LIOC-/f7(J A Special NOAA 20th Anniversary Report Coastal Environmental Quality in the United States, 1990 Chemical Contamination in Sediment and Tissues tm^ -^ .^^ .jiT' 4S '"-*>»k^ ^*PW*S« *«^- ^^O U. S. Department of Commerce National Oceanic and Atmospheric Administration National Ocean Service 1^- National Status and Trends Program Since 1984, the Office of Oceanography and Marine Assessment has monitored, through its National Status and Trends (NS&T) Program, the concentrations of toxic organic compounds and trace metals in bottom-feeding fish, shellfish, and sedi- ments at almost 300 coastal and estuarine locations throughout the United States. The objective of the program is to determine the status and long-term trends of toxic contamination in these important areas. Samples collected annually through the program are analyzed to determine levels of synthetic chlorinated compounds (e.g., DDTs) , polychlorinated biphenyls (PCBs), polynucleararomatic hydrocarbons (PAHs), and toxic trace metals (e.g., mercury and lead). NOAA's NS&T Program is the first to use a uniform set of techniques to measure coastal and estuarine environmental quality over relatively large space and time scales. A "specimen bank" of samples taken each year at about 10% of the sites is maintained at the National Institute of Standards and Technology for future, retrospective analyses. A related program of directed research is examining the relationships between contaminant exposures and indicators of biological responses in fish and shellfish (i.e. bioeffects) in areas that are shown by the NS&T monitoring results to have high levels of toxic chemicals. This report, based on six years of results from the NS&T Program and other monitoring efforts, describes the spatial extent and severity of chemical contamina- tion and changes in concentrations of contaminants over the last decade. Additional information on NOAA's NS&T Program and related activities is available from: Thomas P. O'Connor, Coastal and Estuarine Assessment Branch, Ocean Assessments Division, Office of Oceanography and Marine Assessment, National Ocean Service, National Oceanic and Atmospheric Administration, 6001 Executive Boulevard, Rockville, MD 20852. A Special NOAA 20th Anniversary Report Coastal Environmental Quality in the United States, 1990 Chemical Contamination in Sediment and Tissues Thomas P. O'Connor Manager National Status and Trends Program / W^^\..\.:>^^ .^p"j;'^^^ Coastal and Estuarine Assessment Branch Ocean Assessments Division Office of Oceanography and Marine Assessment National Ocean Service National Oceanic and Atmospheric Administration Rockville, Maryland 20852 Introduction Reports of beaches being closed, trash washing ashore, prohibitions on shell- fishing, health warnings to seafood con- sumers, waste discharges to the sea, ocean dumping, and habitat losses have aroused considerable public concern about the quality of the coastal environ- ment in the United States. To assess the effects of human activities on the quality of coastal and estuarine areas throughout the Nation, the National Oceanic and Atmospheric Administra- tion (NOAA) created the National Status and Trends (NS&T) Program to monitor trends of chemical contamination in space and time and to determine bio- logical responses to that contamination. Since 1984, annual chemical analyses for trace metals and organic contami- nants, e.g., pesticides, have been made on surface sediments, on livers of ben- thic fish, and on whole soft-parts of mussels and oysters collected from a network of almost 300 sites around the U.S. The need for this type of national moni- toring of ambient environmental quality was recently emphasized by the U.S. National Research Council. Its report (NRC, 1990) indicated that the United States annually spends more than $1 30 million on coastal environmental moni- toring, but that most is devoted to com- pliance monitoring, i.e., testing waste- waters and other materials prior to dis- charge or to performing measurements prescribed by regulation very near to discharge points. Since compliance monitoring, by design, covers very small spatial scales and short time periods, programs such as NOAA's NS&T Pro- gram are required to focus on wider public concerns about the long-term effects of coastal pollution throughout the U.S. This report, based on six years of results from the NS&T Program and other monitoring efforts, describes the spatial extent and severity of chemical con- tamination and changes in concentra- tions of contaminants over the last dec- ade. While conclusions are always subject to new information, it appears that, on a national scale, high and bio- logically significant concentrations of contaminants measured in the NS&T Program are limited primarily to urban- ized estuaries. In addition, levels of those contaminants have, in general, begun to decrease in the coastal U.S. Sampling Sites NOAA's NS&T Program is designed to describe national, rather than local, dis- tributions of contamination. Since Its inception, the primary criterion for NS&T site selection has been the collection of samples from places that are "represen- tative" of large coastal areas and the avoidance of small-scale patches of con- tamination, or "hot spots." In particular, no sites were knowingly selected near waste discharge points. For the "Mus- sel Watch" component of the NS&T Pro- gram, a site also has to have a suffi- ciently large and robust population of mussels or oysters to provide annual samples for an indefinite period. NOAA sampling sites are not uniformly distributed. Almost half of them are in urban estuaries, within 10 miles of the centers of populations in excess of 1 00,000 people. This choice is based on assumptions that contamination is 1 higher, more likely to be causing biologi- cal effects, and more spatially variable in urban, as opposed to njral, coastal areas. The same assumptions have led to sites being closer together in estuar- ies and bays than along open coasts. Contaminants Measured The NS&T Program monitors concen- trations of trace metals and organic compounds in sediment and in tissues. Except for most chlorinated organic compounds — DDT and PCB, for ex- ample, whose existence is due to