EPA-600/3-80-060
July 1980
-4
O
AN EVALUATION OF HAZARDOUS CHEMICALS
IN LAKE ONTARIO DURING IFYGL
by
G. Fred Lee
Environmental Engineering
Department of Civil Engineering
Colorado State University
Fort Collins, Colorado 80523
Grant No. R-803187
Project Officer
Michael D. Mullin
Large Lakes Research Station
Environmental Research Laboratory-Duluth
Grosse lie, Michigan 48138
ENVIRONMENTAL RESEARCH LABORATORY
OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
DULUTH, MINNESOTA 55804
77Westj£c:. .,,,..
Chicago, IL 6,. , - .-*' Uth Floor
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DISCLAIMER
This report has been reviewed by the Large Lakes Research
Station, Environmental Research Laboratory-Duluth, U.S. Environ-
mental Protection Agency, and approved for publication. Approval
does not signify that the contents necessarily reflect the views
and policies of the U.S. Environmental Protection Agency, nor
does mention of trade names or commercial products constitute en-
dorsement or recommendation for use.
11
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FOREWORD
The presence of hazardous materials in the environment is a
topic of major interest to the Environmental Protection Agency.
Elevated levels of chlorinated hydrocarbon pesticides, poly-
chlorinated biphenyls (PCBs) and heavy metals in some species of
Great Lakes fish have necessitated the recommendation that persons
limit, or eliminate, their dietary intake of these fish. In
order to develop an understanding of the extent of the contamina-
tion of the Great Lakes by these substances, it is necessary to
better define the relationship of contaminant input and the
effect of this contaminant load on Great Lakes water quality.
This report presents the results of a detailed evaluation
of a comprehensive set of hazardous chemical data that were
obtained on Lake Ontario during the International Field Year for
the Great Lakes (IFYGL).
Michael D. Mullin, Ph.D.
Project Officer
Large Lakes Research Station
Environmental Research Laboratory
Grosse lie, Michigan
111
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ABSTRACT
Data collected during the Internationa] Field Year for the
Great Lakes (IFYGL) studies (1972-73) on hake Ontario are sumna-
rized relative to either recommended International Joint Commis-
sion (IJC) Research Advisory Board water quality objectives or
USEPA Quality Criteria for Water. Data from 247 stations are
used to summarize information on the following parameters: cad-
mium, zinc, chromium, copper, fluoride, iron, lead, nickel, man-
ganese and ammonia. Chlorinated hydrocarbon data for DDT, di-
eldrin, and PCBs are discussed relative to concentrations deter-
mined in water samples and three fish speeier,.
Summaries indicate that almost all reported measurements for
total cadmium, regardless of the region of the lake from which
the samples were collected (i.e., open water, shoreline or river
mouth), exceed the IJC water quality objective of 0.2 yg/1 by at
least five times. Values reported for copper also showed a high
percentage of measurements from all regions of the lake equal to
or in excess of the recommended IJC water quality objective.
Other metals showed more regional patterns of values equalling or
exceeding water quality objectives. The concentrations of PCBs,
dieldrin and DDT and its metabolites in Lake Ontario water and
fish were found to exceed the IJC water quality objectives and
the USEPA water quality criteria.
The significance of this situation at this time is unknown.
Additional research needs to be done to determine the reliability
and representativeness of the hazardous chemical data collected
during IFYGL in describing water qualiry in Lake Ontario. If the
IFYGL data are found to be representative, studies need to be
conducted to evaluate whether the "excessive" concentrations are
indicative of water quality deterioration.
This report was submitted in fulfillment of Contract No.
R-803187 by the Center for Environmental Studies, University of
Texas at Dallas under the sponsorship of the U.S. Environmental
Protection Agency, Large Lakes Research Station, Environmental
Research Lab-Duluth. This report covers The period November
1974 to April 1977 and work was completed is of May 1978.
IV
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CONTENTS
Foreword iii
Abstract iv
Figures vi
Tables vii
Acknowledgments viii
1. Introduction 1
2. Conclusions and Recommendations 3
3. Review of Hazardous Chemical Data
Gathered on Lake Ontario During IFYGL ... 5
References 25
v
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FIGURES
Number Paige
1 Lake Ontario sampling sites for chlorinated
hydrocarbon analysis 9
VI
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TABLES
Number Page
1 Parameters and Numbers of Values Used in
Summarizing IFYGL Data from Lake Ontario 8
Comparison of the Concentrations of Selected
Inorganic Parameters with IJC Water Quality
Objectives or USEPA Quality Criteria for
Water 12
Comparison of River Mouth Measurements to
Total Measurements 13
Evaluation of the Relationship Between Selected
Parameters from the IFYGL Studies on Lake
Ontario and the IJC Water Quality Objectives
or the USEPA Quality Criteria for Water for
the Open Waters and Shoreline Stations 15
Comparison of the Number of Stations on the
Niagara, Genesee, Oswego and Black Rivers
with Concentrations of Contaminants Equal to
or Greater than the IJC Water Quality Ob-
jectives for Selected Heavy Metals and
Ammonia and the USEPA Quality Criteria for
Water for Manganese 17
Comparison of Concentrations of Selected
Heavy Metals and Ammonia for the Lake Ontario
Stations near the Mouths of Major U.S.
