases the occurrence of disease could not be
clearly associated with a specific concentration of water
quality indicator organisms. Moreover, many infections and
toxicities are subclinical in nature, producing only brief or
mild illness and going unreported. Most of these diseases
can be transmitted by routes other than recreational water use.
Consequently, it is difficult to establish a direct statistical
relation between recreational water quality, as indicated by
the levels of indicator organisms, and the incidence of in-
fectious disease (178). Cabelli et al . (178) have recently
embarked on an epidemic!ogical study that is designed to
overcome these problems by using improved control populations
and a range of indicator organisms. Other authors (434, 1455)
have also attempted to develop mathematical models to assess
the health risk posed by a particular level of contamination.
These models are based on critical assumptions about the
probability of infection from a given dose of pathogen and
the probability of acquiring such a dose. However, Fuhs (434)
admits that there are few accurate estimates of infectious
doses of organisms that are of concern in water sanitation.
In fact, Envirogenics Co. (1455) used dose-response data
derived from non-water-related health programs in their model.
Despite the present lack of precise bacteriological and
epidemic!ogical data, authorities have felt obliged to establish
345
-------
standards for recreational water quality. Geldreich (457)
argues that the fecal coliform indicator is more reliable than
salmonella, fecal streptococcus, or total coliform indicators.
He recommends a limit of 200 fecal coliform/100 mi for primary
contact recreational use.
Pseudomonas aeruginosa has also been proposed as an
indicator. This organism is associated with ear infections.
It is present in swimming pools and natural swimming areas and
is found in human feces. More than half of the illnesses
associated with swimming are eye and ear infections, according
to a study cited by Cabelli (180). However, no conclusive
evidence relates P. aeruginosa to swimming-related infections,
and the establishment of a reliable standard based on this
indicator remains unsupported.
In summary, research has been unable to establish the
frequency with which swimming-related infections occur or the
hazard associated with a particular level of contamination.
The risk of contracting serious or fatal disease appears small,
even from waters with poor bacteriological quality. Such
severely contaminated beaches have been occasionally used by
bathers, without reported ill effects (434). Present standards,
although arbitrary, are assumed by authorities to be important
in preventing outbreaks of less serious waterborne disease or
infection.
346
-------
FISH
INTRODUCTION
Wastewater and sludge disposal to aquatic environments
provides the potential for fish to ingest trace metals,
synthetic-organic compounds, biocides, and pathogenic micro-
organisms present in municipal wastes. This disposal of
municipal wastes by direct discharge to surface water bodies
is a direct contaminant pathway. There are also less direct
pathways, e.g., transport of waste constituents in land
runoff, groundwater, or air. In general, the available
literature has not been concerned with these less direct
pathways, although they may occasionally be significant.
For this discussion, attention will be centered on the public
health-impairing contaminants that may accumulate in fish to
levels hazardous to man. Table 123 is a listing of the
literature that was reviewed relevant to fish contamination
from wastewater and sludge.
Trace elemental, synthetic-organic, and biocidal con-
taminants often have the tendency to be bioaccumulated by
aquatic organisms, i.e., to be concentrated into their tissues
to levels much higher than those in surrounding water. This
results from the high solubility of contaminants in lipids
relative to their solubility in water. Bioaccumulation is
a multistage process: the contaminants are taken into the
organism, circulated in the blood, transferred into and out
of various organs, and finally metabolized and/or excreted.
Under conditions of constant exposure, an organism may
eventually reach a quasi-equilibrium in which the concentra-
tion of the contaminant in the tissues is constant. It is
then possible to define a concentration factor, i.e., the
ratio of the concentration of an element or compound in the
tissues of an aquatic organism compared to its concentration
in the surrounding water under equilibrium or steady state
conditions.
Some contaminants tend to be concentrated into the
tissues of organisms at levels higher than those in the food
ingested by the organisms. This most important phenomenon
is termed food chain biomagnification. There is great
variation in the feeding habits of different fish species;
therefore, the particular feeding habits of each species and
the previous steps in its food chain will strongly influence
the quantities of contaminants ingested by the species.
347
-------
TABLE 123. LITERATURE REVIEWED
PERTAINING TO FISH
Contaminant Reference Number
Water Quality Parameters
Ammonia 1397
BOD 1937
Chlorides 1397, 1398
COD 435
Iodides 647
Phosphates 527
Other (general) 647, 873, 1246
Elemental Contaminants
Aluminum 995, 1128, 1380, 1390
Antimony 303, 777, 995, 1128, 1380, 1390, 1408
Arsenic 118, 303, 409, 995, 1128, 1380, 1390,
1408
Barium 995, 1128, 1380
Beryllium 995, 1128, 1380
Boron 995, 1113, 1114, 1128, 1380, 1390
Cadmium 118, 207, 303, 365, 472, 539, 859, 873,
995, 1121, 1128, 1247, 1319, 1380, 1390,
1408
Chromium 19, 77, 303, 365, 777, 859, 873, 995,
1121, 1128, 1247, 1307, 1380, 1390, 1408
Cobalt 303, 365, 647, 859, 995, 1121, 1128,
1380, 1390
Copper 19, 77, 274, 365, 472, 504, 505, 712,
777, 859, 873, 995, 1121, 1128, 1380,
1390, 1408
348
-------
TABLE 123 (continued)
Contami nant Reference Number
Germanium 995, 1128, 1380, 1390
Iron 19, 274, 647, 995, 1121, 1128, 1380,
1390
Lead 118, 234, 365, 472, 539, 748, 777, 859,
873, 995, 1043, 1045, 1121, 1128, 1380,
1390, 1408
Manganese 274, 365, 600, 647, 995, 1121, 1128,
1380, 1408
Mercury 365, 369, 455, 995, 1128, 1251, 1295,
1380
Molybdenum 303, 995, 1128, 1380, 1390
Nickel 19, 365, 859, 873, 995, 1121, 1128,
1380, 1390, 1408
Selenium 995, 1114, 1128, 1380, 1408
Thorium 995, 1128, 1380
Tin 995, 1128, 1380, 1390, 1408
Uranium 995, 1128, 1380, 1408
Zinc 77, 118, 274, 303, 365, 472, 504, 505,
539, 647, 777, 859, 995, 1121 , 1128,
1380, 1390, 1408
Other (general) 303, 365, 647, 873, 893, 1128, 1307,
1380, 1390, 1454, 1456
Biocidal Contaminants
Chlorinated 44, 199, 365, 387, 512, 772S 789, 851,
hydrocarbons 871, 873, 893, 998, 999, 1065, 1163,
1198, 1280, 1294, 1307, 1539, 1561
ODD 425, 429
DDE 199, 421, 429, 851 , 972, 12RQ
DDT 199, 32S, 421, 429, 843, 851 s S7U §73,
874, 972, 1147, 1198, 1280, 1294, 1307,
1530. 1539
349
-------
TABLE 123 (continued)
Contami nant Reference Number
Dieldrin 199, 208, 421, 429, 972, 1280
Endrin 1163
Herbicides 855, 1551
Organophosphorus 1550
pesticides
Other (general) 365, 512, 600, 641, 1454, 1456
Synthetic/Organic 49, 235, 319, 387, 537, 789, 893, 998,
Contaminants 1163, 1397, 1398, 1564
Biological Contaminants
Bacteria 131, 1397
Coliforms 1345, 1397, 1458
Fecal 1397
streptococci
Parasitic worms 161
Salmonella 161, 1397
Shigella 161, 1345, 1397
Virus 161
Other (general) 161
350
-------
ELEMENTAL CONTAMINANTS
Lambou and Lim (748) discussed contaminated fish as one
of the concentrated sources of lead in man. They found that
although lead is relatively insoluble in water, it can be
biologically concentrated at all levels of the aquatic food
chain. They used limited data from isotopic lead experiments
and derived the concentration factors listed below:
Concentration Factor
Bone
5,400
1 ,400
Soft tissue
35
15
Marine fish
Fresh-water fish
Bioaccumulation of cadmium by bass and bluegill has been
observed in the laboratory. For six months, Cearley and Coleman
(207) kept largemouth bass and bluegill in aquaria containing
various concentrations of cadmium in solution. The fish were
exposed to solutions of 805, 80, 8, and 0.5 ppb cadmium, solu-
tion was used as a control . The two most highly concentrated
solutions were toxic to specimens of both species of fish. The
fish accumulated cadmium in concentrations greater than those of
the exposure water. The quantity of metal accumulated increased
as the exposrue concentration increased. At exposure to 8 ppb
cadmium, the maximum total body accumulation by the bass was
8 times greater than that observed in controls; at exposure
to 80 ppb cadmium, the accumulation was 15 times greater. At
exposure to 8 ppb cadmium, the maximum accumulation by the blue-
gill was 6 times greater than that observed in controls; at expo-
sure to 80 ppb cadmium, the accumulation was 210 times greater.
An equilibrium developed between the cadmium concentrations in
the water and in the tissues, as evidenced by the absence of
significant additional accumulation after the second month of
exposure.
The Illinois River has been receiving municipal and
industrial wastes containing trace metals for many years.
Mathis and Cummings (859) used atomic absorption spectro-
photometry to determine the concentrations of copper, nickel,
lead, chromium, lithium, zinc, cobalt, and cadmium in water,
sediments, and fish from the river. Ten fish species were
examined. Five were carnivorous species, feeding mainly on
smaller fish, and five were primarily omnivorous, feeding
mainly on insect larvae, molluscs, algae, and aquatic plants.
The mean metal concentrations in muscle tissue of these fish
are presented in Table 124. All metals were more highly
351
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concentrated in the fish muscle tissue than in the river
water. When carnivorous and omnivorous groups were compared
statistically, it was shown that zinc, chromium, nickel, and
copper concentrations were significantly higher in the
omnivorous than in the carnivorous fish. Concentrations of
the eight metals in bottom sediments were considerably
higher than in fish muscle. Bottom-dwelling worms and clams
closely reflected the concentrations of metals in sediments.
A concentration gradient ranging from highest levels in worms,
intermediate levels in clams, and lowest levels in fish
fillets was observed for copper, nickel, lead, chromium,
lithium, cobalt, and cadmium. Zinc was present at highest
levels in clams and at lowest levels in fish fillets.
Gavis and Ferguson (455) reviewed the knowledge of the
mercury cycle in the aquatic environment. They point out that
mercury does not often exist in hazardous concentrations in
natural waters; however, in places where mercury compounds
have been released to the environment, fish have been able to
obtain and concentrate enough mercury to make them a hazardous
food source. Furthermore, even after mercury discharge was
stopped at these locations, mercury continued to be available
from the bottom sediments, where it had been methylated by
anaerobic bacteria.
Inorganic mercury in the zero or 2 + oxidation state or
methylated mercury can be adsorbed on particles or absorbed by
plankton and then ingested by higher organisms. This accumu-
lation of inorganic mercury by organisms may be facilitated
by the affinity of zero oxidation state mercury for lipids;
however, it is not likely that this is an important factor
since the 2+ oxidation state is predominant in oxygenated
water where most organisms must live. Forms of methyl mercury,
on the other hand, are highly soluble in lipids, facilitating
their absorption and bioaccumulation by aquatic organisms
(455).
Although available data indicate that algae may be able
to bioaccumulate inorganic mercury with concentration factors
reaching 100, Gavis and Ferguson could find no data indicating
the amount of methylated mercury that organisms are able to
bioaccumulate. Further up the food chain the mercury con-
centrations in organisms increase, indicating that biomag-
nification occurs. Fish concentrate mercury from food and
directly from water. Data were cited which showed that at least
90 percent of the total mercury in contaminated Swedish fresh-
water and marine fish was usually of the methylated form.
Additional data showed that fish accumulated higher mercury
concentrations in their tissues as they grew older. None of
the literature reviewed by Gavis and Ferguson was concerned
with municipal waste discharges (455).
353
-------
Shin and Krenkel (1251) conducted laboratory studies to
determine the uptake rates by fish of methyl mercury bio-
synthesized in sediments. They found that the higher the
mercury concentration in sediment, the more methyl mercury
was produced and the greater was the methyl mercury uptake by
fish.
long et al. (1390) measured the concentrations of 36
trace metals in Lake Cayuga trout aged from 1 to 12 yr. Their
studies showed that the concentrations of most metals are not
related to fish age. A significant positive correlation with
age was found only for chromium, while molybdenum and tin had
significant negative correlations. No significant correlations
were found for other metals. Mercury concentrations were not
determined.
The effects of arsenic in aquatic environments were com-
pared with those of mercury by Ferguson and Gavis (409).
Their review indicated that, unlike mercury, arsenic is not
concentrated up the food chain. They cited research which
showed that arsenic concentrations in organisms are con-
siderably higher than those in the water in which they live.
Concentration factors ranging from 2 to 20 have been reported
for fresh-water fish. Concentrations in marine plants and
animals are generally higher than those in fresh-water species,
but evidently little or no food chain biomagnification occurs.
The National Academy of Sciences presented average concentra-
tion factors for the elements in marine fish muscle. These
factors were taken from a large number of references (1128)
and are reported for trace metals in Table 125.
The elemental contaminants have been studied by the
Southern California Coastal Water Research Project (SCCWRP)
as part of an extensive monitoring program of the effects of
waste discharges upon Southern California coastal waters (1307).
Municipal wastewaters are a major source of trace metals to
the Southern California coastal ecosystem. McDermott and
Young (873) studied Dover sole living in contaminated sediments
around major submarine sewage outfalls in Southern California.
They compared the concentrations of seven metals in flesh,
gonads, and livers of Dover sole collected around the Palos
Verdes sewage outfall with concentrations of the metals in
Dover sole collected from a control region in the Santa Barbara
channel. Table 126 gives these concentrations as well as the
multiplication factors for metal enrichment of the sediments
near the outfall relative to the control sediments. In general,
no significant metal enrichments were found in the flesh of
the outfall specimens compared to the control specimens,
although the higher median value for chromium in liver tissue
of outfall specimens is significant at the 95 percent level.
354
-------
TABLE 125. AVERAGE CONCENTRATION FACTORS
FOR TRACE METALS IN FISH MUSCLE (1128)
Trace Metal Concentration Factor
Aluminum 10,000
Arsenic 33,000
Cadmium 1,000
Chromium 70
Cobalt 10
Copper 1,000
Iron 1,600
Manganese 80
Molybdenum 10
Zinc 500
355
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Dover sole was also selected by de Goeij et al. for a
study of trace element concentrations in fish samples from
areas down current from and around the major Los Angeles
sewage outfalls (303). Neutron activation analysis of Dover
sole liver tissue and bottom sediment from both contaminated
and uncontaminated areas was performed. No significant
differences were observed in the levels of 11 trace elements
between the two samples, although sole is a "bottom feeder"
fish, and the ocean sediments in the areas around the sewage
outfalls had trace metal concentrations sometimes 10 to 150
times higher than in uncontaminated areas. Table 127 gives
the measured trace element concentrations in liver tissue
and 95 percent confidence levels for samples from an area
with only natural sediment trace metal accumulation and from
areas near sewage outfalls with intermediate to very high
trace metal accumulation. These data indicate that the con-
centrations of 11 metals in livers of Dover sole did not
increase as a result of exposure to and feeding in contaminated
sediments.
In the 1aboratory,Sherwood and Wright (1247) exposed
another type of marine flatfish, the speckled sanddab, to
dissolved hexavalent chromium and measured the bioaccumulation
of the element. The fish were exposed to 16, 95, 550, and
3,000 ppb of dissolved potassium dichromate for 44 days.
These levels are above the range of common levels for world
ocean waters (0.05 to 0.5 ppb) and are above the level for
water in the immediate vicinity of a Southern California waste-
water outfall. The latter would average 5.0 ppb if the waste-
water were diluted 100:1 Immediately upon discharge. During
the experiment, even at the lowest exposure concentration,
there was significant proportional accumulation of chromium
1n both external and Internal tissues: intestine, skin,
liver, and muscle. These tests confirmed the biological
availability of low concentrations of dissolved hexavalent
chromium to fish. Sherwood and Wright (2147) also exposed
speckled sanddabs to precipitated trlvalent chromium 1n the
form of chronic chloride. Hydroxide precipitate was produced,
added to test tanks, and allowed to settle 1n a layer on the
bottom. Seawater was added on a flow-throuqh basis. Bio-
accumulation did not occur in skin, muscle, or liver, suggest-
ing that the trlvalint chromium precipitate was not biologi-
cally aval Table.
In summary, the Information reviewed appears contradictory,
High concentration factors indicate a tendency for significant
b1oaeeumu1at1on of metals at all Uvels of the food chain,
However, the environmental significance of measured concen-
tration factors, ii discussed by the National Academy of
Selenets (1128), is difficult to establish. Than factors are
often determined 1n thi laboratory, eliminating tht complex
367
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set of relationships that determines the total availability of
a trace element to an organism. Few studies have tried to
identify municipal waste as the source of contaminants to
fish. Studies by the SCCWRP (1307), and by de Goeij et al .
(303) are fairly unique. The studies show no significant
increase in the metal concentrations of fish that live and
feed in contaminated sediments near wastewater outfalls.
BIOCIDAL AND SYNTHETIC/ORGANIC CONTAMINANTS
Polychlorinated byphenyls (PCB's) are an important con-
taminant because of their potentially serious public health
effects and ability to concentrate heavily in fish tissue.
During the period from 1973 to 1975, the Food and Drug
Administration found that 3 percent of the interstate commerce
fish tested exceeded the PCB limit of 5 ppm. All of the
contaminated fish were from the Great Lakes area (1163).
Severe contamination of fish by PCB's in the Hudson River has
also been reported (387). Over 80 percent of the fish sampled
at one point on the river contained more than 5 ppm PCB's
(a rock bass reportedly contained 350 ppm PCB's). In the
past, industrial effluent discharges have been responsible
for much of the PCB loading to aquatic systems; however, as
restrictions on these discharges are more rigidly enforced,
a greater percentage of PCB's discharged to water bodies may
be contained in municipal wastes. According to Nisbet (998),
PCB's have a high tendency for bioaccumulation because of
their high solubility in lipids. Within fish, PCB's are
further concentrated into certain organs, especially those with
high lipid content. Nisbet further points out that fewer
laboratory experiments and more field measurements are needed
to quantify the degrees of bioaccumulation that can be ex-
pected in different circumstances. They cite numerous
studies which showed that under laboratory condi ti ons, f i sh
bioaccumulate PCB's to whole-body concentrations of 30,000
to 300,000 times higher than those in surrounding water.
Concentration factors of up to two million were measured for
lipids.
Chronic exposure of fish to Aroclor 1061 was investigated
by Hansen et al. (537). In a 42-day experiment, when fish were
exposed to concentrations of 32 and 100 mg/i, mortality began
in the second week. The fish that died exhibited symptoms of
poisoning and showed severe liver and pancreatic alterations.
The maximum whole-body residue (wet wt) of PCB was 17,000
times the nominal PCB concentration in test water. The
actual body burden for toxicity was several percent PCB by
weight. When placed in PCB-free water, the fish were able to
remove some of the PCB from their tissues and after 56 days
showed an average reduction of 51 percent in PCB concentration.
359
-------
Lieb et al . (789) reported PCB accumulation in rainbow
trout that were fed Aroclor 1254 at 15 ppm. The total re-
tention of PCB's from the diet was 68 percent for a 32-week
feeding period. The PCB whole-body concentration stabilized
at 8.2 ppm during that period. PCB did not appear to be
eliminated after exposure ceased, even when the fish were
starved. The fish did not appear to be adversely affected
by the PCB.
The results of the above-mentioned laboratory studies
can be compared to results from studies of the natural aquatic
environment. Concentrations of PCB in Cayuga lake trout re-
ported by Bache et al . (49) are listed in Table 128. PCB
concentrations were found to be strongly related to fish age,
with higher concentrations being observed in older fish.
Plankton are an important link in the introduction of
PCB's into the aquatic food chain. Direct surface adsorption
of PCB's by plankton allows these substances to remain in
the pelagic environment for long periods of time. Linko et al
(804) measured PCB concentrations in sediment and plankton
from the southwestern coast of Finland. They found the
concentrations in sediment samples to be lower than those in
piankton samp!es.
Greichus et al. (512) measured organochlorine insecticide
and PCB concentrations in water, bottom sediments, and fish
at Lake Poinsett, South Dakota. As shown in Table 129,
insecticide concentrations in bottom sediments are about 7
times higher than those in the water column, and concentra-
tions in the fish range from 10 to 60 times higher than those
in the bottom sediments. The levels of PCB are higher than
those of insecticides in both sediments and fish.
The persistence of DDT and its metabolites in aquatic
ecosystems and the tendency for food chain biomagnification
was investigated by Dimond et al. (325). The effect of a
single application of DDT to forestland on trout in streams
was studied for 10 yr. Upon application of DDT, the mean
concentration in trout rose to 8.21 ppm; 1 yr later, it
decreased to 3.51 ppm; and after 2 yr, it was 2.10 ppm.
Further reduction in DDT levels was gradual. Even after 10
yr, concentrations were still from 3 to 9 times higher than
those in streams never contaminated with DDT. The average
concentration after 10 yr was 0.35 ppm in treated streams,
compared to an average of .07 ppm in untreated streams.
Laboratory studies by Chadwick and Brocksen (208)
indicate that food organisms are a much less important source
O'f the pesticide dieldrin to aquatic organisms than water.
Dieldrin in solution appears to be immediately and directly
360
-------
TABLE 128. RESIDUES OF PCB's IN CAYUGA LAKE TROUT
AS A FUNCTION OF MATURITY; J. JUVENILE; M. MALE;
F. FEMALE (49)
Age
(yrs)
1
1
1
1
2
2
2
3
3
3
4
4
4
5
6
6
6
7
7
7
8
8
8
9
11
12
12
12
Sex
0
J
J
J
J
J
J
J
0
J
J
J
J
M
M
M
F
M
M
F
M
F
F
M
M
M
F
Length
(cm)
27.7
28.7
33.5
44.5
44.5
41.1
53.8
50.3
55.1
61.0
63.5
66.4
68.3
63.5
68.9
59.7
75.2
71.6
69.0
71.2
80.3
71.6
75.5
70.6
Weight
(q)
181
226
407
815
725
770
1310
1160
1359
2030
2440
2850
2310
2260
3300
1990
3390
2805
3300
3390
4200
2535
3120
3440
PCB
(ppm)
0.6
1.6
0.5
1.2
2.0
1 .3
2.5
2.2
2.4
1 .2
3.5
4.1
5.1
5.7
3.4
9.7
8.6
4.0
5.5
10.0
17.5
13.4
4.5
30.4
12.4
13.4
26.2
7.4
361
-------
TABLE 129. LEVELS OF PCB's AND INSECTICIDES
IN FISH AND BOTTOM SEDIMENTS (512)
Material
Sampled
Water
Bottom
No. of
Samples
6
6
Avg. Total
Insecticides
ppm
0.00023
0.0016
Average
PCB's
ppm
<0.0005
0.0064
sediments *
Fish**
Carp
Crappie
Buffalo
Bui 1 head
2
2
2
2
0.092
0.016
0.032
0.031
0.11
<0.05
0.06
0.11
*
**
Dry wt
Each
t basis.
sample is a composite of 10 fish (wet wt basis).
362
-------
available for accumulation in aquatic animals; however, accumu-
lation of dieldrin via food organisms may be slower since food
is consumed in smaller amounts.
Frank et al . (429) report data on organochlorine in-
secticide residues in fish tissue at four study areas in
southern Ontario, Canada, which had received different
quantities of DDT and dieldrin. The concentrations of
dieldrin, and DDT and its metabolites in the fish tended to
depend on the feeding habits, fat content, and age of the
fish. Low total DDT concentrations (0.1 to 1.0 ppm) were
found in low-fat carnivores; higher concentrations (1.0 to
10 ppm) were found in high-fat bottom and plankton feeders;
and the highest concentrations (over 10 ppm) were found in
high-fat carnivores. A general trend of increasing tissue
concentrations with increasing body weight was also noted.
Yu et al. (1551) investigated the fate of the herbicide,
dicamba, in a model aquatic ecosystem. They found no evidence
that dicamba and its metabolites are biomagnified in the
food chain.
SCCWRP demonstrated that the discharge of chlorinated
hydrocarbons in municipal wastewaters resulted in increased
concentrations of the chlorinated hydrocarbons in sediments
around Southern California sewage outfalls. A close
correspondence between DDT and PCB concentrations in fish and
in sediments of the outfall areas has been observed (365).
SCCWRP collected Dover sole from around Southern
California's five major submarine sewage outfall systems and
at control areas off Dana Point and Santa Catalina Island
(871). Concentrations of DDT and PCB compounds in fish
muscle tissue were measured in 1971-72 and 1974-75, as
shown in Table 130. The highest PCB concentrations were in
specimens collected near the Palos Verdes, Santa Monica, and
Oranqe County submarine sewage outfalls. These concentrations
were significantly higher than those found at the control
areas.
The major municipal wastewater discharge point for DDT
is at Palos Verdes. Approximately 75 percent of the muscle
tissue samples from Dover sole caught in 1971 and 1972
near Palos Verdes contained over 5 ppm DDT (1530). As shown
in Table 130 , the median concentration was 9.0 ppm in
1971-72 and 12 ppm in 1974-75, despite an 8C percent reduc-
tion between 1971 and 1973 in the amount of DDT discharged
annually at Palos Verdes.
DDT concentrations in the flesh of bottom-feeding fish -
such as black perch and kelp bass caught off Palos Verdes
363
-------
TABLE 130. CHLORINATED HYDROCARBON CONCENTRATIONS
IN MUSCLE TISSUE OF DOVER SOLE (871)
(mg/wet kg)
Region
Pt. Hueneme
1971-72
Median
(Range)
0.4
(0.3-0.4)
1974-75
Medi an
(Range)
0.1
(0.1)
1971-72
Median
(Range)
0.1
(0.1)
1974-75
Median
(Range)
0.06
(0.05-0.07)
Santa Monica 1.5
(0.9-7.2)
Palos Verdes 9.0
(3.2-45)
Orange Co. 0.8
(0.7-4.4)
Dana Pt. 0.2
(0.2-0.3)
San Diego
Santa Catalina 0.1
Island (0.1-0.2)
1.4 1.5 2.0
(0.6-1.7) (0.4-2.8) (1.0-2.3)
12 1.9 1.3
(9.7-25) (0.7-6.6) (0.06-2.2)
3.6 0.8 0.6
(0.7-26) (0.2-1.2) (0.3-2.6)
0.2 0.06 0.2
(0.1-2.7) (0.03-0.09) (0.05-0.6)
0.05
(0.04-0.3)
0.1
(0.1)
0.2
(0.08-0.4)
0.04 0.05
(0.04) (0.03-0.07)
364
-------
in 1973 - ranged from 0.82 to 87 mg/wet kg (black perch) and
from 0.37 to 29 mg/wet kg (kelp bass). Concentrations in
approximately half of all specimens exceeded 5 mg/wet kg.
By contrast, a surface feeding predator, the bonita, had
a median DDT concentration of 15 to 500 times lower than the
median concentrations found in the bottom feeders (1530).
BIOLOGICAL CONTAMINANTS
Many of the biological contaminants, when ingested by
fish, may survive in fish viscera, since fish do not have
a permanent coliform or streptococcus flora in their in-
testinal tracts. The population of microorganisms in fish is
a reflection of the population in the external environment.
Bacteria that are indicators of human fecal contamination,
including Streptococcus faecal is and Salmonella ty p h i m u r i u m,
have been found in the intestinal tract of various species
of fresh-water fish (1397).
The intestinal contents of 78 fish from a moderately
polluted river were examined in a study cited by Tsai (1397).
The fecal coliform densities were lowest in bluegill sunfish
(less than 20/g) and highest in catfish (1,090 ,000/g );
levels of fecal streptococci for the two species were 200
and 240,000/g, respectively. Apparently, these differences
were due mainly to habitats and feeding habits of the species.
In another study cited by Tsai, carp were artificially
infected with typhoid bacteria. The bacteria were present
in all organs from 24 to 48 hours after infection and per-
sisted for 8 to 14 days; they did not disappear until after
four to six weeks, although the fish remained healthy.
Temperatures attained by cooking are not, in general,
high enough to destroy typhoid bacteria; therefore, it
is theoretically possible for bacteria to be transmitted
to humans. Research cited by Tsai showed that fish taken from
heavily polluted streams contained specific antibodies to
the bacteria that cause human pseudotuberculosis, paratyphoid
fever, bacillary dysentery, and a variety of chronic infec-
tions. Fish taken from mildly polluted streams were free of
such antibodies.
Shigella and enteropathogenic Escherichia coli were
isolated in fish from contaminated ri ver water (161). Certain
parasitic diseases are maintained by the cycle: human feces
to fresh water; water to copepods or snails; and copepods
or snails to fish. C1 i n o r c h i s s i ni enisi s, Diphyl1obothri urn
1 a t u m, and Echinostoma 11 oc an urn" are" "human parasites with
such life cycles. An outbreak of diphyllobothriasis was
reported from eating fish caught in sewage-polluted water,
365
-------
The research indicated that fish living in contaminated
water can be vectors of pathogenic bacteria to man. However,
this has not been a health problem in the United States
because fish are customarily cleaned (removal of viscera)
and cooked before eating. Obviously, improper cleaning or
storage of fish, which allows pathogenic organisms to enter
the flesh and/or multiply, may create health problems.
366
-------
SHELLFISH
INTRODUCTION
Filter-feeding shellfish (oysters, clams, etc.) are a
major potential pathway of contaminants from wastewater to
man. Such shellfish filter large volumes of water through
their bodies to obtain food and oxygen. In this process
they retain suspended particulate matter. A significant
portion of the biological, trace-elemental, synthetic-organic,
and biocidal contaminants discharged to water bodies in
municipal wastes are associated with the particulate phase,
so there is the potential for shellfish to effectively con-
centrate these contaminants.
While there is relatively little research directly
linking shellfish contamination with municipal wastewater
discharges, the evidence is clear that shellfish taken from
contaminated waters will be contaminated. Table 131 is a
listing of the literature that was reviewed relevant to shell-
fish contamination from wastewater and/or wastewater sludges.
ELEMENTAL CONTAMINANTS
Pringle et al . (1121) reported the ability of estuarine
shellfish to concentrate trace elements to levels many
hundreds of times the levels found in estuarine water and sea-
water. Average concentrations of trace metals in shellfish
taken from Atlantic coastal waters are shown in Table 132.
Species differences in the amount of bioaccumulation are evi-
dent. The averages in Table 132 reflect shellfish accumula-
tion of metals at hundreds of locations along the Atlantic
Coast of the United States, with widely varying degrees of
pol1ution.
Table 133 shows the range of metal concentrations in
samples from Atlantic and Pacific waters. The varieties of
environmental contamination at different locations are a
factor contributing to the broad range of metal concentra-
tions in shellfish shown in Table 133.