hu- man activity — some concentration of chemicals in sediments and organisms is natural and would be present even in the absence of human activity. Only sediments and tissues that contain chemical concentrations in excess of natural levels are considered to be "contaminated." The exact line demarcating natural concentrations from contamination is not easily drawn because it depends on many local and regional conditions. This report highlights NS&T sites where concentrations are highest and, while cases exist where high concentrations might be natural, for the most part, they are due to discharges to coastal waters from human activities. Data on concentrations of the seven trace metals and four groups of organic compounds listed in Table 1 are used in this report to describe the status and trends of contamination in the coastal and estuarine areas of the U.S. Con- centrations of all of these chemicals can serve as indicators of human activity. While the metals all have different uses, they can be categorized as chemicals whose discharge to the environment has been enhanced through industriali- zation. The groups of organic compounds can- not be categorized so generally. Two of those groups, total DDT (tDDT) and chlordane (tCdane), are chlorinated pesticides. Use of DDT in the United States was banned in 1970. The use of chlordane on crops and ornamental plants was first restricted in 1974. Its major use as a termiticide came under severe restriction in 1988. Polychlorinated biphenyls (tPCB) are a mixture of compounds based on the biphenyl molecule chlorinated to vari- ous extents. It was first used in 1 929 for a number of industrial purposes. Its high heat capacity and low dielectric con- stant were exploited for its major use in electrical transformers and capacitors. Its use in the United States began to be phased out in 1971 and it has been banned in new devices since 1976. All of these banned compounds — tDDT, tCdane, and tPCB — continue to be used in other countries and still exist in the environment. In the United States, chlordane is still in the ground as a ter- miticide, PCB-containing devices are still in use, and DDT, while no longer used, remains in the environment be- cause (like chlordane and PCB) of its resistance to degradation. The pesti- cide DDT is metabolized to DDE and DDD in the environment, but the tDDT group of compounds resists further degradation. Polycyclic aromatic hydrocarbons (.PAHs) are like metals in the sense that they are not synthetic but occur natu- rally. They are found in fossil fuels such as coal and oil. Their existence, though. Table 1 . Chemicals measured in NOAA's National Status and Trends Program. Trace Metals Cadmium (Cd) Chromium (Cr) Copper (Cu) Lead (Pb) Mercury (Hg) Silver (Ag) Zinc (Zn) Organic Compounds Total DDT (tDDT) The sum of concentrations of DDT (dichloro-diphenyl-trichloroGthane) and its metabolites DDE (dichloro-diphenyl-trichloroethylene) and DDD (dichloro-diphenyl-dichloroethylene). Total chlordane (tCdane) The sum of concentrations of two major constituents of chlordane mixtures: alpha- chlordane and trans-nonachlor. Total polychlorinated biphenyls (tPCB) The sum of the concentrations of di-, tri-, tetra-, penta-, hexa-, hepta-, octa-, and nona- chlorobiphenyls. Since 1988, the equivalent tPCB has been calculated from the sum of concentrations of 18 individual PCB congeners. Total polycyclic aromatic hydrocarbons (tPAH) The sum of concentrations of 18 PAH compounds: six 2-ring compounds (biphenyl, naphthalene, 1-methylnaphthalene, 2-methylnaphthalene, 2,6-dimethylnaphthalene, and acenaphthene); four 3-ring compounds (flourene, phenanthrene, 1-methylphenanthrene, and anthracene); three 4-ring compounds (flouranthene, pyrene, and benz(a)anthracene); and five 5-ring compounds (chrysene, benzo(a)pyrene, benzo(e)pyrene, perylene, and dibenz(a,h)anthracene). is also attributable to human activity be- cause they are produced when organic matter is burned. A multitude of human activities, from burning coal and wood to incineration of wastes, create PAH compounds in excess of those that would exist naturally. Often, the lower molecu- lar weight compounds (2- and 3-ring compounds in Table 1) are classified separately from the higher-weight com- pounds (4- and 5-rings) because the lower-weight compounds have a higher association with petroleum and the higher-weight compounds with combus- tion products. Since high concentrations of both types of compounds tend to be found in the same locations, all PAH compounds have been combined into a single group for this report. All of these trace metals and groups of organic compounds can be acutely or chronically toxic to marine life and even to people under some conditions. Those conditions include the total concentra- tion of chemical that is biologically available and the ability of each species to accommodate increased chemical exposure. An important aspect of the NS&T Program is to determine the dis- tribution of locations where contamina- tion is of biological consequence. Nationwide Distribution of Contaminants in Sediment The nationwide results from NOAA analyses of surface sediments can be used to define the spatial distribution of contamination. Before simply using the data, however, it is important to know that contaminants are associated with particle surfaces. Sand-sized particles have less contamination per unit weight of sediment than silt or clay. To account for this, the NS&T sediment data have been adjusted in two ways. First, no data for contaminants in sediment were used forcomparisons among sites when the sediment contained more than 80% sand (particles with diameters less than 63 microns). Secondly, contaminant levels in sediments containing less than 80% sand have been adjusted by divid- ing the fraction of sediment that is fine- grained (i.e., divided by a number be- tween 0.20 and 1 .00). That adjustment is the equivalent of considering sand to be only a dilutant of sediment contami- nation. The exclusion of very sandy sediments acknowledges that some contamination may be associated with sand, but cannot be accounted for in this method of comparing among sites. The NS&T results of sediment analyses have already been reported (NOAA, 1988). Those