Tributary Inputs and the St. Lawrence River
near the Outlet of Lake Ontario 18
Chlorinated Hydrocarbons, Pesticides, PCBs
and Fat in Lake Ontario Fish . . . . 20
Chlorinated Hydrocarbons, Pesticides and
PCBs in Lake Ontario Water 21
Limit of Detection for the Chlorinated
Hydrocarbon Pesticides and PCBs 23
VII
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ACKNOWLEDGMENTS
Support was given to this study by the USEPA Large Lakes
Research Station, Grosse lie, Michigan; the University of Texas
at Dallas; and the EnviroQual Consultants and Laboratories, Fort
Collins, Colorado. Special recognition is given to various
members of the USEPA Large Lakes Research Station, especially
Nelson Thomas, Michael Mullin and William Richardson, for their
assistance in various aspects of this project.
The review of the IFYGL hazardous chemical data for Lake
Ontario was co-authored by William T. Waller of the University
of Texas at Dallas and G. Fred Lee of the Department of Civil
Engineering, Colorado State University. The remainder of the re-
port was authored by G. Fred Lee. Numerous individuals have re-
viewed various sections of this report and have provided valuable
suggestions which have improved the quality of the report. The
assistance of these individuals is greatly appreciated. The
assistance of P. Wernsing and M. Jaye in typing and editing is
also appreciated.
Vlll
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SECTION 1
INTRODUCTION
The North American Great Lakes are unique bodies of water
which, in some locations, have undergone significant water qual-
ity deterioration arising from man's activities on the lakes
both within and outside of their watersheds. In 1972 the U.S.
and Canada, through the IJC Water Quality Agreement, made a sig-
nificant commitment toward improving water quality in the Great
Lakes. In addition, both the U.S. and Canadian federal govern-
ments as well as many of the states and the province of Ontario
have adopted legislation which, when implemented, will result in
improved water quality in the Great Lakes. For the U.S., the
1972 Amendments to the Federal Water Pollution Control Act es-
tablish as a goal, where economically feasible, technically at-
tainable and socially desirable, zero pollutant discharge from
municipal and industrial sources by the mid-1980's. In order to
implement this goal in a meaningful way, a much better under-
standing of the relationship of contaminant input to the Great
Lakes and the effect of this contaminant load on Great Lakes
water quality must be available. Particular attention must be
given to these relationships for the chemicals which tend to be
persistent in Great Lakes waters and show toxicity to Great Lakes
organisms. Further, more emphasis must be given to those chem-
icals which bioaccumulate in Great Lakes organisms to the extent
that their use as a source of food for man is inhibited or their
effect on other animals in the food chain, such as fish-eating
birds, is adverse.
This report presents the results of a detailed evaluation of
a comprehensive set of hazardous chemical data that were obtained
on Lake Ontario during the International Field Year for the Great
Lakes (IFYGL). Review of this data has provided additional sup-
port for the fact that some of the Great Lakes are showing con-
centrations of contaminants which are classified as hazardous
chemicals, in excess of IJC Research Advisory Board water quality
objectives and the ,"!uly 1976 USEPA Quality Criteria for Water.
The approach used during the IFYGL studies on the Great Lakes was
more or less the one used previously for other Great Lakes
studies. This approach has numerous, significant deficiencies
which, while generally adequate for control of gross pollution,
are inadequate for control of the more subtle aspects of pol-
lution, especially those associated with chronic toxicity to
aquatic organisms. Since future pollution control efforts will
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be directed toward more subtle aspects, a markedly different ap-
proach will have to be used in IFYGL-type studies if future water
quality management programs are to be based on technically sound
information.
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SECTION 2
CONCLUSIONS AND RECOMMENDATIONS
1. Hazardous chemicals such as the chlorinated hydrocarbon
pesticides, PCBs and heavy metals are currently causing signifi-
cant water quality problems in Great Lakes waters. These prob-
lems are the direct result of discharge of excessive amounts of
these chemicals to the Great Lakes or their tributaries in munic-
ipal or industrial wastes, runoff from urban and rural areas and
direct input from the atmosphere. These problems have been pri-
marily manifested in the bioaccumulation of excessive concentra-
tions of selected chemicals in fish, preventing edibility based
on FDA limits. Commercial fisheries in Lake Michigan have been
virtually eliminated because of buildup of excessive levels of
DDT and its analogs and PCBs in fish. Although much less well
documented, it is reasonable to assume that excessive concentra-
tions of various chemicals have had significant effects on Great
Lakes water quality arising from acute and chronic toxicity to
various forms of aquatic life. While problems of this type are
expected to be localized near the source of input, it is possi-
ble, even though not documented, that lakewide effects have
occurred due to the presence of excessive amounts of hazardous
chemicals in Great Lakes waters.