A survey for the U.S. Environmental Protection Agency
(EPA) (1241) of shellfish beds in San Francisco Bay reported
metal concentrations in shellfish similar to those reported by
367
-------
TABLE 131. LITERATURE REVIEWED
PERTAINING TO SHELLFISH
Contaminant Reference Number
Water Quality Parameters
BOD 226
Iodides 647
Other (general) 226, 435, 828, 919, 1459
Elemental Contaminants
Aluminum 995, 1128, 1380
Antimony 995, 1128, 1380
Arsenic 409, 995, 1128, 1380
Barium 995, 1128, 1380
Beryllium 995, 1128, 1380
Boron 995, 1113, 1128, 1380
Cadmium 135, 136, 162, 365, 502, 539, 698, 699,
732, 828, 995, 1128, 1135, 1241, 1378,
1380
Chromium 162, 365, 502, 611, 698, 699, 732, 828,
859, 995, 1128, 1137, 1307, 1380,
1537, 1540
Cobalt 162, 365, 647, 859, 995, 1128, 1380,
1538
Copper 135, 136, 162, 365, 502, 611, 698, 699,
732, 828, 995, 1128, 1135, 1137, 1307,
1380, 1537, 1540
Germanium 995, 1128, 1380
Iron 55, 135, 136, 162, 365, 611, 647, 995,
1128
Lead 88, 135, 136, 162, 365, 502, 539, 611,
698, 732, 828, 859, 995, 1128, 1241,
1537, 1540
368
-------
TABLE 131 (continued)
Contaminant
Reference Number
Manganese
Mercury
Molybdenum
Nickel
Selenium
Thorium
Tin
Urani urn
Zinc
Other (general )
Biocidal Contaminants
Chiori nated
hydrocarbons
ODD
DDE
DDT
D i e 1 d r i n
Endrin
Herbicides
136, 365, 502, 600, 647, 828, 853, 995,
1128, 1380, 1538
285, 369, 370, 431, 437, 625, 731, 995,
1128, 1264, 1295, 1380
995, 1128, 1380
135, 162, 267, 365, 698, 699, 828, 859,
995, 1128, 1537
995, 1114, 1128, 1380
995, 1128, 1380
995, 1128, 1380
995, 1128, 1380
135, 162, 365, 502, 539, 611, 647, 698,
732, 828, 859, 995, 1128, 1135, 1380,
1537, 1538, 1540
647, 828, 859, 1121, 1241, 1380, 1454,
1456, 1537
173, 432, 537, 554, 804, 851, 997, 998,
1065, 1146, 1163, 1197, 1438, 1529,
1531 , 1532
346, 422, 1408
316, 422, 713, 1408
346, 422, 554, 654, 713, 798, 922,
1044, 1045, 1074, 1306, 1307, 1390,
1408, 1446, 1525
421 , 422, 1081
173, 1163
806, 1197
369
-------
TABLE 131 (continued)
Contaminant Reference Number
Other (general) 600, 806, 1197, 1454, 1456
Synthetic/Organic 319, 402, 570, 1306, 1307, 1564
Contaminants
Biological Contaminants
Bacteria 161, 238
Coliforms 177, 973, 1241 , 1307
Coxsackie virus 905
(A & B)
ECHO virus 905
Parasitic worms 161
Polio virus 322, 323, 905
Salmonella 161, 1241
Shigella 161
Virus 161, 177, 238, 322, 468, 973, 1307
Other (general ) 161
370
-------
TABLE 132. AVERAGE TRACE METAL CONCENTRATIONS IN
SHELLFISH TAKEN FROM ATLANTIC COAST WATERS
IN PPM (WET WT)(1121)
Element Eastern Oyster Soft Shell Clam Northern Quahaug
Zinc 1428 17 20.6
Copper 91.50 5.80 2.6
Manganese 4.30 6.70 5.8
Iron 67.00 405 30
Lead 0.47 0.70 0.52
Cobalt 0.10 0.10 0.20
Nickel 0.19 0.27 0.24
Chromium 0.40 0.52 0.31
Cadmium 3.10 0.27 0.19
371
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372
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Pringle et al. (1121). The data represents 16 sampling
stations. The ranges of trace metal concentrations are as
fol1ows:
Concentration
Element (mg/kg wet)
Cadmium 0.06 to 1.41
Chromium 0.10 to 6.63
Copper 1.12 to 48.2
Lead 0.23 to 18.7
Mercury 0.01 to 0.15
Zinc 8.48 to 157
Cadmium in shellfish meat from two stations exceeded 0.5
ppm (0.58 ppm and 1.41 ppm), and lead concentrations exceeded
7 ppm. All levels of mercury from the specimens, however,
were below 0.5 ppm. Zinc concentrations were high in oysters,
as was found earlier by Pringle et al. (1121).
Mathis and Cummings (859) analyzed fresh-water clams
taken from the Illinois River, which has been receiving
municipal and industrial wastes containing trace metals for
many years. Metal concentrations in the clams (Table 134)
reflected the levels found in the river bottom sediments
(Table 135); concentrations in the clams exceeded levels
found in the water, but were similar to or less than the
concentrations in the sediments.
The uptake of mercury by shellfish depends upon the
chemical and physical form of the metal. The uptake of
mercury and its compounds has received a great deal of atten-
tion as a consequence of the Minamata Bay incident in Japan.
Irukayama (625) reported that abundant inorganic water-
soluble mercury compounds had accumulated in the mud of Mina-
mata Bay, although these compounds were scarcely accumulated
by shellfish cultured experimentally in seawater containing
the mud. Further experimentation led to the conclusion that
an organo-mercury compound -- probably methyl or ethyl
mercury -- dissolved in the seawater of the bay had accumu-
lated directly in fish and shellfish. This compound was
finally identified as methyl mercury chloride, a somewhat
water-soluble compound that had been discharged to the bay
in sludge from an acetaldehyde manufacturing plant. After the
discharge from the plant was discontinued, the mercury content
in shellfish decreased in two years from 85 to 10 ppm,
although abundant inorganic mercury compounds were still
present in the sediment.
Further research has indicated that any form of mercury
that is discharged to water bodies may be converted to methyl
373
-------
TABLE 134.
CONCENTRATION
(859)
OF METALS IN CLAMS
Fusconaia flava
No
Metal
Copper
Nickel
Lead
Chromium
Lithium
Zinc
Cobalt
Cadmium
No
Metal
Copper
Nickel
Lead
Chromium
Lithium
Zinc
Cobalt
Cadmium
. of Samples
Analyzed
17
17
17
17
17
17
17
17
. of Samples
Analyzed
25
25
25
25
25
23
25
25
Concentration
Mean (ppm)
1 .7
2.1
3.7
7.7
0.109
66
1 .2
0.69
Amblema plicata
Concentration
Mean (ppm)
1 .2
1 .1
2.7
4.4
0.076
95
0.7
0.38
Concentration
Range (ppm)
0.9 to 2.0
0.7 to 3.0
1 .8 to 5.1
1.1 to 11.6
0.042 to 0.190
25 to 120
0.6 to 1 .6
0.36 to 1.17
Concentration
Range (ppm)
0.3 to 3.2
0.4 to 2.3
1.1 to 7.6
0.6 to 9.9
0.0005 to 0.260
40 to 178
0.4 to 1 .2
0.15 to 1 .41
No. of Samples
Metal Analyzed
Quadrula guadrula
Concentration
Mean (ppm)
Concentration
Range (ppm)
Copper
Nickel
Lead
Chromi urn
Lithium
Zinc
Cobal t
Cadmium
20
20
20
20
20
19
20
20
1 .
0.
2.
4.
0.
48
0.
0.
7
9
2
7
063
8
56
1.1 to 3.6
0.4 to 1 .6
0.9 to 3.8
1.8 to 8.3
0.036 to 0.1
28 to 64
0.5 to 1 .3
0.31 to 1 .37
00
374
-------
TABLE 135. MEANS AND RANGES OF METAL
CONCENTRATIONS IN BOTTOM SEDIMENTS OF THE
ILLINOIS RIVER AND THREE NONINDUSTRIAL-USE STREAMS (859)
Metal
Concentration (ppm)
11 1 inoi s River
Mean Range
Three Nonindustrial -
Use Streams
Mean
Range
Copper
Nickel
Lead
Chromium
Lithium
Zinc
Cobalt
Cadmium
19 1 to 82 7.7
27 3 to 124 16
28 3 to 140 17
17 2 to 87 6
3.8 0.5 to 16.3 3.8
81 6 to 339 30
6 1 to 18 6
2.0 0.2 to 12.1 0.4
3,5 to 11.2
10 to 22
13 to 27
3 to 7
1 .7 to 5.7
18 to 41
4 to 8
0.3 to 0.5
375
-------
mercury by microorganisms living in bottom sediments (437,
731). Metallic, inorganic, and phenyl mercury can thus be
made available for accumulation in shellfish. Kopfler (731)
exposed oysters to different seawater S9lutions containing
mercury as (1) inorganic mercuric chloride, (2) methyl
mercuric chloride, and (3) phenyl mercuric acetate. When
exposed to 1 ppb mercury in any of these three forms, oysters
rapidly concentrated mercury in their tissues far in excess
of the 0.5 ppm limit recommended by the U.S. Food and Drug
Administration (FDA).
Los Angeles County's submarine discharge of municipal
wastewater off Palos Verdes Peninsula is the single largest
man-related source of trace metals to Southern California
coastal waters. Bottom sediments around the outfall system
are highly contaminated by a number of trace metals. Young and
Jan (1537) reported abnormal levels of seven metals in three
tissues of filter-feeding rock scallops (Hinites multirugosui)
that were collected in the discharge zone and ^hui~hTd~¥eerT
exposed to suspended wastewater partlculates. The trace metal
concentrations in these scallops were compared with concen-
trations from control regions. The "contamination ratios"
(outfall-to-control region ratios of mean metal concentrations
1n scallops) are presented 1n Table 136. This data shows
that rock scallops liv'-ic! 1n the wastewater discharge area
accumulated trace metaiS above normal levels; 16 of the 19
contamination ratios are greater than 1.0.
TABLE 136. "CONTAMINATION RATIOS" (OUTFALL-TO-CONTROL
REGION RATIOS OF MEAN METAL CONCENTRATIONS) FOR SEVEN
METALS IN THREE SCALLOP TISSUES (1537)
Metal
Silver
Cadmium
Chromium
Copper
Nickel
Lead
Zinc
D1 gestl ve
Gland
7.4
0.93
19
3.0
0,87
3.0
1.3
Gonad
4,4
0.48
6.7
1 .4
2.8
2.3
Adductor
Muscle
3.2
2.8
7.0
2.6
1 .8
1 .1
The average mercury concentrations 1n tissues of mussels
from Palos Verdes were reported by Eganhouse and Young (370).
Concentrations 1n digestive gland tissues, adductor muscle,
and gonadal tissues were 62.8, 61,8, and 14.2 ug/wet kg,
respectively -- two to three times higher than levels in
mussels from control regions, The high values appeared to be
376
-------
related to the sewage outfall. Experiments were performed to
determine the availability of mercury discharged in the Palos
Verdes effluent to mussels (Myti1 us ca1i f orn i a nu s) (370).
Mussels from an area of relatively low mercury levels were
suspended near the wastewater outfall and monitored for
mercury uptake as a function of time. Of three tissues
analyzed, digestive gland tissues accumulated mercury at the
fastest rate and contained the highest levels. Adductor muscle
and gonadal tissues had markedly slower accumulation rates.
The mercury concentrations in various tissues of crabs,
prawns, snails, urchins, and sea slugs from the Palos Verdes
shelf measured in 1975 (369) were quite low, in no case
approaching 0.5 ppm (FDA guideline for edible seafood).
Organic mercury constituted the major fraction of total mercury
in muscle tissues of several of the animals. An analysis of
the data with respect to proximity to the wastewater outfall
showed no distinct pattern. Thus, the investigators concluded
that the tissue mercury content of these benthic animals was
not governed significantly by sediment concentrations.
Similarly no significant correlations were found between
concentrations of 12 trace metals in bottom sediments and
in six shellfish species growing at five locations in the San
Francisco Bay estuary. Mercury concentrations in two harvest-
able shellfish species -- Mya arenaria and Tapes japonica -- at
all sampling locations were below 0.5 ppm, wet weight. Cadmium
concentrations in both species from several locations reached
3 ppm, dry weight, and lead levels at several sites ranged
between 12 and 19 ppm. Metal concentrations in oysters
(Crassostrea gigas) from a relatively contaminated area inside
San Francisco Bay and a relatively clean area outside the bay
were dramatically different. For example, the heptopancreas of
bay oysters had concentrations of silver, cadmium, copper,
mercury, and zinc that were respectively 103, 8, 31, 17, and
22 times higher than the concentrations observed in the
hepatopancreas of clean-water oysters.
SCCWRP (1307) found that submarine discharges of waste-
water near two of California's harbors did not appear to have
caused increased copper levels in intertidal mussels (Myti1us
e_d u 1 i s) growing at the bases of these outfalls; vessel anti-
fouling paints evidently caused increased copper levels in
mussels within the harbors. A third wastewater outfall off
Palos Verdes Peninsula near San Pedro harbor did seem to cause
increased copper concentrations in mussels at the base of
this outfall system; the mussels contained an average of 47
ppm copper compared to the 20 ppm of the control mussels.
377
-------
SYNTHETIC/ORGANIC AND BIOCIDAL CONTAMINANTS
The synthetic-organic or biocidal compounds most often
studied as shellfish contaminants are DDT and PCB's. Heesen
and McDermott (554) reported that relatively large concentra-
tions of DDT were found in a variety of shellfish collected in
coastal waters of Los Angeles and Orange Counties in California
They measured concentrations of chlorinated hydrocarbons in
the market crab (Cancer anthonyi ), which feeds on bottom
material that can be significantly contaminated with trace
constituents. The results indicated that DDT and PCB concen-
trations in the flesh of crabs collected around major submarine
sewage outfalls were not above 5 ppm. Concentrations of DDT
were several times higher in crabs around sewage outfalls
than in those around other coastal areas; however, PCB con-
centrations were similar.
Studies performed by SCCWRP (1306) suggest that inter-
tidal mussels (Myti1 us cali forni anus ) rapidly reflect changes
in the seawater concentrations of chlorinated hydrocarbons
by changes in their own tissue concentrations. A 1971 survey
of the Los Angeles Bight (1531) revealed a distinct correla-
tion between the concentrations of both DDT and PCB 1254 in
mussels and the proximity of the station from which the mussels
were taken to the Palos Verdes submarine sewage outfall
system, a major source of DDT and PCB's to the region. For
over 100 km in most directions from the discharge area, DDT
concentrations above baseline levels were detectable; a
maximum concentration of 4,200 ppb total DDT was found in
mussels near the discharge. In comparison, the median con-
centration at six control stations was only 70 ppb.
Since 1971, there has been significant reduction in the
concentrations of these chlorinated hydrocarbons in municipal
wastewater effluent discharged off Palos Verdes. The input
of total DDT compounds to the Bight decreased by approximately
90 percent. Decreases in DDT and PCB concentrations in
mussels sampled from a beach at the base of the outfall system
between 1971 and 1973 were similar to concentration decreases
in the effluent. A follow-up experiment was performed that
similarly showed elimination of DDT metabolite from mussel
tissue when exposure to contaminated water ceased.
Although greatly reduced, the influence of the waste-
water discharge was still evident in 1974 (1307); in Palos
Verdes mussels, DDT concentrations and PCB 1254 concentrations
were 10 and 100 times above baseline values. Both these
studies (1306, 1323) demonstrated the usefulness of the
mussel as an indicator of chlorinated hydrocarbon contamina-
tion of nearshore waters. As a result, an offshore caged
mussel biomonitoring program was set up (1307). The results
378
-------
of the program, as expected, showed a direct relationship
between uptake of DDT and PCB and proximity to contaminated
bottom sediments or a wastewater plume. Specimens suspended
near the bottom became approximately 10 times as contaminated
as did surface specimens. A concentration factor of over
100,000 was estimated for DDT and PCB in soft mussel tissues.
BIOLOGICAL CONTAMINANTS
Mussels and other shellfish are efficient concentrators
of bac^ria and viruses from seawater. SCCWRP (1307), in
testing mussels (Mytil us californianus and Myti 1 us edulis)
from three nearshore 1ocati ons , d e t e c t e d enteroviruses in
mussels from a channel where coliforms in the mussels exceeded
275,000/g (most probable number) of digestive gland tissues.
However, no enteroviruses were detected in mussels from a
beach where coliforms in the mussels were about 30 times
lower, or 8,600/g (most probable number). The beach site was
at the base of a large sewage outfall system, yet microbial
contamination was quite low compared to that of samples from
the channel , which was much further removed from a known source
of contamination.
Further experiments involving the suspension of caged
mussels in outfall areas were conducted by Morris et al.
(973). Viruses were detected and quantified in 16 of 39
samples taken from mussels suspended at various depths.
Table 137 lists concentrations of total coliforms and viruses
in these 16 samples. It also shows that the ratio of coliforms
to virus particles ranged from 11,400 to 10.1 million.
Calculations indicated that viruses were more concentrated
with respect to coliform bacteria in mussels than in sewage
and that mussels positive for viruses contained 0.1 to 8
virus particles per individual mussel.
A survey by the EPA (1241) of shellfish beds in San
Francisco Bay reported bacterial levels in shellfish from
16 sampling stations. Total coliform, fecal coliform, and
salmonella densities were determined. Shellfish from the
bay commonly had fecal coliform levels that exceeded the
standard of 230/100/g of meat set by the National Shellfish
Sanitation Program. Fourteen of 16 stations sampled were
in violation on at least one occasion. A high value of 23,000
fecal coliforma/g of shellfish meat was found at two locations.
Salmonel1 a kentucky and Salmonella typhimuri urn , pathogenic
bacteria, were each found at one location.
There have been several disease outbreaks associated
with the consumption of shellfish contaminated with waste-
water microorganisms. Bryan (161) in a literature review
cited 10 instances in which shellfish, particularly oysters,
transmitted typhoid fever to humans; 13 instances in which
379
-------
TABLE 137. CONCENTRATIONS OF TOTAL COLIFORMS AND
ENTEROVIRUSES IN SEAWATER AND IN DIGESTIVE GLANDS
OF MYTILUS CALIFORNIANUS SUSPENDED FROM BUOYS (973)
Location and
Water Depth
Total Col i form
Date Seawater
Sampled (No./£)
Viruses in
Mussels Mussels
(No. /kg) (PFU/kg)*
Ratio
Col i forms
to Viruses
in Mussels
Santa Monica Bay
15 m
45 m
45 m
Pal os Verdes
Buoy 1
30 m
Buoy 2
16 m
16 m
32 m
32 m
32 m
Buoy 3
17 m
25 m
32 m
32 m
Orange County
Surface
15 m
45 m
* Values gi
** ND. nn Ha
6
6
11
1
3
17
3
17
1
3
30
3
30
6
6
6
Mar
Mar
Feb
Mar
May
May
May
May
Jun
Oct
Oct
Oct
Oct
Feb
Feb
Feb
76
76
76
76
76
76
76
76
76
75
75
75
75
76
76
76
4 x 103
8 x 10
ND**
7 x
1 x
1.2 x
5.9 x
7 x
8.4 x
5 x
3.7 x
1.1 x
1.7 x
ND
ND
ND
103
io32
106
103
102
102
103
103
7.9
3.5
7
1.1
x
x
X
X
3.48x
1.2 x
3.48x
7.8 x
8.6 x
4.9
1.2
8
4
9.2
9.2
3.1
ven do not reflect an estimated
ta.
X
X
X
X
X
X
X
107
107
107
108
107 1
106
10*
106
106
108
108
10'
efficiency
263
140
30
114
620
552
,475
210
321
41.7
105.3
315.8
263.2
91
476
25
3
2.5
2.33
9.65
5.61
2.17
2.36
3.71
2.68
1.18
1.14
2.53
1.52
1.01
1.93
1.24
of recovery of
X 10r
x 10?
x 106
x 104
x 10?
x 10J
x 10*
x 10,
x 10
x 10*
x ID/,
x 10J
x 10
x 107
x 106
35%.
380
-------
clams and oysters were responsible for viral hepatitis out-
breaks; and 3 instances in which cholera was transmitted
by shellfish. The bacterial or viral agents of these diseases
(Salmonella typhi, Vibrio cholerae, and hepatitis virus A) can
be retained by shellfish as they filter large volumes of water
through their bodies. This filtering action can result in the
accumulation of bacteria and virus concentrations in shell-
fish tissues that are greater than the concentration in the
water being filtered. The potential public health consequences
are obvious.
When two-year-old Cal1forn1a mussels were placed in water
containing approximately 3.5 x 10^ polio virus, plaque- *
forming units (pfu) per m£, the mussels accumulated 2.6 x 10
units/g of tissue after 48 hr. West Coast shore crabs, after
residing in water containing 1.4 x 104 polio-virus pfu/m£ for
48 hr, accumulated 4.9 x 10* pfu/g of tissue. Crabs fed
virus containing mussels accumulated 74 to 94 percent of the
virus present in the mussels (322).
Coxsackle virus survival 1n live oysters was studied
by Metcalf and Stiles (905). Oysters exposed to water con-
taining vlrlons 1n the laboratory were then Immersed in an
estuary for two months. Vlrlons survived in the oysters for
the two months during the winter, but less than one week during
summer. At no time were vlrlons Isolated from control oysters.
It was postulated that the shellfish were dormant 1n cold water
during winter, favoring virus retention, but that warmer summer
water temperatures brought on oyster feeding activity and
depuration of vlrlons.
Virus survival 1n chilled, frozen, and processed oysters
has also been studied (DIGirolamo et al.»323). Polio virus
was found to survive 1n raw oysters refrigerated at tempera-
tures between 5 and -17.5°C for 30 to 90 days. The survival
rate varied from 10 to 13 percent. The survival rate of
vlrlons 1n the oysters that withstood stewing, frying, baking,,
and steaming ranged from 7 to 10 percent. It was concluded
that, 1f they are harvested from contaminated areas, not only
fresh, but also refrigerated and cooked oysters can transmit
virus diseases.
331
-------
CROPS
INTRODUCTION
Disposal of wastewater and sludge to agricultural land
is presently practiced at over 400 locations in the United States.
The majority of these locations grow crops that are not consumed
directly by man, e.g., forage, animal feed, etc. There are,
however, examples of municipal waste application to over 25
different edible fruits and vegetables.
This municipal waste application can cause surface contami-
nation of plants by viable pathogenic microorganisms, as well
as accumulation of various trace metals in plant tissues. There
is some concern over the possibility that humans may consume
pathogenic bacteria and viruses or hazardous amounts of metals
when they eat crops grown on waste-supplied land. There is also
concern over the adverse effects of feeding such crops or contami-
nated forage to animals intended for human consumption. Iden-
tification of the contaminant levels that may be associated with
the surfaces or tissues of crops grown on waste-supplied soils
is still in progress. The pertinent literature reviewed is
listed in Table 138.
WATER QUALITY PARAMETERS
High nitrate content in food has been identified as a
potential public health concern (133, 1432); however, no research
was found in the course of this review which indicates that
nitrate accumulation to high levels is a problem in crops grown
on sludge or wastewater-amended soil. On the contrary, nitrate
uptake by crops is generally considered desirable, since it
protects groundwater from nitrate contamination.
Although municipal sewage sludge contains significant
quantities of nitrogen, the amount of nitrogen that is made
available to plants at typical land application rates does not
approach the amount that is made available by inorganic nitrogen
fertilizers. Viets and Hagemen (1432) examined the potential
for nitrate contamination of crops resulting from the use of
inorganic nitrogen fertilizers. They concluded that the current
heavy use of chemical fertilizers has caused no overall increase
in the nitrate content of foods and livestock feeds.
ELEMENTAL CONTAMINANTS
Applications of sanitary wastes to soils affect the metal
content of crops directly by serving as a source of trace metals
382
-------
TABLE 138. LITERATURE REVIEWED
PERTAINING TO CROPS
Contaminant Reference Number
Water Quality Parameters
Ammonia 267, 272, 352, 366, 563, 586, 665, 666,
755, 1299, 1347, 1556
BOD 272, 352, 361, 485, 916, 1215, 1556
COD 87, 190
Chlorides 55, 56, 272, 362, 365, 665, 666, 684,
1072
Fluorides 142
Iodides 1229
Nitrates 55, 56, 133, 151, 190, 267, 362, 366,
500, 579, 586, 658, 665, 666, 684, 690,
755, 916, 1000, 1042, 1072, 1115, 1124,
1141, 1256, 1299, 1347, 1381, 1424, 1432,
1440, 1556
Nitrites 55, 56, 352, 366, 690, 755, 1124, 1299,
1556
Phosphates 55, 56, 87, 116, 190, 267, 272, 352,
366, 684, 690, 711, 755, 916, 1042, 1072,
1115, 1140, 1347, 1409, 1424
Suspended 87, 190, 352, 361, 485, 1215, 1556
sol ids
Total dissolved 55, 56, 272, 352, 1215, 1256
sol ids
Total organic 352, 877
carbon
Other (general) 55, 56, 551, 552, 665, 666, 1376
Elemental Contaminants
Aluminum 366, 634, 710, 720, 1108
Arsenic 267, 366, 720, 790, 1040, 1042
383
-------
TABLE 138(continued)
Contaminant Reference Number
Barium 267, 1040, 1042, 1421
Beryllium 267
Boron 137, 211, 267, 272, 352, 366, 528, 581,
684, 939, 1040, 1088, 1113, 1347, 1495
Cadmium 56, 151, 190, 211, 212, 232, 267, 366,
417, 433, 451, 581, 586, 619, 690, 710,
724, 737, 854, 1040, 1105, 1124, 1144,
1381, 1424, 1556, 1557
Chromium 151, 211, 212, 267/366, 417, 451, 586,
690, 737, 854, 1040, 1042, 1105, 1109,
1124, 1424, 1556, 1557
Cobalt 211, 267, 366, 634, 1040, 1042, 1422
Copper 40, 55, 56, 151, 190, 211, 212, 232, 267,
366, 417, 451, 454, 528, 583, 634, 690,
710, 737, 854, 916, 939, 1038, 1040,
1088, 1105, 1124, 1144, 1154, 1229, 1424,
1495, 1557
Germanium 595
Iron 212, 232, 267, 366, 417, 451, 528, 580,
583, 634, 665, 666, 710, 737, 854, 916,
939, 1038, 1105, 1229, 1409, 1424, 1444,
1495, 1557
Lead 143, 151, 190, 211, 212, 267, 366, 417,
451, 634, 710, 737, 854, 1040, 1042,
1124, 1144, 1409, 1556
Manganese 190, 212, 267, 366, 417, 451, 580, 581,
583, 634, 701 , 703, 710, 744, 939,
1040, 1042, 1105, 1124, 1229, 1409,
1495, 1S56
Mercury 151, 211, 212, 366, 417, 451, 1040,
1042, 1160, 1295, 1557
Molybdenum 267, 366, 648, 711, 1040, 1042, 1050,
1229
384
-------
TABLE 138(continued)
Contaminant Reference Number
Nickel 55,56, 151, 190, 211, 212, 267, 366,
417, 583, 634, 690, 710, 1040, 1042,
1124, 1144, 1423, 1424, 1556, 1557
Selenium 124, 366, 489, 518, 711, 743, 993, 1001
Tin 267, 1445
Uranium 7
Vanadium 7
Zinc 55, 56, 151, 190, 211, 212, 217, 267,
273, 351, 353, 366, 417, 451, 528, 581,
583, 586, 619, 634, 701, 703, 710, 724,
737, 854, 916, 939, 1038, 1040, 1105,
1124, 1144, 1229, 1381, 1409, 1424,
1468, 1495, 1557
Other (general) 55, 151, 205, 211, 212, 267, 365, 417,
485, 583, 586, 619, 634, 918, 1042, 1098,
1110, 1299, 1381 , 1409, 1556, 1557
Biocidal Contaminants
Aldrin 916
Chlorinated 918, 1397, 1534
hydrocarbons
DDT 17, 453, 916, 1534
Dieldrin 916, 1534
Herbicides 916, 1256
Synthetic/Organic 16, 934, 1256, 1457, 1564
Contaminants
Biological Contaminants
Adeno virus 916
Bacteria 74, 161, 399, 428, 665, 666, 738, 913,
918, 1184, 1234
385
-------
TABLE 138 (continued)
Contaminant Reference Number
Coliforms 17, 155, 200, 357, 399, 459, 665, 666,
913, 916, 1006, 1184, 1234, 1556
Coxsackie virus 161, 357
(A&B)
ECHO virus 357
Escherichia coli 200, 913, 1184, 1189
Fecal
streptococci 200, 656, 913
Hepatitis virus 357, 459, 916, 918
Leptospirosis 200, 357, 913, 1189
Mycobacterium 200, 913, 916, 1234, 1361
Parasitic worms 161, 200, 417, 459, 913, 918, 1186, 1188,
1189, 1234
Polio virus 161, 357
Protozoa 417, 459, 913, 1184, 1185, 1189, 1234
Salmonella 161, 200, 357, 361, 459, 913, 916, 918,
1006, 1184, 1189, 1234
Shigella 161, 200, 459, 685, 913, 1006, 1184, 1189
Vibrio cholerae 161, 198, 200, 459, 916
Virus 161, 428, 459, 485, 738, 913, 983, 1184,
1256
Other (general) 46, 161, 433, 665, 666, 913, 918, 1030,
1256, 1556
386
-------
and indirectly by altering the soil chemistry, which in turn
alters the solubility and mobility of metals (1409).
Many metals are essential micronutrients for plant and
animal growth. Increasing their levels in the soil solution
may remedy deficiencies in the plant "diet," resulting in an
improved food supply that can remedy trace element deficiencies
in animal diets. There are, however, limits to the amounts of
trace metals that plants and animals can accumulate without
showing symptoms of metal toxicity. Selenium, for example,
is easily accumulated by certain plants that are adapted to
growth in soils which naturally contain relatively large amounts
of this element. The selenium doesn't affect the plants, but
is toxic to livestock eating the plants. Urinary selenium
levels appear higher in humans ingesting foods raised in
naturally seleniferous soils, and chronic and acute cases of
poisoning have been reported (1114).
The levels of various metals that are toxic to plants
vary with plant species and soil conditions and have not been
fully outlined. The levels that are safe in plants entering
the human food chain are also undecided in many cases. Accord-
ing to several investigators (151, 211, 1042), the elements
that pose a potential hazard to the food chain through plant
accumulation are cadmium, copper, boron, nickel, molybdenum,
and zinc.
Municipal sludges usually contain trace elements in
concentrations higher than those found in typical agricultural
soils (586). Small applications of sludge would normally
be sufficient to correct any trace element deficiencies of the
soil. Land application as a form of sludge disposal, however,
is practiced on a continuing basis; therefore, large cumulative
quantities of sludge are applied. Large metal concentrations
do eventually build up in soils that receive sludge applica-
tions continually. In fact, many of the trace metals remain
near the soil surface (309).
This long-term, heavy accumulation of metals within the
plant root zone of the soil has led to speculation that the
continued application of sludge will eventually result in
adverse crop and food chain effects, even though no effects
are seen in the initial years of sludge application. However,
there is strong evidence that in many soils, plant-available
metal remains constant from year to year despite cumulative
increase in the total metal content of the soil.
From 1968 through 1973, over 160 dry tons of sludge/ac
have been applied to corn at the University of Illinois North-
east Agronomy Research Center in Elwood, Illinois (1557). Metal
levels in corn grown at the Elwood site have not inceased as the
387
-------
cumulative total of applied sludge has increased each year;
the levels have only been increased by the sludge applied in
any one growing season. In particular, the cadmium concentra-
tion of the corn grown did not exceed 1.1 ppm through 1973,
after reaching a level of 1.0 ppm in 1970. Experiments conducted
with soybeans yielded the same conclusion: plant-available
metal levels in soils are not closely related to cumulative
total sludge applications.
Similarly, experiments conducted at the Hanover Park
research farm by the Metropolitan Sanitary District of Greater
Chicago (1557) showed that after a cumulative total sludge
application of 90 tons/ac in 6 yr, there were no unusual
concentrations of metal in the corn grown. There was no
significant difference between the metal concentrations of corn
from sludge-supplied soil and from control soil receiving
no sludge.
Soybeans were grown annually for 6 yr on field plots
irrigated with digested sludge at three application rates (586).
Applications of digested sludge significantly increased soil
levels of zinc and cadmium, which was reflected by increased
concentrations of these elements in plant tissues. For a
particular annual loading rate, the amounts of cadmium and
zinc in plant tissues reached relatively stable levels during
the 6 yr. The magnitude of annual sludge applications was
a more important determinant of amounts of elements in plants
than were the amounts of zinc and cadmium accumulated in the
soil from previous years. Some of the zinc and cadmium accumu-
lated in the soil as a result of sludge applications in previous
years was maintained in forms available to plants. But when
annual sludge applications were terminated, zinc and cadmium
concentrations were significantly decreased in plant tissues.
