. "3. Dimensions of the Problem: Exposure Assessment." Environmental Epidemiology, Volume 1: Public Health and Hazardous Wastes. Washington, DC: The National Academies Press, 1991.
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ENVIRONMENTAL EPIDEMIOLOGY: Volume 1
3
Dimensions of the Problem: Exposure Assessment
EXPOSURE ASSESSMENT IS A crucial component of environmental epidemiology studies that seek to establish causal relationships between exposure to chemical and physical agents from hazardous-waste sites and adverse consequences to human health. The discipline of exposure assessment encompasses numerous techniques to measure or estimate the contaminant, its source, the environmental media of exposure, avenues of transport through each medium, chemical and physical transformations, routes of entry to the body, intensity and frequency of contact, and spatial and temporal concentration patterns. Exposure to a contaminant is defined as “an event that occurs when there is contact at a boundary between a human and the environment at a specific contaminant concentration for a specified period of time; the units to express exposure are concentration multiplied by time” (NRC, 1991, p. 3).
In environmental epidemiology, exposure assessment has proved difficult. Epidemiologic research typically involves retrospective studies. When data are gathered retrospectively, there is an enormous opportunity for exposure assessment to be influenced by apparent disease occurrence, and vice versa. Records of environmental pollution can sometimes provide a surrogate for exposure, but these surrogates are not always available, and direct measures of past exposures have not usually been recorded.
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3
Dimensions of the Problem: Exposure Assessment
EXPOSURE ASSESSMENT IS A crucial component of environmental epidemiology studies that seek to establish causal relationships between exposure to chemical and physical agents from hazardous-waste sites and adverse consequences to human health. The discipline of exposure assessment encompasses numerous techniques to measure or estimate the contaminant, its source, the environmental media of exposure, avenues of transport through each medium, chemical and physical transformations, routes of entry to the body, intensity and frequency of contact, and spatial and temporal concentration patterns. Exposure to a contaminant is defined as “an event that occurs when there is contact at a boundary between a human and the environment at a specific contaminant concentration for a specified period of time; the units to express exposure are concentration multiplied by time” (NRC, 1991, p. 3).
In environmental epidemiology, exposure assessment has proved difficult. Epidemiologic research typically involves retrospective studies. When data are gathered retrospectively, there is an enormous opportunity for exposure assessment to be influenced by apparent disease occurrence, and vice versa. Records of environmental pollution can sometimes provide a surrogate for exposure, but these surrogates are not always available, and direct measures of past exposures have not usually been recorded.
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Rothman (1990) noted estimates of exposure are very often heterogenious, poorly described, and involve low concentrations of toxicants. Although essential to well-designed epidemiologic investigations, exposure assessment has been and continues to be an inadequately developed component of environmental epidemiology, because
the temporal characteristics of site discovery and investigation make it difficult;
the conceptual framework and techniques for evaluation have only recently been established;
epidemiologists often have not understood or given sufficient attention to exposure evaluation.
This chapter has three sections. The first describes the potential for human exposure by identifying toxic chemicals found at hazardous-waste sites. This includes direct site contamination, contamination by unidentified or uncharacterized pollutants, and groundwater contamination from other sources. The second section discusses approaches to exposure assessment and their attendant problems. The third section examines reported exposure assessments associated with hazardous-waste sites and reviews the strengths and weaknesses of the reports.
TOXIC-CHEMICAL EXPOSURE AT WASTE SITES
Although much of the waste produced annually in the U.S. is not listed as hazardous, the U.S. Environmental Protection Agency (EPA) estimated in 1988 that the amount of hazardous waste managed by approximately 3000 licensed facilities was 275 million metric tons (EPA, 1988). In addition, there are a substantial number of uncontrolled disposal sites that contain hazardous wastes and that could present serious environmental or public health problems. For example, municipal waste sludge and incinerator ash can contain toxic materials such as lead, cadmium, mercury, and other toxic materials.
In the late 1970s there was widespread publicity about the indiscriminate dumping of waste that was resulting in release of toxic agents into the environment. The national failure to address the many known and suspected hazards from uncontrolled hazardous waste sites led Congress to pass the Comprehensive Environmental Response, Compensation, and Liability Act of 1980 (CERCLA), generally known as the Superfund law. Under CERCLA's terms, more than 31,000 sites have been reported to EPA's CERCLA Information System (CERCLIS) inventory of sites that could require cleanup. EPA
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has completed more than 27,000 preliminary assessments, and more than 9000 sites have been investigated in detail (EPA, 1988). As of June 1988, EPA's National Priorities List (NPL), included 1236 sites, about 30 percent of which have had initial actions to reduce immediate threats. The number of identified sites represents a small proportion of the sites that are expected to be identified in the future (OTA, 1989).
