Document 3JBxpKKvrVeN4gzwBLG2Gj3z0

U ENVIRONMENTAL LEVELS OF PCB's Doris J. Ruopp Vincent J. DeCarlo U.S. Environmental Protection Agency Washington, D.C. 20460 ABSTRACT Since . the 1966 discovery in Sweden that chlorinated biphenyls were widely dispersed in the etwironment their environmental levels have been the subject ' of many studies with the results indicating that PCB's can have adverse ecological and toxicological effects. However, a well planned national approach to environmental sampling has not been attempted thus hindering making a national assessment of the PCB problem. This paper reviews the levels that are currently being found in. the environment. ' INTRODUCTION Since the 1966 discovery in Sweden that chlorinated biphenyls were widely dispersed in the environment, their levels have been the subject of many studies both abroad and in the United States. Extensive laboratory and environmental measurements indicate that PCB's can have adverse ecological and toxicological effects, are very resistant to environmental degradation and ore being discharged by many different sources. This paper will focus on the current PCB data base in an effort to assess the PCB levels in the environment on a national basis. ENVIRONMENTAL PCB SOURCES Before the PCB data base is examined, it would be of interest' to review bow these chemicals get into the environment. The major sources contributing to the environmental levels of PCB's are industrial effluents, manufacturing processes, consumer and industrial waste materials, sewage -treatment facilities and accidental spills. Lacking extensive air and soil data from these sources, available water data arc shown in Table 1. The 5 major PCB spills in 1973-75 all involved transformers. In 4 of those incidents, the PCB's were spilled on soil while in the fifth the transformer was dropped on a pier and the contents were spilled into the water. In the latter incident, 283 gallons were spilled and it was estimated that only 70-90 gallons were recovered. In all cases the material that could be recovered was drummed up and entombed at a cost approaching $2.3 million. . REVIEW OF THE PCB DATA BASE To assess the scope and . extent of PCB's in the environment, all national surveys and national data "bases maintained by the U.S. Environmental Protection Agency (EPA) were examined, including STORET, the national water quality storage and retrieval system, the National Soils Monitoring Program for Pesticide Residues and the Human Monitoring Program. In addition, data from special data bases maintained by the United States Geological Survey and the open literature were also examined along with available unpublished reports. Using these data, maps were constructed showing the concentrations of PCB's in urban soils and the aquatic environment. The data from the national . surveys show that a great deal of effort has been expended and continues to be expended but that the data are very limited. On examination, all States are believed to show some level of PCB contamination. In Table 2 States which had significant levels in at least one medium are listed with their reported PCB levels for surface and ground water, bottom sediments and fish. In Table 3, a number of localized studies are listed along with the reported environmental data. In all these studies the most extensive measurements have been In fish. TABLE 1 ENVIRONMENTAL SOURCES OF PCB's SOURCE EFFLUENT WATER CON CENTRATIONS (ppb) PAPER MILLS Wisconsin WASTE PAPER MILLS Wisconsin INDUSTRIAL EFFLUENTS 2 California 2 Wisconsin Ohio2 " Michigan-5 MUNICIPAL WASTE ,WATER TREATMENT PLANTS Michigan ^ Wisconsin Ohio2 2 California CAPACITOR AND TRANSFORMER FACILITIES , . New Yorx ^ Massachusetts 0.1 - 18.5 18.5 0- .04 0- .1 - 76 0.25 17 7000 0.5 .05 - 10 . 