Hinesly et al. therefore concluded that if hazardous concen-
trations of zinc and cadmium are to occur in plants as a result
of metal accumulation in soils, they will occur during the
time sludge is being applied rather than later as had previously
been suggested.
According to Zenz et al. (1557), there is no data available
to support the assumption that the long-term enrichment of soil
considerably beyond normal concentrations of heavy metals will
result in correspondingly high levels of these metals in plants.
Brown (151) explored this point further. He states that
plant uptake of metals from soils depends on the portion of soil
metal that is plant available rather than on the total metal
content of soils. It is not known how to measure plant-available
metal directly. Several investigators have tried to correlate
plant uptake of zinc, copper, or nickel with the quantities of
these metals that are extracted from soils by various salts,
388
-------
acids, and organic metal-complexing agents. This approach
for estimating the portion of soil metal that is available
for plant uptake has not been completely successful. However,
the results are much more meaningful than are estimates based
on water solubility considerations. Brown cites data to show
that almost all of the zinc, copper, and nickel in sludge that
were applied to a Blount silt loam soil over a period of 3-
yr were still extractable by 0.1 N HC1 at the end of the
third year. He cites another 2-yr study in which over
100 percent of the applied zinc was extractable by 0.1 N HC1
at the highest application rate used.
A study cited by Chaney et al. (212) reported the metal
content of sludge, soil, and corn tissues at a 35-yr-old
sludge disposal farm at Dayton, Ohio. The treated soils were
very high in total metals: 2,065 ppm zinc, 843 ppm copper,
and 70.5 ppm cadmium. Control soils contained 158 ppm zinc,
51 ppm copper, and 2.0 ppm cadmium. The corn leaves grown on
the control and treated soils contained 67 and 196 ppm zinc,
10 and 40 ppm copper, and 2.1 and 13,9 ppm cadmium, respectively;
the corn from control and treated soil contained 12 and 79
ppm zinc, 8 and 12 ppm copper, and 0.8 and 0.9 ppm cadmium,
respectively. This data appears very encouraging 1n regard to
the long-term low availability to corn grain of sludge-borne
cadmium. A difference between cadmium buildup 1n leaf tissue
relative to grain was very evident.
Chaney et al. (212) recognized the need for research that
would examine the plant availability of sludge-applied cadmium
at sites that were 1n use for 10 or 25 yr, rather than for
2 or 3 yr. Therefore, they located long-term sludge use sites
with a wide range of soil cadmium contents, established plots
to which no new sludge would be applied, and grew a number of
crops representing a range of cadmium accumulation characteristics
on these plots and matched control plots. Results of this
Important research program are discussed below.
Table 139 shows the trace element concentrations of oat
grain from several sampling points at one particular long-term
disposal site. These results show the effect of past sludge
applications, since no new sludge was applied once the experi-
mental plots were established. Oat cadmium at this site
reached 2.1 ppm (mg/kg dry weight of plant tissue) when grown
1n soil containing 8.4 ppm DTPA-extractable cadmium at pH 6.4.
Control soils contained only 0.10 ppm DTPA-extractable cadmium.
Oat normally contains only 0,01 ppm cadmiur..
389
-------
TABLE 139. TRACE ELEMENT CONCENTRATIONS OF OAT GRAIN
AFTER SUSPENSION OF SLUDGE APPLICATIONS AT A
LONG-TERM DISPOSAL SITE (212)
Soil pH
6
6
6
6
6
.9
.6
.4
.2
.1
Zn
30.
32.
49.
46.
45.
Oat grain
Cd Pb
3
8
8
0
6
0
0
2
1
1
ppm
.22
.10
.13
.32
.68
Dry
0.
0.
0.
0.
0.
Cu
Ni
Crop
71
61
56
56
50
4.
4.
4.
4.
4.
0
2
7
3
8
2.
1 .
7.
5.
5.
1
5
5
6
8
The zinc and cadmium concentrations of corn at another
site are shown in Table 140. The sampling locations of low pH
yielded corn with relatively low cadmium concentrations. Soil
DTPA-extractable cadmium was found to be a poor predictor of
corn cadmium. Corn normally contains about 0.03 to 0.10
ppm cadmium.
TABLE 140. ZINC AND CADMIUM CONCENTRATIONS OF CORN
AFTER SUSPENSION OF SLUDGE APPLICATIONS AT
A LONG-TERM SLUDGE DISPOSAL SITE (212)
Soi
Zn
147
124
238
134
156
125
_
77
90
156
75
1 total
Cd
ppm
6.7
4.9
10.8
5.6
6.9
5.9
9.1
3.1
3.9
5.7
2.3
pH
5.3
5.5
5.2
5.1
5.5
5.2
6.1
5.2
5.1
7.4
6.9
Soil
Zn
ppm
43
37
74
37
44
39
34
22
27
33
14
DTPA
Cd
2.15
1 .67
2.92
1 .68
2.03
2.08
2.42
1 .18
1 .32
1.67
0.70
Corn gra
Zn
ppm
34
21
26
23
24
34
23
23
21
21
17
in
Cd
0.42
0.21
0.31
0.72
0.75
0.85
0.50
0.39
0.62
0.062
0.048
390
-------
As shown in Table 141, the soil pH was high at a site where a
large amount of low-metal sludge was applied. Fescue was some-
what higher in zinc and copper on sludge-amended plots, but for
cadmium and lead there was no significant difference between
sludge-amended and control plot fescue.
TABLE 141. TRACE ELEMENTS IN SOILS AND TALL FESCUE AT A SITE
WHERE HIGH LIME FILTER CAKE SLUDGE WAS APPLIED AT
200-400 DRY T/A (212)
pH Zn Cd Pb Cu Ni
ppm dry weight
Mn
Fe
Total metal content
Sludged soil
Control soil
DTPA-extractable metal
7.8
5.3
128.
28.
1.01
0.08
42.0 45.6
10.4 3.1
12.4
4.8
339
186
Sludged soil
Control soil
Grass metal content
Sludged soil
Control fertilized
Control unfertilized
7.8
5.3
7.8
6.2
6.1
19
2
61
23
13
.3
.3
0.
0.
0.
0.
0.
28
07
24
18
11
5.5
3.2
3.5
6.1
4.6
15.8
0.9
7.7
4.7
4.1
0
0
1
1
0
.44
.41
.0
.2
.18
15
20
116
87
no
174
81
410
112
194
Table 142 shows the trace element concentrations of soy-
bean and corn and associated soils at various sampling spots
at another long-term disposal site. The very low pH of the
corn field may have been partly responsible for the substantial
enrichment of corn above normal cadmium levels of 0.03 to 0.10 ppm,
The soybean shows little or no enrichment above normal levels of
0.2 ppm cadmium.
and soybean
The chard
Table 143 shows the cadmium results for chard
tissues grown at sites near three different cities
cadmium results at City 4 show no effect of sludge-applied
cadmium. At City 13, chard cadmium was increased at low pH,
but not at high pH; at City 9, it was very high (73 ppm) at low
soil pH, but dropped to 5.5 ppm at high soil pH,
Soybean leaves and grain were substantially enriched in
cadmium at Cities 9 and 13, raising the soil pH lowered grain
cadmium about 60 percent at City 9 and about 75 percent at
City 13. Soybean grain normally contains up to 0,2 ppm cadmium
391
-------
TABLE 142. TRACE ELEMENT CONCENTRATIONS OF SOYBEANS AND
CORN AT A LONG-TERM SLUDGE DISPOSAL SITE (212)
DTPA-extractable
Soil Zn Cd Cu N1 Zn
pn - " " ppnl» air dry 501 i- - - - -
6.4 8.8 0.22 5.3 0.8 48
5.5 13.6 0.33 8.1 1.2 67
5.9 9.6 0.23 5.2 0.6 56
6.2 5.9 0.17 4.2 0.5 51
6.3 3.7 0.11 2.3 0.4 45
6.4 3.9 0.11 3.0 0.5 44
Soybean grain
Cd Pb Cu
0.30 0.50 12.0
0.19 0.84 14.3
0.23 0.74 12.8
0.23 0.60 13.9
0.18 0.89 11.8
0.37 0.57 12.7
Ni
1,8
2.4
2.8
2.0
1.5
1,4
Soil
DTPA-extractable
Zn
5.2 7.1
5.0 6.4
5.0 10.2
Cd
ppm, air
0.13
0.17
0.22
Cu
dry soil-
3.8
4.1
7.1
Ni
Zn
1.2 19
0.9 18
0.8 16
Cd
0.23
0.56
0.43
Corn
ppm,
0
0
0
grain
Pb
dry crop
.87
.78
.77
Cu
1.8
2.0
1.7
Ni
0.
0.
0.
7
4
4
High cadmium and cadmium to zinc ratio sludges were used
at Cities 9 and 13. At City 9, sludqe had not been applied for
nearly 3 yr at harvest time, yet soybean grain contained
3.7 ppm cadmium at low pH and 1.5 ppm at high pH. Chaney et al
came to the following conclusions regarding cadmium:
• Soil pH significantly affected crop concentrations
of cadmium;
• Crops differed widely in cadmium uptake, in the
relative transport of cadmium to the grain, and
in the influence of pH on cadmium uptake;
• Cadmium remained available to crops, even though
sludge application had ceased; and
• High cadmium and cadmium/zinc sludges produced
higher crop cadmium levels than did ordinary
municipal sludges.
392
-------
TABLE 143. CADMIUM CONCENTRATIONS (PPM DRY CROP) OF
CROP TISSUES GROWN AT THREE LONG-TERM SLUDGE DISPOSAL SITES (212)
City
4 Control
4 Control
4 Sludged
4 Sludged
9 Control
9 Control
9 Sludged
9 Sludged
13 Control
13 Control
13 Sludged
13 Sludged
Soil
DTPA-extrac-
table Cd
0.13
0.14
0.53
0.57
0.13
0.10
1.13
1.19
0.09
0.10
7.15
5.45
PH
5.7
6.7
5.2
6.2
5.3
6.7
4.8
6.6
5.3
6.4
5.6
6.6
Chard leaf
0.6
0.5
1.9
0.6
3.6
1.2
73.0
5.5
0.9
0.5
7.0
1.8
Soybean
Leaf
0.27
0.26
—
--
1.04
0.55
10.7
1.87
0.24
0.17
5.70
2.38
Grain
0.17
0.15
--
--
0.36
0.28
3.70
1.51
0.16
0.13
2.64
0.65
Regarding trace metals other than cadmium, Chaney et al
concluded the following:
• Crops were not
sludge lead.
influenced by additions of
With the exception of
higher in copper from
a large proportion of
DTPA-extractable.
chard, crops were not
sludge use, even though
added copper remained
• Where sludges high in nickel were used, plant
levels of nickel were increased only at
low soil pH.
• Zinc remained available over many years of sludge
use and for many years after sludge use stopped.
Crops differed widely in zinc uptake from the same
sludge treated soil; grain zinc increased less
than foliar zinc.
The results of a study cited by Page (1040) are presented
in Table 144. The trace element concentrations of leeks, globe
beets, potatoes, and carrots grown on soil treated with 66 t
of sludge/ha/yr over a period of 19 yr are reported. The
carrots were grown on soil that had not received sludge for 7 yr,
yet metal concentrations in carrot tops were higher than the
concentrations in carrot tops from untreated soil.
393
-------
TABLE 144. TRACE ELEMENT COMPOSITION OF CROPS GROWN ON
SOIL TREATED WITH SLUDGE AT AN AVERAGE RATE OF
66 METRIC TONS/HA/YR FOR 19 YRS* (1040)
Treatment
Untreated
Treated
Untreated
Treated
Untreated
Treated
Untreated
Treated
Untreated
Treated
Untreated
Treated
Untreated
Treated
Concentrations of Trace Element in Plants
Chromium Copper Molybdenum Nickel Zinc
0.71
0.54
0.85
1.0
0.3
0.8
1.70
3.0
0.09
0.03
0.41
0.88
0.03
0.06
5.7
16.0
8.5
10.0
11
18
4.2
8.2
9.5
9.5
8.2
9.9
6.3
4.6
H-y ' y u>j ma v. us i —
Leeks
0.50
1.10
Globe Beet Tops
0.45
0.65
Globe Beet Roots
0.1
0.25
Potato Tops
0.37
1 .0
Potato Roots
0.40
0.27
Carrot Tops
0.58
0.84
Carrot Roots
0.12
0.12
2.0
7.0
3.2
16.5
1.65
13.0
1.7
5.2
0.25
0.57
1.28
3.0
-
46
135
169
> 505
102
250
90
120
30
27
47
99
34
42
* Leeks, beets, and potatoes are means of two plots.
Carrots were grown on soil 7 yr after treat-
ments were discontinued.
394
-------
In contrast to the studies of long-term disposal sites by
Chaney et al, (212), Zenz et al. (1557), and Hinesley et al.
(586), several researchers have presented data from short-term
sites, where sludge was applied during the same year in which
crops were grown. This type of data cannot show long-term
effects.
In 1973 and 1974 corn plants were grown on digested sludge-
amended soils and analyzed for their trace metal concentrations
(365). In both years, sludge application increased the cadmium
concentration in the whole corn plant but had no effect on the
grain concentration.
Baier (55) conducted a study that involved one-time sludge
applications at three rates to irrigated dryland pasture plots.
Results are presented in Table 145.
TABLE H5. AVERAGE CONCENTRATIONS OF TRACE METALS IN
FORAGE FROM DRY AND IRRIGATED PASTURE PLOTS
RECEIVING SLUDGE AT THREE APPLICATION RATES (55)
AVERAGE CONCENTRATIONS IN DRYLAND FORAGE
(mg/kg dry wt of plant tissue)
Application Rate 22 T/A 12 T/A 3 T/A 0 T/A
Cadmium
Copper
Nickel
Lead
Zinc
.15
7.61
3.26
.66
51 .63
.40
11 .03
4.96
1 .38
74.42
.19 .12
7.67 6.55
1.64 2.73
1.21 .66
39.43 30.02
IRRIGATED LAND FORAGE
Application Rate 22 T/A 12 T/A 3 T/A 0 T/A
Cadmium
Copper
Nickel
Lead
Zinc
.24
3.39
5.08
.80
53.67
.22
7.34
5.65
.91
58.76
.21
4.51
3.38
.85
41 .10
.09
7.22
2.78
.78
27.20
The data show that only cadmium and zinc were found in
consistently higher concentrations in forage from sludge-treated
rather than control plots; however, the concentrations did not
increase proportionately to the amount of sludge applied,
suggesting that the metals were being complexed in an unavailable
form.
395
-------
Cadmium was held in a very shallow layer of soil,
probably the top h in. The resulting high concentration may
have been toxic enough to plant roots so that the roots did
not grow in that zone, making the metal less available to the
pi ant.
Solid municipal waste was applied to Sagehill sand at
rates of 0, 100, 200, and 400 tons/ac (267). Sewage sludge
was applied at 55 gal/ton of solid waste. Winter wheat was
planted as a cover crop in October 1971 and was followed by
spring-seeded fescue and alfalfa. Ammonium sulfate fertilizer
was applied, and the plots were irrigated for two crop seasons.
Wheat harvested in June 1972, and all fescue and alfalfa con-
tained 100 to 300 ppm iron. Some alfalfa samples, especially
in September 1972, contained up to 900 ppm iron. These
samples raised the averages and may indicate local spots of
high iron concentration in the soil. However, alfalfa may
normally contain up to 1,000 ppm iron. Iron uptake in
general did not increase with the addition of municipal wastes.
The manganese content of the fescue and alfalfa harvested
in June increased with waste application and with nitrogen
fertilization. Fescue from plots that received the highest
cumulative nitrogen contained 300 to 400 ppm manganese,
approaching levels toxic to the plants. Manganese availability
increased with decreasing pH.
The copper content of the wheat, fescue, and alfalfa
ranged between 5 and 15 ppm. Normal plant copper levels
range between 5 and 20 ppm.
The zinc content of the fescue and alfalfa also in-
creased wtih waste application and nitrogen fertilization.
The fertilizer increased zinc uptake primarily by its effect
on soil pH. The zinc content of both crops grown on plots
that received 400 tons solid waste/ac was over 100 ppm.
Zinc levels in plants grown on control plots were closer to
25 ppm.
Plant content of iron and copper was not affected by
the waste treatments. Manganese and zinc uptake by wheat,
fescue, and alfalfa increased with waste addition and with
nitrogen fertilization. The copper content of the wheat,
fescue, and alfalfa ranged between 5 and 15 pptr. Normal
plant copper levels range between 5 and 20 ppm. Apparently
copper added in the waste materials is released very slowly
and/or is rapidly immobilized in the soil, remaining un-
available to plants.
The boron content of wheat sampled in April 1972 in-
creased dramatically with addition of municipal wastes.
396
-------
Wheat from control plots contained 4 to 6 ppm boron while
wheat from plots that received 100 tons solid waste/ac con-
tained a moderately phytotoxic level of about 20 ppm boron. Wheat
from plots that received 200 or 400 tons solid waste/ac con-
tained up to 100 ppm boron. The normal boron content of wheat
is 3 to 5 ppm. Boron uptake by alfalfa Increased only slightly.
Molybdenum uptake by alfalfa grown with the higher waste
treatments reached levels potentially hazardous to livestock
during the first growing season but decreased to safe levels (2.0
ppm) the second year. The highest level during the first
season was 10.8 ppm molybdenum. Molybdenum is toxic to live-
stock at 5 ppm.
The cobalt content of wheat, fescue, and alfalfa ranged
from 0.4 to 0.7 ppm. Normal levels are 0.02 and 0.29 ppm
cobalt in alfalfa, fescue, and wheat.
Chromium uptake by fescue and alfalfa was affected very
little by waste additions.
Digested sludge has been applied to a land reclamation site
at Fulton County, Illinois, since 1971 (1556). Crop tissue
samples have been taken each year since the project began.
The metal content of corn grown on nonsludged and on sludged
fields was compared in 1972 and 1973. The amount of sludge
applied ranged from 0.49 to 5.8 dry tons/ac. The data from
the analyses reveals no significant difference between the
sludged and nonsludged fields in the levels of zinc, iron,
manganese, copper, nickel, chromium, lead, and cadmium in
corn grain.
A 1-yr study of five existing sludge disposal sites
receiving various quantities of sludge was conducted by Keeney
et al. (690). Cadmium, chromium, copper, nickel, and zinc
were measured in grass samples and in soil. The concentrations
of these metals were increased in the surface soil of each
sludge disposal area. The two sites receiving the highest
sludge application rates -- 500 and 290 dry t/ha of sludge --
were of lower pH (4.6 and 4.4), At these two sites, trace
element uptake by plants was greater than in the control
areas. At other sites receiving less sludge, the trace
element concentrations of grasses, except for zinc, compared
more favorably to grasses in the control areas. At two of
these sites, the average zinc concentration of grass increased
when compared to the control areas, from 28 to 80 ppm and
from 16 to 30 ppm.
The average cadmium, copper, manganese, and zinc content
of the grass collected from the site receiving the most sludge
increased when compared to the control samples, from 0.2 to
397
-------
1 ppm, 5.8 to 14 ppm, 70 to 240 ppm, and 19 to 290 ppm,
respectively. The average chromium and nickel content of
grass compared closely with the control samples.
Dowty et al. (1409) studied the uptake of metals by seven
vegetable crops after 0, 112, 225, and 450 tons/ha of sludge
was applied to coarse sandy soil. Generally, metal contents
of the vegetable tissues were higher than those of fruiting,
root, and tuber tissue. In most edible tissue, heavy metal
accumulations did not increase more than two- to threefold
as a result of amending the soil with 450 tons/ha sludge.
Lettuce tissue was an exception, with increases of 11-, 7.5-,
and 4.4-fold for zinc, copper, and cadmium, respectively.
Lettuce seems to be an accumulator of metals, whereas
potatoes and carrots seem to be excellent nonaccumulators.
Approximately three times as much zinc accumulated in pea vine
tissue as in edible fruit. The cadmium to zinc ratios of
edible tissues of potatoes, carrots, and peas were less than
0.01 at all sludge application rates. The ratio for lettuce
was 0.029 for the control treatment of 0 tons of sludge
applied, and 0.012 for the highest application rate.
Shredded municipal refuse and primary sludge were applied
to Sagehill loamy sand before the planting of wheat, fescue,
and alfalfa during a 1-yr study conducted by Halvorson (528).
The concentrations of iron, copper, boron, and zinc in fescue,
and of iron, molybdenum, boron, and zinc in alfalfa were
affected by the waste treatments. Results of the study are
shown i n Table 1 46 .
TABLE 146. AVERAGE TRACE ELEMENT CONCENTRATIONS
(mg/kg DRY WT PLANT TISSUE) IN
FESCUE AND ALFALFA GROWN ON PLOTS RECEIVING
400 T/A SHREDDED MUNICIPAL WASTE PLUS SLUDGE
AND ON CONTROL PLOTS (528)
Appl
0 ga
200
SI
ica
I/A
gal
udge
tion Rate
Fe
122
/A 208
Cu
9
25
Fescue
B
3.4
37
Zn
Fe
29 190
268 452
0
14
Alfal
Mo
.9
.5
fa
B
34
60
Zn
44
320
Table 147 shows the heavy metal concentrations in the
seeds of soybeans that received a maximum of 228 mm of liquid
digested sludge during the year 1970. Sludge was applied to
plots at 0, 25, 50 or 100 percent of the maximum loading
rate (1557).
398
-------
TABLE 147. AVERAGE TRACE METAL CONCENTRATIONS
OF SOYBEAN SEEDS FERTILIZED WITH DIGESTED
SLUDGE AT VARIOUS APPLICATION RATES (1557)
Percent of Maximum
Application Rate
0%
25%
50%
100%
Metal
Zinc
59
68
73
83
Concentrati
Copper
13.1
14.9
12.5
12.2
on (mg/kg
Nickel
6.1
9.4
10.5
10.5
dry wt)
Cadmi urn
0.12
0.38
0.60
1 .08
An examination of this data shows that zinc, nickel, and
cadmium contents of soybean seeds were much increased by sludge
application. Copper contents in plant tissues were not in-
creased above the levels in plants from control plots.
Sludge application to pasture from August 1, 1973 through
September 1974 was studied by Fitzgerald and Jolley (417).
Sudan pasture grass, corn stubble, rye pasturage, corn silage,
and alfalfa hay were analyzed for chromium, copper, iron,
lead, nickel, manganese, and zinc. Increases of metal con-
centrations in plants other than the Sudan grass were not
apparent over the test period. The metal concentrations found
in Sudan grass are reported in Table 148. In most cases,
control Sudan grass contained higher peak levels of metals
than test Sudan grass.
TABLE 148. TRACE ELEMENT CONCENTRATIONS IN
SUDAN GRASS GROWN ON SLUDGE-IRRIGATED AND CONTROL
PLOTS (mg/kg OVEN-DRIED SUDAN) (417)
Trace Metals SIudge-Irrigated Control
Zinc
Copper
Chromium
Iron
Nickel
Lead
Manganese
42.4 -
4.63-
5.37-
177 -2
2.98-
3.81-
32.8 -
98.1
33.0
39.6
,666
11.2
13.4
96.2
69.7 -
1 .0 -
1.95-
484 -11
2.68-
3.40-
77.6 -
100
20.0
20.0
,794
20.3
19.3
251 .0
Chaney et al. (212) suggested that farmers must be
educated to use sludge properly. Presently, farmers are often
not aware that sludge has a tendency to lower soil pH and that
liming the soil can remedy the situation. This is important
399
-------
because increased plant uptake of metals has been observed at
low pH. Nonuniform spreading practices used on fields by
farmers can result in localized regions of extremely high
metal content, especially because added metals tend to remain
in the surface layers of the soil.
BIOLOGICAL CONTAMINANTS
In Europe and other parts of the world outside the United
States, epidemics of typhoid and infectious hepatitis have
reportedly been caused by the application of human wastes to
agricultural crops (361). These outbreaks have been attributed
to the consumption of raw vegetables fertilized by night soil
(human feces) or grown on farms irrigated with raw wastewater.
Night soil used on vegetables and fruits has been responsible
for recurrent outbreaks of amoebic dysentery, bacillary
dysentery, gastroenteritis, cholera, and roundworm (ascaris)
in the Orient (459). Sewage irrigation of vegetable crops
was found to be linked with an outbreak of cholera in
Jerusalem in 1970 (198).
A partial summary of the disease outbreaks linked to foods
contaminated with sewage is presented in Table 149, adapted
from Bryan (161). These outbreaks results from the surface
contamination of vegetables with enteric pathogens. Normal,
healthy vegetables are internally sterile, even when their
surfaces and the surrounding soil are contaminated with
bacteria and viruses (1184).
Bryan states that outbreaks of food-borne illness may
continue to occur sporadically, if raw or partially treated
wastewater is used for irrigation of foods that are consumed
raw (161). The true extent of disease infection from raw
produce is unknown (459). Many infections may be experienced
as mild intestinal upsets that do not require medical treat-
ment and therefore go unreported. In the United States, the
most recently reported disease outbreak associated with waste-
water irrigation occurred in 1919. Allegedly, blackberries
or vegetables grown on a sewage farm at Pasadena, California,
caused typhoid in eight, employees (200).
Enteric pathogens survive some stages and sometimes the
entire process of wastewater treatment. Viable pathogens are
therefore applied to the land in the process of irrigation
with wastewater. After application, these pathogens must
survive long enough to be present on the crops when they are
harvested. Adverse environmental conditions considerably reduce
the survival rate of these organisms. Salmonella, shigefla,
enteropathogenic Escheri chia coli , amoebic cysts, ascaris ova,
and enteroviruses have been detected on garden produce growing
in soil contaminated or irrigated with sewage effluents, but
400
-------
TABLE 149. OUTBREAKS ASSOCIATED WITH FOODS
CONTAMINATED BY SEWAGE OR WASTEWATER (Adapted from 161)
D1sease
Source of Contamination
Typhoid fever
Typhoid fever
Typhoid fever
Typhoid fever
Sewage sludge fertilizer
and irrigation
Sewage-contami nated
watercress beds
Human manure
Privy-polluted water-
cress beds
Typhoid fever Sewage irrigation
Typhoid fever
Amebiasis
Taeniasi s
Typhoid fever,
Paratyphoid
fever
Shigellosis
Amebiasi s
Fascioliasis
Taeniasi s
Fascioliasi s
Salmonellosis
(Animal in-
fection)
Sewage irrigation
Sewage irrigation
Sewage irrigation
Secondary sewage treat-
ment (activated sludge)*
plant effluent irriga-
tion and wash water
Irrigation water
(Primary treatment plant
effluent)**
Night soil
Sewage-polluted water
Human feces contaminated
trench silo
Animal feces contami-
nated watercress bed
Animal dung slurry used
to irrigate pastures
Food
Celery
Watercress
Rhubarb
Watercress
Vegetables,
blackberries
Raw vegetables
Vegetables
Beef
Vegetables
Cabbage
Vegetables
Watercress
Rare beef
Watercress
Grass
401
-------
TABLE 149 (continued)
Disease
F a s c i o 1 i a s i s
Ouch-ouch
disease
(cadmi um
poisoning)
F a s c i o 1 i a s i s
Viral
hepatitis
Salmonellosis
(Animal in-
fection,*
possible
human cases)
Viral
hepati ti s
Cholera
Source of Contamination
Food
Animal feces contami-
nated water used for
watercress beds
Mining waste used to
flood rice fields
Animal feces contami-
nated watercress bed
Septic tank effluent
contaminated water**
Human sewage flowing
over grazing land
Sewage-polluted water
Raw sewage irrigation
Watercress
Rice
Watercress
Watercress
Grass
Oysters
Vegetables
* Secondary treated sewage
** Primary treated sewage
+ Implied
402
-------
their detection is infrequent (459). When pathogens are found,
they are found in a low percentage of samples and usually
for only a short time after irrigation (161).
Studies have been made on the viability of various in-
dicator and pathogenic organisms on crops irrigated with
wastewater. The viability of such organisms varies from
several days to a few months, depending on the type of
organism and its resistance to environmental factors e.g.,
climatic conditions, soil moisture, amount of protection pro-
vided by crops, etc. Research has shown that salmonella may
persist for up to 70 days in soil irrigated with sewage under
moist winter conditions, and for about half that period
under drier summer conditions (1256).
In 1949, Falk (399) conducted experiments at a small
sewage irrigation farm outside a southern New Jersey state
institution. Three plots were established for the growth of
tomatoes. One plot was treated throughout the growing season
with raw, settled sewage; the second was treated with sewage
only before planting; and the third was never treated with
sewage. Similar coliform densities were found on the surfaces
of normal tomatoes from all three plots, indicating no sig-
nificant contamination from the sewage. When the stem ends of
the tomatoes were abnormally split, however, high coliform
densities were found on tomato surfaces. On broken tomatoes,
the coliform density was three times higher when the soil
was treated with sewage durinq growth than when it was treated
prior to planting or not at all.
In later experiments at this site, Rudolfs et al. (1184)
applied feces or Eschericnia col i suspensions directly to
the surfaces of growing tomatoes. By the end of 35 days, the
residual coliform concentration on the surfaces decreased
to or below that of uncontaminated controls. The representa-
tives of salmonella and shigella on tomato surfaces in the
field did not survive more than 7 days, even when the organisms
were applied with fecal organic material, which might have
afforded some protection. The investigators concluded that
cessation of sewage application to crops one month before
harvest will offer a considerable margin of safety for pro-
tection against enteric bacterial diseases even though vege-
tables are consumed raw.
Rudolfs et al. (1189) found that the maximum survival
time of End amoeba histolytica on lettuce or tomatoes in the
field was 18 hr. Ascaris eggs, in some cases, remained on
tomatoes for more than a month after application, but were
unable to develop into a mature, infective state. It appeared,
therefore, that cessation of sludge application to crops a
month before harvest should greatly reduce the probability
403
-------
of transmission of ascaris, one of the hardier parasitic
worms.
According to Foster and Engelbrecht (428), cessation of
sludge application to crops a month before harvesting probably
would not offer safety against the transmission of
Mycobacterium Tuberculosum. They reported that when waste-
water containing tubercle bacilli was applied to a radish
patch, some bacilli were discovered after three months of ex-
posure to the elements.
The use of settled chlorinated sewage effluent for vegetable
crop irrigation was studied. Over 50 percent of the irrigation
water samples tested contained salmonella bacteria, ascaris eggs,
or Endamoeba coli cysts. Yet only 1 of the 97 samples of vegeta-
bles tested yielded salmonella, and ascaris eggs were recovered
from 2 of 34 vegetable samples tested. Ascaris was found only
when raw sewage was mixed into the irrigation water.
Wei 1-digested sludge may contain fewer viable pathogenic
organisms than raw sludge and therefore present a lesser
hazard when land applied. Carroll et al. (200) cited a study
of the persistence of pathogens in liquid-digested, sludge-
amended soil. Fecal coliforms were found in the soil 18
weeks after application of liquid-digested sludge;
Pseudgmonas aeruginosa were found after 16 weeks, and sal-
monella were found for up to 19 weeks after application.
Before application, the soil had contained none of these
bacteria.
On the basis of his literature review, Shuval (1256)
concluded that sufficient numbers of pathogens can survive
under the conditions normally expected in agricultural
practice to result in a potential health hazard, if crops
recently irrigated with wastewater are consumed without
cooking. However, he states that no clear-cut epidemiological
evidence is available to indicate that the carefully regulated
use of wastewater to irrigate crops not used for direct human
consumption or crops consumed only after cooking and pro-
cessing has ever led to disease outbreak. In addition, no
records exist of diseases having been caused by using
digested sludge as a soil conditioner or fertilizer (339).
Irrigation practices play an important role in minimizing
the health risks involved in the use of wastewater in
agriculture. For instance, surface irrigation techniques
applied to fruit trees can produce uncontaminated fruit pre-
senting no public health risk. However, if spray irrigation
is used, there is a definite possibility of contaminating the
fruit. Similarly, certain vegetable crops might be irrigated
404
-------
by the ridge and furrow technique in such a way as to avoid
any direct contact between the wastewater and the crop.