2. Previously used and in some instances current programs
for control of hazardous chemicals in the Great Lakes are not
adequate to eliminate future problems of the type experienced
over the past few years.
3. Because of an inadequate data base on current concentra-
tions of hazardous chemicals in many parts of the Great Lakes
water, aquatic organisms and sediments, estimates have not been
made of the current degrees of contamination and the changes in
contamination levels over time. Many of the previously con-
ducted studies on Great Lakes water quality have been improperly
planned and executed. Further, there have been several examples
of studies on Great Lakes water quality where inadequate funds
were made available for data presentation and interpretation.
In addition, coordination among the various groups conducting
studies on hazardous chemicals in the Great Lakes should be in-
creased to obtain maximum benefit from the efforts expended.
4. Based on the IFYGL data, the concentrations of certain
heavy metals and chlorinated hydrocarbon pesticides and PCBs are
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present in Lake Ontario water equal to and in some instances
many times in excess of the IJC water quality objectives and the
USEPA water quality criteria. Information is not available on
the significance of these apparently high concentrations. Work
should be done to determine how much of the total contaminant
concentration present in a water sample is available to affect
water quality.
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SECTION 3
REVIEW OE HAZARDOUS CHEMICAL DATA GATHERED ON LAKE ONTARIO
DURING IFYGL
In 1972-73 the U.S. and Canada conducted the International
Field Year for the Great Lakes (IFYGL) studies on Lake Ontario.
The IFYGL was a large, multicomponent study which included de-
tailed measurements of the physical, biological and chemical
characteristics of this lake. As part of the USEPA studies con-
ducted during the IFYGL, samples of water, aquatic organisms and
sediments of the lake were collected and analyzed by the USEPA
or under contract. This report summarizes the results of these
studies with particular reference to the concentrations of vari-
ous types of contaminants which are normally considered hazard-
ous to aquatic life and man.
The results of the chlorinated hydrocarbon studies are
based on the work of Haile et al. (1975) and Moore (Personal com-
munication, 1974) of the State University of New York at Oswego.
The data used for comparison of inorganic parameters were
derived from analyses of the U.S. Environmental Protection
Agency's Rochester Laboratory as retrieved from the STORET data
system. The data contained numerous errors. Obvious errors
were omitted from the summaries, while less obvious ones, if
present, are included. The magnitude of the influence of the
less obvious errors on the summaries presented is unknown. As
with any summary attempt of this type, the methods used can
greatly influence the results obtained. In addition, data taken
out of their spatio-temporal frame sometimes yield poor statis-
tical correlations, indicating potential collection and storage-
analytical problems or high variability in the water of a par-
ticular area.
Robertson et al. (1974) compared the analytical results ob-
tained from various laboratories for parameters investigated
during IFYGL. They found, "statistically significant differences
among the results from the three laboratories for many of the
parameters." They attribute the significance to differences in
the analytical methods used by the participants. For most of the
inorganic constituents compared, the results from the EPA Roch-
ester Laboratory were higher in concentration than the results
from the other two laboratories. The results on inorganic con-
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stituents summarized in this report are based on data from the
EPA Rochester Laboratory and, therefore, likely reflect the
higher concentrations.
OVERALL APPROACH
Summaries of the parameters reported were made relative to
the proposed water quality objectives recommended by the Inter-
national Joint Commission (1977). Those parameters included ir
the summaries for which recommendations were made are: total
cadmium, 0.2 yg/1; total chromium, 50 yg/1; total fluoride, 1.2
mg/1; total lead, 25 yg/1; and total zinc, 30 yg/1.
The Water Quality Objectives Subcommittee (1976) of the
International Joint Commission Water Quality Board has made the
following recommendations: total copper, 5 yg/1; total iron,
300 yg/1; and total nickel, 25 yg/1. Ammonia was compared to a
proposed objective of 0.02 mg/1 as unionized ammonia. In the
case of manganese, a specific recommendation was not made by the
committee. These parameters were analyzed relative to criteria
suggested in Quality Criteria for Water (USEPA, 1976). The
recommended criterion for manganese is 50 yg/1 for domestic
water supplies.
The data summarized in this report are expressed in terms of
the percentage of measurements exceeding a specific water quality
objective or criterion by differing amounts, for different areas
within Lake Ontario. This approach was taken in lieu of express-
ing the results in terms of means, standard deviations and con-
fidence levels because it was felt more relevant trends regarding
potential problems would be obtained.
From an aquatic toxicity point of view, means, standard de-
viations and ranges have little meaning since they do not con-
sider duration of exposure. To properly interpret water quality
data of the type generated during the IFYGL studies on Lake
Ontario, it would be necessary to know the amount of time that
the concentrations exceeded the toxicity threshold for aquatic
organisms. Unfortunately, very little information is available
on the toxicity of fluctuating concentrations of various chemi-
cals to aquatic life as a function of time of exposure, magnitude
of change in concentration and life history state exposed. With-
out this type of information it is difficult to judge the environ-
mental significance of a particular concentration of a contamin-
ant which may only periodically exceed a water quality objective
or criterion.