0.16 - 17.0 17 76 2800 42.5 PCB MANUFACTURING FACILITY East St. Louis'5 ' .87 SPILLS . Variable 1. Kleinert, S. J.Environmental Status of PCB in Wisconsin, May 8, 1975, Wisconsin Department of Natural Resources. 2. PCB's and tlie Environmental, Report of the Interdepartmental Task Force on PCB's, National Technical Information Service, 1972. 3. Statement of Concerns of the Lake Michigan Toxic Substances Committee Related to Poly chlorinated Biphenyls, June 1975. Prepared by Karl F. Bremer, USEPA, Chicago, 111. 4. Unpublished Data - Royal J. Nadeau and Robert P. Davis, Investigation of Polychlorinated Biphenyls In the Hudson River, Hudson FallsFt. Edward Area, August 1974. 5. Field Sampling and Analysis of Toxic Pollutant's Interim Report, Battelle, Pacific Northwest Laboratories, August 1974. DSW 362047 STLCOPCB4098106 WATER On the basis of the national aquatic environmental data collected in 1971-1972 and in 1974, a continuing widespread accumulation of PCB's in water, sediment and fish appears to be occurring. However, no trend analysis is possible with the available measurements. For example, whole water measurements have been taken throughout most of the country but- those states reporting non zero readings are few in relation to the number of states shoving zero concentrations. This is due both to the low solubility of PCB's and to the usual analytical procedure that limits detectability to the 0.1 ppb level. More meaningful water concentrations were obtained in .the Lake Ontario^ and Orange County, California^ studies where concentrations in water at the ppt (ng/1) level were measured. At these levels, changes in PCB concentrations could be found with distance and time and could be related to other measurable parameters such as PCB concentrations in sediment, flora and fauna. SEDIMENTS Since PCB's are relatively insoluble, it is not surprising that bottom deposits have shown significant concentrations. Although 30 states collected samples in the 1974 study, 15 had less than 4 stations reporting and showed zero readings. Of the remaining 15, with at least 4 reporting stations, 13 showed detectable concentrations. Since the 13 states involved were not necessarily the same in both studies, only a very broad comparison may be made, i.e., five states had lower concentrations, four states were higher and four did not sample again. 3 We may conclude, then, that in those states with any monitoring effort in the 1974 study, PCB's are present in bottom deposits and the levels are not any lower than in the 1971-72 study. Considering the persistence of PCB's, a significant proportion of the nation's waters are now affected and will continue to be. SOILS The National Soils Monitoring Program is a small sampling effort studying only 5 urban areas each year. However, PCB's were detected in three of the five cities sampled in each of the years for which data are available, 1971-73. Of the 22 positive readings 17 of them were below 1 ppm. Of the cities sampled in 1973, Pittsfield, Mass., was of particular interest because it has a large transformer and condenser plant using large quantities of' PCB's. Six different sampling sites within one mile of the plant show no detectable PCB- residues. In contrast, the soil surrounding another facility in Illinois using PCB's in the manufacture of investment casting waxes was recently measured for,, PCB content. Samples taken in an '.area one-quarter mile radius around the plant ranged in value from 0.77-5.2 ppm. The