data, plus new data from NOAA Mussel Watch sites occupied in 1988 and 1989 and NOAA Benthic Sur- veillance data from 1986, provide infor- mation on chemical concentrations in sediments at 287 sites. Fine-grained sediment was collected at 232 of those sites. Each time sediments were sampled at a site, three separate samples of surface sediment were col- lected. The overall total number of samples per site varies som.ewhat de- pending on how often a site was sampled and on the availability of fine-grained sediment, but in general, the mean concentrations used in this report are based on analyses of six samples at each site. Data on cadmium and tPCB are used in Figure 1 to show that, for both trace metals and organic chemicals, concen- trations are distributed in such a way that there are few high concentrations that stand out from the rest. When dis- tributions of concentrations are highly skewed toward the lower concentra- tions, it is useful to examine the distribu- tions of the logarithms of the data. As exemplified in Figure 1 , when the loga- rithms of the concentrations are plotted, the distributions become bell-shaped. In statistical analyses such distributions are referred to as normal distributions and, in this case because logarithms were required, the distributions are log- normal." The advantage of the fact that the con- centrations are log-normally distributed is that it allows a statistically objective Figure 1 . Distributions of Cadmium and tPCB concentrations in sediment on aritiimetic and logaritiimic scales 200^ 150 H B '^ 100 o a5 E 50 Cd 0 "1 \ \ r 8 12 16 20 Concentration (|jg/g-clry) Arithmetic scale 200 150 CO ■"^ 100 o CD E 3 50 tPCB 0 800 1600 2400 3200 4000 Concentration (ng/g-dry) Aritlimetic scale w a> ■^ 'en ^_ CD E 3 w (D ■t— ' High Concentration 1 .3 MQ/g-dry 50 n 40 30- 20- 10- .016 0.10 0.63 4.00 25.0 160 Concentration (pg/g-dry) Logarithmic scale High Concentration 200 ng/g-dry ° 30 CD -| 20 ^ 10 0.25 1.60 10.0 63.0 400 2500 Concentration (ng/g-dry) Logarithmic scale and convenient definition of "high" concentrations as those whose logarith- mic value is more than the mean plus one standard deviation of the logarithms for all concentrations. In practice, be- cause we are dealing with normal distri- butions, about 1 7% of all the concentra- tions for each chemical will fall into the "high" category. ForcadmiumandtPCB, for example, the "high" concentrations correspond to 1 .3 ^ig/g (dry) and 200 ng/g, respectively, as shown in Figure 1 . For those and the rest of the chemicals being used in this report, the "high" concentrations are listed in Table 2. Table 2. Concentrations in sediment that are defined as "high" for NS& T sites. Concentrations are in units of[ig/g (dry) for trace metals and ng/g (dry) for groups of organic compounds. Chemical Hiqh concentration Cd 1.3 Cr 230 Cu 87 Pb 87 Hg 0.51 Ag 1.2 Zn 280 tDDT 40 tCdane 5.5 tPCB 200 tPAH 3900 That definition of "high" in a listing of all the NS&T sites can be used to indicate which ones have sediments with "high" concentrations of each chemical. The Appendix lists, in clockwise geographic sequence from Maine to Hawaii, all sites sampled in 1984 through 1989. It also indicates which chemicals, if any, had concentrations in the "high" range. That information is displayed graphically in Figure 2 where NS&T sites are shown on a map of the U.S. On a national scale, particularly for sites with three or more high concentrations, it is clear that contamination is associ- ated with urbanized areas of the North- east states; near San Diego, Los Ange- les, and Seattle on the West Coast; and, except at a few sites, relatively rare in the Southeast and along the Gulf of Mexico Coast. The association of higher levels of sediment contamination with highly populated areas is not a surpris- ing result. Nevertheless, it is important to note that these results come from sites that are considered to be "repre- sentative." However, some NS&T sites may not be representative. One could doubt that the NS&T site in the Elizabeth River, VA, is typical of the southern end of Chesap- eake Bay, because no chemicals are at high concentrations in sediments at other sites in that area. Sediments from sites near Los Angeles, the one off Palos Verdes and one in Santa Monica Bay, were taken within about a mile of the ends of discharge pipes from major sewage treatment plants. In those cases concentrations are very high, but other sites in the area, away from major dis- charges, also have sediments with high concentrations. The high concentrations in St. Andrews Bay, FL, were unex- pected but are confirmed by data from other sites near Panama City. The high concentrations at one site in Choc- tawhatchee Bay, FL, have not been confirmed by results from other sites. If our objective had been to identify the most contaminated sediments in the Nation, even the highest concentrations at NS&T sites could have been ex- ceeded. For example, Rodgerson et al. (1985) found levels of tPAH, tPCB, cadmium, copper, lead, and zinc in Black Rock Harbor in Bridgeport, CT, that are higher than any found at NS&T sites. Levels of tPAH, silver, mercury, and lead in industrial waterways of Seattle and Tacoma have been found in excess of all NS&T concentrations (Malins et al., 1982). As already stated, the NS&T site in the Elizabeth River may not be a represen- tative site, but a detailed sampling of that river by Huggett et al. (1 987) yielded levels of tPAH that exceed those re- ported at any NS&T site. While sedi- ments at all NS&T sites in Boston Har- bor show high levels of tPAH, they are not as high as some of those reported by Shiaris and Jambard-Sweet (1 986) who analyzed a similar suite of PAH com- pounds in sediments from around piers and other inner parts of Boston Harbor. There are many NS&T sites in Southern California, but with a single exception, none have high levels of tPAH in sedi- ments. Nevertheless, high concentra- tions have been found near discharges and centers of industrial activity (Ander- son and Gossett, 1 987). Sampling on a much finer spatial scale than the NS&T Program could yield much higher levels of contamination, but they would be of little spatial significance from a national perspective. However, this