Food-borne disease organisms must survive processing
and cooking steps,and often have to multiply to reach in-
fective levels. If wastewater-contaminated foods are cooked
so that the contaminated portions reach 165°F, vegetative
bacteria (but not spores), protozoa, helminth eggs, and most
viruses will be killed. In South Africa, only three cases of
enteric fever were observed over a period of 9 yr in 28,000
mine workers consuming cooked, sewage-irrigated vegetables.
The vegetables were cooked in a thick stew for about 20 min.
Little work has been done on the transmission of enteric
viral diseases by foods contaminated with wastewater (1256).
Viruses as a group, however, are generally more resistant
to environmental stresses than many of the bacteria (428),
and therefore there is a potential for the spread of water-
borne viral diseases, including infectious hepatitis or
poliomyelitis, by this route. Once again, however, proper
irrigation practices and the use of wastewater only for
raising foods that are not consumed raw can reduce the hazard,
405
-------
LIVESTOCK
INTRODUCTION
Pasture, forage, and grain for livestock consumption are
often grown with wastewater or sludge applied either to soil
or crop. However, there is little information on the possible
accumulation of contaminants in the livestock consuming these
feeds (200). The levels to which contaminants accumulate
before the animals show symptoms of toxicity are not of direct
public health interest. But before contaminant concentra-
tions reach such levels, they may reach levels at which animal
products can become unsafe for incorporation into the human
diet and may, therefore, be of public health concern. What
these levels are, and what the likelihood is that contaminants
will accumulate to these levels in livestock are basically
unexplored questions. The pertinent literature that has been
found is recorded in Table 150.
ELEMENTAL CONTAMINANTS
Trace metals in small quantities are required for
metabolic activities of animals. Copper and zinc are fre-
quently added to pig and poultry feeds; livestock eating
forage on selenium-deficient soils have been known to have
severe deficiency diseases (1114). Therefore, in certain
instances, it can be advantageous to add trace metal-bearing
municipal waste to livestock pasturage.
Although the ingestion of feed containing excessively
high concentrations of trace metals is known to produce
diseases in livestock, no adverse effects from land applica-
tion operations involving municipal wastes have been reported
in the literature. Cottrell (267) found that when 200 tons
of solid waste/ac and 11,000 gal of municipal sludge/ac
were applied to Sagehill sand, alfalfa raised thereon con-
tained 5 to 6 ppm molybdenum. These elevated levels of
molybdenum are possibly high enough to induce a copper
deficiency disease in cattle.
Spray application of fluid sludges to pastures and hay
fields is an important component of most all-season, all-
weather fluid sludge systems. Adherence of sludge particles
from spray application onto grass surfaces can increase
levels of persistent organic compounds far above those reached
when sludge is not sprayed directly onto pasturage. A study
406
-------
TABLE 150. LITERATURE REVIEWED PERTAINING TO LIVESTOCK
Contaminant Reference Number
Elemental Contaminants
Boron 1113
Cadmium 737
Chromium 737
Copper 737
Lead 737
Mercury 1295
Molybdenum 267, 1040
Selenium 1114
Zinc 737
Other (general ) 212, 918
Biocidal Contaminants
Chlorinated 918, 998
hydrocarbons
SS synthetics 417, 1564
Biological Contaminants
Hepatitis 918
Salmonella 161, 200, 913, 918
Shigella 161, 200, 913
Lepto 200
Escherichia coli 147, 200, 913
Vibrio cholerae 200
Mycobacterium 288, 913
407
-------
TABLE 150(continued)
Contaminant Reference Number
Fecal 200, 913, 918, 1356
streptococcus
Proto.zoa
Parasitic worms
Vi rus
Col iforms
Bacteria
Other (general )
913
161 ,
161,
H7,
161 ,
161
200,
908,
200,
913,
913,
913,
913
918,
918
918
1356
of the adherence of sludge particles directly onto grass and
hay was carried out by Chaney et al. (212). They found that
sludge comprised as much as 32 percent, by weight, of the
harvest from the tested pasture,and rainfall was ineffective
in removing the adhering sludge. Because such surface con-
tamination can increase trace element contamination of forage,
sludge use on pastures may require special technologies, such
as injection into sod.
The effect of sludge application to pasture for 14 months
was reported by Fitzgerald and Jolley (417). Levels of PCB's
in sludge-irrigated Sudan pasture grass were measured. Sludge-
irrigated pasture produced grass containing 0.1 to 1.2 ug
PCB/gm = ug PCB/gm of dry plant tissue, while the grass grown
on control soil receiving no sludge contained 0.2 to 0.4 PCB =
yg PCB/gm. The investigators stated that little data exists
with which to compare these PCB levels.
BIOLOGICAL CONTAMINANTS
The most prevalent mode of bacterial, viral, or parasitic
transmission from land-applied wastes to humans appears to
be through consumption of sewage-contaminated fruits and
vegetables. However, certain parasites may reach humans
via a parasitic life cycle involving humans, feces, and un-
cooked beef or pork. Livestock that have grazed on land-
application sites or fed recently contaminated forage crops
have high infection rates of salmonel1osis, tuberculosis,
ascaris, hookworm, and liver fluke.
408
-------
In a review of literature, reports of beef tapeworm
(Taem'a saginata) infections of beef cattle in Great Britain
fed on grasslands fertilized with sludge that had undergone
mesophilic digestion for 20 days were cited (913). The mode
of transmission from pasture to beef was not elaborated on,
although it is known that the life cycle of the beef tapeworm
involves transmission from man to-feces, to cattle, and back
to man. The pork tapeworm (Taem'a sol uim) has a similar
life cycle involving uncooked pork rather than beef (161).
Echinococcus graniilosis is another parasitic helminth
found in domestic sewage. It is cyclically transmitted
between sheep and dogs, but can incidentally infect humans
working in sludge-supplied pastures (913).
409
-------
PUBLIC HEALTH CONSIDERATIONS
EPIDEMIOLOGICAL AND PATHOLOGICAL EVALUATION
OF WASTEWATER CONTAMINANTS
Many contaminants contained in municipal wastewater are
known to produce adverse human health effects. A number of
elemental, biocidal, and synthetic/organic constituents have
been clearly identified as potential carcinogens; some have
even been identified as being mutagenic or teratogenic.
Although the epidemiological effects of various viruses and
bacteria are known and predictable, knowledge of the health
risks of certain other contaminants is incomplete or lacking.
Moreover, some chemical substances work not only in isolation
within the human body, but may react synergistically (two or
more chemicals combining to produce a net effect that is
greater or lesser than that produced if the chemicals act
independently). A multiplicity of factors is involved in
such reactions, and knowledge of potential health risks is
scant.
Literature detailing the epidemiological and pathological
effects of wastewater constituents has been surveyed; the
principal health problems posed by these contaminants are
summarized below. A sound understanding of human physio-
logical reactions and consequent public health threats will
better prepare responsible authorities to assess treatment
performance and set acceptable standards.
Present standards controlling wastewater discharges and
drinking water supplies have been assumed by many to guarantee
adequate protection of public health. However, recent in-
vestigation has shown that some residual organics, carcinogenic
chlorinated hydrocarbons, synthetic compounds, trace elements,
and biocides are harmful even in extremely small concentra-
tions. Existing standards are called into question by this
increasing knowledge: there may be no "safe" threshold for
some of these chemicals. Growing epidemiological and patho-
logical evidence must be taken into account if discharge and
drinking water standards are to safely ensure public well-
being.
WATER QUALITY PARAMETERS
Suspended solids, BOD, TOC, and most other constituents
of general water quality have no direct effect on public
410
-------
health. However,, certain constituents may become associated
with other, more directly harmful, contaminants. The sur-
vival and potential health threat of such contaminants may be
magnified as a result of this process. Moreover, nitrogen
species present in wastewater can directly affect human
health.
Jiltrggen
Nitrogen in wastewater effluent is usually found in one
of the stable forms (ammonia, nitrate, or organic nitrogen)
rather than the more hazardous nitrite form. Nitrates and
nitrites occur in drugs, food, and water. Man is continually
exposed to small amounts of these substances, which usually
cause no harm. In high concentrations and under special cir-
cumstances, however, they may cause illness and even death.
Sepp (1233) and the Hazardous Waste Advisory Committee of the
EPA (1002) consider nitrite, in particular, a significant
health problem.
Nitrite toxicity is the major health problem associated
with these nitrogen species since nitrate easily reduces to
the toxic nitrite form. Such a conversion mav occur outside
the human body in food or water containing nitrates. Con-
version can also take place inside the body through the
action of intestinal bacteria on Ingested nitrates.
Nitrate/nitrite conversion that occurs during digestion
requires special conditions likely to be present only in
infants. The foremost prerequisite is the presence of
nitrate-reducing bacteria in the upper gastrointestinal
tract. Such bacteria are not normally present there, but
lower 1n the intestinal tract. They may occur 1n the upper
GI tract of infants, particulary those with gastrointestinal
infections and a gastric pH insufficiently acidic to kill
the bacteria.
Acute nitrite toxicity (methemoglobinemia) occurs when
hemoglobin (the oxygen-carrying red pigment of blood) is
oxidized into methemoglobin (a brown pigment incapable of
carrying oxygen). Methemoglobin constitutes about 1 percent
of the total hemoglobin of a healthy adult and up to
approximately 4 pe»cent of that of a healthy newborn infant.
Cyanosis results when roughly 15 percent of the hemoglobin
in blood is converted into methemoglobin; when methemoglobin
constitutes 70 percent or more of the total hemoglobin,
oxygen transport is severely impeded, and death may occur
(1002).
Infants, then, are particularly prone to nitrate-
induced methemoglobinemia. In addition to the presence of
411
-------
nitrite-reducing bacteria in the upper gastrointestinal
tract as mentioned above, (1) the hemoglobin of very young
infants is oxidized twice as rapidly as that of adults by
nitrate to form methemoglobin; (2) the red blood cells of
infants are not able to reduce methemoglobin into hemoglobin
as well as adult cells; and (3) the total fluid intake of
infants per unit of body weight is much greater than that of
adults. Thus, for a given concentration in fluids, infants
consume proportionately more nitrate than adults.
The consumption of water containing high levels of
nitrates has accounted for many more cases of methemoglobin-
emia than all other causes combined. Methemoglobinemia of
such etiology has been reported only in infants, although one
study documents one occurrence resulting from the use of
nitrate-contaminated well water for peritoneal dialysis in
an adult. In the United States only one case has been
associated with water from a public water supply; all the
rest (about 300) have been due to well water (1002).
Standards for nitrates in drinking water limiting nitrate
to 10 mg/£ expressed as nitrate nitrogen (45 mg/£ expressed
as nitrate) were set by the U.S. Public Health Service in
1962. The 10-mg/£ nitrate nitrogen level was set because
there had been no reports in this country of infantile
methemoglobinemia associated with the ingestion of water
containing nitrate at levels below 10 mg/l. In addition,
this level was set because it was a standard that could be
met easily by most municipal water supplies. After publica-
tion of these standards, however, data reported from other
countries revealed that a small percentage of cases had
occurred where the water nitrate nitrogen content had been
below 10 mg/t.
As a consequence, the 1962 standards are currently under
reevaluation. Several studies have been designed to determine
more specifically the exact nitrate levels in water required
to cause elevated levels of methemoglobin and clinical
evidence of methemoglobinemia in infants. Preliminary re-
sults suggest that the 1962 standards provide adequate pro-
tection against clinical methemoglobinemia. However, sub-
clinical elevations of methemoglobin have been found in
infants with diarrhea or respiratory disease, consuming water
with a nitrate content below the 10 mg/t level (1002).
In contrast to the relative wealth of data on acute
toxicity in humans, reliable data are lacking on the physio-
logic effects, if any, of chronic nitrate/nitrite toxicity
or of mild, noncyanotic methemoglobinemia. Studies in
animals indicate that nitrates and nitrites may, on occasion,
cause vitamin A deficiency, and that nitrates may have an
412
-------
antithyroid effect by increasing the need for iodine. No
data are available to indicate whether such effects can
occur i n man.
Chronically elevated levels of methemoglobinemia may
have some effect on the human brain: abnormal changes on
electroencephalograms have been observed in rats given 100 to
2,000 mg/£ of sodium nitrite each day for two weeks. A
Russian study purports to show decreased response to visual
and auditory stimuli in school children with a mean methemo-
g.lobin level of 5.3 percent of total hemoglobin. However, the
study was poorly controlled, and the results are inconclusive.
There have been patients with hereditary methemoglobinemia
and mental retardation, but the association may be coincidental
Most patients with hereditary methemoglobinemia show no
mental or neurologic abnormalities (1002).
Nitrosamines formed by the reaction between nitrites and
amines have been proven hazardous to human health. Nitrites
and/or precursor nitrates are found in foods, water, and drugs?
amines are found in tobacco smoke, beer, tea, wine, and tooth-
paste as well.
Nitrosamines have potent biological effects, including
acute cellular injury (primarily involving the liver), car-
cinogenesis, mutagenesis, and teratogenesis. To date,
approximately one hundred nitrosamines have been tested in
animals. The vast majority has proved to be carcinogenic.
Many organs (liver, esophagus, and kidneys) that are common to
diverse species of animals are susceptible to the cancer-
producing effects of these compounds. These effects can be
elicited experimentally by various routes of nitrosamine
administration (oral, intravenous, inhalation) at extremely
low doses. In some instances, cancer can develop after a
single exposure (1002).
Concerns about potential nitrosamine hazards to human
health arise from the possibility for (1) contact with pre-
formed carcinogenic nitrosamines and (2) the formation of
carcinogenic nitrosamines within the human body after exposure
to precursor nitrites and amines. The possible formation of
carcinogenic nitrosamines in the human gut through the
combination of ingested nitrites and amines is of critical
concern. Such reactions have been demonstrated to occur
both in vitro and in vivo (in animals).
Studies in humans that were fed nitrate and a noncarcino-
genic nitrosamine precursor amine (diphenylamine) have shown
that diphenylnitrosamine can be formed in the human stomach.
Nitrosamine determinations in these studies were made by
413
-------
thin-layer chromatography, a'method now known to give false
positive results. Unfortunately, these data have not yet
been confirmed using the newer and more reliable techniques
of gas-liquid chromatography and mass spectrophotometry (1002).
ELEMENTAL CONTAMINANTS
It is often difficult to assess the health effects of
metals and their compounds: many metals are essential to
life at low concentrations but toxic when concentrations ex-
ceed tolerance in man. The situation is further complicated
because the various chemical states of metals (pure metal,
inorganic or organic-metallic compounds) react differently
within the body. Individual differences between subjects,
incubation periods, and sites of accumulation of the sub-
stances in the body are also significant factors in toxicity.
In addition, results from experiments with animals may not
be readily applicable to humans. Experimental animals such
as rats and mice have a much shorter life-span than man and
react and respond differently to chemicals because of their
own distinctive physiological processes.
Table 151 gives a comprehensive summary of the presence
of metals in the environment, their toxicity to humans, and
their half-life in the body (the time it takes for one-half
the chemical to be excreted). Five heavy metals -- cadmium,
lead, mercury nickel as nickel carbonyl , and beryllium --
represent known hazards to human health. Lead, mercury, and
cadmium are particularly insidious,because they can be re-
tained in the body for a relatively long time and can
accumulate as poisons. Antimony, arsenic, cadmium, lead, and
mercuric salts are the most toxic. Discussions of fatal
doses and other considerations can be found in each individual
metal section.
Lead
Except in cases of prolonged exposure at high concen-
trations, most ingested lead is absorbed into the blood and
is later excreted in the urine. The blood lead does not rise
to acute levels; however, a small portion of the daily lead
intake gradually accumulates in bones, where it is normally
insoluble and harmless. Under certain conditions, such as
periods of high calcium metabolism in feverish illness, cor-
tisone therapy, or old age, this accumulated lead can be
released suddenly into the blood at toxic levels. A fatal
dose of absorbed lead has been estimated to be 0.5 g; inges-
tion of more than 0.5 mg/£/day may, because of the above-
mentioned accumulation, cause toxicity and death.
414
-------
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Lead prevents the formation of hemoglobin in the blood
by Interfering with the synthesis of certain precursors
(prorphyrins). This leads to the anemia present in chronic
lead poisoning. Lead also inhibits the sulfhydryl enzymes
that catalyze many of the metabolic pathways, including the
biosynthesis of heme. The effects of lead on the brain and
peripheral nervous system are most serious, manifested as gas-
trointestinal or central nervous system disturbances and
anemia. Symptoms of acute poisoning include metallic taste,
abdominal pain, vomiting, diarrhea, black stools, oliquria,
collapse, and coma. Symptoms of chronic poisoning in early
stages include loss of appetite and weight, fatigue, head-
ache, lead line on gums, loss of recently developed skills,
and anemia. In advanced stages, there is intermittent vomit-
ing, irritability; nervousness; lack of coordination; vague
pains in arms, legs, joints, and abdomen; paralysis; disturb-
ances of menstrual cycle; and abortion. Exposure to tetra-
ethyl lead or tetramethyl lead causes insomina, disturbing
dreams, emotional instability, hyperactivity, and even toxic
psychosis. Severe symptoms include persistent vomiting,
papilledema, encephalopathy (any disease of the brain), ele-
vated blood pressure, cranial nerve paralysis, delirium, convul
sions, and coma (343).
There are up to 100 cases of lead poisoning reported
annually; an average of 10 are fatal. Most of the fatalities
are related to children who ingested lead-based paint from
homes built before 1940; however, 7 cases of lead poisoning
were reported from drinking well water in Australia in 1973
(104, 270). The well water contained a soluble lead content
of about 14 mg/£.
Mercury
Neither methyl nor elemental mercury is normally found
in dangerous concentrations in air, water, or most common
foodstuffs. There are three principal ways in which man can
be poisoned by methyl mercury: (1) when food is consumed that
has been contaminated with methyl mercury, e.g., seed con-
taining mercury fungicides (HgCl2); (2) when methyl mercury
used or formed in industrial processes is intentionally or
unintentionally dumped into natural waters, reaching man
directly through the water and indirectly through the food
chain; and (3) when nontoxic inorganic or organic phenyl
mercury is converted into toxic alkyl mercury compounds by
microorganisms in the environment and is passed on to man
through the food chain (644).
416
-------
The acute toxicity of methyl mercury is the result of
almost complete (98 percent) absorption of the compound from
the gastrointestinal tract. Ingested metallic mercury is not
toxic since it is not absorbed. Mercurous chloride and organic
mercurials such as acetomeroctol, ammoniated mercury, merbromin,
mercocresol, and mercury protoiodide are not likely to cause
acute poisoning because they also are poorly absorbed. The
single fatal dose of these compounds is 3 to 5 times the fatal
dose of soluble mercury salts. The mercurial diuretics (mersalyl,
meralluvide, mercurophyl1ine, mercumati1 in, mercaptomerin, chlor-
merodrin, and merethoxyl1ine) are almost as toxic as mercury
salts. Volatile diethyl and dimethyl mercury are 10 times as
toxic as mercuric chloride (1503). The fatal dose of mercuric
salts is 20 mg to 1 g. The biological half-life of methyl mer-
cury compounds is estimated to be about 70 (30 to 100) days
(1323, 1586).
Acute poisoning by ingestion of mercuric salts causes metal-
lic taste, thirst, severe abdominal pain, vomiting, and bloody
diarrhea. Death is from uremia (an excess of urea and other
nitrogenous waste in blood). Ingestion of insoluble or ooorly
dissociated mercuric salts (including mercurous chloride and
organic mercurial compounds) over a prolonged period causes urti-
caria progressing to weeping dermatitis, stomatitis, salivation,
diarrhea, anemia, liver damage, and renal damage progressing to
acute renal failure with anuria (total suppression of urine).
In children, repeated administration of calomel (Hg2Cl2) appears
to be the cause of a syndrome known as erythredema polyneuropa-
thy. In fatalities from mercury poisoning, the pathologic find-
ings are acute tubular and glomerular degeneration or hemorrha-
gic glomerular nephritis. The mucosa of the gastrointestinal
tract shows inflammation, congestion, coagulation, and corrosion
(343).
Mercurialism is manifested primarily in kidney, liver, or
brain damage in animals. Exposure to inorganic mercury compounds
usually results in kidney damage, while alky! mercurialism is
characterized by brain damage. However, some degree of both
kidney and neurological injury results from exposure to either
category of mercurials. Mercury poisoning apparently damages
Kreb's cycle enzymes (which catalyze the oxidation of tricarbox-
ylic acids) and protein synthesis, leading to kidney and brain
damage.
417
-------
The tragedy of Minamata Bay, Japan, which occurred from
1953 to 1961, is one of the best documented cases of mercury
poisoning. In essence, it was concluded that the disease --
which had felled many inhabitants of the fishing villages
on the shores of Minamata Bay -- had resulted from mercury
poisoning. A chemical plant in the area used mercury chloride
as a catalyst in the production of vinyl chloride. The waste
containing the mercury washed off the product was discharged
into the bay, and was ingested by the shellfish therein.
Some 114 cases of "Minamata disease" were reported, as well
as 44 deaths and 22 cases of brain damage in 400 live births
(625, 780, 863).
A similar disaster struck at Niigata, Japan, where 120
persons were poisoned (780, 863).
Nickel
The fatal dose of nickel is not known, but its whole
body half-life is about 667 days (as shown in Table 157 ).
Inhaled nickel carbonyl decomposes to metallic nickel, which
deposits on the epithelium of the lung. This finely divided
nickel is rapidly absorbed and damages the lung and brain.
The principal manifestation of nickel carbonyl poisoning is
dyspnea (difficult respiration). Workers exposed to nickel
carbonyl show a high Incidence of lung cancer, and some
workers develop dermatitis (343). Very little is under-
stood about the adverse health effects of nickel in waste or
water supplies.
Cadmlurn
Cadmium has become the most recent menace among the
widely used heavy metals. Unlike lead and mercury, relatively
little is known about the fate and distribution of cadmium
in the environment, and what is known is often contradictory.
There is very little information available concerning
the health hazards of cadmium present in wastewater and water
supplies. However, the daily averaqe American citizen's in-
take of cadmium from foods and water supplies is estimated
to be between 0.02 and 0.1 mg/£. The oral dose of cadmium
producing toxicity is about 3 mg, but its fatal dose is not
known. ThP whole body half-life of cadmium is 25yrs (433).
418
-------
Currently, there is no agreement as to whether cadmium
is linked to hypertension in man. Some of the conflicting
data are discussed in Friberg's work (433). Circumstantial
evidence points to some link between trace metals of cadmium
and hypertension: levels of cadmium or ratios of cadmium to
zinc were much higher in the kidneys of persons dying from
hypertension-related diseases (1323). Inhalation of tobacco
smoke is a major source of cadmium accumulation in man. Only
about 2 percent of the cadmium ingested through food or drink
is absorbed by the body, while 10 percent to perhaps as much
as 50 percent of inhaled cadmium is retained (1323).
Cadmium tends to accumulate in liver and kidney tissues
because of its very long biological half-life in man (esti-
mates range from 10 to 25 yr, compared with about 70 days
for methyl mercury). Excessive levels in the kidney cortex
(over 200 ug/g wet weight) result in proteinuria. Therefore,
the cadmium concentration in water must be kept low (1323).
The Environmental Protection Agency (EPA) in its 1975 Interim
Primary Drinking Water Standards set a mandatory limit of
0.010 rng/a for cadmium concentrations in drinking water; the
World Health Organization set a limit of 0.05 mg/fc. The results
of a U.S. geological survey investigation of 720 waterways
showed that 4 percent had concentrations above EPA standards
(863).
Cadmium has reportedly caused a number of deaths from
orgal ingestion of the metal in food or water. For example,
Japanese people living along the Jintsu River suffered for
years from an unknown malady characterized by kidney mal-
function, a drop 1n the phosphate level of the blood serum,
loss of minerals from the bones, and osteomalada (resulting
in pathologic bone fractures causing Intense pain). Impli-
cated as one of several sources of the malady was a cadmium,
zinc, and lead mine that was discharging wastewater Into the
river. The disease, known as 1ta1 itai , was contracted either
by drinking water from the r 1 ver" or By eating rice that had
accumulated the metal from irrigation water (863). In another
situation, there was an outbreak of acute gastroenteritis in
13 children who drank orange soda contaminated with cadmium
at a concentration of 16 mg/s,. The contamination was caused
by the orange soda coming in contact with the soldered joints
in the tank of the soft drink machine (104, 111).
Chromium
Chromium, which exists in various oxidation states
(+2+3 and +6), appears to be most toxic to man as the hexa-
valent chromium ion. The fatal dose of a soluble chromate
such as potassium chromate, potassium bichromate, or chromic
acid is approximately 5 g. Acute poisoning from ingestion is
manifested by dizziness, intense thirst, abdominal pain,
vomiting, shock, oliguria (scanty urination), or anuria.
Hemorraghic nephritis occurs, and death 1s from uremia.
419
-------
Repeated skin contact with chromium leads to incapacitat-
ing eczematous dermatitis with edema and slowly healing ulcer-
ation. Breathing chromium fumes over long periods of time
causes painless ulceration, bleeding, and perforation of the
nasal septum accompanied by a foul nasal discharge (343).
Whether chromium is carcinogenic is questionable at
this time. However, the incidence of lung cancer in workers
exposed to dusty chromite, chromic oxide, and chromium ores
is reported to be up to 15 times the expected rate (343).
Experiments on rats showed no toxic response from
drinking water containing 0.45 to 25 mg/i in chromate and
chromium ion form (831).
Although a potential .health hazard exists, evidence of
health problems resulting from chromium present in waste-
waters is lacking in the literature.
Arsenic
Arsenic is widely distributed in nature. It is present
in toxic concentrations in many water supplies: cattle in
New Zealand have died from drinking water containing natural
arsenic, and there are several areas of the world where there
is a high incidence of skin cancer among people drinking well
water that contains natural arsenic (863). In 1971 the U.S.
Geological Survey found that 2 percent of the samples drawn
from 720 waterways were above their standard of 0.05 ppm for
arsenic.
Before the advent of modern insecticides, arsenic com-
pounds were widely used to treat food crops. Although arsenic
can stimulate plant growth in very low concentrations, in
excessive quantities, as little as 1 ppm of arsenic trioxide
can be injurious. Organic arsenicals, such as arsphenamine
and dimethylarsinic acid, release arsenic slowly and are less
likely to cause acute poisoning. But arsenic accumulates in
the body, so small doses can be lethal. Repeated or prolonged
intake has a cumulative toxic effect, presumably caused by the
arsenic combining with sulfhydryl (-SH) enzymes and interfer-
ing with cellular metabolism.
Chronic poisoning from ingestion or inhalation of
arsenic can cause anemia, weight loss, polyneurit1s, optic
neuritis, dermatitis, cirrhosis of the liver, abdominal cramps,
chronic nephritis, and cardiac failure (343).
420
-------
Arsenic is suspected to be carcinogenic but not tumori-
genic (66, 679, 733). Chronic exposure to arsenic-contaminated
water of 0.3 mg/£ is also suspected to be related to the
increased incidence of hyperkeratosis (hypertrophy of the
horny layer of the epidermis) and skin cancer (1569); chronic
exposure at levels of 0.8 mg/t may be related to gangrene of
the lower limbs (503).
Arsenic is one of the impurities in mineral phosphate
deposits, a source of commercial water softeners. Concen-
trations of 10 to 70 ppm of arsenic have been detected in
several common household detergents. Baby rash-, hand rash,
skin eruptions, and other types of dermatitis allergies are
associated with arsenic in detergents. Much of the sewage
containing such detergents is dumped into waterways (863).
There is a danger that arsenic in laundry water may be
absorbed through unbroken skin.
The principal oxidation states of arsenic are +3 and +5.
In the +3 state, arsenic forms arsenious oxide; in the +5
state, arsenious acid; and in the -3 state, arsine gas.
The fatal dose of arsenic trioxide is about 20 mg. Arsenic
poisoning is manifested by gastrointestinal disturbances;
death is due to circulatory failure as a result of hemolysis
(destruction of the red blood cells).
Copper
The biological properties of copper are such that it is
a useful biocide, especially as an algicide. Various salts
of copper (one of the most common being copper sulfate -
CuS04) are used as astringents, deodorants, and antiseptics.
These salts are all water soluble, and their protein-
precipitating characteristics form the basis of their astrin-
gent and antiseptic effects. The copper mined in the United
States for these effects alone amounts to some 15 million
Ib/yr and accounts for about 40 percent of all chemical uses
of the metal.
Trace amounts of copper are essential for normal
metabolism, and relatively large concentrations can be
tolerated by most animals including vertebrates. The effect
of copper on aquatic organisms varies greatly; microorganisms,
including algae, are highly susceptible.
Small quantities of copper are not considered toxic,
but higher concentrations are known to cause vomiting and
liver damage (1586). Fatalities have been reported following
the ingestion of 10 g of zinc or copper sulfate (343). An
outbreak of acute copper poisoning occurred in a school in
Mesa, Arizona. The outbreak began 10 min after the students
421
-------
drank an orange-flavored drink that had been kept in a brass
container for 17 hr (104). An 8-oz glass of the drink
contained 8.5 mg of copper.
Copper salts in natural waters occur in small concentra-
tions, from a trace to about 50 ppb. Their presence in injur-
ious amounts is almost always due to pollution.
Selenium
Selenium is an excellent example of the fine balance
that can occur in nature between the beneficial and injurious
effects of a natural substance. An essential micronutrient
for some plants, selenium is one of the most toxic substances
to occur naturally in the environment; concentrations only
slightly above those needed for growth of plants may be
poisonous to animals. A selenium compound that was used to
kill insect pests in fruit orchards left a residue in the
fruit. Cattle that were feeding on this fruit contracted
a chronic form of livestock poisoning called alkali disease.
Ingestion of forage containing about 25 ppm can cause this
disease when the forage is eaten for several weeks or months
(863).
As long ago as 1936, inhabitants of seleniferous areas
of South Dakota and Nebraska complained of gastrointestinal
symptoms and were found to excrete large quantities of selenium
in their urine (863). There is also a report of selenium
toxicity from a three-month exposure to well water containing
9 mg/£ of selenium.
The American Conference of Governmental Industrial
Hygienists recommends a selenium limit of 0.2 mg/cu m in
air and 0.01 ppm in water.
Beryl 1i urn
Although the fatal dosage of beryllium is not known,
in 1971 the EPA placed beryllium on the list of hazardous
pollutants. From 1941 to 1967, 760 cases of berylliosis
were recorded (343).
Soluble beryllium salts are irritating to the skin and
mucous membranes, and induce acutepneumonitis with pulmonary
edema. At least part of the changes present in acute
pneumonitis and berylliosis (chronic pulmonary granulomatosis)
develop from hypersensitivity to beryllium in the tissues.
Weight loss and marked dyspenea , which are symptoms of
berylliosis, begin 3 months to 11 years after the first ex-
posure (inhalation). Eczematous dermatitis with a maculopop-
ular, erythematous visicular rash appears in a large percentage
of workers exposed to beryllium dusts.
422
-------
Bari urn
Absorbable salts of barium, such as the carbonate,
hydroxide, or chloride, are used in pesticides; the sulfide
is sometimes used in depilatories for external application.
A soluble barium salt such as the carbonate or hydroxide may
be present as a contaminant in the insoluble barium sulfate
used as a radiopaque contrast medium.
The fatal dose of absorbed barium is approximately 1 g.
The principal manifestations of barium poisoning are tremors
and convulsions. Barium presumably induces a change in
permeability or polarization of the cellular membrane that
results in stimulation of all cells indiscriminantly (343).
Other Elements
Antimony will be considered a potential hazard if levels
of the element increase. It is present chiefly in industrial
wastes, typesetting metal, pewter, and enamel ware. Antimony
is suspected to cause a shortened life-span and heart
disease in rats (343).