PCB's identified were mixtures of Aroclor 1260 and decachltrrobiphenyl. Levels up to 1.8 ppm Aroclor 1260 were found at 1-1/4 miles from the plant. Samples were collected ,from this facility as part of a study being conducted for the Office of Toxic Substances at sites i suspected to have PCB concentrations. Other sites sampled in March of 1975 were in the vicinity of an investment casting company in Michigan arjd the PCB manufacturer in Illinois. Surface soil samples were collected at each site up to a distance of approximately one mile from the plant boundary*' at 1/4 mile intervals in all directions. PCB's 3e detected in soils at both sampling locations." Concentrations ranged from the detection limit of 0.001 ppm to over 20 ppm. The distribution of all PCB's analyzed appears higher near .the plant site and generally decreases with distance from the site.4 Details of the sampling sites and the concentration levels measured are- shown in Figure 1. TABLE 2 . SELECTED STATE DATA ON ENVIRONMENTAL LEVELS OF PCB's State Surface and Ground Water Ng/1 Bottom Sediment Ng/kg Fish3 ppm AL AR CA CO CT fl . GA ' IL . IA ' MD MA MI MN MS NB NJ NY OH OR PA PR SC TX - UT VA wv . WI 0.1 0.3 0.1-0.2 0.1-2.1 0.1 0.2 0.1-0.3 - 0.1 0.1-4.0 0.2 0.1 0.1-3.0 0.1 20-2,400 20-190 5-3502 5-3,200 10-1,300 10-1,200 1.53-5.48 1.69-3.88 2.16-5.34 0.10-1.25 0.52-1.18 1.21-11.3 0.35-1.41 0.56-1.31 50-170 3-8002 3-13,0002 1-5-140 6-7002 t 30-200 7.9-290 5-80 10 4.00-11.7 0.44-1.09 0.47-4.58 0.10-4.00 2.68-9.50 1.73-8.07 0.71-3.62 1.94-2.48 0.10-7.3 0.10- .22 0.15-2.14 0.31_1.20 1.24-14.8 All data in this column taken from Hans J. Crurnp--Wiesner, Herman R. Feltz and Marvin L. Yates,, A Study of the Distribution of Poly- chlorinated Biphenyls in the Aquatic Environ ment, Jour. Research U.S. Geol. Survey 1^, ' 603 (1972, unless otherwise noted. 2. USGS Sediment data, 1974. 3. All data in this column taken from Croswell Henderson, Anthony Inglis and Wendell L. Johnson, . Organochlorine Insecticide Residues in -Fish Fall 1969 National Pesticide Monitoring Program, . Pesticide Monitoring Journal 5^, 1(1971). O 2 DSW 362048 STLCOPCB4098107 U - TABLE 3 SELECTED PCB STUDIES O - Fish Water Sediment Plankton lake's Lake Ontarioif 4 - (ppm) ,0.14 - 9.17 (UB/1) 0.035 - 0.097 (yg/kg) 43 - 245 (ppm) 3.4 - 11, Lake Erie3 4 0.2 - 7.8 Lake Superior5 0.3 - 5.6 Lake Huron^ Lake Michigan^. 9 0.16 - 11.0 0.1 - 165.3 3.72 - 636 ... Cayuga LakelO Lake St. Clairl6 3.4 - 9.7 tr - 3.8 0.1 - 0.2 . RIVERS Iowa Mississippi River?-?- 0.9 - 5.5 _ Texas ' Brazos River?? 0.1 -- 0.5 Utah Green River?? 0.1 New York Hudson *-3 7 - 350 1.0 - 2800 6.6 - 6,700,000 Michigan Saginaw River^ ?^ Kalamazoo River? ?5 6.9 - 165.3 <0.01 - 164.56 0.1 - 0.21 0.1 - 0.45 100 - 560 Portage Creek? 0.1 - 0.48 10 - 475,400 Wisconsin Milwaukee .02 - 2.17 MARINE ENVIRONMENT Atlantic Oceania* 18 _ 0.038 - 0.190 0.0009 - 0.0036 Bay of Fundy?9 0.07 - 1.54 Gulf of Mexico/Carib bean Sea?*?> 21 0.032 - 0.059 Southern California?? 0.04 - 6.6 .1 Clarence L. Haile, Gilman Veith, G. Fred Lee and William C. Boyle, Chlorinated Hydrocarbons in ' 0.0015 - 0.019 0.157 - 1. '" 13. Unpublished data - Royal J. Nadeau and Robert P. Davis, Investigation of Polychlorinated Bi the Lake Ontario Ecosystem, EPA-660/3-75-002, phenyls in the Hudson River (Hudson Falls - Ft. . June 1975, U.S. E.P.A., Corvallis, Oregon. 2 Klaus L. Kaiser, Mirex, An Unrecognized Contami nant of Fishes from Lake Ontario, Science 18, Edward Area, August 1974. 14. Unpublished data - John L. Hesse, Monitoring for Polychlorinated Biphenyls in the Aquatic Envi 523 (1974). ronment, Kay 1973. 