HAZARDOUS-WASTE SITES
Within the past decade, estimates of the number of potential NPL sites have shifted dramatically. The Office of Technology Assessment (OTA, 1989) concludes that there could be as many as 439,000 candidate sites. This is more than 10 times that estimated earlier by EPA. These sites include Resource Conservation and Recovery Act (RCRA) Subtitle C and D facilities, mining waste sites, underground leaking storage tanks (nonpetroleum), pesticide-contaminated sites, federal facilities, radioactive release sites, underground injection wells, municipal gas facilities, and wood-preserving plants, among others.
One recent EPA survey found that more than 40 million people live within four miles and about 4 million reside within one mile of a Superfund site. Residential proximity does not per se mean that exposures and health risks are occurring, but the potential for exposure is increased. As of December 1988, the Agency for Toxic Substances and Disease Registry (ATSDR) concluded that 109 NPL sites (11.5 percent) were associated with a risk to human health because of actual exposures (11 sites) or probable exposure (98 sites) to hazardous chemical agents that could cause harm to human health. These NPL sites were listed in the categories of “urgent public health concern” or “public health concern.”
The states with the largest number of NPL sites are New Jersey, Pennsylvania, California, Michigan, and New York. They accounted for 464 of 1236 (37.5 percent) sites as of 1991 (Figure 3-1). The activities associated with these sites are shown in Table 3-1. Figure 3-2 depicts the observed contamination of various media as a percentage of 1189 final sites on the NPL as of February 1991. Note that a site can have more than one type of contamination.
Data derived from the 951 ATSDR health assessments at hazardous-waste sites indicate the existence of more than 600 different chemical substances. Some of them are listed in Table 3-2. The documented migration of substances into water, soil, air, and food also is listed in Table 3-2. Most of the identified agents are toxic and represent potential threats to the public health, depending on the degree of expo-
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FIGURE 3-1 Few Superfund sites completely cleaned up. Source: Adapted from Viviano, 1991, with permission.
sure. Of the compounds identified at more than 100 sites, lead, chromium, arsenic, cadmium, nickel, trichloroethylene (TCE), perchloroethylene (PCE), vinyl chloride, methylene chloride, chloroform, benzene, ethylene dichloride (EDC), and polychlorinated biphenyls (PCB) have been identified as either human or animal carcinogens and are classified in group 1 of the ATSDR-EPA list of the 100 most hazardous substances. A list of agents identified at more than 10 proposed and final NPL sites is listed in Appendix 3-A to this chapter, and the original ATSDR list of priority substances can be found in Appendix 3-B.
Buffler et al. (1985) have reviewed the adverse health effects associated with specific toxicants identified at hazardous-waste sites. While discussing the types of chemicals found, the review addresses whether health effects could be detected in studies of populations exposed to these chemicals at waste-disposal sites. Skin and central nervous
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TABLE 3-1 Types of Activities at Hazardous-Waste Sites in the United States (Includes 1177 Final and Proposed Sites Placed on the National Priorities List as of June 1988)
Activity
Final
Proposed
Total
Surface impoundments
295
137
432
Landfills, commercial/industrial
299
113
412
Containers/drums
229
64
293
Other manufacturing/industrial
102
137
237
Landfills, municipal
157
56
213
Spills
111
73
184
Chemical processing/manufacturing
82
78
160
Waste piles
73
46
119
Leaking containers
80
36
116
Tanks, above-ground
80
28
108
Tanks, below-ground
46
42
88
Groundwater plumes
63
12
75
Electroplating
36
27
63
Wood preserving
39
16
55
Waste oil processing
34
16
50
Ore processing/refining smelting
27
9
36
Open burning
24
12
36
Solvent recovery
24
11
35
Outfall, surface water
20
15
35
Military ordnance production/storage/disposal
19
14
33
Military testing & maintenance
16
10
26
Landfarm, land treatment/spreading
18
7
25
Battery recycling
17
6
23
Incinerators
17
1
18
Mining sites, surface
11
4
15
Underground injection
11
2
13
Drum recycling
8
4
12
Sand and gravel pits
7
3
10
Mining sites, subsurface
6
3
9
Road oiling
7
1
8
Laundries/dry cleaners
2
5
7
Sinkholes
6
1
7
Explosive disposal/detonation
2
1
3
Tire storage/recycling
2
0
2
Total sites a:
799
378
1177
a Since each site may have more than one activity, the number of activities is greater than the number of sites.