Metal alloys and smoke suppresant in power plants are
the major sources of manganese as a pollutant. Although
manganese in trace amounts is an essential element to man,
increased levels may imperil health. The findings in one
death - suspected to be caused by the ingestion of manganese-
contaminated drinking water - were atrophy (a wasting of the
tissues) and disappearances of cells of the globus pallidus
(in the brain). Experimental animals show inflammatory
changes in both gray and white matter (343).
BIOCIDAL CONTAMINANTS
There is significant information in the literature
concerning biocidal contaminants, their chemical and physical
characteristics, toxicology, analytical chemistry, and
impacts on health and the environment. In both chemical and
medical literature, hundreds of cases of acute poisoning
resulting directly or indirectly from such pesticides have
been reported (see Table 152).
Chlorinated Hydrocarbons
Because of their persistence and nondegradational
characteristics, many of the relatively less toxic chlorinated
hydrocarbons, such as DDT, aldrin, and dieldrin, have been
banned and are being replaced by highly toxic but less per-
sistent organophosphorus pesticides. The U.S. EPA is pre-
sently conducting a program to identify new, less harmful
423
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425
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pesticides that can act as substitutes for those causing
the problems.
This decision to remove aldrin and dieldrin from the
market has been highly criticized. The idea that these com-
pounds pose "an unreasonable risk of cancer" is based on the
presence of tumors in the livers of mice that were given food
containing aldrin and dieldrin; some of these tumors metasta-
sized to the lungs. However, it has been noted that similar
tumors can be produced by other compounds, such as DDT and
phenobarbitone, and can occur in mice on normal diets.
There is, then, some question as to whether the production
of tumors in the livers of mice given aldrin or dieldrin is
a reliable indicator of a hazard to man. The general dietary
intake of all major pesticides except aldrin and dieldrin
is well below the allowable standards that were established
in 1972 by the World Health Organization Council on Environ-
mental Quality. Much of the DDT uptake (about 85 to 90
percent) comes from food; the remainder comes from air,
water, aerosols, cosmetics, and clothing.
Because of DDT's extremely low solubility in water
(about 2 ppb), the body, which is essentially a water system,
cannot handle the liquid soluble substance and deposits it
in fat. Quantities of DDT and other related pesticides do
not appear to build up continuously; instead, the pesticides
reach a plateau or steady state (storage equilibrium) at
which they are being excreted and degraded at levels equal
to their intake. Children may take 5 to 10 yr to reach
storage equilibrium. Little is really known about these
levels, which undoubtedly vary with different pesticides,
exposure, intake conditions, and individuals.
Of real concern are the possible effects of long-term
exposure to low levels of DDT and other pesticides. Some
sublethal effects have been observed in animals (cellular
changes in liver tissue and other physiological and histologi-
cal effects); however, these effects cannot be extrapolated
to man. Of course, there is still the suspicion that DDT
might eventually cause damage to human physiology. It has
been suggested, for instance, that long-term exposure to
low levels of pesticides may cause cancer. Research nei-
ther supports nor contradicts this possibility, because
it is difficult to control or document experiments on humans
over a longer period of time.
Based on animal experiments, the average lethal amount
of DDT is a single dose of about 8,000 to 14,000 mg/150-lb
person, although quantities as high as 109 ppm have been
found in sampling a general population. A study was conducted
of persons accidentally or violently killed in Dade County,
Florida, from 1965 to 1967. The average concentration of
426
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DDT in the fat of the bodies ranged from 5 to 22 ppm; there
was more in adults than in children, more in nonwhites than
in whites.
Because the use of chlorinated hydrocarbon pesticides
has been sharply curtailed, it is therefore expected that
smaller quantities of DDT are being ingested and that
residues in human fat will decline. However, the average
value of DDT, DDE, and isomers in human fat samples in India
was 21.8 + 2.9 mg/kg in 1973 and 24.3 mg/kg in 1965. This
would seem to indicate that the DDT storage status had not
undergone any significant change in those years.
A comparative study was performed of DDT and its
derivatives in human blood samples. The study was conducted
in two areas of Ontario where DDT has been used in large
amounts. The mean values of total DDT in the adipose tissue
and blood samples were found to be 5.83 and 0.032 ppm,
respectively. There was a significant correlation between
total DDT in the fat and blood, but there was no evidence
of any adverse effects of DDT on either of the populations
(150).
In another study, tap water samples collected in the
Washington, D.C., area before treatment showed the presence
of DDT (0.17 mg/£), TDE (0,27 mg/£), and DDT-derived compounds
(.15 mg/£); no evidence of these compounds was found after
treatment.
The EPA's ban on DDT has been modified since the insti-
tution of the ban in 1972. In 1974, DDT was used against
the tussock moth in northwestern forests and against the pea
leaf weevil in Washington and Idaho. The EPA, however, states
that DDT will be used only against pests that cannot be
controlled by other means and that will do economic damage
or threaten human health or safety. Also, despite the
suspension of aldrin and dieldrin, the EPA will permit their
use against termites and clothes moths, under certain circum-
stances .
The toxic effects of carbaryl, which is used against
DDT-resistant lice, were found to be minimal at the levels
of 75 mg/£ (256).
The residues of mirex - a chemical which is used to
control the imported fire ant - were discovered in the
fatty tissue of six persons from 1971 to 1972. It was con-
cluded that the residues came from routes other than direct
pesticide usage (994).
427
-------
The maximum allowable concentration of most of the
pesticides (as determined by biological tests) lies below
1 mg/l, but is as low as about 0.01 mg/l for such preparations
as atrazine, malathion, and thiometon (1096).
Workers occupationally exposed - through manufacturing
processes - to aldrin, dieldrin, endrin, and telodrin
(isobenzan) for up to 15 yr were studied by Versteeg and
Jugar (1431). No persistent adverse effects on health were
observed in 52 workers who had left the company and were
traced. The average pesticide exposure in this group of
workers was 6.6 yr, and an average of 7.4 yr had elapsed
since exposure. No hepatic disease or convulsions occurred,
and no-new cases of malignant disease developed. Most of
the workers experienced no unusual illnesses.
Exogenous leukemogenic agents such as pesticides (DDT,
lindane, organophosphates) are being considered as potentially
contributory etiological factors that may activate a latent
leukemia virus in certain cells (1329).
Organophosphorus Pesticides
The organophosphates attack the neural transmission
system of mammals and arthropods and thus interfere with
the function of the target organs. Especially active are
those organophosphates that function by inhibiting carboxylic
ester hydroxylases (including acetylcholinesterase , which
is present in human erythrocytes, nerves, synapses, and
skeletal muscle; and cholinesterase, which is present in human
plasma and in the liver). Miosis (contraction of the pupil),
is found in about 90 percent of the patients with moderately
severe or severe cases of organophosphate poisoning (1521).
Tamura et al. (1358) conducted a statistical and epidemic-
logic investigation of the relationship between the changes in
the use of organophosphorus insecticides and the recent increase
in cases of myopia in 40,000 Japanese children from 1957 to 1973.
The study showed that in the year following any period when large
amounts of organophosphorus insecticides were used, the morbidity
from myopia in school children increased rapidly, conversely,
decreased use of the insecticides resulted in decreased morbidity,
Thus it appears that the recent increase in myopia in school chil-
dren was due, at least in part, to chronic intoxication or organ-
ophosphorus insecticides (1358).
Pediatric hazards associated with organophosphates are
often reported (1578). Signs of toxicity are overaction of
the parasympathetic nervous system, nausea, vomiting, diarrhea,
sweating, and abdominal cramps. Large doses may lead to
428
-------
muscular paralysis and death from respiratory failure
(1578).
Because organophosphorus pesticides are readily absorbed
through the skin, as well as by ingestion and inhalation,
these pesticides present a particular hazard to agricultural
workers who engage in mixing, loading, and applying the con-
centrated materials (1309).
The incidence of organophosphorus insecticide poisoning
varies considerably throughout the world. During 17 yr in
Japan there were 19,000 cases of organophosphorus poisoning
reported, resulting in more than 9,000 deaths. By contrast,
during 17 yr in Great Britain there were only five deaths
reported from this poisoning (1415). Increased chromosome
aberrations were observed in patients suffering acute
organic phosphate insecticide intoxication. The frequency
of stable chromosome aberrations showed a significant increase
with malathion, trichlorfon,mevinphos, and methylparathion;
malathion induced an outstandingly high number of structural
chromosome aberrations. Patients less seriously intoxi-
cated suffered milder chromosome alterations (1585). Even
in the absence of clinical siqns of organophosphate poison-
ing by dichloros at low levels, the cholinesterase values were
much lower than those of a nonworker control population. The
decrease in enzyme levels was significantly correlated with
subjective health complaints: sore throat and loss of memory
(1567).
Herbicides
Today over 40 weed killers are available, but the most
widely used are 2, 4-0 (2, 4 - dichlorophenoxyacetic acid)
and 2, 4, 5-T (2, 4, 5 - trichlorophenoxyacetic acid). In
general, these chemicals are rarely lethal to humans or
animals, do not persist for long periods of time 1n the
environment, and do not build up in the food chain.
During the Vietnam war, South Vietnam suffered massive
military herbicide spraying. It has been estimated that at
least one-th^rd of the timber forests was destroyed, as
well as 10 percent of all cultivated land and at least 25
percent of the coastal Mangrove forests, which are the
breeding or nursery grounds for most offshore fish and
crustaceans (1485). However, there was no evidence in
Vietnamese hospital records that were examined by Thimann
(1372) that birth defects could be attributed to the herbicide
sprayi ng.
Humans are exposed minimally to the phenoxy herbicides
through food; air and water are the primary sources of
429
-------
exposure to these herbicides. On the basis of air samples
collected from wheat-growing areas in the state of Washing-
ton, it was estimated that an average person would be ex-
posed to 1.8 mg of phenoxy herbicide/day. Rain and wind carry
the herbicides into water (215). Workmen who were engaged
in the manufacture of herbicides were examined; the clinical
results were compared to those of a control population that
was not exposed to the 2, 4-D or 2, 4, 5-T. No meaningful
differences were obtained; moreover, there were no chromosomal
effects (215).
In the fall of 1969, the National Institute of Cancer
reported that 2, 4, 5-T was teratogenic and was responsible
for fetal toxicity at levels of 27 +_ 8 ppm. The manufacturer
claimed that this herbicide was not teratogenic; that the
fetal toxicity was caused by 2, 3, 7, 8-tetrachlorodibenzo-p-
dioxin, known as dioxin (653).
At the dose level of 100 mg/kg/day of silvex, there
were no effects on either the dams or fetuses of rats.
Similar observations were also made with picloram. Picloram,
however, is much more persistent in soil than the other com-
pounds. Unlike DDT, it forms soluble salts and does not con-
centrate in fat; in addition, the toxicity of picloram is
very low when compared to that of most other herbicides (653).
The widespread use of phenoxy herbicides has produced
no demonstrable evidence of potential harm to man. The
herbicides used most widely (2, 4-D and 2, 4, 5-T) are
degraded to nontoxic components and do not bioconcentrate
(653).
An epidemiological investigation was made of tumor
incidence and mortality in Swedish railway workers exposed
to various herbicides. Among workers exposed to amitrole
(3-amino-l, 2, 4-triazole),tumor incidence and mortality were
significantly increased and were slightly dose related. Nearly
normal conditions were found in those exposed to phenoxy
acids. Animal experiments suggest that amitrole may produce
malignant tumors in several different organs, but tumors
of the thyroid and liver have received the most attention
(48).
To receive a letal dose of 2, 4, 5-T, a 125-lb woman
would have to eat the equivalent of her body weight of material
containing 380 ppm of the herbicide (based on the acute oral
toxicity expressed in mg/kg). Both 2, 4, 5-T and DDT in
technical form are relatively nontoxic on skin contact (3,800
mg/kg for 2, 4, 5-T and 2,500 mg/kg for DDT). There have been
no human deaths and remarkably few human illnesses from the
agricultural or public health uses of either of these chemicals,
A no-effect level of 50 mg/kg/day of 2, 4, 5-T containing less
430
-------
than 1 ppm dioxins has been proposed as providing ample pro-
tection for human embryos (215).
The first recognized incident in which significant
poisoning resulted from the improper disposal of waste
residues containing TCDD (tetrachlorodibenzodioxin) was in
eastern Missouri. In this incident, a salvage oil company
sprayed waste-oil sludge on an arena at a horse-breeding
farm, to control dust. Birds, cats, dogs, and rodents were
killed; 62 out of 85 horses became ill, and 48 died. The
horses had been exposed to the arena in the summer of 1971,
and they continued to die as late as January 1974. The horses
showed chronic weight loss, loss of hair, skin lesions,
dependent edema, intestinal colic, dark urine, gross hematuria
(the passage of blood in the urine), conjunctivitis, joint
stiffness, and laminitis (inflammation of one side of the
neural arch of a vertebra). In addition, the horses' feet
were inflamed. Human illness, although less severe, included
one case of hemorrahagic cystitis in a 6-yr-old girl who
played in the arena. The soil of the arena contained 3.18
to 3.3 percent TCDD by weight and 2, 4, 5-tri chlorophenol
(TCP) and related chemicals (1431).
Paraquat, a widely used bipyridyl herbicide, produces
a low-dose, chronic illness in rats, primarily manifested
by pulmonary fibrosis (414). Paraquat is also known to
cause severe lung damage in rats, leading to death (599).
Although it causes proliferation of fibroblasts, no
carcinogenic action has been demonstrated. Taken orally,
paraquat causes ulceration in the digestive tract, diarrhea
and vomiting, renal damage, and jaundice.
Pesticidal Viruses
Tinsley and Mel nick(1387) found some antibodies that
reacted with insect viruses in domestic and wild animals and
in several laboratory workers handling insect viruses.
There is always a possibility that changes in the patho-
genicity and specificity of pesticidal insect viruses could
occur, causing a wider spectrum of host involvement. No
collaborative research programs on the in vitro specificity
of insect viruses were recommended (1387).
Fungicides
In Iraq during a two-month period, 6,530 poisoning
victims werehospitalized, and 459 hospital deaths occurred.
The source of the poisoning was found to be homemade bread
prepared from seed wheat treated with methyl mercurial
fungicides (1358). In another case, diphenyl (or biphenyl)
poisoning from fungicides in a Finnish paper mill was reported
431
-------
by Seppalainen and Hakkinen (1235). Workers were employed in
areas of the mill where the average concentration of diphenyl
measured in the air varied from 0.6 to 123.0 mg/m^. The
workers developed EEG abnormalities that were compatible with
generalized cerebral disturbance (1235).
Polychlorinated Biphenyls (PCB's)
Relatively high concentrations of a group of widely used
industrial chemicals known as PCB's have been found in fish,
birds, and man. The widespread presence of these PCB's has
tagged them,like DDT, as truly global pollutants. In fact,
it has been speculated that sunlight might convert DDT to
PCB's. PCB's are insoluble in water, soluble in fats and
oils, and very resistant to chemical and biological degrada-
tion. Due to their solubility, PCB's accumulate in the
environment, especially in aquatic organisms and birds (in
which cumulation factors up to one billion may be reached).
PCB's, like DDT, can inhibit photosynthesis of marine
phytoplankton and can kill shrimp, trout, minks, and birds.
PCB's may be twice as effective as DDT in causing thinning of
bird eggshel1s.
In 1968, over 1,000 people in Japan suffered from a
skin disease and from liver damage caused by rice oils. The
oil was heavily contaminated with PCB's; however, these
effects were not due to the PCB's but to a highly poisonous
contaminant - chlorinated dibenzofurans. This contaminant
is found in some PCB's manufactured in other countries.
To date limited study in this area indicates that
uncontaminated PCB's have a very low toxicity to man.
According to the Food and Drug Administration, the average
PCB concentration in a normal American diet is only about
10 percent of the strict safety levels set in 1971 for food,
food packaging materials, and animal feeds.
SYNTHETIC/ORGANIC CONTAMINANTS
Recently diverse compounds identified in water supplies
drawn from the Mississippi River have been discovered in
the blood serum of local residents using the water supply.
This has created great concern over chemicals found in
drinking water. The presence of small amounts of synthetic/
organic chemicals in treated reclaimed water has been
recognized as a potential health hazard.
The list of compounds identified in drinking waters is
rapidly growing larger. This is due primarily to the
continual introduction of new chemicals but also to the
development of sensitive analytical techniques that measure
432
-------
trace quantities of the chemicals. There is very little
evidence available concerning the relation between the
presence of these compounds in water and human disease.
Information on classical acute health effects of relatively
toxic chemicals can be obtained from physicians' manuals.
However, knowledge of the chronic health effects associated
with long-term exposure to low-level concentrations of
chemical substances is not well documented. The possibility
that cancer may result from long-term exposure to low con-
centrations of carcinogens is of utmost concern.
Carbon-Chloroform Extractables (CCE) and Carbon Alcohol
Extractables (CAE)'
The Committee on Water Quality Criteria (1586) suggested
that absorbable organic carbon in public water supply sources
should not exceed the carbon chloroform extractables (CCE)
level of 0.7 mg/l. (No level has been established for carbon
alcohol extractables - CAE.) The establishment of this level
was based upon the adverse physiological effects of CCE as
well as aesthetic considerations.
To date, laboratory testing of the pathological effects
of trace organics has been restricted to mice and fish.
Hueper and Payne (609) conducted a study of mice that were
exposed subcutaneously, cutaneously, and orally to extracts
of CCE and CAE obtained from both raw and finished water
supplies. Results of this study indicated that these extracts
had a potential for carcinogenicity (see Table 153). The
cutaneous dose used in the experiment was one drop of extract
every 2 weeks for 56 weeks with 72 mice; the subcutaneous
dose was 2 to 4 mg every 2 weeks for 56 weeks with 72 mice;
and the oral dose (only one instance) constituted 2 percent
of the regular food and was available to 40 mice. The control
group consisted of 40 unexposed mice. No tumors were observed
among the 40 mice in the control group or among those exposed
orally. Carcinogenic effects in subcutaneous and cutaneous
groups included one papilloma (a circumscribed overgrowth of
the papilla) of the bladder; four spindle-cell sarcoma (fusi-
form cell tumor) at the site of subcutaneous injection; and<
leukemia, lymphoma, or reticulum-cel1 sarcoma of the liver in
all other instances. However, it is very difficult to extra-
polate the experimental data of animals to humans. Thus, the
question still remains as to whether such extracts would cause
similar abnormalities in humans.
Another experiment was conducted to investigate the
toxicity of CCE and CAE from processed water supplies (355).
A total of 5 mg of either CCE or CAE was introduced sub-
cutaneously during the first 20 days after birth of the
test mice. No tumors were found to be induced during the
433
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TABLE 154. LONG-TERM TOXICITY OF TRACE ORGANICS (1570)
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TABLE 155. ACUTE AND PREDICTED LONG-TERM
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436
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period, but varied death rates of the test animals were ob-
served. The studies were conducted over a 1-yr period using
New Orleans drinking water supplies (355).
Organohalides
Occurrence and formation of organohalides such as
CHC13, CHClgBr, CHClBr^i and CHBrs were reported when water
containing organic substances was chlorinated (83, 1176).
Of the haloforms, chloroform (CHC^) was reported as the
predominant organohalide, with concentrations ranging from
54 yg/£ to 150 yg/£. The level of risk for chloroform -
estimated from consideration of the worst case and for the
expected cancer site, such as the liver - might be ex-
trapolated to account for up to 40 percent of the observed
liver cancer. The toxicity of chloroform has been well
demonstrated in lethal-dose studies.
An 1050 value ranging from 89 to 35 mg/kg was observed
by Tardiff and Deinzer (1362), when CCE obtained from the
Kanawha River in West Virginia was introduced into mice via
an interperitoneal route. The difference amonq these LDso
values was shown to be due to the amount of chloroform pre-
sent in the extract, indicating the toxicity of chloroform.
The CAE obtained from the same river showed an LDsg of 84 ma/kg.
The LD5Q for the concentrated organics from Cincinnati tap water
was shown to be 65 to 290 mg/'-g.
The same authors also reported the identification of 60
compounds from drinking water. Of the compounds, 1 was classi-
fied as nontoxic; 14, moderately toxic; 16, very toxic; 2,
extremely toxic; and 27, unknown (135). However, it is diffi-
cult at this time to determine the relationships of the toxici-
ties of these compounds in humans to the level of the compounds
present in water and wastsv/ster.
Careful interpretation of the toxicity data, such as
the 1050 value obtained from concentrated extracts, is
necessary when these values are to be used to set toxicity
levels in drinking water.
Polynuclear Aromatic Hydrocarbons (PAH)
Occurrence, formation, concentration, activity, carcin-
ogenicity, and degradation of polynuclear aromatic hydro- .
carbons (PAH) in water are well documented (29). Minimal car-
cinogenic doses of three of the most potent hydrocarbons in
susceptible experimental animals are shown in Table 156.
437
-------
TABLE 156. THE MINIMAL CARCINOGENIC DOSE FOR
THREE OF THE MOST POTENT CARCINOGENIC HYDROCARBONS
IN SUSCEPTIBLE EXPERIMENTAL ANIMALS (1564)
Least Amount which
3,4
3,4
1,2
20
Carcinogen
- Benzpyrene
- Benzpyrene
,5,6 - Dibenzanthracene
- Methyl cholanthrene
Animal
Mouse
Rat
Mouse
Mouse
Rat
Caused Cancer*
4.0 yg
50.0 yg
2.5 yg
4.5 yg
20. 0 yg
* Only one dose was administered subcutaneously.
Miscellaneous Organic Compounds
A preliminary experiment was designed to study the
toxicity of organic compounds present in a secondary treat-
ment plant effluent. Rats were supplied with filter-
sterilized effluent from an activated sludge plant as the
sole source of drinking water. Two of the 10 rats developed
massive tumors. Also, the exposed female rats developed
significantly smaller adrenal glands than the control rats
that were provided with the local water supply (1037).
An epidemiologic study on the toxicity of compounds
present in drinking water was cited by Andelman and Suess
(29). This study indicated fewer cancer mortalities in a
London borough that was supplied with well water than in
boroughs supplied with river water. This could mean that
the river water receives more carcinogenic waste material.
Similar findings reported by Tromp (1584) showed that
areas using municipal water systems had lower cancer death
rates than those using other systems. However, the cancer
death rate was higher among areas that received municipal
water from a river than among those that received municipal
water from wel1s.
438
-------
When other factors such as food, air quality, and
individual habits (i.e., cigarette smoking) are considered,
the importance of trace carcinogens in water supplies may
not be significant. However, several observations have been
made correlating water supply quality and cancer incidence.
For example, Talbot and Harris (1357) established
a correlation between cancer mortality in white males and
water supply source, between mortality and urbanization, and
between mortality and income. When occupational variables
are not considered, lung cancer mortality rates were found
to be correlated with surface water sources, but there were
no correlations found in other cancers.
Halogenated. Hydrocarbons
In a study that was designed to investigate the correla-
tion between levels of halogenated hydrocarbons in New
Orleans drinking water and levels of halogenated hydro-
carbons in blood plasma of individuals drinking the water,
13 halogenated hydrocarbons were isolated. Researchers also
detected the presence of carbon tetrachloride and tetra-
chloroethylene (2 of the 13 compounds) in the pooled sera
of eight people. It is probable that biomagnification was
involved if the chemicals in the plasma originated from the
drinking water (1573).
Low Molecular Sulfurated Hydrocarbons
A case history study of the waterborne goitrogens and
their role in the etiology of endemic goiter was recently
reported from Colombia, South America (442). The potential
presence of low molecular weight compounds (less than 220),
such as sulfurated hydrocarbons in water and wastewater,
received careful evaluation. The compounds (sulfurated hydro-
carbons) were known to be related to the high incidence of
goiter among children and were regarded as waterborne goitro-
gens. The study also reported a 10-fold increase in cancer
of the thyroid where endemic goiter was observed (442).
BIOLOGICAL CONTAMINANTS
Epidemics of waterborne diseases have largely been elimi-
nated, due mainly to the advancement of sanitary engineering,
enforcement of public health regulations, and preventive
medical practices; however, waterborne disease data from the
last three decades indicate that outbreaks are no longer on
the decline in the United States (271, 425). As shown in Table
157,during the 25-yr period from 1946 to 1970, there were 358
recognized outbreaks (72,358 individuals involved) of disease
or chemical poisoning attributed to contaminated drinking water
439
-------
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440
-------
According to the reports of the Center for Disease Control
(426), during the past four years (from 1972 to 1975), 105
waterborne disease outbreaks were reported, involving 22,650
cases. As shown in Table 158, in 1975, 24 waterborne disease
outbreaks were reported, involving 10,879 cases.
TABLE 158. WATERBORNE DISEASE OUTBREAKS
1972-1975 F AND M (426)
1972 1973 1974 1975 Total
Outbreaks
Cases
29
1 ,638
24
1 ,720
28
8,413
24
10,879
105
22,650
Table 159 shows the number of outbreaks and cases by
etiology and type of water system. The category with the most
outbreaks is acute gastrointestinal illness. This category
includes outbreaks characterized by upper and/or lower gastro-
intestinal symptomatology for which no specific etiologic agent
was identified. In previous years, these outbreaks were
considered sewage poisoning. One outbreak each was caused by
giardiasis, shigellosis, enterotoxigenic E. coli, and hepatitis /
There were no reported deaths associated with waterborne disease
outbreaks in 1975 (426).
Most outbreaks involved semipublic (67 percent) and
municipal (25 percent) water systems; some involved individual
(8 percent) systems. Outbreaks attributed to water from muni-
cipal systems affected an average of 1,218 persons; those
attributed to semipublic systems involved 221 persons; and those
associated with individual water systems affected 13 persons.
Of those 16 outbreaks associated with semipublic water supplies,
11 (69 percent) involved visitors to areas used mostly for
recreational purposes.
441
-------
TABLE 159. WATERBORNE DISEASE OUTBREAKS, BY ETIOLOGY AND
TYPE OF WATER SYSTEM, 1975 (426)
Disease
Municipal
Outbreaks
Cases
Semi public
Outbreaks
Cases
Individual
Outbreaks
Cases
Total
Outbreaks
Cases
Acute gastro- 4 7,300
intestinal
illness
Chemical 2 11
poisoning
Giardiasis
Shigellosis
Enterotoxi-
genic E. coli
Hepatitis
Total 6 7,311
13
1
—
1
1
—
16
2,460
26
1 9
56
1,000 ' --
1 17
3,542 2 26
17
3
1
1
1
1
24
9,760
37
9
56
1,000
17
10,879
The object of this section is to compile a comprehensive
summary of research into the health effects of biological contami-
nants in wastewater treatment. Diseases transmitted by water and
wastewater largely originate in the intestinal discharge of man
and/or animals. These diseases are caused by bacteria, viruses,
fungi, and protozoan and other parasites.
Protozoan and Other Parasites
A number of.intestinal parasite infections can be introduced
into man directly from water supplies and indirectly through
wastewater discharges. Under normal conditions, the potable-water
route of infection is quite unimportant. However, the reuse of
treated waste effluents for irrigation and groundwater recharge
requires that this problem be reexamined.
Ascariasis (a disease caused by infection with ascaris),
trichuriasis (a disease caused by infection with trichuris), and
hookworm diseases are some of the infections that originate from
direct soil pollution by feces. This pathway has been virtually
eliminated in the United States, due to the introduction of modern
sewage disposal and water supply systems. When there is a break-
down in sanitation, these diseases may reappear (1509).
Studies in foreign areas affirm the relative unimportance
public water supplies as a route of infection for intestinal
parasites. A study by the World Health Organization (WHO) in
of
442
-------
Sudan, in which a modern water supply was provided to one test
city, showed that parasitic infections were not decreased. The
study indicated, instead, the need for sanitary waste disposal
facilities. This finding was substantiated by the substitution
of a modern water supply system for an older system in Western
Transvaal. The substitution had no effect on the prevalence
of helminths among the Bantu population studied - children 7
to 16 years (1509).
Amoebic dysentery (amoebiasis) appears to be the most
important parasitical disease associated with wastewater in the
United States. It is caused by Entamoeba histolytica, a proto-
zoan. Today, the prevalence rate of E. histolytica in the
general population of the United States is considered to be
around 3 to 5 percent (1577). The prevalence of the intestinal
protozoa varies considerably in different population groups
and is generally correlated with socioeconomic conditions.
Higher rates are found in areas of poor sanitation and in regions
without sewage systems, and potable water. Higher, rates are also
noted in groups of people with poor personal hyoiene (e.g.,
patients in institutions for the mentally retarded).
The amoeba can form small cysts (5 to 20 vm) with a speci-
fic gravity of about 1.06. Each mature cyst is capable of pro-
ducing four motile amoebae. The cysts are resistant to adverse
environmental conditions and are excreted with feces into water
and/or remain in the human digestive tract to become vegetative
amoebae. These amoebae multiply and may become invasive, caus-
ing erosion of the superficial mucous membranes. They may even-
tually invade the tissue with consequent ulceration.
The vegetative forms do not survive outside the digestive
tract. As with most parasitic diseases, the symptomatology
produced by pathogenic intestinal protozoa is too nonspecific
to enable the physician to make an accurate clinical diagnosis.
In 1974, there were 2,743 reported cases of amoebiasis in the
United States (1580); because of non-clinical manifestations,
the actual figure is undoubtedly considerably higher.
In an experiment with volunteers, it has been demonstrated
that up to 25 percent could be infected by a dose containing
less than 10 organisms of endamoeba; the remainder required a
minimal dose of 10,000 organisms to become infected. However,
as shown in Table 160, the infected volunteers did not manifest
any signs of illness.
Giardia lamblia, a flagellated protozoan of the small intes-
tine, often implicated epidemic!ogically with drinking water is
the etiologiccl agent for giardiasis. An outbreak has recently
been reported (1581) in Rome, New York, where the water supply
could have been contaminated by untreated human waste. Another
443
-------
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outbreak of giardiasis by G. lamblia was reported in September
1976 in Idaho. The source was purported to be from untreated
surface water of an individual water system (561).
Apparently, the cysts of G_._ lamb!ja survive in water and
re'main infective for 16 days. During 1969 to 1973, seven out-
breaks involving 193 people were reported in the United States.
During October 1954 to March 1955, there was a suspected water-
borne outbreak of 50,000 cases of giardiasis in Portland, Oregon.
The outbreak was not reported, because of the failure to isolate
the organism from the suspected water source (909). Epidemic
giardiasis among American travelers to the Soviet Union has been
reported since 1970; the latest outbreak was reported in
October 1975 (1581). Sporadic single cases or occurrences of
giardiasis with recent exposure to untreated mountain or pond
water have been noted (941). In an experiment where adult
humans were given challenge doses of Giardia lamblia, 76 to 100
percent Infected with a dose containing 10 organisms did not
become 111. Similar results were observed with doses containing
up to a million organisms (see Table 160).
Human schistomlasis is another parasitic infection. Although
it does not occur naturally in North America, human schistomiasis
1s a difficult problem to control in other parts of the world.
Schistosoma mansoni in Africa and S_._ japonicum in Japan are the
principal etiologlcal agents of schistosomal dysentery, parasi-
tic periportal cirrhosis, and secondary portal hypertension. S.
haematoblum 1s the etiologlcal agent of schistosomal haematuria
(the passage of blood In urine due to schistosoma) and schisto-
somal carcinoma (cancer due to schistosoma) of the bladder. The
schistosomal worms are known as blood flukes; their primary hosts
are aquatic snails (1212). "Swimmer's itch," a schistosomiasis
1n which the primary hosts are waterfowl, is an accidental infec-
tion by the cercariae. Because man is not a natural host, their
development results 1n local irritation and itching.