3. Richard L. Carr, Charles E. Finsterwalder and Michael J. Schibi, Pesticides Monitoring Jour 15. Unpublished data - Michigan Water Resources Com mission, Evaluation of the Aquatic Environment, nal 6:23 (1972). of the Kalamazoo River Watershed, May 1972. 4. John R. M. Kelso and Richard Frank, Organochlorine 16. Michigan Department of Agriculture, Bureau of . Residues, Mercury, Copper and Cadmium in Yellow Consumer Protection, 1973 Great Lakes Environ Perch, White Bass and Smallmouth Bass, Long mental Contaminants Study. . Point Bay, Lake Erie, Trans. Amer. Fish. Soc., 17. T. F. Bidleman and C. E. Olncy, Chlorinated Hyrdo- 103:577 (1974). carbons in the Sargasso Se^ Atmosphere and Sur 5. Unpublished data. Gilman D. Veith and G. E. Glass, face Water, Science 183:516, 1973. PCB's and DDT in Fish from Western Lake Superior, 18 George R. Harvey, Helen P. Miklas, Vaughan T. Bowen . U.S. E.P.A., Duluth, Minnesota. 6 Unpublished Data - John L. Hesse, Bureau of Water and William G. Steinhauer, Observations on the Distribution of Chlorinated Hydrocarbons in Management, Michigan Department of Natural Re Atlantic Ocean Organisms, Journal of Marine Re sources, June 1973. . search 32:103 (1973). 7. Unpublished data - State of Michigan Water Re 19. V. Zitko, 0. Htttzinger and P.M.K. Choi, Contamin sources Commission, Polychlorinated Biphenyl Sur ation of the Bay of Fundy - Gulf of Maine Area vey of the Kalamazoo River and Portage Creek in with Polychlorinated Biphenyls, Polychlorinated . the Vicinity of the City of Kalamazoo, 1972. . 8 Gilman D. Veith and Fred G. Lee, Chlorohiphenyls Terphenyls, Chlorinated Dibenzodioxins and Dibenzofurans, Environmental Health Perspectives, in the Milwaukee River, Water Research, 1971. 1:47 (1972). .9. Unpublished data - Schacht 1974, EPA 600/3-74-002. 10 Carl A. Bache, James W. Serum, William D. Youngs and Donald J. Link, Polychlorinated Biphenyl. 20. C. S. Giam, A. R. Hanks, R. L. Richardson, W. M.Sackett and M. K. Wong, DDT, DDE, and Polychlor inated Biphenyls in Biota from the Gulf of Mex Residues: Accumulation in Cayuga Lake Trout ico and Caribbean Sea - 1971. Pesticides Moni . --Vith Age, Science 177:1191 (1972). 11 Lauren G. Johnson and Robert L. Morris, Chlorin toring Journal 6:139 (1972). 21. C. S. Giam, M. K. Wong, A. R. Hanks, W. M. Sackett': ated Insecticide^Residues in the Eggs of Some and R. L. Richardson, Chlorinated Hydrocarbons Freshv;ater Fish, Bulletin of Environmental Con in Plankton from the Gulf of Mexico and Northern tamination and Toxicology 11:503 (1974). California, Bulletin of Environmental Contam 12. Jean A. Schulze, Douglas B. Manigold and Freeman ination and Toxicology 9:376 (1973). L. Andrews, Pesticides in Selected Western 22. the Ecology of the Southern California Bight: Streams 1968-197.1, Pesticides Monitoring Jour Implications for Water Quality Management, nal 7:73 (1973). Southern California Coastal Water Research Pro- ' ject, 1500 East Imperial Highway, El Segundo, 1973. DSW 362049 STLCOPCB4098108 Figure 1 Concentration of PCB's in Soil with Distance (ppm) Investment Casting Company Arcelor 1260 Investment Casting Wax Manufacturer DSW 362050 STLCOPCB4098109 AIR PCB measurements in air along with the related transport studies are practically nonexistent. Harvey and Steinhauer-* have reported levels ranging from 3.9 - 5.3 ng/m3. Air measurements by Bidleman and Olney for Rhode Island ranged from 2.1-9.4 ng/m3 and from 0.21 - 0.65 ng/m3 at Bermuda.