Another significant problem with the IFYGL hazardous chemi-
cal data, which is true of most data of this type, is that for
some parameters a large number of less than values were reported.,
This makes interpretation of normal statistical parameters such
as means, standard deviations, etc. less meaningful, especially
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when the detection limits used in the analytical procedures are
greater than the water quality objective or criterion.
Data from 247 stations on Lake Ontario were used in this
summary effort. One problem in summarizing the data was the fre-
quency with which collections were made and consequently, the
number of values reported. The inorganic data, as summarized,
does not distinguish between samples collected from different
depths. The data base summarized by depth was too fragmentary to
provide any meaningful comparisons. Table 1 shows the parameters
and number of values for each that were used in these summaries.
Figure 1 presents a map of Lake Ontario showing some of the
sampling stations.
ANALYTICAL PROCEDURES
Inorganic Parameters
Inorganic parameters were analyzed by the Rochester New
York field office of the USEPA Region II. Ammonium was deter-
mined using the Technicon Autoanalyzer by the indophenol pro-
cedure. Fluoride was determined on the Technicon Autoanalyzer
using the alizarin blue-lanthanum procedure. The heavy metals
(Cd, Mn, Pb, Zn, Cr, Cu, Ni, Fe) were determined by atomic ab-
sorption procedures after digestion of unfiltered samples with
concentrated nitric acid. The digested solution was concen-
trated by evaporation. HC1 was added and the sample was directly
aspirated into the atomic absorption instrument. The APDC-MIBK
procedure was not used; therefore, the results of these analyses
are somewhat suspect since the direct aspiration procedure used
by the USEPA Rochester Laboratory was found to yield incorrect
results for certain types of aquatic samples. Further details
on analytical procedures can be obtained from the USEPA (Un-
dated). The results of the heavy metal analyses would approach
and in many instances equal the total heavy metal content except
for that part of the heavy metals bound in the silicate matrix.
Chlorinated Hydrocarbon Studies
Sampling and analytical procedures used for the chlorinated
hydrocarbon analyses performed by Haile have been described in
detail by Haile et al. (1975). Water samples were taken with a
Van Dorn sampler just below the surface and at 10 meters above
the bottom. Fish were collected by trawling at 18 to 73 meters
depth. All samples were transported and stored at or near M- C
in glass or metal containers.
Whole fish samples were homogenized, extracted with ethyl
ether-hexane and cleaned up on an activated florisil column.
Further cleanup was accomplished on silicic acid columns using
dichloromethane-hexane.
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TABLE 1. PARAMETERS AND NUMBERS OF VALUES USED IN SUMMARIZING
IFYGL DATA FROM LAKE ONTARIO
Parameter
Iron
Lead
Manganese
Nickel
Zinc
Fluoride
Cadmium
Chromium
Copper
Ammonia
Number of values
1937
593
2032
1978
2041
7687
614
114
2067
3645
Samples collected from Spring 1972 through Spring 1973.
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Water samples were passed through a column containing poly-
urethane foam plugs which had been coated with DC-200 silicone
oil. The foam plugs were extracted with ethyl ether-hexane.
The extracts were cleaned up in a similar manner as used for the
fish samples. Studies were not performed to evaluate the effi-
ciency of the polyurethane foam plug recovery of chlorinated
hydrocarbons from Lake Ontario waters. It is therefore possible
that some chlorinated hydrocarbons were not completely recovered
by this procedure and the results presented here are minimum
concentrations present in the water.
The chlorinated hydrocarbon determination for the above
samples from the silicic acid cleanup were chromatographed on
Varian Aerograph gas chromatographs on four different GC columns
using electron capture. Some of the samples were examined by
GC-MS using the Finnigan quadropole mass spectrometer.
PCS determinations were made on perchlorinated samples.
The results of PCB analyses are reported as equivalent Aroclor
1254.
Veith (Personal communication, 1977) has questioned the
reliability of the PCB analyses conducted by Haile e_t al. (1975)
of Lake Ontario water. He has concluded, based on sTudTes con-
ducted under his supervision, as well as others, that either the
polyurethane foam plug yielded high results for PCBs or the con-
centrations of PCBs have decreased substantially between 1972
and 1976. Since the likelihood of the latter is small, it is
felt that the water PCB data during IFYGL is high due to con-
tamination problems arising from the analytical procedure used
by Haile e_t al. (1975). On the other hand, the PCB data for
fish appear to be reliable.
RESULTS OF INORGANIC PARAMETERS
The initial review of the data for the 247 stations was
directed toward determining the number of values which equalled
or exceeded the water quality objectives or criteria used as
listed previously. This method showed that none of the 247
stations contained values for fluoride and chromium equal to o:°
greater than the water quality objectives or criteria.
The ammonia data from the STORET system are presented as
total ammonia expressed as N. In order to compare these data
with the water quality criterion of 0.02 mg/1 as unionized
ammonia, tables from Thurston et al. (1974) and the pH and water
temperature values from the STORET data were used. This pro-
cedure permitted calculation of the percentage of total ammonia
that was unionized. In many cases temperature, pH and total
ammonia concentrations were not available for the same dates.