In mid-May 1976, 11 Girl Scouts noticed a transient, prui-
t1c, erythematous macular rash on their lower extremities 15 to
20 m1n after wading In a lake 1n Shadow Cliffs Regional Park,
California, Four days later, 7 of the girls developed superim-
posed papules, The lesions cleared after a few days. Several
other Individuals were similarly affected after swimming in Cas-
talc Lake, California (183), These eases are typical of "swim-
mer's Itch" of schlstosome dermatitis, caused by a variable aller-
gic response to schlstosome eercariae whose definitive hosts are
birds and small sem1aquat1e mammals. The short-lived, free swim-
ming cercariae are liberated from snails (the intermediate hosts)
and penetrate the human skin during water contract in Infected
fresh water lakes or man-made water Impoundments. Afttr §k1n
penetration, the cercariae die.
448
-------
TABLE 161. AVERAGE VALUES FOR C. ALBICANS, COLIFORM
AND FECAL COLIFORM COUNTS AND TOC (TOTAL ORGANIC CARBON)
DETERMINATIONS IN THE ESTUARINE WATER SAMPLES,
LONG ISLAND, NEW YORK (631)
Estuari ne
Stations
Station 1
Station 2
Station 3
C. al bi cans
cells/£
4,245
4,003
9,555
Col if orm
Total
MPN/100 ml
338
298
1,962
Col i form
Fecal
MPN/100 ml
33
12
490.5
TOC
mg/£
8
8.4
8.7
This fungus retained an infectivity and pathogenicity to
mice after it was exposed to sea water for eight weeks (631).
In the open ocean, there is a concentration of 200 to 300 fungal
cells/£; in moderately contaminated beach areas, there are
levels of 10,000 to 20,000 cells/£; and in heavily contaminated
estuaries, up to 100,000 cells/£ (631). The overall trend was
a gradual increase in concentrations during summer months, from
June to September, after which the concentration declined (631).
Bacteria
Salmonellosi s--
A wide variety of species pathogenic to man and
animals belongs to the genus salmonella. Water and food, as
well as personal contact, are the main routes for transmission
of the species from man to man.
Among the three distinct forms of salmonellosis in man,
typhoid fever - caused by S_._ typhosa - is the most severe
enteric fever form, and man is the only host. Salmonella
septicemia, most commonly caused by S. choleraesuis, is
relatively rare. This bacteria is not particularly common in
humans, but has a predilection for swine. Salmonella are most
commonly encountered in acute gastroenteritis. Serotypes (types
based on antibodies) in excess of 1,500 have been identified.
Most, in contrast to S. typ h o s a, are not host specific.
The death rate, due to typhoid fever in the United States
in 1900, was 31.3/100,000 population; however, at present, death
due to this disease is practically nonexistent, as shown in
Table 162 (308, 613).
449
-------
Cau
Typhoi
TABLE 162. U.S.
RELATED TO
se of Death
1
d & paratyphoid
MORTAL
WATER
920 1
7.6
ITY FROM SEL
POLLUTION (
De
930
4.8
ath
1
Rate
940
1 .1
ECTED
308).
per 1
1950
0.1
CAUSES
00
,000
1960
0.0
1967
0
.0
fever
Dysentery
Gastritis ,
enteriti s ,
duodenitis,
& colitis
4
53
.0
.7
2.8
26.0
1
10
.9
.3
0
5
.6
.1
0
4
.2
.4
0.1
3.8
Amoebic meningoencephalitis has been reported in different
parts of the world, including the United States. The etiologic
agent is Naegleria fowleri, a free-living soil amoeba. Epidemi-
ologically, the amoebae have been aspirated by swimmers into
their nasopharynx, resulting in such clinical conditions as
meningoencephalitis, brain abscesses, and lung abscesses (277}.
The disease can be contracted by the intensive passage of
amoebae from one human to another in overcrowded swimming pools.
The disease is also associated with streams connected to canals
that receive warm industrial effluent. In addition, reptiles
that harbor such amoebae can transmit the disease.
An outbreak of ascariasis occurred after World War I;
one out of every three surgical patients at a hospital in
Le Havre, in the 2 yr following cessation of the war, was found
to have the disease (1509). Also, following World War II, a
40 percent incidence of ascariasis was reported in Darmstad
and was attributed to a widespread breakdown of sanitation
practices that occurred in Germany during the latter part of the
war (1509).
Ova from the giant roundworm A s c a r i s 1umbricoides , the
pinworm Oxyuris vermicularis , the whipworm Trichuris trichuria,
the tapeworm Taenia sag1nata . and possibly the hookworm
are reported to be present in wastewater (428). Heavy infestations
of roundworms found in some European cities are related to the use
of night soil, which is also known to be responsible for about
20 percent of the recurrent infections of amoebiasis and hookworms
(459), The cestode eggs are transmitted to the intermediate host
(swine or cattle), and man is infected by eating the meat of the
intermediate host. This is of greatest concern when sewage sludge
is spread in agricultural areas.
450
-------
Man is known to be the host and reservoir of A. lumbricoides,
whose ova are excreted in the feces of infected indTviduals. Ova
of these intestinal parasites require several days before maturing
to an infective stage. Under the most favorable conditions,
ascarids require 10 days to mature; trichurids, 21 days; and
hookworms, 6 days. Hence, these parasites are unlikely to pose
health threats if the water is used for drinking, since they would
be eliminated from the human body before maturation. However, use
of such water for food processing, garden watering, or simple
aesthetic activities may require the effective removal or destruc-
tion of the parasites (1509).
Free-living nematodes are widely found in municipal water
supplies. Their potential as carriers of enterococci , salmonella,
and shigella has been demonstrated (1509). Although free-living
nematodes are not important as health threats in conventional
waterworks practice, their significance in a reclaimed water
situation needs evaluation.
Dracontiasis, or guinea worm infection, is a disease
primarily associated with poverty (especially inadequate water
supplies and wastewater treatment), and is common in India and
West Africa. Vector species of Cyclops persisting in ponds
drinking water must be controlled (usually by the use of Abate
at a concentration of 1 mg/£).
In moderate climates, the human contribution of ova to
wastewater would appear to be no greater than 10 percent, but
may reach 30 percent in subtropical regions such as the southern
extremities of the United States. The remainder of the ova is
of animal origin. Various authors have reported 59 to 80 worm
eggs/£ sewage (428). The eggs are generally resistant to
environmental conditions, having a thick outer covering to
protect them against desication. In one study, 90 percent of
ascaris ova was destroyed after 15 days at 29°C; the ova may
survive for up to 60 days at 40°C (428).
In summary, it may be stated that a large quantity of a
variety of ova from parasitic worms may be present in waste-
water, and that the ova possess a high degree of resistance to
many environmental stresses.
Candida albicans. a pathogenic, yeastlike fungus, is an
asporogenous T"non-spore-f ormi ng) yeast that develops pseudohyphae
(a kind of filamentous structure). Large, round, thick-walled
chlamydospores - the morphological characteristic of the genus
Candida - are frequently, though not always, present.
451
-------
C. albicans has been found in the feces and skin of several
animalspecies other than man. The fungus rarely occurs in
soil. The prevalence of Candida in feces in different regions of
the United States varies from 19.3 to 44.6 percent of the total
population (631). Seventy percent of the inhabitants of Baghdad
have the fungus in their feces. Another important infective
area in the human body is the female vagina; 43 percent of the
female population in the United States are carriers (631).
C. albicans may cause oral thrush, corneal ulcers, and
other ocular infections. One survey analyzed 20 weekly samples
collected at three stations on the North Shore of Great South
Bay, Long Island. It was reported that the estuarine water
samples contained between 1,000 to 11,000 or more cells/£ (631).
These results are shown in Table 161 .
Relatively few outbreaks of typhoid fever and salmonellosis
associated with drinking water were reported in the United States
during 1971 to 1973 (425, 910). The reported isolation rates
for humans in the United States in 1972 was 12.5/100,000; the
fatality rate between 1962 and 1972 was 0.43 percent, mostly
among the very young and very old.
In 1974, 23,833 isolations of salmonella were reported to
the Center for Disease Control, a decrease of 2,855 cases
(10.7 percent) from the previous year. As in 1973, S. typhimurium
(30.8 percent), S. newport (6.9 percent), and S. enteritides
(6.0 percent) were the first, second, and thircfmost commonly
isolated serotypes, respectively (1192). The annual incidence of
reported human isolations of salmonella has remained relatively
constant since 1963 (1192). The seasonal incidence for the
period from 1967 to 1974 shows a consistent pattern, with
the greatest number of isolations reported in July through
November, and the fewest reported in February through
April (1192).
The ages of infected persons reveal that 66.8 percent of
the 17,229 isolations was from persons less than 20 yr of age.
Similarly, this age group showed the highest infection incidence
for the years from 1963 through 1973 (1192).
Several serotypes (e.g., S_._ we! tevreden, S. panama, and
ij. oslo in Hawaii; §_._ newport and S. javiana in the southern
states) have definite regional patterns, for reasons that are
not clear.
From 1962 to 1974, 143 deaths were reported in 34,291
persons involved in 499 outbreaks. This resulted in a case-
fatality ratio of 0.42 percent.
452
-------
In 1974, in 18 of the 34 outbreaks of salmonellosis (involv-
ing at least 4,011 persons), 5 outbreaks were caused by contami-
nated poultry, 5 by beef or beef products, and 3 by dairy products
In 6 of these outbreaks, person-to-person transmission was thought
to be responsible; none was reported to be transmitted by water.
In 1973, 3 typhoid outbreaks (totalling 217 cases) and 1 out-
break of salmonellosis (3 cases) occured in semipublic or
individual water supplies. In 1974, an outbreak involving several
hundred people on a cruise was reported; epidemic!ogic investiga-
tion failed to clearly implicate either food or water. Three
epidemiologic investigations of turtle-associated salmonellosis
were also found in the literature (270).
According to experimental data, the dose required to bring
about human cases of typhoid fever is surprisingly high (1576).
Human volunteers were challenged with one dose of a given number
of Salmonella typhosa. The results are summarized in Table 163.
TABLE 163. RELATION OF DOSAGE OF
S_^ TYPHOSA TO DISEASE (1576)
Number of Viable Cells Total Volunteers Number with Disease
S. typhosa Challenged
109
108
107
105
103
42
9
32
116
14
40
8
16
32
0
(95%)
(89%)
(50%)
(28%)
(---)
With the salmonella species Isolated from spray-dried eggs,
human volunteers were challenged orally; the results are
summarized 1n Table 164. Existence of varying degrees of
virulence among the species and strains are shown. Similar
results are shown 1n Table 160.
453
-------
TABLE 164. DOSE OF VARIOUS SPECIES AND STRAINS OF
SALMONELLA THAT CAUSED DISEASE IN HUMAN VOLUNTEERS (1571)
Dose at Which
Salmonella 50% or More Develop'
Species/Strain Clinical Disease
S. meleagridis I 50,000,000
S. meleagridis II 41,000,000
S. meleagridis III >10,000,000
S. anatum I 860,000
S. anatum II 67,000,000
S. anatum III 4,700,000
S. newport 1,350,000
S. derby 15,000,000
S. bareilly 1,700,000
S. pullorum I >1 ,795,000 ,000
S. pullorum II >163,000,000
S. pullorum III >1 ,295 ,000 ,000
S. pullorum IV 1,280,000,000
Shiqellosis
Shigella cause bacillary dysentery in man and in higher
apes. Although person-to-person transmission is the predominant
mode of spreading shigellosis, waterborne outbreaks have played
a significant role in the overall epidemiology of the disease in
the United States (1320, 1582). In 1975, 14,757 shigella isola-
tions from humans were reported to the Center for Disease Con-
trol (CDC). This was a decrease of 24.0 percent from the 19,420
isolations reported in 1974 (1249). Utilizing population esti-
mates for July 1, 1975, approximately 69.2 isolations were repor-
ted for each million population of the United States in 1975.
Shi gel 1 a sonnei (60.3 percent) was the most common etiological
agent followed by S. f1exneri (38.2 percent). Between January
17 and March 15, 1974, approximately 1,200 cases of acute gas-
trointestinal illness occurred in Richmond Heights, Florida.
The outbreak was caused by a failure in the chlorination process
454
-------
of well water, which allowed insufficiently chlorinated water
from a contaminated well (located near a church's septic tank)
to be distributed to the community (270).
Most instances of Shigel1a-induced illnesses reported in the
past several years have involved small wells, temporary break-
downs of chlorination systems in water supply, and swimming in
waters contaminated with sewage. The isolation rate in the United
States is approximately 15/1,000,000 population. Up to. 25 per-
cent of adult humans may be infected and show clinical response
to S h i g e 11 a dysenteriae doses of 10 cells; 25 to 50 percent, to
doses of 100 eel Is; and up to 100 percent, to doses of 10^ cells
(see Table 160). These results indicate that it would take
smaller doses to show clinical response for shigella than it
would take to show response for salmonella.
Cholera
Cholera, which is fully controlled in the United States,
has created a major global public health problem in India, Italy,
Portugal, and many other countries. In the United States, only
one case (in the Gulf Coast town of Port Lavaca, Texas) has
been reported since 1911. Transmission was associated with a
well that was contaminated by leachate from a septic tank system.
The etiological agent of cholera is Vibrio cholerae, Biotype
El Tor, Serotype Inaba or Ogawa. Man is the only known natural
host, and, since a prolonged carrier state is uncommon, the
disease must be maintained by an unbroken chain of mild, subtle
infections. Cholera is a serious disease, similar to typhoid
fever but more rapid in onset, more virulent, and more often
fatal. Death rates of 25 to 85 percent are commonly reported
(1571).
The primary means of cholera transmission is the drinking
of contaminated water. Also associated with cholera is the
eating of fish caught in contaminated waters. In the event that
imported cases occurred in the United States, it is felt that
the risk of spread would be minimal because of modern, indus-
trialized sanitary engineering as well as responsible medical
therapy. It is also reported that vaccination is not needed
to control imported cases or outbreaks that may occur in the
United States (270).
The minimum doses of vibrio that cause clinical symptoms
in adult humans may vary (depending upon the strains of vibrio
that are used) from 103 cells (in up to 50 percent of the indi-
viduals) to 105 cells (in up to 75 percent of the individuals),
as shown in Table 160.
455
-------
Gastroenteritis
There are many reports of waterborne gastroenteritis of
unknown etiology in which bacterial infections are suspected.
These include outbreaks characterized by nausea, vomiting,
diarrhea, and fever, for which no specific etiologic agent
could be identified.
An epidemiological study of the. impact of wastewater
pollution on marine bathing beaches was conducted during the
summers of 1973 and 1974 at the Coney Island and Rockaways
beaches in New York (179). A statistically significant finding
was observed: the rate of gastrointestinal symptoms among
swimmers compared to nonswimmers was higher at Coney Island,
where the densities of the indicative organisms such as E. co1i
and fecal streptococci were significantly higher than the
densities at Rockaways Beach (Tables 165 and 166). It was
concluded that there were measurable health effects associated
with sewage polluted waters (179).
In 1971, a waterborne gastroenteritis outbreak was
reported in Pico Rivera, California, in which 11,000 residents
became ill with diarrhea and abdominal cramps. No pathogens
were isolated from any cases. The source of water was
responsible for the outbreak; chlorination at the reservoir had
been interrupted when the chlorine supply was exhausted. One
of the major outbreaks involving over 1,000 persons occurred
at Crater Lake National Park, Oregon, in July 1975. The
illness was reported to be associated with sewage-contaminated
water (945). Enterotoxigenic E. c o1i , Serotype 06:H16, was
isolated from ill park residents and from the park's water
supply (426).
It was noted that the attack rate of acute "summer diarrhea"
on the Fort Apache Reservation, Arizona, during 1971, rose
simultaneously with rainfall, temperature, and bacterial
contamination of water sources (1520). Nonenteropathogenic
E. coli capable of producing enterotoxin was isolated.
In the study of clinical response of adult humans to
challenge doses of E. co1i , it has been demonstrated that very
large doses of cells (about 10°) would be necessary to show
clinical response in 75 percent of the individuals tested
(Table 161 ). With the E^ coli strain of 0111:84, doses of
only 106 cells were necessaryfor a similar response. However,
it should be noted that the digestive tract in most individuals
is populated by normal flora, of which E. col 1 is the most
abundant and most characteristic; about~TO^/g of feces is
common (85).
456
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Leptospirosis
Etiologlcal agents of 1eptospirosis (an infection caused
by leptospira) constitute approximately 150 different serotypes
categorized on the basis of their agglutinogenic properties
(1577). The pathogenic serotypes are otherwise indistinguishable
by morphology or biochemical activity.
Recognition of two species, Leptospira interrogans and
L. biflexa, has been proposed for the so-cal1ed pathogenic and
saprophytic leptospires, respectively (1577).
Generally, 1eptospirosis, typically a disease of animals,
has been regarded as an occupational disease that occurs
primarily in workers associated with wastewater, rice, sugar
cane, farms, and slaughter yards. The disease is transmitted
to man by direct contact or via water contaminated by urine
from infected wild and domestic animals. Leptospirosis is
endemic in some parts of the world. However, 11 outbreaks in
nonendemic areas during 1939 to 1959 were associated with
swimming or wading in contaminated water (270, 1577), indicating
the potential for contacting the disease as a result of
recreational activity.
At the same time, leptospirosis has become a more recognizable
human health problem in recent years, because of better identifi-
cation of symptoms and improved methods of diagnosis. In rural
populations in France, the percentage of infection by source was
as follows: water or mud, 21 percent; animals, 53 percent; and
water and animals, 25 percent. In nonrural populations, how-
ever, 80 percent of the infections was acquired by contact
with contaminated water (1572). It was also noted that sub-
clinical leptospirosis in humans was not infrequent and may be
a significant public health hazard (1572). Information on the
infective dose of leptospira to humans is not available from the
literature surveyed. Leptospira can apparently penetrate intact
skin, assisted by cuts, abrasions, and immersion. Incidences of
infection from swimming also suggested penetration via the
mucous membranes of the mouth or nasopharynx (270). The nesting
site of leptospires in natural hosts is the lumen of nephritic
tubules, from which they are shed into the urine (1577). Patho-
genic leptospires can survive for three or more months in neutral
or slightly alkaline waters, but do not persist in brackish or
acidic water (1577). In 1975, two outbreaks of 1eptospirosis
were attributed to swimming in contaminated surface water. Seven
children in Tennessee developed infection with L. interrogans
serotype grippotyphosa after swimming in a smalTTocalstream.
Two persons in Louisiana became infected with leptospires of the
serotype icterohaemorrhagiae after bathing in a man-made lake (426)
459
-------
Tuberculosi s
The possibility that tuberculosis may be transmitted by
sewage has frequently been considered in connection with the
disposal of wastewaters from hospitals, tuberculosis sanitaria,
dairies, and slaughter houses; the possibility has even been
considered in connection with domestic sewage in general.
Concern has been expressed about the danger of human and animal
infection, particularly where these waters are reused (509).
The presence of mycobacteria in wastewater has been
extensively studied since around 1900 - the time of the first
findings of the bacteria in feces (428). The recovery of
Mycqbacterium tuberculosis (the bacteria that cause tuberculosis)
is difficult, even from favorable sources such as sputum;
recovery from sewage is much more difficult because of the
presence of other bacteria.
The tubercle bacilli are present in the sputum and feces
of tuberculosis patients. The wastes from institutions that
treat the patients will almost always contain large numbers
(4 x 105 to 10'/£) of tubercle bacilli (509). Significant
numbers (about 3/1 in the effluent of a plant producing about
7,600 gpd of milk) of virulent tubercle bacilli are also found
in the wastes from some dairies. A cow suffering with tuber-
culosis of the udders discharges about 1.5 x 10^ tubercle
bacilli/day (509). M. balnei , which causes granuloma, may be
present in chlorinate~d~ water used for swimming pools (580). Much
of the data on survival of tubercle bacilli in sewage indicate
that, under laboratory conditions, the bacteria can be infective
for 6 months in sewage and for up to 24 months in feces (509).
Contaminated water can produce typical tuberculosis in
humans in some instances. The first clear-cut cases of human
infection were reported in 1947. From 1947 to 1953, nine cases
of tuberculosis were described in humans who aspirated polluted
water into their lungs after swimming and nearly drowning in
contaminated water (509).
There were not much data available in the literature on
the infectious dose to humans of tubercle bacilli in wastewater.
In an experiment with guinea pigs, it was reported that 80 per-
cent of the animals contracted the disease when they were fed
with grass that had been sprayed with more than 4 x 10^ tubercle
bacilli. Calves that had been similarly fed also succumbed (509)
The majority of studies carried out on mycobacteria has
focused on the presence of M. tuberculosis in sanitarium wastes.
These studies may not provicTe a realistic picture of the danger
of infection from contaminated water.
460
-------
The potential health hazards of M. tuberculosis being
transmitted through sanitarium wastewaters, to drinking supplies,
and back to man in general appears to be quite remote.
Other Sources of Bacterial Infection
Vibrio garahaemplyticus is a marine bacteria that is known
to be associated with common-source gastroenteritis outbreaks
when contaminated seafoods are consumed. The bacteria 1s not
directly involved with wastewater; however, its frequent
occurrence in the coastal waters and aquaculture farms alarms
consumers of seafoods as well as bathers in contaminated waters
(270). Between 1969 and 1972, 13 common-source outbreaks were
recognized in the United States. This infectious agent has
been the leading cause of food poisoning in Japan for some years.
Klebsiel la pneumoniae is one of the coliform group members,
closely resembling Enterobacter aerogenes. In one case, it was
reported that K. pneumoniae were isolated from pulp and paper
wastewater effluents and represented as much as 80 percent of
the total coliform bacteria present (722). Although the origin
of the bacteria in the pulp mill wastewaters was not resolved,
fecal origin was a strong possibility. Whether ingested K. pneu-
moniae are pathogenic and a hazard to human health should be
determined. They are a respiratory pathogen.
Pseudomonas aeruginosa has been an etiological agent for
many types of infections in hospitals. Contaminated sinks and
flower vases are some of the well-known sources of P. aeruginosa
(270, 1572). The microbiological characteristics of sewage
discharged by hospitals are interesting when compared with those
of residential wastewaters, because counts of all the organisms
tested, except P^ aeruginosa. were lower in the hospital
effluent (493).
C1ostrid ium perfringens is known to cause gas gangrene and
is found in anaerobic environments such as sludge, mud, and
sediment in aquatic and marine environments. It has been shown
that a dose of at least 10- cells of the bacteria would be
necessary to demonstrate clinical response in 75 to 100 percent
of the individuals tested (see Table 160).
Viruses
In the past, transmission of waterborne viral diseases was
rarely recognized, due largely to lack of sensitive virus-detection
methods and precise quantification. With improved techniques for
concentrating viruses from large water samples, increasing
occurrences of viruses in water and wastewaters have been reported.
Viral transmission through water may take place 1n various ways:
bathing in contaminated water, eating contaminated seafoods,
461
-------
drinking from untreated or improperly treated water sources,
or contacting contaminated waters. Enteric viruses have been
investigated with greater emphasis than any other group of
viruses, mainly because any virus excreted in the feces and
capable of producing infection when ingested is theoretically
transmissible by water. The human enteric viruses and the
diseases associated with them are listed in Tables 167 and 168.
TABLE 167. THE HUMAN ENTERIC VIRUSES
AND THE DISEASES ASSOCIATED WITH THEM (1571)
Virus Subgroup
No. of
Types
Disease
Polio virus
Coxsackie virus
Group A
Group B
ECHO virus
Infectious hepatitis
Reovirus
Adenovirus
26
6
34
K?)
3
32
paralytic poliomyelitis,
aseptic meningitis
herpangina, aseptic meningitis,
paralysis pleurodynia,
aseptic meningitis, acute
infantile myocarditis
aseptic meningitis, rash and
fever, diarrhea! disease,
respiratory illnesses
infectious hepatitis
fever, respiratory infections,
diarrhea
respiratory and eye infections
Infectious Hepatitis
Apart from theoretical considerations, there are very few
viruses for which epidemiological evidence suggests transmission
by water. Infectious hepatitis (hepatitis A) is the only disease
caused by an agent having the characteristics of a virus for
which evidence of waterborne transmission has been accepted by
all workers in the field (976). Therefore, it is regarded as the
viral disease of greatest importance in wastewater.
In 1973 alone, a total of 59,200 cases of viral hepatitis A,
B, and a type unspecified were reported (426). In 1974, a total
of 59,340 cases of viral hepatitis - hepatitis A, B, and type
unspecified - were reported to CDC. This represents a rate of
28.1 cases/100,000 population, approximately the same rate as for
1973. Since 1971, 1974 is the first year to have shown rate
462
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increases for two quarters; the increase in cases began in the
fourth quarter of 1973. The seasonal variation noted in the
1950s and early 1960s was not seen in 1974. The 48,709 cases
of acute hepatitis A and hepatitis, type unspecified, consti-
tuted 82.1 percent of the total cases of viral hepatitis repor-
ted in 1974 (562). Waterborne outbreaks of hepatitis A con-
tinue to occur in the United States. From 1971 to 1973, these
documented outbreaks were associated with contaminated drink-
ing water from either municipal, semipublic, or individual water
systems (270, 910). Use of contaminated spring or groundwater
without proper treatment or disinfection, and back-siphonage of
contaminated water into the distribution system were reported
to be the causes of the outbreaks. The majority of documented
hepatitis A outbreaks in municipal water systems in the United
States between 1946 and 1971 occurred as a result of distribu-
tion system contamination, primarily through cross connections
and back-siphonaqe.
Two outbreaks of shellfish-associated hepatitis involving
285 cases were reported in 1973 (426). Both outbreaks - one
in Georgia and the other in Texas - were associated with the
eating of raw oysters. Epidemiologic evidence suggested that
two particular bays contaminated by flooding were the source of
the contaminated oysters.
A recent hepatitis outbreak of 14 cases was reported to be
associated with swimming in a grossly contaminated lake in North
Carolina, and with ingesting water from that lake. This is the
first time that such a definite case has been made for the poten-
tial of contracting this disease while swimming in sewage-pollu-
ted water. The probable fecal-oral transmission of infectious
hepatitis made the waterborne route possible. This mode of
transmission was vividly illustrated by several large epide-
mics that took place in 1955 to 1956, especially in India where
28,745 cases occurred (976).
As far as the magnitude of waterborne infectious hepatitis
is concerned, the water route still only accounts for up to
1 percent of reported cases at any time for which information
is available (976).
Despite the increased interest and concern in infectious
hepatitis, its infectious agent has not yet been isolated and
cultured. One recent report (404) using microscopic techniques
was able to show the presence of virus!ike particles, immunolo-
gically distinct from hepatitis B, in infected stools.
Poliomyelitis
The infectivity of feces from persons with poliomyelitis
and the characteristic fecal excretion of the diseased persons
466
-------
have been documented for years. The polio virus has been sought
and detected in sewage. Accordingly, the water route of trans-
mission has been implicated in several outbreaks of poliomyelitis
(see Table 169). Many cases of epidemics of poliomyelitis were
attributed to waterborne transmission through contaminated or
untreated water, but the evidence is not sufficient. It appears
that water transmission of the polio virus may be a rare occur-
rence in the United States, but common in' parts of the world
lacking adequate sanitary facilities. Six of the outbreaks
attributed to drinking water occurred in Sweden during the 1930s
and 1940s (976) and led to the early recognition of the impor-
tance of the fecal-oral route in poliomyelitis.
Viral Gastroenteritis
When a recognized pathogen cannot be isolated in cases
of gastroenteritis and diarrhea, the term vira 1 is often used
to describe the symptoms. It is quite possTbTe" that forms
of gastroenteritis and diarrhea transmissible from person to
person are due to viruses.
Gastroenteritis and diarrhea! disease are believed to
have accounted for approximately 60 percent of all epidemics
of waterborne diseases throughout history. The number of
these cases that was due to viral agents is not known; if,
however, only a small portion of the cases was due to viral
agents, this number would still be quite substantial.
A virus-like particle, similar in appearance but immuno-
logically distinct from the hepatitis A, has been reported to
be associated with an acute infectious nonbacterial gastro-
enteritis (680). Shellfish-associated gastroenteritis has also
been reported (332).
Other Viral Diseases
Outbreaks of pharyngo-conjunctivitis, caused by adenovirus
are reported in association with swimming in contaminated pools
(1568). The implication of waterborne transmission of the
disease was based on epidemiologic evidence; no viruses were
obtained from the water.
Successful isolation of the causative virus demonstrated the
water transmission of coxsackie virus type A16 to children who
swam in lake water with relatively high fecal coliform counts.
InfectiveDose of Viruses
Virologists feel that one plaque-forming unit (pfu) - one
viral particle that grows in the laboratory media - constitutes
an infectious viral dose. However, there is a difference between
infection and disease (1366): the diseased person manifests
467
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a variety of symptoms and readily recognizes that he is sick;
an infected person has the material in his system, but does
not necessarily show symptoms of the disease. It has been
estimated that of every 100 to 1,000 people who are infected,
only one will manifest the clinical symptoms of disease. How-
ever, it is not quite as simple as these statistics suggest,
for an infected individual can serve as a carrier or source
within the community and transmit this disease to other people
(1366).
Table -170 shows the minimal infective doses of attenuated
polip virus for human hosts by oral routes. The infected rate
with 20 or more pfu was 100 percent; with 2 pfu, 67 percent
of the individuals was infected.
TABLE 170. MINIMAL INFECTIVE
POLIO VIRUSES FOR HUMAN HOSTS
DOSES OF ATTENUATED
BY ORAL ROUTES (1366)
Subject
Adults
Premature
Infants
Poll
(SM
Poli
(Fox
Virus
o virus Type I
Strain)
o virus Type III
Strain)
Dose
(pfu)
200
20
2
0.2
10
2.5
1
Carrier*
Rate
4/4
4/4
2/3
0/2
2/3
3/9
3/10
Infected
Percent
100
100
67
0
67
33
30
* Number of persons developed into carrier for the
virus/number of persons who had taken the virus orally.
It has been mentioned that infection with small amounts
of virus in water would probably immunize individuals rather
than produce disease. This may be substantiated by the fact that
sewage workers continually exposed to small amounts of infected
material had the lowest rate of absenteeism among all the occu-
pation groups studied (98).
An ad
waters is
made to fi
phages to
have been
coliforms
well as a
water, resi
viruses.
wastewater
equate biologi
not currently
nd better indi
human enteric
investigated (
and coliphage
yeast and two
st chlorinatio
This suggests
chlorination
cal indicator for viruses in various
available; however, efforts are being
cators. For example, ratios of coli-
viruses and the col iform-virus ratio
734, 1574). Also, a high degree of
occurring in water samples (693), as
acid-fast bacilli recovered from waste'
n at a level sufficient to inactivate
that they may be useful indicators of
efficiency (383).
470
-------
Infection From Microbial Aerosols
An investigation was made of the morbidity risk factors
from spray irrigation with treated wastewater (1320). It was
pointed out that no instances of disease have been reported from
spray irrigation with chlorinated secondary effluent. This is
not surprising. If aerosolized pathogens constituted a public
health risk from drift and spray of aerosolized particles
generated from sewage, the clinical risk would be greatest where
the concentration is greatest -- in the sewage works, near the
aerobic treatment unit. No evidence has been found that either
long-term or newly employed operators have diseases attributed to
aerosol ingestion. Indeed, some experts have suggested that the
morbidity rate of sewage plant operators is less than the
morbidity rate of the general public. Perhaps a more sensitive
indicator would be the health of adolescent school children
visiting a sewage plant for a science course field trip. A
letter from the National Science Teachers Association told us
that "from inquiries to the U.S. Public Health Service and the
Montgomery County (Maryland) Health Department, we have learned
of no reported illnesses to students following visits to sewage
treatment plants, nor could we find that any guidelines have be^en
developed or are in practice as precautions for such visits.
Also, the student tours director for the Washington Suburban
Sanitary Commission told us that no special precautions have been
observed in their tour program, nor did he know of any illnesses
to students following tours of that facility" (1320).
Many factors influence the survival of bacterial and
viral pathogens in the air. Aerosols remain viable and travel
greater distances with increased wind velocity, increased
relative humidity, lower temperatures, and darkness. Some
bacteria such as £_._ col i have been shown to have an extremely
short life-span in aerosol form (545, 1099, 1302, 1303, 1304).