fact illus- trates the need for more detailed moni- toring programs in selected areas for local decision-making. Fifty-five sites yielded only sandy sedi- ments and have not, therefore, contrib- uted to defining the spatial distribution of contamination. For the most part this is not a severe problem because, on a national scale, those sites are near other sites that have fine-grained sediment. On the California coast, however, only sand was collected at most sites on the offshore islands and along the rocky shore north of Point Conception. There are no samples to reveal whether any of these sites are among the more con- taminated. We can, with some reserva- tion, use data from analyses of mussel tissues to gauge contaminant levels at these sites. The reservations are due to the fact that mussels and oysters do not accumulate chemicals with equal profi- ciency (NOAA, 1 989) , and so we cannot usually compare chemical concentra- tions in oysters with those in mussels. This same problem limits our ability to compare results across the Nation from different fish species sampled through the Benthic Surveillance component of the NS&T Program. NOAA has collected mussels at a total of 96 sites. If the data for those 96 sites are treated as we have treated the data fromthe 232fine-grained sediment sites, "high" concentrations can be defined in the same way. Mussels at sandy sites on the offshore islands and along the northern coast of California often con- tain high concentrations of tDDT. This is consistent with data from the few sites in that areathat did have fine-grained sedi- ment and is related to the major histori- cal discharges of DDT from production facilities in Los Angeles. Except for 8 tDDT, however, mussels at these sites are not highly contaminated. If fine- grained sediment had been available, it is unlikely thattheirchemical concentra- tions would be among the high concen- trations. NS&T sites along the stretch of coast from Point Conception, CA, to the Hood Canal, WA, provide an example of sedi- ment concentrations that are high due to natural, rather than human, causes. Levels of human population and indus- trialization are low, but a few metals appear at high concentrations. Chro- mium concentrations in sediments are high, most likely because mineralsform- ing the bedrock of that region are also enriched in chromium (USGS, 1981). High chromium concentrations in sedi- ments elsewhere in the nation can be attributed to human activity and consid- ered to be contamination, but in the Northwest chromium is naturally high and is not a contaminant. This point will become important as we discuss levels of chemicals in sediments that have been found to produce biological re- sponses. Biological Effects Of Contaminants A crucially important aspect of chemical contamination is whether or not it is causing any biological effects. One approach to that question is to collect and examine organisms living at each site. The other is to expose test organ- isms to sediment samples and use the organism's response as a measure of toxicity. Both methods are being used in NOAA's NS&T Program. The presence of tumors in fish is usually interpreted as a response to contamina- tion (Susani, 1 986) , and livers of fish col- lected at all NS&T sites have been examined for them. They were found in only 36 of the approximately 5,600 fish examined between 1984 and 1986. Fourteen of those were found in winter flounder in Boston Harbor, MA, and five in English sole in Elliott Bay, WA. These two areas do appear in the Appendix and Figure 2 as having sediments with high concentrations of chemicals. Two fish with liver tumors were found at each of four other sites: Raritan Bay, NJ; Great Bay, NJ; Bodega Bay, CA; and Commencement Bay, WA. Two of those sites. Great Bay and Bodega Bay, have not shown evidence of chemical con- tamination. So, while there is a general connection between contamination and liver tumors in fish, tumors are not al- ways found in places where contamina- tion is high, and they are occasionally found in what might be considered uncontaminated areas. Complicating factors include the facts that older fish have a higher frequency of tumors than younger fish, and that even under identical exposures to con- tamination, different species of fish metabolize contaminants at different rates and are more likely than others to develop tumors (Varanasietal., 1987). The observations in the NS&T Program are not all on older fish and, because it is a national program, the focus cannot be on a single species, i.e., no single species of fish is found at all sites. The infrequent occurrence of liver tumors is related to the species examined, but is due also to liver tumors being an ex- treme response to contamination and the fact that NS&T sites are not isolated areas of extreme contamination. Recent work by Long and Morgan (1 990) allows us to extrapolate from chemical data describing the nationwide distribu- tion of contamination to give us a sense of the distribution of sediment toxicity. They reviewed 1 50 scientific papers and reports on sediment toxicity and found 85 with data on both biological response and chemical concentrations in the sediment. They examined all of this in- formation and found chemical con- centrations, listed in Table 3, that corre- spond to concentrations above which effects were frequently observed. Since the values in Table 3 (except for chro- mium) are all greater than those defined in this report as "high" concentrations, it follows that sediment toxicity will be found at fewer sites than are highlighted in the Appendix and Figure 2. The di- chotomy between "high" and "possibly biologically effective" concentrations is actually somewhat larger because the sediment data used by Long and Mor- gan were not adjusted for their sand content. The middle column in Table 3 shows that the "high" NS&T concentra- tions would have been about 40% lower if the data had not been adjusted. As noted in Table 3, the exception of chromium is probably due to its naturally high levels in the Northwest combined with the fact that many tested sediments have been collected in that region. As Long and Morgan indicated, chromium probably was not causing