In these cases decisions as to whether or not water quality ob-
jectives were equalled or exceeded was based on monthly average
10
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temperature and pH values.
Data for the nine parameters are presented in Table 2. This
table shows the relationship between the number of stations re-
porting a parameter and the number and percentage of stations
showing a parameter equal to or in excess of the water quality
obj ective.
Examination of Table 2 reveals that 40 percent of the sta-
tions had iron greater than the IJC water quality objectives
while 15 percent of the stations showed manganese greater than
the USEPA criteria. Nickel and zinc had 44 and 79 percent of
the stations, respectively, reporting concentrations in excess
of the IJC water quality objectives. Essentially all stations
had copper and cadmium concentrations in excess of the IJC water
quality objectives, while eight stations had concentrations of
unionized ammonia greater than the objective for this compound.
Further review of these data was undertaken in which the
247 stations were divided into four major groups. The first
group was comprised of 60 main lake water quality stations lo-
cated in an approximately equally spaced grid in the open waters
of Lake Ontario. The second group was made up of 90 nearshore
individual stations grouped into three's along the U.S. side of
Lake Ontario. The three station triplets are positioned per-
pendicular to the shore with the nearest shore station in each
triplet spaced approximately 10 kilometers apart. These triplet
stations began at Point Weller, in Western Lake Ontario (43°13'
26.0", 079 13' 48") and continue to Eastern Lake Ontario (43
50' 30.0", 076° 23' 50.0"). The third group of stations was
comprised of five stations; four of which are located near the
mouths of rivers feeding Lake Ontario. The locations of these
stations were generally at a gaging station and, therefore, the
concentrations found represent the characteristics of the river
rather than the lake. These include the Niagara River at the
Fort Niagara gaging station, the Genesee River mouth at the Navy
Militia, the Oswego River at the Main Street Bridge in Oswego,
New York, and the Black River mouth. The fifth station was lo-
cated at Cape Vincent on the St. Lawrence River (lake outlet).
These five stations were analyzed individually. The fourth
group of stations was comprised also of nearshore stations, and
these are clustered near the mouths of the major rivers entering
Lake Ontario along the U.S. side of the lake.
The number of values reported in Table 1 associated with
the 247 stations were not distributed equally among the stations.
The five stations associated with the Niagara, Genesee, Oswego,
Black and St. Lawrence Rivers were sampled for the most part at
three-day intervals. As a result, for some parameters the five
stations represent a large percentage of the total data base re-
ported. The percentage of the total data base reflected in anal-
yses from these five stations is given in Table 3.
11
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TABLE 3. COMPARISON OF RIVER MOUTH MEASUREMENTS TO TOTAL
MEASUREMENTS
Parameter
Iron
Lead
Manganese
Nickel
Zinc
Cadmium
Chromium
Copper
Ammonia
Percent of total number of
measurements from five
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26
89
24
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77
39
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Table 4 shows the total number of measurements associated
with eight parameters from the 60 main lake stations and the 90
shoreline stations. The table also shows the number and per-
centage of these measurements which equal or are greater than
the water quality objective; are equal to or greater than 1.5
times the objective; and are equal to or greater than 5 time?;
the recommended objective.
Examination of Table 4 shows that based on this set of pa-
rameters, essentially the same water quality exists at the open
60 main lake stations and the 90 shoreline stations. These 90
shoreline stations are generally in areas not directly influ-
enced by major rivers entering the lake. Table 6 gives the re-
sults of shoreline stations clustered near the mouths of major
rivers. A comparison of the percent of the stations with values;
equal to or greater than the recommended objectives with those
in the column with 1.5 times the recommended values shows that
approximately 50 percent of the stations which are equal to or
in excess of the objectives have values near the objectives.
There were few stations with values in excess of five times the
objectives for these parameters. On the other hand, cadmium
always exceeded the water quality objective by at least five
times. In addition, a significant number of the copper values
exceeded the objectives by 1.5 times. Table 4 also shows that
based on these data, ammonia is not a problem in either the oper
lake or for the 90 shoreline station waters.
Table 5 presents a comparison of the number of stations on
the Niagara, Oswego, Black and Genesee Rivers with concentra-
tions of contaminants equal to or greater than the IJC water
quality objectives for selected heavy metals and ammonia. These
stations are located at gaging stations for each of these rivers
and thereby reflect the concentrations of the parameters enter-
ing Lake Ontario from the major U.S. tributaries of this lake.
Examination of this table shows that of these tributaries, the
Genesee River is the most contaminated for these parameters, with
exceptionally high concentrations of iron, lead, manganese, zinc,
cadmium and copper. The other rivers show a large number of
samples with excessive amounts of cadmium and copper. Many cf
the values for the Oswego River lie between 1.5 and 5 times the
IJC recommended objectives. It is interesting to note that the
only river that consistently shows large numbers of samples with
excessive concentrations of ammonia is the Genesee River.