Specific pathogenic bacteria of klebsiella form a large
capsule that apparently protects the organism from desication
in flight. All species of this genus are known pathogens of
the respiratory tract (1304).
Another pathogen of the respiratory tract, mycobacterium
species, has been known to cause infections associated with
contaminated water but not with aerosols (509).
A direct means of human infection by biological aerosols
is inhalation. The infectivity of an aerosol is further depen-
dent on the depth of respiratory penetration (1304). Biological
aerosols in the 2 to 5y size range are primarily captured in
the upper respiratory tract. These particles are removed by
bronchial cilia and may pass into the digestive tract through
the pharynx (2). If gastrointestinal pathogens are present
471
-------
in these aerosols, a certain degree of infection may result.
However, a much higher incidence of infection results when
respiratory pathogens are inhaled into the alvioli of the lung.
The greatest alveolar deposition occurs in the 1- to 2-u.
range and then decreases to a minimum at approximately 0.25u.
Belo.w 0.25y, alveolar deposition again increases due to
Brownian movement. Approximately 82 percent of 1.0 particles,
28 percent of 0.1 to 0.3y particles, and 51 percent of O.OSy
particles are deposited in the broncheoles or the alveoli.
This aspect of aerosol deposition becomes significant when viral
size particles (about 0.01 to O.ly ) are considered. Attention
must therefore be paid to viral deposition, with the possible
resultant infection (1304).
A summary of virus infections by the respiratory route
demonstrates that extremely low doses of virus can cause
infection in man (161, 1366). The tissue culture infective doses
(TCID5Q) cited ranged from 1.0 to 790.0 pfu. The number of
infectious virus particles necessary to initiate an infection
in man, as determined by antibody production or a disease state,
has been reported by Sorber et al. (1304). The study utilized
human volunteers who ha:, no detectable antibody levels against
the test viruses. It was observed that 28 TCID5Q of coxsackie
virus A-21 in small particle aerosols (0.3 to 2.5y) were
required for a 50 percent human infective dose (HIDso). Only
one TCIDcg of adenovirus Type IV was required for a HIDso when
generated in small particle aerosols. Both of these enteric
viruses required a higher TCIDso to give a respiratory tract
infection than did Reo virus strain NIH 1734, which required only
0.68 TCID5Q. The study emphasized the importance of droplet
size upon the nature of the clinical and dose response.
It is reasonable to postulate that, if disinfection of
sewage is not complete and the pathogenic organisms are
aerosolized, even very low numbers of these organisms may be
a public health hazard (1304). Unfortunately, there are
essentially no quantitative date that can be used to evaluate
the risk at the present time.
472
-------
SECTION III
REPORT BIBLIOGRAPHY
473
-------
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1056. Parker, M. and A.D. Hasler. Studies on the Distribution
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572
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1068. Pavoni, J.L. and D.J. Hagerty. Absorption of Pesticides by
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1078. Perspectives on the Control of Viral Hepatitis, Type B.
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1088. Pietz, R.I., J.R. Peterson, and C. Lue-Hing. Groundwater
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1111. Preliminary Assessment of Suspected Carcinogens in Drinking
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Health Eng., 1^:105-113, 1975.
1678. Tchobanoglous, G. and R. Eliassen. The Indirect Cycle
of Water Reuse. Water Wastes Eng., _6(2):35-41, February
1969.
1679. Thayer, S.E. and O.J. Sproul. Virus Inactivation in
Water-Softening Precipitation Processes. J. Am. Water
Works Assoc., 5^(8):1063-1074, August 1966.
630
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1680. Thiem, L.T. Removal of Mercury from Drinking Water
Using Powdered Activated Carbon. In: Proceedings pf
the 96th Annual Conference of the American Water Works
Association, June 20-25, 1976. pp. 17-3.
1681. Thiem, L.T. Removal of Mercury from Drinking Water
Using Powdered Activated Carbon. Water Sewage Works,
12_3(8):71, August 1976.
1682. UOP, Inc. Fluid Systems Division. Reverse Osmosis.
San Diego, California, 1977. 4p.
1683. Van Loon, J.C. Mercury Input to the Environment
Resulting from Products and Effluents from Municipal
Sewage Treatment Plants. Environ. Pollut., 7^:141-147,
1974.
1684. Water Purification Associates. Innovative Technology
Study Prepared for the National Commission on Water
Quality. August 1975.
1685. White, G.C. Disinfection: The Last Line of Defense for
Potable Water. J. Am. Water Works Assoc., 67(8):410-
413, August 1975.
1686. Wilkinson, L. Nitrogen Transformations in a Polluted
Estuary. Adv. Water Pollut. Res., 1962(3):405-422.
1687. Wozniak, D., M. Kievak, C. Cahoon, and R.H. Edgerton.
Water to Air Bacterial Transfer by Bursting Bubbles. J.
Environ. Eng. Div., Am. Soc. Civ. Eng., 102(EE3):567-
570, June 1976.
631
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SECTION IV
CURRENT RESEARCH
€32
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INTRODUCTION
In this section are listed research projects currently
being conducted, the results of which are not included in the
report text. Project titles, principal investigators, and
research locations are listed under relevant headings. This
information was primarily derived from an NTIS computer
search and an extensive mail survey (see Section II, Introduc-
tion) conducted in November of 1975.
EXISTING LITERATURE AND RESEARCH PRESENTLY UNDERWAY
PRIMARY TREATMENT
Research programs currently being conducted are concerned
primarily with dissolved air flotation and microstraining.
This work is being conducted by the following organizations:
Rex Chainbelt, Incorporated
Technical Center
Treatment of Combined Sewer Overflows Using New
Techniques of Screening and A1r Flotation
W. J. Katz (Principal Investigator)
Milwaukee, Wisconsin
FMC Corporation
Environmental Equipment Division
Study of Activated Sludge Separation by Dynamic Straining
A. H. Strom and J. E. Dumanowski (Principal Investigators)
Itasca, Illinois
Philadelphia Water Department
Microstraining Pilot Tests of Combined Sewers
C. F. Guarino and G. W. Carpenter (Principal Investigators)
Philadelphia, Pennsylvania
Metropolitan Sanitary District of Greater Chicago
Performance Analysis of 15 MGD Microstralner for Tertiary
Treatment
C. Lue-hing (Principal Investigator)
Chicago, Illinois
633
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Crane Company
Cochrane Division
Microstraining and Disinfection of Combined Sewer Overflows
VI. A. Keilbaugh (Principal Investigator)
Norristown, Pennsylvania
Fram Corporation
Feasibility Investigation of a Self-Cleaning Strainer
and Filter
S. S. Blecharczyk (Principal Investigator)
Providence, Rhode Island
American Process Equipment Corporation
Fabrication and Evaluation of an Ultrasonic Microstaining
System for Treating Sewage
R. Robert (Principal Investigator)
Hawthorne, California
Cornell, Howland, Hayes and Merryweather
Fine-Mesh Screening for Primary Treatment of Storm Water
O.verf low
Hernandez (Primary Investigator)
Corvallis, Oregon
SECONDARY TREATMENT: ACTIVATED SLUDGE PROCESS
Research programs currently being conducted concerning the
activated sludge processes are largely directed at the utiliza-
tion of the activated sludge process in tandem with tertial
processes. Current work is being conducted by the following
organizations:
U.S. Environmental Protection Agency
National Environmental Research Center
Nitrogen Removal by the Three Stage Activated Sludge
System and by a Single Stage Activated Sludge Process
D. F. Bishop (Principal Investigator)
Ci nci nnati, Ohio
University of Pittsburgh
Department of Civil Engineering
Aqueous Heavy Metal Removals by Biological Slimes
R. D. Neufeld (Principal Investigator)
Pittsburgh, Pennsylvania
Oklahoma State University
School of Civil Engineering
Metabolism of Components of Extended Aeration Activated
SIudge
A. F. Gaudy and P. Y. Yang (Principal Investigators)
Stillwater, Oklahoma
634
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University of New Hampshire
Department of Chemistry
Fate of Metal Ions During Treatment of Water Containing
Organics
0. H. Weber (Principal Investigator)
Durham, New Hampshire
Dallas City Water Utilities Department
Removal of Heavy Metals by Activated Sludge Processes
H. W. Wolf (Principal Investigator)
Dallas, Texas
Oklahoma State University
School of Civil Engineering
Biological Treatment of a Wastewater Containing Phenol
J. H. Sherrard (Principal Investigator)
Stillwater, Oklahoma
Southwest Research Institute
Department of Chemical Engineering
Health Implications of Activated Sludge Systems
D. E. Johnson and J. T. Goodwin (Principal Investigators)
San Antonio, Texas
University of Texas
Department of Civil Engineering
Application of Oxygen to Treat Waste from Military Field
Instal1ations
J. F. Malina (Principal Investigator)
Austin, Texas
U.S. Environmental Protection Agency
National Environmental Research Center
Identification of Organic and Inorganic Compounds in
Activated Sludge Treated Wastes
A. W. Garrison (Principal Investigator)
Corvallis, Oregon
Oklahoma State University
School of Engineering
Response of Completely Mixed Activated Sludge Systems to
Changes in the Environment
A. F. Gaudy (Principal Investigator)
Stillwater, Oklahoma
U.S. Army
Waterways Experiment Station
Effects of Intermittent Loading on an Activated Sludge
Treatment System
A. J. Green and J. L. Maloch (Principal Investigators)
V i c k s b u r g, Mississippi
635
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U.S. Environmental Protection Agency
National Environmental Research Center
Chlorinated Organics in Chlorine Waste Activated Sludge
A. W. Garrison (Principal Investigator)
Corvallis, Oregon
U.S. Department of Agriculture
Eastern Utilization Research Division
Recovery of Proteins from Lime-Sulfide Unhairing Effluents
W. F. Happich (Principal Investigator)
Wyndmoor, Pennsylvania
University of Texas
Department of Civil Engineering
Virus Removal 1n the Conventional Activated Sludge
Process
J. F. Malina and K. R. Ranganathan (Principal
Investigators)
Austin, Texas
FMC Corporation
Environmental Equipment Division
Activated Sludge Separation by Dynamic Straining
A. H. Strom and J. E. Dumanowski (Principal Investiga-
tors)
Itasca, Illinois
Rexnord, Incorporated
Industrial Waste Treatment by Activated Sludge
R. W. Agnew (Principal Investigator)
Milwaukee, Wisconsin
Koppers Company, Incorporated
Activated Sludge Treatment of Wood Preserving
Waste Water
X. P. Laskaris (Principal Investigator)
Carbondale, Illinois
State Department of Environmental Conservation
High Performance Bio-Treatment of Municipal Sewage
C. Beer (Principal Investigator)
Albany, New Yprk
Chino City Government
Reclamation of Wastewater by Controlled Biological
Kinetics
D. Feuerstein (Principal Investigator)
Chino, California
636
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U.S. Environmental Protection Agency
National Environmental Research Center
Installation of Instrumentation and Control Devices
for Three-Stage Activated Sludge
W. W. Schuk (Principal Investigator)
Cincinnati, Ohio
Wyoming City Government
Disinfection of Activated Sludge Effluent
J. A. Sheeran (Principal Investigator)
Grand Rapids, Michigan
U.S. District of Columbia Government
Department of Environmental Services
BOD Removal, Nitrification and Denitrification in
a Single Stage Activated Sludge System
A. B. Hals (Principal Investigator)
Washington, D.C.
U.S. Environmental Protection Agency
National Environmental Research Center
A Three-Stage Activated Sludge System for Removing
Virus and Heavy Metals
S. Roan (Principal Investigator)
C1ncinnati, Ohio
University of Connecticut
Department of Chemical Engineering
Addition of Powdered Activated Carbon to Activated
Sludge Reactors
D. W. Sundstrum and H. E. Kiel (Principal Investigators)
Storrs, Connecticut
University of Connecticut
Department of Agricultural Economics
Efficient Pricing for Urban Waste Water Ranovatlon
R. L. Leonard and R, Laak (Principal Investigators)
Storrs, Connecticut
University of California
Department of Chemical Engineering
Size of Bacterial Aggregations on Rates of growth
and Bio-Oxidation
A. P, Jackman (.Principal Investigator)
Davis, California
Beaunlt Fibers
Activated Sludge Treatment Qf Nylen Wastewtters
Using Enriched A1r
R. K. Priest (Principal Investigate^
Etowah, Tennessee
637
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Lehigh University
Center for Surfacing and Coating Research
Effect of Various Additives on the Improved
Dewatering of Activated Sludge
F. J. Micale (Principal Investigator)
Bethlehem, Pennsylvania
Purdue University
Joint Highway Research Project
Treatment of Sanitary Wastes at Interstate Rest Areas
J. E. Etzel and A. J. Steffen (Principal Investigators)
Lafayette, Indiana
U.S. Environmental Protection Agency
National Environmental Research Center
Determination of the Effects of Doses of Sludge on
the Activated Sludge- Process
B. V. Salotto (Principal Investigator)
Cincinnati, Ohio
York City Department of Water Resources
Demonstration of the Oxygen Aeration Process to
Upgrade Existing Waste Treatment Plants
W. Pressman (Principal Investigator)
New York, New York
Los Angeles County Sanitation District 2
Operation of Two-Stage Activated Sludge System
J. Gasser (Principal Investigator)
Los Angeles, California
Los Angeles Board of Public Works
Characterization of the Activated Sludge Process
at the Hyperion Treatment Plant
A. D. Leipzig (Principal Investigator)
Los Angeles, California
U.S. Environmental Protection Agency
National Environmental Research Center
Microscopic Examination of and Characterization of
Batch Flux Settling Properties on Activated Sludges
R. F. Lewis (Principal Investigator)
Cinri nnati , Ohio
U.S. Environmental Protection Agency
National Environmental Research Center
Investigate the Effectiveness of Process Control by
Computation
R. Smith (Principal Invetigator)
Cincinnati, Ohio
638
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U.S..Environmental Protection Agency
National Environmental Research Center
Identification of Pollutants in Petroleum Refinery
Waste Waters After Activated Sludge Treatment
L. H. Keith (Principal Investigator)
Corvallis, Oregon
Hydrotechnic Corporation
High Rate Deep Bed Filtration of Activated Sludge
Plant Effluent
P. J. Harvey (Principal Investigator)
New York, New York
Michigan State University
Institute of Water Research
The Characterization of Soluble Phosphorus Compounds
i-n Biological Waste Treatment Processes
F. M. Ditri (Principal Investigator)
East Lansing, Michigan
University of Puerto Rico
Department of Civil Engineering
Relationship Between BOD Removal and LAS Detergent
Removal
N. Tang (Principal Investigator)
Mayaguez, Puerto Rico
University of Kentucky
Department of Chemical Engineering
Process Control of Activated Sludge Treatment
R. I. Kermode and R. W. Brett (Principal Investigators)
Lexington, Kentucky
U.S. Army Plans and Studies Directorate
Emission of Viruses from Sewage Treatment Plant
Facili ties
C. J. Spendlove and P. A. Adams (.Principal Investigators)
Dugway Proving Ground
Dugway, Utah
University of Texas
Department of Civil Engineering
Hydrocarbons Emitted During Aeration of Refinery
Wastewater
J. 0. Ledbetter and J. W. Kim (Principal Investigators)
Austin, Texas
639
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University of Maine
Department of Civil Engineering
Adsorption as a Protective Mechanism for VJater-
Borne Viruses
0. J. Sproul (.Principal Investigator)
Orono, Maine
SECONDARY TREATMENT: TRICKLING FILTERS
Research programs currently being conducted are being
performed by the following organizations:
Georgia Institute of Technology
Environmental Resources Center
Bark as a Trick!ing-Filter Dewatering Media
for Pulp and Paper Mill Sludge
G. R. Lightsey (Principal Investigator)
Atlanta, Georgia
Georgia Institute of Technology
Department of C1v1l Engineering
Sanitary Landfill Leachate Treatment by Trickling
Filter
F. G. Pohland (Principal Investigator
Atlanta, Georgia
Harris Company Water Control and Improvement
Removal of BODs, Suspended Solids, Nitrogen, and
Pho'sphorous by Trickling Filter
N. 0. Swennes
Seabrook, Texas
U.S. Army Plans and Studies Directorate
Emission of Viruses from Sewage Treatment Plant
Facilities
C. 0. Spendlove and P. A. Adams CPHndpal Investigators)
Dugway, Utah
SECONDARY TREATMENT: AERATED LAGOONS
There 1s a significant amount of research presently
underway .which 1s directed towards Industrial waste application!
of aerated lagoons and upgrading of lagoon effluents through
tertiary treatment. Research 1s being conducted by the follow-
ing organizations:
640
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University of Arizona
Department of Civil Engineering
Tertiary Treatment of Aerated Lagoon Effluent by Soil
Filtration to Permit Reuse for Park and Playground
Irrigation
Tucson, Arizona
U.S. Environmental Protection Agency
National Environmental Research Center
Organic Pollutants in Refinery Wastewater Following
Aerated Lagoon Treatment
L. H. Keith (Principal Investigator)
Corvallis, Oregon
University of Texas
Department of Civil Engineering
Hydrocarbons Emitted During Aeration of Refinery
Wastewater
J. 0. Ledbetter and J. W. Kim (.Principal Investigators)
Austin, Texas
University of Washington
Department of Forest Products
Natural, Acidic, and Water Soluble Compounds Resulting
from Aerated Lagoon Treatment
B. F. Hruthfiord (Principal Investigator)
Seattle, Washington
Auburn University
Department of Agricultural Engineering
Pollutlonal Characteristics of Swine Waste following
Treatment in a Two-Stage, Anaerobic-Aerobic Lagoon
System
R. E. Hermanson and J. L. Koon (Principal Investigators)
Auburn, Alabama
Utah State University
Utah Center for Water Resources Research
Performance Evaluation of an Existing Lagoon
J. H. Reynolds and E. J. Middlebrooks (.Principal
Investigators)
Logan, Utah
Clemson University
Department of Horticulture
Treatment of Wastewaters from Food Processing Plants
by Aerated Lagoon
L. Vanbularicom and T. L. Senn (.Principal Investigators)
Clemson, South Carolina
641
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Crown Zellerbach Corporation
Coliform Organisms in a Full-Scale Aerated Stabilization
Basin
H. Amberg (Principal Investigator)
Camas, Washington
Kent Cheese Company
The Effectiveness of Aerated Lagoons for the Treatment
of Industrial Wastewater
F. R. Paul (Principal Investigator)
Mel rose Park, Illinois
University of Texas
Department of Civil Engineering
Hydrocarbons Emitted During Aeration of Refinery
Wastewater
J. 0. Ledbetter and J. W. Kim (.Principal Investigators)
Austin, Texas
University of Washington
Department of Forest Products
Natural, Acidic, and Water Soluble Compounds Resulting
from Aerated Lagoon Treatment
B. F. Hruthfiord (Principal Investigator)
Seattle, Washington
Auburn University
Department of Agricultural Engineering
Pollutional Characteristics of Swine Waste following
Treatment in a Two-Stage, Anaerobic-Aerobic Lagoon
System
R. E. Hermanson and J. L. Koon [Principal Investigators)
Auburn, Alabama
Utah State University
Utah Center for Water Resources Research
Performance Evaluation of an Existing Lagoon
0. H. Reynolds and E. J. Middlebrooks (.Principal
Investigators)
Logan, Utah
Clemson University
Department of Horticulture
Treatment of Wastewaters from Food Processing Plants
by Aerated Lagoon
L. Vanbularicom and T. L. Senn (.Principal Investigators)
Clemson, South Carolina
642
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Crown Zellerbach Corporation
Coliform Organisms in a Full-Scale Aerated Stabilization
Basin
H. Amberg (Principal Investigator)
Camas, Washington
Kent Cheese Company
The Effectiveness of Aerated Lagoons for the Treatment
of Industrial Wastewater
F. R. Paul (Principal Investigator)
Mel rose Park, Illinois
W. E. Reeves Packinghouse
The Suitability of Anaerobic-Aerobic Lagoons in
Meatpacker Waste Treatment Systems
W. E. Reeves (Principal Investigator)
Ada, Oklahoma
East Central State College
Department of Environmental Science
Aerated Aerobic Oxidation Pond Treatment of Packinghouse
Wastes
R. H. Ramsey (Principal Investigator)
Ada, Oklahoma
SECONDARY TREATMENT: ANAEROBIC LAGOONS
Research concerning anaerobic lagoons is currently being
conducted by the following organizations:
W. E. Reeves Packinghouse
Demonstration of the Suitability of an Anaerobic-
Aerobic Lagoon System for Treating Meat Packer
Wastes
W. E. Reeves (Principal Investigator)
Ada, Oklahoma
University of Georgia
Department of Agricultural Engineering
Design and Operation Criteria for an Anaerobic Lagoon
for Swine Waste Treatment
R. E. Smith (Principal Investigator)
Athens, Georgia
Auburn University
Department of Agricultural Engineering
A Swine Waste Treatment System Consisting of a Series
Connected Anaerobic Lagoon, Aerated Lagoon or Oxidation
Ditch, and Final Aerobic Lagoon
R. E. Hermanson and K. L. Koon (Principal Investigators)
643
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Utah State University
Utah Center for Water Resources Research
Performance Evaluation of an Existing Lagoon
J. H. Reynolds and E. 0. Middlebrooks (Principal Investi-
gators)
Logan, Utah
SECONDARY TREATMENT: PONDING
Several current research projects concerning the removal
of contaminants by lagooning procedures are listed below:
University of Kentucky
Department of Civil Engineering
Tertiary Treatment Using Oxidation Ponds
R. A. Lauderdale (Principal Investigator)
Lexington, Kentucky
Asian Institute of Technology
Nitrogen Uptake through the Regrowth of Algae in Secon-
dary Ponds
M. G. McGarry and S. Pinkayan (.Principal Investigators)
Bangkok, Thailand
University of Texas
Department of Civil Engineering
The Presence of Pathogenic Organisms Including Virus
and the Susceptibility of the Effluent in Stabilization
Ponds to Chemical Disinfection
J. F. Malina (Principal Investigator)
Austin, Texas
University of North Carolina
Department of Environmental Sciences and Engineering
Suspended Solids Removal fn Settling Ponds
J. C. Brown (Principal Investigator]
Chapel Hill, North Carolina
Gorgas Memorial Institute
Stabilization Pond Operation in Tropical Areas
M. D. Young and K. W. Langley (.Principal Investigators)
Washington, D. C.
U.S. Environmental Protection Agency
National Environmental Research Center
Organic Pollutant Discharge in industrial Wastewater
Following Lagoon Treatment
L. H. Keith (Principal Investigator)
Corvallis, Oregon
644
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TERTIARY TREATMENT: FILTRATION
The removals of various contaminants have been the
subject of several research projects because of the increasing
interest in filtration as a process for tertial wastewater
treatment. Organizations performing this research include the
following:
Dallas City Water Utilities Department
Heavy Metals Removal Using a Combination of Processes
Including Dual Media Filtration
H. W. Wolf (Principal Investigator)
Dallas, Texas
Colorado State University
Agricultural Experiment Station
Reduction of COD and BOD from Animal Feed Lot
Runoff by Ultrafiltration
S. M. Morrison and R. P. Martin (Principal Investigators)
Fort Collins, Colorado
University of Illinois
Department of Civil Engineering
The Role of Polymers in the Removal of Viruses by
Filtration
R. S. EnglebrecHt and D. Amirhor (.Principal Investigators)
Urbana, Illinois
Water Pollution Research Laboratory
Department of the Environment
Fundamentals of Biological Filtration Mechanisms
Stevenage, England, United Kingdom
University of Wyoming
Department of C1v1l and Architectural Engineering
The Effectiveness of Sand Filters for Removal of
Colloidal Manganese Oxides when Selected Cations
are Used as Chemical Conditioners
S. R, Jenkins (Principal Investigator)
Laramle, Wyoming
U.S. Environmental Protection Agtney
National Environmental Reitareh Canter
Identification of Organic and Inorganic Compounds
Remaining 1n Physical-Chemical Treated Municipal
Wastes
A. W. Garrison (Principal Investigator)
CorvalUs, Oregon
645
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U.S. Department of Agriculture
Western Regional Research Center
Evaluation of the Uni-Flow Filter System for the
Separation of Solids from Food Processing Waters
and Waste Effluents
K. Popper (Principal Investigator)
Berkeley, California
Asian Institute of Technology
Filtration Processes in Tertiary Treatment Under
Tropical Conditions
M. G. McGarry and S. Pinkayan (.Principal Investigators)
Bangkok, Thailand
Minneapolis-St. Paul Sewer Board
Physical-Chemical Treatment Evaluation Including
Multi-Media Filtration
R. M. Susag (Principal Investigator)
St. Paul , Minnesota
Woods Hole Oceanographic Institute
Department of Biology
Virus and Bacteria Removal from Secondary Effluent by
Photoinactivation and Sand Fil tering
B. H. Ketchum (Principal Investigator)
Woods Hole, Massachusetts
Hatfield Township Municipal Authority
BODs, COD, Suspended Solids and Phosphorus Removal
by Filtration
T. Greenland (Principal Investigator)
Colmar, Pennsylvania
.U.S. Environmental Protection Agency
National Environmental Research Center
Removal of Toxic Metals by Filtration
S. A. Hannah (Principal Investigator)
Cincinnati, Ohio
University of Delaware
Department of Biological Sciences
The Use of Blue-Green Algal Viruses as Indicators of
the Efficiency of Water Treatment in Elimination
of Human Enteric Viruses
D. S. Herson and J. Nobleharvey (.Principal Investig.ators)
Newark, Delaware
University of North Carolina
Department of Environmental Sciences and Engineering
Tertiary Solids Removal by Filtration
J. C. Brown (Principal Investigator)
Chapel Hill, North Carolina
646
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J. P. Stevens and Company, Incorporated
BODs and Suspended Solids Removal by Filtration
W. R. Hogue (Principal Investigator)
Greensboro, North Carolina
Roy F. Weston, Incorporated
Treatment of Storm Runoff by Filtration
R. Weston (Principal Investigator)
Westchester, Pennsylvania
Fram Corporation
Feasibility Investigation of Self-Cleaning Strainer
and Filter
S. S. Blecharczyk (.Principal Investigator)
Providence, Rhode Island
U.S. Environmental Protection Agency
National Environemntal Research Center
Chlorination and Filtration of Effluent from
Denitrification through Dual or Tri Media Filters
D. F. Bishop (Principal Investigator)
Cincinnati, Ohio
American University
Department of Chemistry
Identification of Trace Organics Following Lime
Clarification, Filtration and Carbon Adsorption
M. H. Aldridge and T. A. Pressley (.Principal
Investigators)
Washington, D.C.
State Department of Iron Range Resources
Peat and Peat Soil Mixtures as Filter Media
R. Scuffy (Principal Investigator)
St. Paul, Minnesota
Auburn University
Department of Civil Engineering
The Effectiveness of Sand Filters for the Removal
of Specific Viruses from Water Using Selected
Cations as Filter Aids
S. R. Jenkins (Principal Investigator)
Auburn, Alabama
647
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University of Maine
Department of Civil Engineering
Controlled Filtration Experiments Using Uniform
Sand Columns and Chemically Conditioned Influent
Suspensions of Latex Monodispersions and
Polydispersions, Secondary Effluents and Virus
Suspensions
M. M. Ghosh and W. F. Brutsaert (Principal Investigators)
Orono, Maine
TERTIARY TREATMENT: ADSORPTION
The removal by carbon adsorption of certain groups of
contaminants has been the topic of many research projects.
This interest arises from the fact that carbon adsorption
offers promise in the tertiary removal of troublesome con-
taminants (i.e., trace organics) in municipal wastewater.
Organizations performing this research include the following:
University of Texas
Department of Civil Engineering
Removal of Mercury by a Combination of Chelation and
Activated Carbon Adsorption
M. J. Humenick and R. Austin (Principal Investigators)
Austin, Texas
University of New South Wales
School of Chemical Engineering
Treatment of Refinery Wastes by Carbon Adsorption
K. A. Buckle and C. 0. Fell (Principal Investigators)
Sydney, New South Wales, Australia
Dallas City Water Utilities Department
Removal of Heavy Metals Using a Combination of Treatment
Processes Including Carbon Adsorption
H. W. Wolf (Principal Investigator)
Dallas, Texas
U.S. Environmental Protection Agency
National Environmental Research Center
The Fate of As, Ba, Cd, Se, Cr, and Hg During Activated
Carbon Treatment
0. M. Symons (Principal Investigator)
Cincinnati, Ohio
U.S. Environmental Protection Agency
National Environmental Research Center
Identification of Trace Organic and Inorganic Compounds
Remaining in Physical-Chemical Treated Municipal
Wastes
A. W. Garrison (Principal Investigator)
Corvallis, Oregon
648
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University of Illinois
Department of Civil Engineering
Removal of Organics from Military Waste Streams Using
Ozone and Activated Carbon
E. S. Chain (Principal Investigator)
llvhana Tll^nn-Jc
t. o. unain \.m
Urbana, Illinois
Asian Institute of Technology
Activated Carbon Adsorption of Color
M. 6. McGarry and S. Pinkayan (.Principal Investigators)
Bangkok, Thailand
Mlnneapol1s-St. Paul Sewer Board
Suspended Solids, BODs, Ammonia, and Phosphate Removal
by Carbon Adsorption
R. H. Susag (Principal Investigator)
St. Paul , Minnesota
U.S. Environmental Protection Agency
National Environmental Research Center
Process Modifications Using Activated Carbon Adsorption
S. A. Hannah (Principal Investigator)
Cincinnati, Ohio
U.S. Environmental Protection Agency
National Environmental Research Center
Removal, of Synthetic Organic Compounds from Wastewater
by Activated Carbon
R. A. Dobbs (Principal Investigator)
Cincinnati, Ohio
InfUco Fuller Company
Activated Carbon Treatment in Slurry Clarifiers
C. F. Garland (Principal Investigator)
Tucson, Arizona
American University
Department of Chemistry
Characterization of Trace Oranics in Wastewater
Following Carbon Adsorption
M. M. Aldridge and T. A. Pressley (Principal
Investigators)
Washington, D.C.