toxicity in any of the tested sediments. This extrapolation from chemistry to biological effect cannot be accepted unequivocally. The exhaustive compi- lation of reports that Long and Morgan used included bioassays based on dif- ferent organisms, different test proce- dures, and different indicators of effect (usually death). The list of reports in- cluded studies where chemicals were added to sediments, cases where sedi- ments were tested as taken from the field, and cases where toxicity was esti- mated from calculations of chemical concentrations in the pore water of sediments. Finally, it included reports where sediment quality was judged on the basis of the species of organisms found (or not found) living in association with it. All of these differences make comparisons precarious. Nevertheless, the conclusion that sediment toxicity is not widespread is consistent with re- sults from NS&T studies that tested sediment toxicity. Scott (1 989) collected sediment at NS&T sites in western Long Island Sound and in the Hudson/Raritan estuary that are listed in the Appendix as having sedi- ment with high levels of contamination. In a standard bioassay based on 1 0-day survival of amphipods these sediments proved nontoxic. It may be that toxic sediments are found in only very local- ized and highly contaminated places. For example, Rodgerson et al. (1985), using that same amphipod test, did find toxicity in Black Rock HarlDor near Bridge- port, CT, a site already mentioned as being highly contaminated. While the NS&T sediment data do not indicate high levels of contamination in San Francisco Bay, Chapman et al. (1987) and Long and Buchman (1989) did find toxic responses to sediments taken from Islais Waterway and the inner parts of Oakland Harbor, two highly industrialized locations within San Fran- cisco Bay. Swartz et al. (1982) found a range of toxic responses within the in- dustrial waterways of Tacoma, WA, off Commencement Bay. 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CO o 8 to 03 3 3 a -o B q O r^ h- d Cvj o o o ir> iri o CO k— o c o> o E 2 E CO en "cO c" o T3 C CO E E o o 2 CO 1= 0 CO cn _Q a> 0 ^ 5. CO cn 0 CO C o 3 CO 00 CX3 00 ■^ o o O) cvj' o CJ) o 03 i5 OJ CvJ Oi CVJ c 0) 0 > J3 * ■^^ CX (0 CO C3) o ^ o ^ J^ to =L J3 3 —I .55 SO is ■•— o CO O «•— cn !c c: to k- CO V) .ti c 3 cvj" CD CO 1- H CO o E "D 3 «,- 0) 8 i 03 to 15 o E sz O TJ O 3 J3 O) Oi c H X 0 CQ o v> o CD o "cO c a> o c o E 8 CD cn 'c CO o o c CO -p tC > 0 IT) 2 W •2^ 1 O O CL X < N Q < Q. 4— « c CO o Q. cn c cn c 0 k- c 0 0 c 0 CO E£ .3 CO 03 n h- c u c 8 C3) X a c (S o c 8 X T3 C CO cn CD k- O c 8 c CO -o CO 8 E 3 E 0 0 « 3 S8 ■^ c:) "0 C- 11 some places. However, sediment toxic- ity is not usually found at NS&T sites be- cause they are chosen to be represen- tative of more than isolated locations. It appears that, on a national scale, biological effects are restricted to ex- tremely contaminated and spatially lim- ited locales. That result is, of course, a welcome assessment of the status of coastal contamination. However, it is very important to continue to test for possible effects, especially non-lethal ones. Ongoing projects at the NMFS Environ- mental Conservation Division in Seattle are seeking to find contaminant re- sponses in fish that are less dramatic than liver tumors, but may be more often found and of possible significance to the longevity or reproductive potential of the species. For example, while there is not yet a nationwide set of data, livers of fish are being biochemically examined for the activity of enzymes produced to me- tabolize organic contaminants. Direct measurements of the reproductive suc- cess of fish are being made in selected locations. The NS&T Program serves as an ex- perimental matrix in which to find bio- logical responses that are being caused by chemical contamination. Research into effects of contaminants is not re- stricted to NS&T sites. Intact, samples are deliberately collected in very con- taminated areas to test whether the hypothesized response occurs under extreme conditions. Once it is known that a response occurs under these conditions, it will be possible to incorpo- rate the measurement into NOAA's national monitoring program. Temporal Trends of Contaminants in Sediments Sediment data can be used to describe the spatial distribution of contamination, but periodic analyses of surface sedi- ments do not reveal temporal trends. Organisms on the seafloor mix newly arrived particles into the existing sedi- ment. Whenthe NS&T Program samples the upper one to two centimeters of sediment, we do not know how much time has been integrated into that sample. It could be, for example, that the upper 10 cm of sediment are all mixed together and that sediment is delivered slowly at that site. Quite pos- sibly, a chemical concentration of the surface represents a 20-year average. Getting chronological data from sedi- ments requires a knowledge of rates of particle deposition and rates of sedi- ment mixing. It is possible, under certain circum- stances, to find sediment that can be specially examined so that layers in vertical sections can be associated with a sequence of years. Generally, the objective is to apply radiological dating techniques to sediments that are not overly disturbed by biological activity and have sufficiently rapid rates of sedi- mentation. The NS&T Program has begun investigations in this field, but there are data collected in other pro- grams that allow an important general observation about trends in contamina- tion. Figure 3 contains data extracted from a number of scientific papers. The impor- tant point is that contaminant concen- trations in sediments, except possibly for copper, have begun to decrease 12 Figure 3. Chronological profiles of chemical concentrations in sediment cores 2000 1990 1980 1970 1960 1950 1940 1930 1920 ro 1910 >■ 1900- 1890- 1880- 1870- I860- 1850- 1840 1830- 1820 1810 1800 Southern California Finney and Huh (1989) tPAH 00 0 5 1 0 1 5 20 25 30 3 5 40 45 5 Concentration relative to 1845 Puget Sound Bates etal. (1984) 4000 tPAH (ng/g-dry) 2000 -, 1990- 1980 1970- 1960- 03 ^ 1950- 1940- 1930 1920 1910 1900 Puget Sound Crecelius and Bloom (19i 2000 1990 1930- 1920 1910- 1900 Southern California