Source: U.S. Environmental Protection Agency, Office of Emergency Response, Washington, D.C. 20460.
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FIGURE 3-2 NPL: Types of activities at 1189 final sites. Source: Environmental Protection Agency, Office of Solid Waste and Emergency Response, 1991.
system (CNS) effects were the most likely effects to occur from direct contact with waste site chemicals. Hepatic, hematopoietic, renal, reproductive, and CNS effects were the most likely indicators of chronic, low-dose exposure through ingestion.
UNIDENTIFIED OR UNCHARACTERIZED CONTAMINANTS
To date, attention has focused on a relatively small number of chemical contaminants identified at hazardous-waste sites. Many identified or unidentified potential contaminants have received little scrutiny. These uncharacterized pollutants include substances that are not on the ATSDR-EPA list of 100 most hazardous substances, compounds that cannot be identified by standardized or accepted analytical methods, previously unidentified substances that result from in situ transformation processes, and by-products of treatment techniques. MacKay et al. (1989) suggest that large quantities of these potentially toxic compounds may be relatively mobile in the subsurface environment, and a potential exists for these compounds to contaminate groundwater.
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One EPA evaluation (Bramlett et al., 1987) of the composition of leachates from hazardous-waste sites documents the potential problem. The chemical composition of leachates from 13 sites located throughout the U.S. was analyzed. Only 4 percent of the total organic carbon (TOC) in the leachate was characterized by gas chromatography/mass spectroscopy according to their chemical structure. More than 200 separate compounds were identified in the 4 percent fraction. This included 42 organic acids, 43 oxygenated and heteroaromatic hydrocarbons, 39 halogenated hydrocarbons, 26 organic bases, 32 aromatic hydrocarbons, 8 alkanes, and 13 metals. The unidentified 96 percent of organic carbon is of unknown toxicity. Overall, the number of chemical agents found in the 4 percent of the leachate studied is large, and yet this represents only a fraction of the overall organic contribution. In addition to the toxicity of these chemical agents, whether the mobile compounds promote transport of chemical toxicants is an important subject for research.
Research in California by MacKay et al. (1989) has documented the examples of uncharacterized compounds that could have important toxicologic properties or significance for transport. Chlorobenzenesulfonic acids have been identified at the Stringfellow Acid Pits in Glen Avon and at the BKK landfill in West Covina; arsenicals were found at a site in Rancho Cordova; and brominated alkanes were found at the Casmalia hazardous-waste disposal site, along with high melting explosive (HMX) (cyclotetramethylene tetramintriamine), research department explosive (RDX) (cyclonite), and mutagenic explosive by-products from the Lawrence Livermore National Laboratory, to name just a few.
NONPOINT SOURCES
As important as the NPL sites are, focusing attention solely on the chemicals identified at these sites understates the potential scope of the problem of groundwater contamination. Toxic contaminants in groundwater can be considered as “hazardous waste” in a public health or toxicologic context, in contrast to the regulatory framework for defining hazardous waste. Secondly, contaminated groundwater close to defined hazardous-waste sites may act as a confounder in environmental epidemiologic investigation. In California, for example, 70 percent of public drinking water comes from groundwater (Leeden et al., 1990). Moreover, recent surveys show that problems with ground-water are not unique to California. In 1986, EPA reported to Congress that groundwater contamination from organic chemicals had occurred or was occurring in 70 percent of the states; 65 percent and
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60 percent had groundwater contamination from metals and pesticides, respectively (EPA, 1987a). Contamination from nonpoint sources, such as agricultural runoff, may not derive from a specific hazardous-waste site, but is toxic waste and could pose significant health hazards unless recognized and controlled. For example, according to EPA (Appendix 3-A), the reproductive toxicant and carcinogen dibromochloropropane (DBCP) has been identified at only one NPL site. Although DBCP use was suspended in California in 1979, it persists in the environment and has been detected in more than one-fifth of drinking water wells in California not related to NPL sites. MacKay and Smith (1990) have reviewed the status of groundwater monitoring in California for “active” ingredients from pesticides, based on samplings from 1975 to 1988 of 10,929 wells. DBCP was detected in 2353 wells; in more than 1000 wells, it exceeded the state maximum contaminant level (MCL) of 0.2 parts per billion (ppb). About 100 of the wells that exceeded the limit were in public supply systems that serve large numbers of customers. One hundred were in smaller public supply systems, and others were private supply wells. It is estimated that approximately 500,000 Californians have DBCP in their drinking water supply.