University of Connecticut
Department of Chemical Engineering
The Addition of Powdered Activated Carbon to Activated
Sludge Reactors
D. E. Sundstrom and H. E. Klei (Principal Investigators)
Storrs, Connecticut
649
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TERTIARY TREATMENT: CHEMICAL TREATMENT
A considerable amount ,of research is currently being
performed concerning the removal of the various public health
impairing contaminants by chemical treatment processes. The
organizations conducting this research include the following:
Life Systems, Incorporated
Use of the Electrochemical Process to Disinfect Water
and Wastewater in Reuse Systems
R. A. Wynveen (.Principal Investigator)
Cleveland, Ohio
University of Illinois
Department of Civil Engineering
Coagulation of Wastewaters Using Fly Ash
J. T. O'Connor and J. H. Gulledge (.Principal Investigators)
Urbana, Illinois
Water Pollution Research Laboratory
Physico-Chemical Processes to Remove Ammonia, Phosphate,
and Organic Matter from Sewage Effluent
Department of the Environment
Stevenage, England, United Kingdom
U.S. Environmental Protection Agency
National Environmental Research Center
Study of Treatment Processes for the Removal of Trace
Metals and Nitrates
J. M. Symons (Principal Investigator)
Cincinnati, Ohio
U.S. Department of the Interior
Metallurgy Research Center
Treatment of Metallurgical Wastes by Chemical Coagulation
A. A. Cochran and L. C. George (Principal Investigators)
Rolla, Missouri
U.S. Environmental Protection Agency
National Environmental Rsearch Center
Identification of Pollutants in Physical-Chemical
Treated Wastes
A. W. Garrison (Principal Investigator)
Corvallis, Oregon
Northeastern University
Department of Civil Engineering
Effects of Interactions of Chemicals for Water Treatment
0. 0. Cochrane and W. Glover (.Principal Investigators)
Boston, Massachusetts
650
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Rex Chainbelt, Incorporated
Technical Center
Chemical Oxidation in the Treatment of Combined Sewer
Overflows
W. J. Katz (Principal Investigator)
Milwaukee, Wisconsin
U.S. National Aeronautics and Space Administration
Urban Systems Project Office
Chemical Coagulation for the Removal of Suspended Solids
J. Poradek (Principal Investigator)
Houston, Texas
Minneapolis-St. Paul Sewer Board
Physical-Chemical Treatment Plant Evaluation
R. H. Susag (.Principal Investigator)
St. Paul, Minnesota
Fairfax County Department of Public Works
Reduction of BODs, Nitrogen, Phosphorus and Suspended
Solids by Chemical Treatment
J. E. Sunday (Principal Investigator)
Fairfax, Virginia
U.S. Environmental Protection Agency
National Environmental Research Center
Physical-Chemical Processes to Remove Potentially
Hazardous Compounds from Wastewater
R. A. Dobbs (Principal Investigator)
Cincinnati, Ohio
U.S. Environmental Protection Agency
National Environmental Research Center
Removal of Toxic Metals by Physical-Chemical Treatment
S. A. Hannah (Principal Investigator)
Cincinnati, Ohio
University of Delaware
Department of Biological Sciences
The Use of Blue-Green Algal Viruses as Indicators of
the Efficiency of Coagulation in Elimination of Human
Enteric Viruses
D. S. Herson and J. Nobleharvey (Principal Investigators)
Newark, Delaware
Roy F. Weston, Incorporated
Treatment of Urban Storm Runoff by Coagulation
R. Weston (PrinicipaJ Investigator)
West Chester, Pennsylvania
651
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Grumman Aerospace Corporation
Chemical Coagulation in the Treatment and Recovery of
Fluoride Industrial Wastes
C. Staebler (Principal Investigator)
Bethpage, New York
U.S. Environmental Protection Agency
National Environmental Research Center
Analysis of Organic Pollutants in Industrial Wastewater
Following Chemical/Biological Treatment
L. H. Keith (Principal Investigator)
Corvallis, Oregon
Dallas City Water Utilities Department
Removal of Heavy Metals by Chemical Treatment Processes
H. W. Wolf (Principal Investigator)
Dallas, Texas
American University
Department of Chemistry
Identification of Trace Organics in Physical-Chemical
Treatment Effluents
M. H. Aldridge and T. A. Pressley (Principal Investi-
gators)
Washington, D.C.
University of Maine
Department of Chemical Engineering
Chemical and/or Chemico-Mechanical Modification of
Sludges
E. G. Bobalek and R. E. Durst (.Principal Investigators)
Orono, Maine
Iowa State University
Department of Civil Engineering
Chemical Treatment for Phosphorus Removals
E. R. Baumann and C. S. Oulman (Principal Investigators)
Ames, Iowa
New York State Agricultural Experiment Station
Physical-Chemical Treatment of Refractory Food Processing
Liquid Wastes
R. H. Walter (Principal Investigator)
Geneva, New York
R.A.I. Research Corporation
Technical and Economic Feasibility Study of Electro-
chemical O'xidation of Whey
S. B. Tuwiner (Principal Investigator)
Long Island City, New York
652
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Aerojet General Corporation
Department of Treatment Systems •
Development of Treatment Process for Chlorinated
Hydrocarbon Pesticide Manufacturing and Processing
Wastes
K. H. Sweeny (Principal Investigator)
El Monte, California
University of Rhode Island
Department of Civil and Environmental Engineering
The Electrochemical Process for Nutrient Removal
C. P. Poon (Principal Investigator)
Kingston, Rhode Island
San Antonio Department of Public Works
Demonstration of Lime Coagulation for Removal of Virus
from Municipal Sewage
H. C. Norris (.Principal Investigator)
San Antonio, Texas
U.S. District of Columbia Government
Department of Environmental Services
Stack Gas Analysis Studies for Air Pollution Control
from Incineration of Wastewater Sludge
A. B. Hais (Principal Investigator)
Washington, D.C.
TERTIARY TREATMENT: ION EXCHANGE
Several research programs are currently being conducted
in regards to the application of ion exchange in municipal
wastewater treatment. This research is being performed by
the following organizations:
U.S. Department of the Interior
Metallurgy Research Center
Treatment of Metallurgical Wastes Using Ion Exchange
A. A. Cochran and L. C. George (Principal Investigators)
Roll a, Missouri
U.S. Department of Agriculture
Western Regional Research Center
Separation of Liquids from Solids in Food Processing
Wastes Using Ion Exchange
K. Popper (Principal Investigator)
Berkeley, California
Grumman Aerospace Corporation
Treatment and Recovery of Fluoride Industrial Wastes
Using Ion Exchange
C. Staebler (Principal Investigator)
Bethpage, New York
653
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Louis Koenig Research
Operations Research for Advanced Waste Treatment Process
Including Ion Exchange
L. Koenig (Principal Investigator)
San Antonio, Texas
Minneapolis-St. Paul Sewer Board
Suspended Solids, 8005, Ammonia, and Phosphate Removal
by Ion Exchange
R. H. Susag (Principal Investigator)
St. Paul, Minnesota
TERTIARY TREATMENT: NITRIFICATION-DENITRIFICATION
The following organizations are currently conducting
research programs on this subject:
Hatfield Township Municipal Authority
Analysis of an Integrated Series of Unit Processes
Including Biological Nitrification
T. Greenlund (Principal Investigator)
Colmar, Pennsylvania
Harris Company Water Control and Improvement
Suspended Growth Nitrification and Column Denitrification
in Trickling Filters
N. 0. Swennes (Principal Investigator)
Seabrook, Texas
U.S. Environmental Protection Agency
National Environmental Research Center
Nitrification and Denitrification by a Single Stage
Activated Sludge Process
D. F. Bishop (Principal Investigator)
Ci ncinnati , Ohio
U.S. Environmental Protection AGency
National Environmental Research Center
Staged Nitrification-Denitrification System for
Removing Virus and Heavy Metals
S. Roan (Principal Investigator)
Cincinnati, Ohio
U.S. District of Columbia Government
Department of Environmental Services
Nitrification and Denitrification by a Single Stage
Activated Sludge System
A. B. Hais (Principal Investigator)
Washington, D.C.
654
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DISINFECTION: CHLORINATION
Research is being performed by the following organizations
Holifield National Laboratory
Environmental Sciences Division
Chlorinated Organic Compounds Present in Natural Waters
C. W. Gehrs and W. W. Pitt (Principal Investigators)
Oak Ridge, Tennessee
Dallas City Water Utilities Department
Removal of Heavy Metals by Chlorination
H. W. Wolf (Principal Investigator)
Dalla-s, Texas
U.S. Environmental Protection Agency
National Environmental Research Center
Identification of Chlorinated Organics in Chlorinated
Waste Activated Sludge
A. W. Garrison (.Principal Investigator)
Corvallis, Oregon
Northeastern University
Department of Civil Engineering
Effects of Interactions of Chemicals for Water Treatment
J. J. Cochrane and W. Glover (Principal Investigators)
Boston, Massachusetts
University of Tennessee
Farm Electrification Research Branch
Tests of Chlorinators on Water from Typical Farm Sources
and on Septic Tank Effluent
R. B. Stone (Principal Investigator)
Knoxville, Tennessee
University of Hawaii
Department of Public Health Science
Characterization of Refractory Organics of Possible
Carcinogenic Significance in Recycled Wastewater
N. C. Burbank and R. E. Green (Principal Investigators)
Honolulu, Hawaii
Asian Institute of Technology
Chlorination Processes as Applied to Tertiary Treatment
for the Reclamation of Drinking Water from Sewage
M. G. McGarry and S. Pinkayan (Principal Investigators)
Bangkok, Thailand
655
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Koppers Company, Incorporated
Pre- and Post-Chlorination
X. P. Laskaris (Prinicipal Investigator)
Carbondale, Illinois
Philadelphia Water Department
Chlorination Treatment of Combined Sewer Overflow
C. F. Guarino (Principal Investigator)
Philadelphia, Pennsylvania
Minneapolis-St. Paul Sewer Board
Evaluation of Chlorination Treatment for Disinfection
R. H. Susag (Principal Investigator)
St. Paul , Minnesota
U.S. Environmental Protection Agency
National Environmental Research Center
Bactericidal Effect of Various Combinations of Gamma
Radiation and Chloramine on Aquaeous Suspension of
Escherichia coli
A. D. Venosa (Principal Investigator)
Cincinnati, Ohio
Fairfax County Department of Public Works
Transportable Advanced Wastewater Treatment Plant for
Interim Use
J. E. Sunday (Principal Investigator)
Fairfax, Virginia
Wyoming City Government
Ozonation and Chlorination with Dechlorination of
Chlorinated Effluent
J. A. Sheeran (Principal Investigator)
Grand Rapids, Michigan
University of Delaware
Department of Biological Sciences
The Use of Blue-Green Algae Viruses as Indicators of the
Efficiency of Water Treatment on Elimination of Human
Enteric Viruses
D. S. Herson and J. Nobleharvey (Principal Investigators)
Newark, Delaware
U.S. Environmental Protection Agency
National Environmental Research Center
Chlorination and Filtration of Effluent from Denitrifica-
tion
D. F. Bishop (Principal Investigator)
Cincinnati, Ohio
656
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U.S. Environmental Protection Agency
National Environmental Research Center
Use of the Membrane Filter for Chlorinated Effluents
R. A. Greene (Principal Investigator)
Cincinnati, Ohio
Dallas City Water Utilities Department
Removal of Heavy Metals by Chlorination
H. W. Wolf (.Principal Investigator)
Dallas, Texas
Dow Chemical Company
Environmental Research Laboratory
Ultraviolet Chlorination of Organic Acids in Waste Brines
R. F. Wukasch (Principal Investigator)
University of Cincinnati
Department of Civil and Environmental Engineering
Inactivation of Viruses in Wastewater by Chlorine and
Chlorine Compounds
P. V. Scarpino (Principal Investigator)
Cincinnati, Ohio
University of Minnesota
Department of Chemistry
Chlorination and Ozonation Products of Municipal Sewage
and their Environmental Impact
R. M. Carlson (.Principal Investigator)
Minneapolis, Minnesota
University of Hawaii
Department of Environmental Health
Use of Bromine Chloride as a Viricide in Hawaii
N. C. Burbank and P. C. Loh (.Principal Investigators)
Honolulu, Hawaii
University of Illinois
Department of Civil Engineering
New Microbial Indicator of Wastewater Chlorination
Efficiency
R. S. Engelbrecht (Principal Investigator)
Urbana, Illinois
University of Connecticut
Department of Biology
Effects of Chlorine Treatment on Organic Molecules
R. P. Collins (.Principal Investigator)
Storrs, Connecticut
656a
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University of Maryland
Department of Agricultural Engineering
Chlorination of Runoff from Livestock Operations as a
Means to Improve the Bacteriological Quality of the
Effluent
J. A. Merkel CPrincipal Investigator}
College Park, Maryland
U.S. Environmental Protection Agency
National Environmental Research Center
The Fate of a Simulated Marine Environment of Chlorinated
Compounds Produced by Wastewater Chlorination
M. A. Horton (.Principal Investigator)
Corvallis, Oregon
DISINFECTION: OZONATION
Recent evidence suggesting that chlorinated effluents
adversely affect aquatic life has increased the research
interest in the possibilities of ozonation. Research is
presently being conducted by the following organizations:
University of Louisville
Department of Biology
Enteric Virus Survival in Package Plants and the
Upgrading of the Small Treatment Plants Using
Ozone
L. S. Cronholm and J. L. Pavoni (.Principal Investigators)
Louisville, Kentucky
University of Tennessee
Farm Electrification Research Branch
Ozone Generators for Purification of Farm Water
Supplies
R. B. Stone (Prinicipal Investigator)
Knoxville, Tennessee
University of Hawaii
Department of Public Health Science
Characterization of Refractory Organics of Possible
Carcinogenic Significance in Recycled Wastewaters
N. C. Burbank and R. E. Green (Principal Investigators)
Honolulu, Hawaii
Philadelphia Water Department
Ozonation Applied to the Treatment of Combined Sewer
Overflow
C. F. Guarino (Principal Investigator)
Philadelphia, Pennsylvania
657
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Wyoming City Government
Ozonation and Chlorination with Dechlorination of
Chlorinated Effluent
J. A. Sheeran (Principal Investigator)
Grand Rapids, Michigan
University of Illinois
Department of Civil Engineering
Virus Inactivation by Ozone
J. T. O'Connor and T. R. Begley (Principal.' Investigators)
Urbana, Illinois
Case Western Reserve University
Department of Chemical Engineering
Ozone Applications for the Treatment of PUlp and
Paper Mill Effluents
P. B. Melnyk (Principal. Investigator)
Cleveland, Ohio
University of Vermont
Department of Biology
The Effectiveness of Ozone in the Oxidation of Lipids
(Fats) in Sewage Effluent Water
T. Sproston and J. J. Stoveken (Principal Investigators)
Burlington, Vermont
Montana State University
Department of Chemistry
An Evaluation of Tertiary Water Treatment Via Ozonation
W. L. Waters and A. Rollin (Principal Investigators)
Bozeman, Montana
University of Illinois
Department of Civil Engineering
Removal of Organics Using Ozone
E. S. Chain (Prinicipal Investigator)
Urbana, Illinois
Westgate Research Corporation
U V - Ozone Water Oxidation/Sterilization Process
0. D. Zeff (.Principal Investigator)
Venice, California
Aerojet General Corporation
Department of Treatment Systems
Development of Treatment Process for Chlorinated
Hydrocarbon Pesticide Manufacturing and
Processing Wastes
K. H. Sweeney (Principal Investigator)
El Monte, California
658
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DISINFECTION: RADIATION TREATMENT
Research into the effect of radiation on any of the
public health impairing contaminants is being conducted by the
following organizations:
University of Hawaii
Department of Public Health Science
Characterization of Refractory Organics of Possible
Carcinogenic Significance in Recycled Wastewater
N. C. Burbank and R. E. Green (.Principal Investigators)
Honolulu, Hawaii
U.S. Environmental Protection Agency
National Environmental Research Center
Bactericidal Effect of Various Combinations of Gamma
Radiation and Chloramine on Aqueous Suspension of
Escherichia coli
A. D. Venosa (Principal Investigator)
Cincinnati, Ohio
U.S. Army
Engineering Research and Development Laboratories
Radiation Treatment of Wastewater
A. J. Vandenberg (Principal Investigator)
Fort Belvoir, Virginia
University of Tennessee
Farm Electrification Research Branch
Ultraviolet Irradiation for Purification of Farm Water
Supplies
R. B. Stone (Principal Investigator)
Knoxville, Tennessee
Florida Institute of Technology
Department of Science Education
Radiation Treatment of Waste Water for Destruction of
Viruses and Bacteria
D. D. Woodbridge and W. R. Garrett CPrincipal Investigators)
Melbourne, Florida
Massachusetts Institute of Technology
Department of Electrical Engineering
Wastewater Treatment With High Energy Electrons
J. G. Trump and K. A. Wright (Principal Investigators)
Cambridge, Massachusetts
THICKENING AND DEWATERING: GRAVITY SLUDGE THICKENER
Ongoing research in the field of gravity thickening of
sewage sludge is being conducted by the following organization:
659
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U.S. District of Columbia Government
Department of Environmental Services
Thickening of Wastewater Sludge
A. B. Hais (Principal Investigator)
Washington, D.C.
THICKENING AND DEWATERING: VACUUM FILTERS
Research is currently being conducted in the field of
vacuum filtration of sewage sludge by:
U.S. District of Columbia Government
Department of Environmental Services
Vacuum Filtration of Wastewater Sludges
A. B. Hais (Principal Investigator)
Washington, D.C.
SLUDGE STABILIZATION: ANAEROBIC DIGESTION
Research projects presently being conducted with regard
to anaerobic digestion are the following:
Georgia Agricultural Experiment Station
Digestion by Anaerobic Systems of Effluents from
Vegetable Processing Operations
W. A. Bough and A. L. Shewfelt (Principal Investigators)
Griffin, Georgia
Dartmouth College
Department of Engineering Science
Anaerobic Digestion and Membrane Separation for the
Treatment of Domestic Sewage
H. E. Grethlein (Principal Investigator)
Hanover, New Hampshire
University of Southern California
Department of Engineering
The Effects of Alkalinity on Anaerobic Digestion
of Primary Effluent
K. Chen and A. Sycip (Principal Investigators)
Los Angeles, California
SLUDGE STABILIZATION: AEROBIC DIGESTION
Ongoing research in the field of aerobic digestion is
being conducted by the following organizations:
660
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Georgia Institute of Technology
Department of Applied Biology
Production and Dispersal of Pathogenic Bacterial and
Viral Aerosols by Aeration of Contaminated Waters
R. King and T. W. Kethley (Principal Investigators)
Atlanta, Georgia
Georgia Agricultural Experiment Station
Digestion by Aerobic Systems of Effluents from
Vegetable Processing Operations
W. A. Bough and A. L. Shewfelt (Principal Investigators)
Griffin, Georgia
SLUDGE STABILIZATION: CHLORINATION
Research projects are currently being conducted in the
field of chlorination of sewage sludge by the following
organizations:
University of Hawaii
Department of Public Health Science
Characterization of Refractory Organics of Possible
Carcinogenic Significance in Recycled Wastewater
N. C. Burbank and R. E. Green (Principal Investigators)
Honolulu, Hawaii
State Department of Environmental Conservation
High Pressure Chlorination Treatment of Primary
Sludge
C. Beer (Principal Investigator)
Albany, New York
University of Massachusetts
Department of Civil Engineering
Sludge Stabilization by High-Dosage Chlorination
T. H. Feng (Principal Investigator)
Amherst, Massachusetts
SLUDGE STABILIZATION: LIME TREATMENT
Research projects are presently being conducted in the
field of lime treatment of sewage sludges by the following
organization:
FMC Corporation
Process to Remove Carbonaceous, Nitrogenous, and
Phosphorous Materials from Anaerobic Digester
Supernatant and Related Process Streams
H. A. Oldenkamp (Principal Investigator)
Santa Clara, California
661
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SLUDGE STABILIZATION: HEAT TREATMENT
Research is currently being conducted with regard to
heat treatment by the following organizations:
U.S. Environmental Protection Agency
National Environmental Research Center
Treatment of Supernatants from Heat Treatment of
Sludge
B. V. Salotto (Principal Investigator)
Cincinnati, Ohio
FMC Corporation
Process to Remove Carbonaceous, Nitrogenous, and
Phosphorous Materials from Anaerobic Digester
Supernatant and Related Process Streams
H. A. Oldenkamp (.Principal Investigator)
Santa Clara, California
University of Texas
Department of Civ4! Engineering
Inactivation of Enteric Viruses and Bacteria During
the Heat Treatment of Sludges
J. F. Malina and R. Cain (Principal Investigators)
Austin, Texas
SLUDGE STABILIZATION: WET AIR OXIDATION
Research projects are currently being conducted in the
field of wet air oxidation by the following organizations:
University of Delaware
Department of Chemical Engineering
Wet and Catalytic Oxidation of Suspended and
Dissolved Wastes
B. E. Anshus and J. R. Katzer (Principal Investigators)
Newark, Delaware
Rose Hulman Institute of Technology
Department of Environmental Engineering
The Influence of Wet-Air Oxidation on the Nitrogen,
Phosphorus, Heavy Metal Content and Attachment in
Domestic Sewage Sludge
E. H. Curtis and L. E. Sommers (Principal Investigators)
Terre Haute, Indiana
662
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FINAL DISPOSAL: INCINERATION
Ongoing research in the field of incineration is being
conducted by the following organizations:
University of Delaware
Department of Civil Engineering
Gravity Thickening of Sludges as a Batch Process
R. I. Dick and C. Tien (Principal Investigators)
Newark, Delaware
U.S. District of Columbia Government
Department of Environmental Services
Stack Gas Analysis Studies for Air Pollution Control
from Incineration of Wastewater Sludges
A. B. Hais (.Principal Investigator)
Washington, D.C.
FINAL DISPOSAL: SANITARY LANDFILL
The migration of public health imparing contaminants
as a result of sewage sludge burial in landfills is only
beginning to be researched and documented. The following
organizations are presently performing contract research work:
SCS Engineers, Inc.
Monitoring and Environmental Impact Evaluation of
Sewage Sludge Disposal in Sanitary Landfills
R. J. Lofy and R. P. Stearns (.Principal Investigators)
Long Beach, California
Georgia Institute of Technology
Department of Civil Engineering
Sanitary Landfill Stabilization with Leachate Recycle
F. G. Pohland (Principal Investigator)
Atlanta, Georgia
FINAL DISPOSAL: LAND RECLAMATION
Present research projects identified that are relevant
to land reclamation are being conducted by the following
organizations:
Metropolitan Sanitary District of Greater Chicago
Agricultural Benefits and Environmental Changes
Resulting from the Use of Digested Sludge on Field
Crops
D. T. Lordi (Principal Investigator)
Chicago, Illinois
663
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University of Texas
Virus Survival in Soils Injected with Municipal Waste-
water Treatment Residuals
B. P. Sagik (Principal Investigator)
San Antonio, Texas
Florida Institute of Technology
Radiation Treatment of Wastewater for Land Use
D. D. Woodbridge, W. R. Garrett (Principal Investigators)
Melbourne, Florida
Pennsylvania State University
Effects of Spray Irrigation of Municipal Wastewater on
the Rate and Total Accumulation of Heavy Metals
W. E. Sopper (Principal Investigator)
University Park, Pennsylvania
Purdue University
Utilization and Disposal of Municipal, Industrial, and
Agricultural Processing Wastes on Land
L. E. Sommer (Principal Investigator)
Lafayette, Indiana
University of Wisconsin
Utilization and Disposal of Municipal, Industrial, and
Agricultural Processing Wastes on Land
D. Keeney (Principal Investigator)
Madison, Wisconsin
U. S. Army
Engineer Power Group
Radiation Treatment of Wastewater for Land Use
A. J. Vandenberg (Principal Investigator)
Fort Belvoir, Virginia
ATMOSPHERIC PATHWAYS
Research presently underway on the generation,, migration,
and/or health effects associated with aerosols from sewage
treatment and disposal processes, is reported by the following
organizations:
U.S. Army Medical Bioengineering and Development
Laboratory
S. A. Schaub (Principal Investigator)
Fort Detrick, Frederick, Maryland
U.S. Army Plans and Studies Directorate
Emission of Viruses from Sewage Treatment Plant Facili-
ties
C. J. Spendlove and P. A. Adams (.Principal Investigators)
Dugway Proving Ground
Ougway, Utah
664
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Southwest Research Institute
Department of Chemistry and Chemical Engineering
Health Implications of Sewage Treatment Plant Facilities
D. E. Johnson and J. T. Goodwin (.Principal Investigators)
San Antonio, Texas
Georgia Institute of Technology
Department of Applied Biology
Production and Dispersal of Pathogenic Bacterial and
Viral Aerosols by Aeration of Contaminated Waters
R. King and T. W. Kethley (Principal Investigators)
Atlanta, Georgia
University of Texas
Department of Civil Engineering
Hydrocarbons Emitted During Aeration of Refinery Waste-
water
J. 0. Ledbetter and J. W. Kim (Principal Investigators)
Austin, Texas
WASTEWATER TO LAND: GROUNDWATER
Research programs currently underway in this field
include:
Pennsylvania State University
Mclntire Stennis Program
Effects of Spray Irrigation of Municipal Wastewater
on the Rate and Total Accumulation of Heavy Metals
W. E. Sopper (Principal Investigator)
University Park, Pennsylvania
San Antonio Department of Public Works
Demonstration of Virus Removal from Municipal Sewage
H. C. Morris (.Principal Investigator)
San Antonio, Texas
Minnesota State Department of Iron Range Resources
and Rehabilitation
Treatment of Wastes Using Peat, and Peat in
Combination with Soil"
R. Scuffy (Principal Investigator)
St. Paul, Minnesota
University of Texas
Department of Civil Engineering
Soil Treatment of Concentrated Organic Wastewaters
H. Applegate (Principal Investigator)
El Paso, Texas
665
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West Virginia University
Mater Research Institute
Effects of Plant Nutrients and Heavy Metals from
Land Application of Sludge
D. J. Horvath and R. N. Singh (Principal Investigators)
Morgantown, West Virginia
University of Wisconsin
Department of Soil Science
Utilization and Disposal of Municipal, Industrial,
and Agricultural Processing Wastes on Land
D. Keeney (.Principal Investigator)
Madison, Wisconsin
University of California
Department of Soil Science and Agricultural Engineering
Heavy Metal and Radlonuclide Pollution in Relationship
to Crop Plants
A. Wallace (Principal Investigator)
Riverside, California
U.S. Environmental Protection Agency
National Environmental Research Center
Bioactivity of Soils In Land Application of Wastewater
W. R. Duffer (.Principal Investigator)
Corvallis, Oregon
U.S. Environmental Protection Agency
Robert S. Kerr Environmental Research Laboratory
Rating Biodegradabil1ty of Wastewater Organics in Soil
R. E. Thomas (Principal Investigator)
Ada, Oklahoma
Purdue University
Department of Agronomy
Utilization and Disposal of Municipal, Industrial, and
Agricultural Processing Wastes on Land
L. E. Sommer (Principal Investigator)
Lafayette, Indiana
U.S. Environmental Protection Agency
National Environmental Research Center
Chemical Changes in Wastewater as it Passes Through
Soil Systems
C. G. Enfield (Principal Investigator)
Corvallis, Oregon
666
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U. S. Army
Waterways Experiment Station
The Effects of Land Disposal on Less Permeable Soils
J. Harrison (Principal Investigator)
Vicksburg, Mississippi
University of Texas
Graduate School
Virus Survival in Soils Injected with Municipal Waste-
water Treatment Residuals
B. P. Sagik (Principal Investigator)
San Antonio, Texas
California Institute of Technology
Metal Occurrences within Natural Ecosystems
C. C. Patterson (Principal Investigator)
Pasadena, California
East Central State College
Department of Environmental Science
Analysis of a Spray-Runoff Irrigation System
R. H. Ramsey (Principal Investigator)
Ada, Oklahoma
Woods Hole Oceanographic Institute
Department of Biology
Determination of the Most Efficient Vegetation for
Nutrient Removal and Water Recharge
B. H. Ketchum (Principal Investigator)
Woods Hole, Massachusetts
Cornell University
Department of Agricultural Engineering
Land Disposal Systems for Animal Wastes
R. C. Loehr (Principal Investigator)
Ithaca, New York
University of Arizona
Department of Civil Engineering
Sand Filtration of Oxidation Pond Effluent for Reuse
1n Park Irrigation
D. R. Kasper and R. A. Phillips (Principal Investigators)
Tucson, Arizona
State Department of Water Management
The Flora Filter System in the Disposal of Wastewater
on Soils
D. Papier (Principal Investigator)
Columbus, Ohio
66'
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South Dakota State University
Department of Civil Engineering
Infiltration Lagoons for Tertiary Treatment of Stabili-
zation Pond Effluent
J. N. Dornbush (Principal Investigator)
Brookings, South Dakota
WASTEWATER DISPOSAL TO LAND: CROPS
Research on this topic is currently under investigation
by the following organizations:
East Central State College
Department of Environmental Science
Analysis of a Spray-Runoff Irrigation System
R. H. Ramsey [Principal Investigator)
Ada, Oklahoma
Woods Hole Oceanographic Institute
Department of Biology
Determination of the Most Efficient Vegetation for
Nutrient Removal and Water Recharge
B. H. Ketchum (Principal Investigator)
Woods Hole, Massachusetts
University of California
Department of Soil Science and Agricultural Engineering
Heavy Metal and Radionuclide Pollution in Relationship
to Crop Plants
A. Wallace (Principal Investigator)
Riverside, California
West Virginia University
Water Research Institute
Effects of Plant Nutrients and Heavy Metals from Land
Application of Sludge
D. J. Horvath and R. N. Singh (Principal Investigators)
Morgantowns West Virginia
Duke University
Marine Laboratory
The Role of Sewage Effluent and Sludge Disposal in the
Introduction of Mercury into Marine and Agricultural
Ecosystems
R. T. Barber (Principal Investigator)
Beaufort, North Carolina
Pennsylvania State University
Mclntire Stenr.is Program
Effects of Spray Irrigation of Municipal Wastewater
on the Rate and Total Accumulation of Heavy Metals
W. E. Sopper (Principal Investigator)
University Park, Pennsylvania
668
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Northeastern Wisconsin Regional Planning
Use of Emergent Vegetation for the Biological Treatment
of Municipal Wastewater
F. L. Spangler and W. R. Duffer (Principal Investigators)
Appleton, Wisconsin
Metropolitan Sanitary District of Greater Chicago
Agricultural Benefits and Environmental Changes
Resulting from the Use of Digested Sludge on
Field Crops
D. T. Lordi (Principal Investigator)
Chicago, Illinois
WASTEWATER DISPOSAL TO LAND: FRESHWATER SYSTEMS
The following organizations are currently conducting
research into the effect on fresh surface water from land
disposal of wastewater.
U. S. Army
Waterways Experiment Station
Overland Runoff of Wastewaters
P. G. Hunt (Principal Investigator)
Vicksburg, Mississippi
California Institute of Technology
Department of Geological and Planetary Science
Metal Occurrences within Natural Ecosystems
C. C. Patterson (Principal Investigator)
Pasadena, California
WASTEWATER DISPOSAL TO LAND: MARINE SYSTEMS
Two organizations were discovered which are currently
conducting research on the subject topic:
Duke University
Marine Laboratory
The Role of Sewage Effluent and Sludge Disposal in
the Introduction of Mercury into Marine and Agricul-
tural Ecosystems
R. T. Barber (Principal Investigator)
Beaufort, North Carolina
California Institute of Technology
Department of Geological and Planetary Science
Metal Occurrences Within Natural Ecosystems
C. C. Patterson (Principal Investigator)
Pasadena, California
669
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SLUDGE DISPOSAL TO LAND: CROPS
On-going research on the agricultural application of
sludge is listed below:
Duke University
R. T. Barber (Principal Investigator)
Beaufort, North Carolina
Metropolitan Sanitation District of Chicago
D. T..Lbrdi (Principal Investigator)
Chicago, Illinois
University of California
A. Wallace (Principal Investigator)
Riverside, California
West Virginia.University
D. J. Horvath and R. N. Singh (.Principal Investigators)
Morgantown, West Virginia
SCS Engineers
R. J. Lofy and R. P. Stearns (Principal Investigators)
Long Beach, California
SLUDGE DISPOSAL TO WATER: MARINE SYSTEMS
Research projects are presently being conducted by the
following organizations with regard to ocean disposal of
sludges :
Duke University
Marine Laboratory
The Role of Sewage Effluent and Sludge in the Introduction
of Mercury into Marine Ecosystems
R. T. Barber (.Principal Investigator)
Beaufort, North Carolina
U.S. Environmental Protection Agency
National Environmental Research Center
Fate of Trace Elements in Placed, Digested Sewage Sludge
in an Experimental Site in the New York Bight
M. H. Feldman (Principal Investigator)
Corvallis, Oregon
SLUDGE DISPOSAL TO WATER: SHELLFISH
Research programs currently underway are primarily
concerned with the introduction of trace elements from sewage
sludges into marine organisms. These programs are listed
below:
670
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Duke University
Marine Laboratory
The Role of Sewage Effluent and Sludge in the Intro-
duction of Mercury into Marine Ecosystems
R. T. Barber (Principal investigator)
Beaufort, North Carolina
U.S. Environmental Protection Agency
National Environmental Research Center
Fate of Trace Metals in Placed, Digested Sewage Sludge
in an Experimental Site in the New York Bight
M. H. Feldman (.Principal Investigator)
Corvallis, Oregon
671
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before c
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