Eganhouse and Kaplan (1988) 0.0 05 10 15 20 2 5 30 35 40 45 50 5 5 50 Concentration relative to 1940 20 40 60 80 100 120 tPDT (nq/g-dry) 13 since the late 1970s or earlier. This point needs to be substantiated with more data from sediment cores. The data in Figure 3 were chosen because the chronologies extend to at least 1 980. There are many reports where the chro- nologies end in the 1 970s. In these latter cases, contaminant concentrations that had been increasing since the industrial revolution appear to have stopped in- creasing, but evidence of decreases is lacking. The reason for studying new cores is to verify or refute the hypothesis that contamination has been decreas- ing over the last decade. Temporal Trends of Contaminants in Molluscan Tissue Except underspecial circumstances, one cannot expect samples of surface sedi- ment collected at a single site to differ on an annual basis even if contaminant inputs change. Mussels and oysters, on the other hand, can change their con- taminant levels in response to changes in their surroundings (Roesijadi et al., 1984; Pruell et al., 1987). This and the fact that they are immobile makes them ideal for monitoring changes in chemi- cal concentrations in the coastal envi- ronment. Figure 4 is an 1 8-year record of tPCB in mussels at the NS&T site in Royal Palms Park on the Palos Verdes coast of Los Angeles. It shows a dramatic decrease that began in 1 971 when the U.S. began to phase out PCB use. The record has been constructed by combining three sets of data from three separate pro- grams. Sericano et al. (1990) have combined data from diverse sources to show similarly dramatic historical changes in the average tDDT concen- tration in oysters in the Gulf of Mexico. In that case as well as in Figure 4, the major decreases occurred in the early 1 970s. Unlike trends found in sediment cores, where all sections would have been analyzed by a single laboratory, trends from annual collections of mol- lusks have had to be based on data from several sources. As explained by Stout (1986), analytical artifacts must be sus- pected because chemical techniques for quantifying organic compounds in environmental samples have improved dramatically overthe same period of the apparent decreases. Nevertheless, the timing and the large magnitude of the decreases lends credibility to the argu- ment that major decreases have oc- curred in concentrations of now-banned chlorinated compounds. Decadal trends in trace metal contami- nation have been sought by comparing NS&T data of 1986 through 1988 with data from analyses of mussels and oysters collected in 1 976 through 1 978 by a previous "mussel watch" program (Goldberg et al., 1983) sponsored by the U.S. Environmental Protection Agency (EPA). Statistically, since the earlierprogramcollected a single sample each year, it was necessary to aggre- gate the three years of data for each decade. With that aggregated data it was possible to estimate differences in trace metal concentrations in mollusks at the 50 sites that were common to both programs. Figure 5 shows the 50 site locations and demonstrates the over- whelming (39 out of 50) dominance of decadal decreases in lead. That excess of decreases over increases or lack of difference is itself statistically sufficient to declare a national decrease in lead concentrations since the late 1970s, a result consistent with the phase-out of 14 Figure 4. Concentrations of tPCB in mussels collected at Palos Verdes State Park since 1971 4000 m 3000 - i; 2000 - C OQ O a. • ■ ■ ■ Young eta. (1988) • Hayes and Phi ips (1987) - NOAA NS&T 1000 - ■ ■ ■ 1 ■ ■ • . • • • _ • A ■ • • • A A • • • 0 19 70 1972 1974 1976 1978 1980 1982 1984 1986 1988 19 90 Year 15 leaded gasoline. For copper, cadmium, silver, and zinc the directions of change were not over- whelmingly in a single direction. How- ever, for cadmium, there were 12 sites where the 1970s data were statistically different from the NS&T data, and in 1 1 of those cases the 1970s concentra- tions were higher. Conversely, for 1 8 of the 22 sites where copper concentra- tions were statistically different they were lower in the 1970s. As pointed out by Lauenstein et al. (1990), the copper increase may reflect the fact that of all the metals measured in both programs, copper is the only one whose annual use in the United States has shown an increase since the mid-1970s. Changes in concentrations of chemi- cals in mollusks at a single site may indicate trends, but they could be ran- dom variations unrelated to chemical inputs. Differences over a 1 0-year time span were considered trends rather than random variations because they occurred at many sites. The data from sediment cores and from mussels at single sites were considered trends because there were data for many years and there were consistent relationships between concentration and time. Changes over short time scales may be found in data on mussels and oysters that have been collected by NOAA at 1 2-month intervals (in the late winter to early spring) at NS&T sites since 1986. This is the beginning of what will be- come an increasingly valuable set of data. At the early stages, however, it is difficult to separate changes that signify trends from those that do not. The first three years of concentration data for 132 sites have been examined for cases where there were statistically significant differences and where the concentration in the middle year was not the highest or lowest (NOAA, 1989). This restriction was imposed so that possible trends cou Id only be those cases where concentrations had continuously increased or decreased over the three years. Even with that restriction, trends cannot be confidently identified at single sites with only three years of data. Some confidence may be associated with cases where groups of sites show simi- lar changes. On the whole, concentrations of each trace metal or group of organic com- pounds changed in a statistically signifi- cant and uniform fashion at about 10% of the sites. There were a few groups of sites showing a common change. For example, cadmium and chlordane con- centrations were decreasing in mussels at sites in Long Island Sound; copper and mercury were increasing at sites in the Hudson/Raritan Estuary. Neverthe- less, without data for more years, re- sults from NS&T analyses, by them- selves, cannot confidently identify trends. Conclusions The spatial distribution of contamination throughout the coastal United States, revealed through analyses of surface sediments, shows the higher levels to be characteristic of urbanized estuar- ies. Those high levels, however, are generally lower than those expected to cause sediment toxicity, and among the NS&Tsites, biological responses to con- tamination, such as liver tumors in fish or sediment toxicity, have not been commonly found. Temporal trends in contaminant levels at NS&T sites are 16 I I I I I ■I I i 8 I I* si 0) CO o r^ O) 1— 0) .c c 03 r ffl C_) f- h- -*— • O) o CO ■I- c o r: 0) t/3 c o '•♦— « CO ■♦— ' c: c o o 0) o CO CO Q) E CO CO CD c CO CD X /^.,w-*-^. 