^ Snow melt water data from Wisconsin ranged from zero to 0.24 ppb. The suggestion has been made that atmospheric fallout may be the most significant source of PCB discharge to the waters of the state of Wisconsin. ^ PISH Fish have been studied on a nationwide basis by the Department of the Interior since 1967. In the 1969 study, PCB levels were identified in fish from 35 states. Data from the nationwide sampling programs, 1970-1973, are currently being prepared but were not available for this report. Consequently, nationwide fish data are not available any more currently than 1969, with the exception of the isolated studies listed in Table 3. The 1969 national study showed PCB levels generally within the FDA 5 ppm guideline. In the Great Lakes area, PCB levels in fish from Lake Michigan were so high, 7.6-10.9 ppm, that FDA seized shipments of coho salmon in May 1975.^ Although transport mechanisms are not well known and would vary through different ecosystems, it is interesting to consider the Lake Ontario Ecosystem Study summarized in Table 4. From this study an estimate of biomagnificalion is possible giving a sediment to fish ratio of 1:120. The FDA guideline of 5 ppm in the edible portion of fish corresponds to a sediment concentration of 41 ppb - a figure exceeded in all 13 states reporting through USGS in 1974. HUMANS With PCB's as widespread across various media as they are, it is expected that levels would be identified in humans as well. 'Hie Human Monitoring Program, in 1972, found that 3035 out of 4102 samples from 31 States showed levels ranging from less than 1 ppm to more than 3 ppm. In 1973, 964 out of 1277 samples from 28 States again showed levels in the same range. In both years approximately 75% of the adipose tissue analyzed contained some polychlorinated biphenyls. Unfortunately we do not know age, occupation or residential histories of the cases involved so It Is difficult to trace the levels back to the potential sources. CONCLUSIONS Although there are many national and state groups collecting environmental PCB data, limitations in the current data base prevent one from making a uniform national assessment of PCB environmental levels. It appears that if a well planned national approach to sampling were attempted, the data base could be improved in a very short period of time. TABLE 4 LAKE ONTARIO ECOSYSTEM1 FISH, yg/g Alewife Smelt Slimy Sculpin .14 - 4.36 1.40 - 3.49 1.58 - 9.17 WATER, ng/1 38 ' - 97 SEDIMENT, ng/g 43 - 245 NET PLANKTON, yg/g 3.4 - 11.8 1. Haile, C. L., Veith, G. D., Lee, G. F., Boyle, W. C., Chlorinated Hydrocarbons in the Lake Ontario Ecosystem (IFYGL) June, 1975. REFERENCES 1. Haile, C.L., Veith, G.D., Lee, G.F., Boyle, W.C., Chlorinated Hydrocarbons in the Lake Ontario Ecosystem (IFYGL), June 1975, 2. McDermott, D.J., and Hansen, T.C., Inputs of DDT, PCB and Trace Metals from Harbors, Coastal .Water Research Project Annual Report, 1975. 3. U.S. Geological Survey. 4. Environmental Polychlorinated Biphenyl Contamination near Sites of Manufacture and Use, Environmental Science and Engineering, Inc., 1975. 5. Harvey, G.R. and Steinbauer, W.G., Atmospheric Transport of Polychlorinated Biphenyls to the North Atlantic, Atmospheric Environment, Vol. 8, 1974. 6. Bidleman, T.F., and Olney, C.F., Chlorinated Hydro carbons in the Sargasso Sea Atmosphere and Sur face Water, Science, Vol. 183, February 1974. 7. Kleinert, S.J., Environmental Status of PCB's in Wisconsin, May 8, 1975, Wisconsin Department of Natural Resources. 8. Henderson, C., Inglis, A., Johnson, W.L., Organochlorir.e Insecticide Residues in Fish - Fall 1969 National Pesticide Monitoring Program, Pesticides Monitoring Journal, Vol, 5, No. 1, June 1971. 9. Bremer, Karl E., Draft copy of "Statement of Con cerns of the Lake Michigan Toxic Substances Com mittee related to PCB's," June 1975. DSW 362051 STLCOPCB4098110