Special attention must be given to the Niagara River because
of its large contribution of water to the lake. In addition to
the high percentages of cadmium (92 percent) and copper (78 per-
cent) measurements which equal or exceed the water quality ob-
jectives, 51 percent of the iron, 23 percent of the zinc, 13 per-
cent of the lead and 8 percent of the nickel measurements report-
ed equalled or exceeded the recommended objectives for this
river.
14
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Most parameters associated with the IFYGL STORET system
data base, on which the inorganic metal portion of this analysis
is based, have values which are presented as less than. This
causes no particular problem relative to the type of analysis
used in this report except for cadmium. In the case of cadmium
the recommended objective is 0.2 yg/1 total cadmium. However,
those values designated as being less than were reported as less
than 1 yg/1 total cadmium or 5 times the recommended objective.
There is no way to tell exactly what the concentration of cad-
mium was in these cases which represent 7 percent of the total
cadmium measurements. It is reasonable to assume that the per-
centage of cadmium values exceeding the objective represent a
conservative estimate.
Table 6 presents an analysis of the Lake Ontario stations
clustered near the mouths of the Niagara, Genesee, Oswego and
Black Rivers and on the St. Lawrence River near the outlet of
Lake Ontario. It is interesting to note that the outlet sta-
tion generally shows a higher frequency of concentration of
these contaminants equal to or exceeding the IJC water quality
objectives than the main lake stations. This could indicate a
local source of contamination for the St. Lawrence River. On
the other hand, the Lake Ontario stations clustered near the
mouths of major U.S. tributary inputs generally show a greater
number of stations with excessive concentrations than the open
lake stations.
RESULTS OF CHLORINATED HYDROCARBON ANALYSES
Fish
Table 7 presents chlorinated hydrocarbon and fat content
for composites of three species of fish collected from Lake On-
tario. Examination of this table shows that all fish extracts
contained DDT group pesticides and dieldrin. The total DDT for
the alewife, smelt and slimy sculpin ranged from 0.11 to 1.65
yg/g based on whole fish. Dieldrin content of these fish ranged
from 0.02 to 0.11 yg/g whole fish. GC-MS confirmed the presence
of DDE, ODD, DDT and dieldrin in these samples.
Several other chlorinated hydrocarbons were identified in
extracts of fish from selected locations in Lake Ontario.
Endrin was found in all fish taken off Prince Edward Point and
Mexico Bay, but was below detection limits in fish taken from
between Galloo and Stoney Islands and other eastern lake sam-
pling sites. Endrin was below the detection limits in fish
taken from western lake sites off Hamilton, Olcott and Roches-
ter. Lindane and heptachlor were also identified in some of the
fish taken from Lake Ontario.
16
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PCB content of fish expressed as equivalent Aroclor 1254
ranged from 0.1 to 9.2 yg/g based on whole fish analysis (see
Table 7). The lakewide average total DDT was 1.4 yg/g in smelt
(1972) which compares favorably with that reported by Reinert
(1970) in Lake Ontario fish collected in 1965-68, which had an
average concentration of about 1.6 yg/g. Reinert (1970) report-
ed dieldrin levels for alewife and smelt captured in 1967-68 of
0.1 and 0.06 yg/g, respectively. These values are comparable to
the concentrations found in this study for 1972 captured fish of
0.04 yg/g for alewife and smelt.
Examination of the data presented in Table 7 in comparison
to the FDA limits for DDT, dieldrin, and PCBs in fish shows that
all of the fish composites analyzed had less total DDT than the
FDA limit of 5 ppm. It was found that all fish composites
analyzed had less dieldrin than the guideline of 0.3 ppm for the
sum of aldrin and dieldrin which has been set by the FDA as an
upper limit on food for human consumption. Several of the fish
composites analyzed had PCBs in excess of the current limit of
2 ppm. Based on this study, the fish in Lake Ontario were not,
in general, suitable for human consumption because of the high
PCB concentrations. This indicates that there has been large
scale contamination of fish by PCBs.
The IJC has recommended a 1 yg/g limit for DDT and its
metabolites for whole fish in Lake Ontario. The basis of this
recommendation is protection of fish consuming birds. Examina-
tion of Table 7 shows that, in general, DDT on a whole fish
basis is approximately equal to this objective. The IJC also
recommended that the aldrin and dieldrin content of edible por-
tions of fish should not exceed 0.3 yg/g. Table 7 shows that,
in general, whole fish dieldrin content was in the order of 0.03
to 0.1 yg/g.
The IJC recommended a water quality objective for whole
fish of 0.1 yg/g PCBs for protection of fish consuming birds -and
animals. Examination of Table 7 shows that, in general, both
the water and fish in Lake Ontario have PCB concentrations in
excess of IJC recommended criteria and objectives.