17 beginning to be drawn from annual analyses of mussels and oysters. Look- ing at trends over decadal and longer time scales indicates that levels of most contaminants measured in the NS&T Program may be decreasing. Except possibly for copper, there is little evi- dence that they could be increasing. New Directions The NS&T Program is continuously evaluating new ideas that could enhance its value to the Nation. Already men- tioned are efforts to identify subtle bio- logical responses to contamination and the program of collecting sediment cores to construct chronologies of contami- nant inputs. New chemicals have also been added to those monitored by NOAA through the NS&T Program. For ex- ample, tri-, di-, and mono-butyl tin are now measured in mussels and oysters. Tributyl tin is a toxic chemical that was often added to marine paints to serve as an anti-foulant on the hulls of boats. Because it has harmed marine life in unintended ways, its use has been severely restricted. Results of those re- strictions should appear as decreasing concentrations of tributyl tin and its break- down products, di- and mono-butyl tin. A major test of NS&T results will be derived from strong interagency coop- eration with the U.S. Environmental Protection Agency's recently inaugu- rated Environmental Monitoring and Assessment Program (EMAP). The Near Coastal Component of that program began in 1990 to collect and analyze biological and sediment samples and perform toxicity tests on sediment and waterf rom about 200 randomly selected estuarine sites between Chesapeake Bay and Cape Cod. For the next few 18 years that sampling intensity will be repeated at another set of randomly chosen locations and, at the same time, the program will expand to other parts of the country. While many of the meas- urements are common to both programs, EMAP is based on random sampling while NS&T is based on annual sam- pling throughout the nation at fixed loca- tions. Data from both programs will be examined to test how well the NS&T results actually represent conditions in the estuarine and coastal United States. Participating Organizations The NS&T samples and data are gath- ered through two major NOAA programs. The Benthic Surveillance Program began sampling fish and sediments in 1984. The Mussel Watch Program started sampling mussels, oysters, and sediments in 1986. The laboratories that have performed Benthic Surveil- lance activities are located at five sites: the NOAA National Marine Fisheries Service laboratories in Gloucester, MA; Sandy Hook, NJ; Beaufort, NC; Char- leston, SC; and Seattle, WA. The Mussel Watch work has been performed at the Battelle laboratories in Duxbury, MA, and in Sequim, WA; the Texas A&M University Geochemical and Environ- mental Research Group in College Station, TX; and the LaJolla, CA, labora- tory of Scientific Applications Interna- tional Corporation. Acknowledgements This report could not have been com- pleted without contributions from innu- merable people and organizations. The several laboratories responsible for collection and analysis of samples have been mentioned. Members of the staff of the National Status and Trends Pro- gram provided invaluable assistance and advice. Bernard W. Gottholm created the graphics in this report using soft- ware and geographic data developed by the Strategic Assessment Branch of the Ocean Assessments Division, NOAA Office of Oceanography and Marine Assessment. Nathalie J. Valette-Silver provided data from her collection of contaminant chronologies in sediment cores. Alan J. Mearns and his col- leagues in the Historical Assessment Group furnished data from various sources required to construct a chronol- ogy of tPCB in mussel tissues. Pamela H. Rubin and Kevin D. McMahon pro- vided editorial support. References Anderson, J.W. and R. W. Gossett. 1 986. Final report on polynuclear aromatic hydrocarbon contamination in sediments from coastal waters of southern Califor- nia. Report to California State Water Resources Control Board. Southern California Coastal Water Research Project. Long Beach, CA. 50 p. & ap- pendices. Bates, T. S., S. E. Hamilton, and J. D. Cline. 1984. Vertical transport and sedi- mentation of hydrocarbons in the cen- tral main basin of Paget Sound, Wash- ington. Environ. Sci. Technol. 18: 299- 305. Chapman, P. M., R. N. Dexter, and E. R. Long. 1987. Synoptic measures of sedi- ment contamination, toxicity, andinfau- nal community composition (the Sedi- ment Triad) in San Francisco Bay. Mar. Ecol. Prog. Ser. 37: 75-96. Crecelius, E. A. and N. Bloom. 1988. Temporal trends in contamination in Puget Sound. \ni Oceanic Processes in Marine Pollution. Vol. 5. Urban Wastes in Coastal Marine Environments. D.A. Wolfe and T.P. O'Connor, eds. Krieger, Malabar, FL pp. 149-155. Eganhouse, R. P. and I. R. Kaplan. 1988. Depositional history of recent sediments from San Pedro Shelf, Cali- fornia: Reconstmction using elemental abundance, isotopic composition, and molecular markers. Mar. Chem. 24: 1 63- 191. Finney, B. P. and C.-A. Huh. 1989. History of metal pollution in the South- ern California Bight: an update. Environ. Sci. Technol. 23: 294-303. Goldberg, E. D., M. Koide, V. Hodge, A. R. Flegal, and J. Martin. 1983. U.S. tAussel Watch: 1977-1978 results on trace metals and radionuclides. Estuar- ine. Coastal and Shelf Sci. 16: 69-93. Hayes, S.P. and P. T. Phillips. 