In addition to the active ingredients in pesticides, so-called “inert” ingredients also contaminate groundwater in California and elsewhere. Cohen and Bowes (1984) have estimated that 200 million pounds of inert ingredients were released to the land in pesticide use between 1971 and 1981. These are rough estimates because the composition of inert ingredients in a commercial pesticide formulation is proprietary. In some cases, materials that have been banned as active ingredients continued to be used as inert ingredients. Reports published by MacKay and co-workers (MacKay et al., 1987; Smith et al., 1990) note that inert ingredients can include TCE, PCE, formaldehyde, pentachlorophenol, ethylene dichloride, and 1,4-dichlorobenzene, all of which are known to be toxic. In 1987, EPA confirmed that these and other inert ingredients can have toxicologic significance (EPA, 1987b). Of the approximately 1200 substances used as inert ingredients in pesticide products, EPA (1987b) has determined that about 50 are of “significant toxicological concern” on the basis of their carcinogenicity, adverse reproductive effects, neurotoxicity, or other chronic effects. An additional 60 compounds were considered “potentially toxic.” These pollutants are not derived from hazardous-waste sites, but they illustrate the potential for groundwater contamination from agricultural chemical waste. They constitute a hazardous-waste hazard in themselves, whereas their impact on epidemiologic investigation of hazardous-waste sites would be that of a confounder.
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Since 1984, public drinking water supplies in California have been investigated by the California Department of Health Services (DHS) to determine the extent of groundwater contamination in the state (Smith et al., 1990). During the period 1984-1988, approximately 7000 large and small supply systems were evaluated, and about 1500 wells were found to be contaminated with organic chemicals. The chemicals identified in this monitoring included pesticides and solvents such as PCE, TCE, chloroform, EDC, TCA, and carbon tetrachloride. A total of 409 (5.6 percent) wells had one or more chemicals exceeding the state's action level or the Maximum Contaminant Level (MCL), and 18.3 percent of the wells had some contamination. Since early 1986, the state has sought to identify the sources of organic chemical pollution of contaminated supply wells identified by the monitoring program, but there is no comprehensive effort to identify new sources of groundwater contamination, and the evaluation of existing sources is slow. The MacKay and Smith study (1990) also documents groundwater contamination from a variety of solvents and toxic active ingredients in pesticides. These include 1,2-dichloropropane and ethylene dibromide (EDB), atrazine, simazine, bentazon, aldicarb, diuron, prometon, and bromacil, all of which have been linked with adverse human health effects. These data indicate the need for periodic screening of groundwater supplies in areas of high chemical use.
Table 3-3 lists the major causes of groundwater contamination reported by states. NPL sites are included, but other sources of contamination are also important. The groundwater contamination from sources other than hazardous-waste sites is relevant to the conduct of exposure assessment in environmental epidemiology. For example, in the city of Santa Maria, California, which is adjacent to the operating Casmalia hazardous-waste site, numerous wells were closed because of contamination by organic solvents (Breslow et al., 1989). Possible sources of well water contamination include leaching from the Casmalia hazardous-waste disposal site (unlikely), use of such solvents as TCE and PCE to clean septic tanks (likely), and runoff of agricultural chemicals (likely). Groundwater contamination of this type from unrecognized nonpoint sources poses a twofold problem. Such contamination may provide important additional exposures that increase the overall health risk and can reduce the likelihood of finding effects in studies that fail to take these exposures into account.
ASSESSMENT OF THE NATURE AND EXTENT OF EXPOSURE
There is no question that large quantities of highly toxic chemicals are found at hazardous-waste sites. Even though it is not always
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exposures in connection with soil, including studies of ingested plants and fish from contaminated water, characterization of chemical transformation, and better measurements of residues.
Weaknesses in data employed on exposure are common to most studies of hazardous-waste sites that the committee has reviewed. The flaws reflect historical tendencies to collect data to conform to environmental needs, rather than to meet the needs of public health assessment. Usually, exposure estimates are made with one medium—water—although others may be critical. Site assessments should use more realistic exposure measures, including direct studies of contaminants at the tap of incoming domestic water supplies, in order to improve their utility for epidemiologic research. In addition, where concerns have been raised, efforts should be made to include relevant soil and airborne measurements, so that integrated exposure assessment can be conducted.