Water
The DDT, dieldrin and PCB concentrations in Lake Ontario
water are shown in Table 8. Examination of this table shows
that the dominant form of the DDT group was DDE, comprising 50
to 90 percent of the total DDT. The lakewide average total DDT
was 35 ng/1 with a range of 16 to 57 ng/1. These results show
that Lake Ontario water has a concentration of DDT 10 times the
USEPA (1976) and the IJC (1976) water quality objectives for DDT,
The USEPA water quality criterion for DDT of 1 ng/1 is based on
the potential for bioaccumulation in fish which could be harmful
to man and birds. The IJC objective for DDT is 3 ng/1 with es-
19
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sentially the same rationale, although the IJC notes that the 3
ng/1 level is equal to the lower quantification limit for DDT
and its metabolites. It is interesting to note that even though
the total DDT in the water is apparently considerably greater
than the EPA or IJC criteria or objectives, the concentrations
in fish were, in general, less than the FDA limit of 5 ppm for
use as human food.
The average dieldrin in Lake Ontario was 4 ng/1 with a range
of approximately 1 to slightly over 12 ng/1. The highest values
were found off Oswego and Cobourg. In July 1976 the USEPA
recommended a dieldrin limit of 3 ng/1 for the sum of aldrin and
dieldrin, while the comparable IJC value is 1 ng/1. Again, the
primary concern is bioaccumulation in fish. It is evident that
the dieldrin content of the water (Table 8) is, in general, equal
to or greater than the EPA and IJC criteria or objectives.
The polychlorobiphenyls (PCBs) content of the water ranged
from 40 to 97 ng/1 with an average of 55 ng/1. This value is 50
times the USEPA water quality criteria. While the IJC Water
Quality Board did not establish a PCB water quality objective,
they did indicate that it should be less than 1 ng/1 which is
considerably below the current reliable minimum quantitation
level. As discussed earlier, it appears that the data reported
by Haile ejt al. (1975) for PCBs in water are high. Veith (Per-
sonal communication, 1977) indicated that other investigators
have found concentrations of PCBs in Lake Ontario water between
2 and 6 ng/1.
Additional pesticide data (101 water samples) (Moore, Per-
sonal communication, 1974) collected during IFYGL from Lake On-
tario were reviewed. The analyses of these water samples for
lindane, heptachlor, aldrin, heptachlor epoxide, dieldrin, P,P'-
DDE, 0,P'-TDE, endrin, 0,P'-DDT, P,P'-TDE, chlordane, toxaphene
and PCBs indicated that these parameters were not present in
detectable quantities. The detection limits for these analyses
are listed in Table 9. In general, it can be determined that
insufficient analytical procedure sensitivity was used in the
studies by Moore to detect chlorinated hydrocarbon pesticides
and PCBs at levels which are now considered to be significant in
natural waters.
DISCUSSION
As discussed in Appendix A of the Fourth Annual Report on
Great Lakes Water Quality (1976), the significance to biological
organisms of the forms of metals in waters remains to be fully
elucidated. In addition, not only is the significance of the
forms of metals and their interactions in water not fully under-
stood, the data presented here are only point estimates in time
and space. These data do not, in general, reflect the continuum
of measurements that would be necessary to establish the percent-
22
-------
TABLE 9. LIMIT OF DETECTION FOR THE CHLORINATED HYDROCARBON
PESTICIDES AND PCBs
Limit of Detection for Study by Moore
(ng/1)
Aldrin
Chlordane
P,P'-DDE
0,P'-DDT
P,P'-DDT
Dieldrin
Endrin
Heptachlor
Heptachlor Epoxides
Lindane
PCBs
0,P'-TDE
P,P'-TDE
Toxaphene
50
1000
50
100
100
50
50
50
50
50
1000
100
100
10,000
After Moore (Personal communication, 1974)
23
-------
age of time an objective was exceeded. The significance of
periodic departures above water quality objectives cannot be
adequately evaluated without data relative to the length of time
an objective is exceeded, the magnitude of the departure above
the objective and the period of time the objective is exceeded
relative to the life history stages of the organisms to be pro-
tected. Therefore, no one should attempt to extrapolate from
these summary data to biological effects.
These summary data can be used to provide guidance relative
to which parameters most frequently deviate from the objectives.
Based on the data analyzed here and assuming that the total con-
centration of a parameter also reflects that a higher concen-
tration of a parameter exists in toxic form leads to the con-
clusion that among the heavy metals studied cadmium and copper
currently hold the greatest risk of becoming problems in Lake
Ontario. Particularly noteworthy is the high percentage of
measurements, including those for all main lake stations, which
equalled or exceeded the water quality objective for cadmium by
more than five times.
For the chlorinated hydrocarbon pesticides and PCBs, con-
cern must be focused on the apparently high concentrations of
DDT and its metabolites, dieldrin and the PCBs found in Lake
Ontario water and fish compared to the IJC water quality ob-
j ectives.
It is evident that there is need for additional work on the
concentrations of the various forms of heavy metals, especially
copper and cadmium, and chlorinated hydrocarbons, PCBs, diel-
drin and DDT present in Lake Ontario water. If it is found that
the concentrations of potentially significant forms of these
compounds present in the lake have a reasonable expectation of
having an adverse effect on water quality, studies should be con-
ducted to determine the dominant contributor of available forms.
Control strategies may then be initiated where possible. It is
important to emphasize that before large scale control measures
are instigated, beyond those already implemented in the U.S. in
compliance with PL 92-500, research should be done along the
above indicated lines to ensure that funds spent in the name of
water pollution control accomplish the intended purpose of lower-
ing the excessive concentrations of available forms and the con-
comitant improvement in water quality for various parts of Lake
Ontario. Failure to take this approach could result in the ex-
penditure of large amounts of money and the utilization of re-
sources with little or no improvement in water quality in Lake
Ontario.
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REFERENCES
Haile, C. L., G. D. Veith, G. F. Lee, and W. C. Boyle. Chlo-
rinated Hydrocarbons in the Lake Ontario Ecosystem (IFYGL).
EPA-660/3-75-002, USEPA, Corvallis, Oregon, 1975. 28 pp.
International Joint Commission Research Advisory Board's Stand-
ing Committee on the Scientific Basis for Water Quality
Criteria. Appendix A of the Fourth Annual Report on Great
Lakes Water Quality. Windsor, Ontario, 1976. 123 pp.
International Joint Commission, New and Revised Great Lakes Water
Quality Objectives, Volume II, October 1977. 155 pp.
Reinert, R. E. Pesticide Concentrations in Great Lakes Fish.
Pesticide Monitoring Journal _3_: 233-240, 1970.
Robertson, A., F. C. Elder, and T. T. Davies. IFYGL Chemical
Intercomparisons (IGYFL). Proc. 17th Conf. Great Lakes
Res. p. 682-696, International Association Great Lakes Res.
1974.
Thurston, R. V., R. C. Russo, and K. Emerson. Aqueous Ammonia
Equilibrium Calculations. Tech. Report No. 74-1, Fish-
eries Bioassay Lab., Montana State Univ., Bozeman, 1974.
U.S. Environmental Protection Agency, IFYGL Methodology Roch-
ester Field Office, EPA Region II. Further information
available from USEPA Large Lakes Research Station, Grosse
lie, Michigan, undated.
U.S. Environmental Protection Agency. Quality Criteria for
Water. EPA-440/9-76-023, Washington, B.C. 1976. 501 pp.
25
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1 REPORT NO.
EPA-600/3-80-060
2.
3. RECIPIENT'S ACCESSI Of* NO.
4. TITLE AND SUBTITLE
AN EVALUATION OF HAZARDOUS CHEMICALS
IN LAKE ONTARIO DURING IFYGL
5. REPORT DATE
July 1980 Issuing Date.
6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
G. Fred Lee
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Department of Civil Engineering
Colorado State University
Fort Collins, CO 80523
10. PROGRAM ELEMENT NO.
11. CONTRACT/GRANT NO.
R-803187
12. SPONSORING AGENCY NAME AND ADDRESS
Environmental Research Laboratory-Duluth
Office of Research and Development
U.S. Environmental Protection Agency
Duluth, Minnesota 55804
13. TYPE OF REPORT AND PERIOD COVERED
Final - 10/74 - 4/77
14. SPONSORING AGENCY CODE
EPA/600/03
15. SUPPLEMENTARY NOTES
16. ABSTRACT
Data collected during the IFYGL studies (1972-73) on Lake Ontario are
summarized relative to the recommended International Joint Commission
(IJC) Research Advisory Board water quality objectives or USEPA Quality
Criteria for Water. Data from 247 stations are used to summarize infor-
mation on the following parameters: cadium, zinc, chromium, copper,
fluoride, iron, lead, nickel, manganese, and ammonia. Chlorinated hydro*
carbon data for DDT, dieldrin, and PCBs are discussed relative to con-
centrations determined in water samples and three fish species. Summa-
ries indicate that almost all reported measurements for total cadmium
exceed the IJC water quality objective of 0.2 yg/1 by at least five
times. Values reported for copper also showed a high percentage of mea-
surements equal to or in excess of the recommended IJC water quality ob-
jective. Other metals showed more regional patterns of values equaling
or exceeding water quality objectives. The concentrations of PCBs, di-
eldrin and DDT and its metabolites in Lake Ontario water and fish were
found to exceed the IJC water quality objectives and the USEPA water
quality criteria. If the IFYGL data are representative of Lake Ontario
conditions, studies need to be conducted to evaluate whether the "ex-
cessive" concentrations are indicative of water quality deterioration.
17.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b.IDENTIFIERS/OPEN ENDEDTERMS
C. COS AT I FiCld/GlOllp
Great Lakes
Water quality
Copper
Cadmium
08/H
13. DISTRIBUTION STATEMENT
Release to public
19 SECURITY CLASS (This Report)
Unclassified
21. NO. OF PAGES
34
20 SECURITY CLASS (This page)
Unclassified
22. PRICE
EPA Form 2220-1 (9-73)
26
fr U.S GOVERNMENT PRINTING OFFICE 1980--S57-165/0040
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