APPENDIX 3-A Frequency of Substances Reported at Final and Proposed NPL Sites * (3/91)
1,1,2-TRICHLOROETHYLENE (TCE)
401
LEAD (PB)
395
CHROMIUM AND COMPOUNDS, NOS (CR)
310
TOLUENE
281
BENZENE
249
TETRACHLOROETHENE
210
1,1,1-TRICHLOROETHANE
202
CHLOROFORM
196
ARSENIC
187
POLYCHLORINATED BIPHENYLS, NOS
185
CADMIUM (CD)
179
ZINC AND COMPOUNDS, NOS (ZN)
159
COPPER AND COMPOUNDS, NOS (CU)
150
XYLENE
136
1,2-TRANS-DICHLOROETHYLENE
134
ETHYLBENZENE
130
PHENOL
126
1,1-DICHLOROETHANE
124
METHYLENE CHLORIDE
107
1,1-DICHLOROETHENE
106
MERCURY
97
VINYL CHLORIDE
92
CYANIDES (SOLUBLE SALTS), NOS
90
NICKEL AND COMPOUNDS, NOS (NI)
83
CARBON TETRACHLORIDE
81
1,2-DICHLOROETHANE
77
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CHLOROBENZENE
65
PENTACHLOROPHENOL (PCP)
62
NAPHTHALENE
60
DDT
50
METHYL ETHYL KETONE
56
TRICHLOROETHANE, NOS
49
MORE THAN 15 SUBSTANCES LISTED
48
BARIUM
47
MANGANESE AND COMPOUNDS, NOS (MN)
44
PHENANTHRENE
41
HEAVY METALS, NOS
40
ACETONE
40
BENZO(A)PYRENE
37
IRON AND COMPOUNDS, NOS (FE)
33
CHLORDANE
33
VOLATILE ORGANICS, NOS
33
BENZO(J,K)FLUORENE
30
CHROMIUM, HEXAVALENT
30
PYRENE
29
CIS-1,2-DICHLOROETHYLENE
29
LINDANE
28
1,1,2-TRICHLOROETHANE
28
ARSENIC AND COMPOUNDS, NOS (AS)
27
BIS(2-ETHYLHEXYL)PHTHALATE
27
DICHLOROETHYLENE, NOS
26
ANTHRACENE
26
1,1,2,2-TETRACHLOROETHANE
26
STYRENE
23
URANIUM AND COMPOUNDS, NOS (U)
22
DDE
22
TETRACHLOROETHANE, NOS
21
CREOSOTE
19
FLUORENE, NOS
19
DIOXIN
18
SELENIUM
19
ETHYL CHLORIDE
18
CHRYSENE
18
RADON AND COMPOUNDS, NOS (RN)
18
ASBESTOS
17
TRINITROTOLUENE (TNT)
17
DDD
17
DICHLOROETHANE, NOS
17
DIELDRIN
17
SULFURIC ACID
17
WASTE OILS/SLUDGES
17
ACENAPHTHENE
16
RADIUM AND COMPOUNDS, NOS (RA)
16
ALDRIN
16
AROCLOR 1260
16
ENDRIN
16
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TRICHLOROFLUOROMETHANE
16
1,4-DICHLOROBENZENE
16
ACID, NOS
15
DI-N-BUTYL PHTHALATE
15
DICHLOROBENZENE, NOS
15
METHYL ISOBUTYL KETONE
15
M-XYLENE
14
1,2-DICHLOROBENZENE
14
ALUMINUM AND COMPOUNDS, NOS (AL)
14
CHLOROMETHANE
14
AMMONIA
13
TETRAHYDROFURAN
12
THORIUM AND COMPOUNDS, NOS (TH)
12
HEXACHLOROBENZENE
12
HEPTACHLOR
11
TOXAPHENE
11
TRIBROMOMETHANE
11
1,2-DICHLOROPROPANE
11
RDX (CYCLOTRIMETHYLENETRINITRAMINE)
10
ANTIMONY AND COMPOUNDS, NOS (SB)
10
BARIUM AND COMPOUNDS, NOS (BA)
10
BERYLLIUM AND COMPOUNDS, NOS (BE)
10
* This list is a frequency of substances documented during HRS score preparation, not a complete inventory of substances at all sites.
“NOS”—Not otherwise specified, e.g., not identified as to specific isomer or congener.
APPENDIX 3-B ATSDR Priority List of Substances for Toxicological Profiles (Listed in Federal Register 52(74), Friday April 17, 1987, p. 12869)
CAS No.
Substance Name
Priority Group 1
50328
Benzo(a)pyrene
53703
Dibenzo(a,h)anthracene
56553
Benzo(a)anthracene
57125
Cyanide
60571
Dieldrin/aldrin
67663
Chloroform
71432
Benzene
75014
Vinyl chloride
75092
Methylene chloride
76448
Heptachlor/heptachlor epoxide
79016
Trichloroethene
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