1987. California State l^ussel Watch Marine Water Quality Monitoring Program 1 965- 86. Wat. Qual. Mon. Rpt. 87-2WQ, Cali- fornia. Water Research Control Board, Sacramento, CA. 58 p. (More recent data in Figure 4 supplied directly to A. J. Mearns by California Mussel Watch.) Huggett, R.J., M. E. Bender, and M. A. Unger. 1987. Polynuclear aromatic hydrocarbons in the Elizabeth River, Virginia. \ni Fate and Effects of Sedi- ment-Bound Chemicals in Aquatic Sys- tems. K.L. Dixon, A.W. Maki, and W.A. Brungs, eds. Pergammon Press, Ox- ford. Lauenstein, G. G., A. Robertson, and T. P. O'Connor. 1990. Comparison of trace 19 metal data in mussels and oysters from a Mussel Watch Program of the 1970's with those from a 1 980' s program. Mar. Poll. Bull, (in press). Long, E. R. and L. G. Morgan. 1 990. The potential for biological effects of sedi- ment-sorbed contaminants tested in the National Status and Trends Program. NOAA Technical Memorandum NOS OMA 52. NOAA Office of Oceanogra- phy and Marine Assessment, Ocean Assessments Division, Seattle, WA. 1 73 p. & appendices. Malins, D.C., B. B. McCain, D. W. Brown, A. K. Sparks, H. O. Hodkins, and S.-L. Chan. 1982. Chemical contaminants and abnormalities in fish and invertebrates from Puget Sound. NOAA Technical Memorandum OMPA-19. NOAA Office of Marine Pollution Assessment, Boul- der, CO. 168 p. National Research Council (NRC). 1990. Managing Troubled Waters: The Role of Marine Environmental Monitoring. Na- tional Academy Press, Washington, DC. 125 p. NOAA. 1 988. National Status and Trends Program for Marine Environmental Quality. A summary of selected data on chemical contaminants in sediments collected during 1984, 1985, 1986, and 1987. NOAA Technical Memorandum NOS OMA 44. NOAA Office of Ocean- ography and Marine Assessment, Ocean Assessments Division, Rockville, MD. 15 p. & appendices. NOAA. 1 989. National Status and Trends Program for Marine Environmental Quality. A summary of data on tissue contamination from the first three years (1986-1988) of the Mussel Watch Proj- 20 ect. NOAA Technical Memorandum NOS OMA 49. NOAA Office of Ocean- ography and Marine Assessment, Ocean Assessments Division, Rockville, MD. 22 p. & appendices. Pruell, R. J., J. G. Quinn, J. L. Lake, and W. R. Davis. 1987. Availability of PCBs and PAHs to Mytilus edulis from artifi- cially resuspended sediments. In: Oce- anic Processes in Marine Pollution. Vol. 1 . Biological Processes and Wastes in the Ocean. Capuzzo, J.M. and D.R. Kester, eds. Krieger, Malabar, FL. pp. 97-108. Rodgerson, P.P., S. C. Shimmel, and G. Hoffman. 1985. Chemical and biologi- cal characterization of Black Rock Har- bor dredged material. U.S. EPA/U.S. Army Corps of Engineers Waterways Experiment Station, Vicksburg, MS. 1 1 0 p. & appendices. Roesijadi, G., J. S. Young, A. S. Drum, and J. M. Gurtisen. 1987. Behavior of trace metals in Mytilus edulis during a reciprocal transplant field experiment. Mar. Ecol. Prog. Ser. 15: 155-170. Scott, K.J. 1989. Report to NOAA Oceans Assessments Division on re- sults of toxicity tests on sediments from Long Island Sound and Hudson Raritan estuary. Science Applications Interna- tional Corporation, Narragansett, Rl. Sericano, J. L., T. L. Wade, E. A. Atlas, and J. M. Brooks. 1990. Historical per- spective on the environmental bioavaila- bility of DDT and its derivatives to Gulf of Mexico oysters. Environ. Sci. Technol. (in press). Shiaris, M.P. and D. Jambard-Sweet. 1 986. Polycyclic aromatic hydrocarbons in surficial sediments of Boston i-iarbor, Massachusetts USA. Mar. Poll. Bull. 17:469-472. Schults, D.W., S.P. Ferraro, G.R. Dits- worth, and K.A. Sercu. 1987. Selected chemical contaminants in surface sedi- ments of Commencement Bay and Tacoma Watenn/ays, Washington, USA. Mar. Environ. Res. 22: 271-295. Susani, L. 1986. Liver lesions in feral fish: a discussion of their relationship to environmental pollutants. NOAA Tech- nical Memorandum NOS OMA 27. NOAA Office of Oceanography and Marine Assessment. Rockville, MD. 20 P- Swartz, R. C, W. A. deBen, K. A. Sercu, and J. O. Lamberson. 1982. Sediment toxicity and distribution of amphipods in Commencement Bay, Washington, USA. Mar. Pollut. Bull. 13: 359-364. USGS. 1981 . Metallogenic map of North America. United States Geological Sur- vey Map G79199. U.S. Geological Sur- vey, Reston, VA. Varanasi, U., J. E. Stein, M. Nishimoto, W. L. Reichert, and T. K. Collier. 1987. Chemical carcinogenesis in feral fish: uptake, activation, and detoxification of organic xenobiotics. Environ. Health Perspect. 71:155-170. Young, D. R., R. W. Gossett, and T. C. Heesen. 1988. Persistence of chlorin- ated hydrocarbon contamination in a coastal California marine ecosystem. In: Oceanic Processes in Marine Pollu- tion. Vol. 5. Urban Wastes in Coastal Marine Environments. D.A. Wolfe and T.P. O'Connor, eds. Krieger, Malabar, FL. pp. 33-41. 21 Appendix The appendix lists all NS&T sites sampled in the Benthic Surveillance Program from 1984-1986 and the Mus- sel Watch Program from 1986-1989. Benthic Surveillance sites are those with only ageneral site name. Mussel Watch sites are given txjth a general and spe- cific site designation. If all sediment samples from a site contained more than 80% sand-sized particles, that site is indicated to be sandy and chemical data from it have not been used when comparing among sites. The last col- umns indicate which chemical concen- trations, if any, at a site exceeded the "high" concentrations listed in Table 2. 22 00 I CO i I CO 00 I "^ 00 i 1 c q> CQ ••^ CO X c 0} Q. 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E OJ -C _C "a3 m o tr c o Q. 2 ■D TO 3 o s O m 0) _c TO 3 _J TO TO CO TO m 3 SZ TO 2 1 TO c 3 N 0 T5 TO > N 0 ■D TO > r o >■ TO E TO 0 "5 r o CL TO X o 3 Q c o CL B b >> TO CO 0 O X) E CL c o CL TO CO TO X 3 3 O c o X 'to 3 TO X < Q. -•-• QQ O Q. ■•-• a c m x> • • O 1— a Q o n T3 r5 0) w cr c < 0) <1) £ > ^ CO Q. • JC 13 d O JZ w I— c () X) r iJ • 0> (0 CL X) 0) 1- 0) w S i ui ui Q) w b nJ k- 3 T' (D o > U- (1> c *— • r cc d W o CL o Q. c nj o _l LU »4— o Oh > o o CO 0) 0) CO CO CO LL CO 1^ 0) ■a E CO 2 c O CO I— O &— 0) CO 0) > E CO c X CL 2 (0 o Q C o k- E a c CO CD (D (0 o o CD ^ CO j_ z 34 -■;•'"■ / ■^'. !».•'■•-' )-A , oemCO - ^>. IkTMOsiH,. '""■WENT Of '^° October 1990 A Special NOAA 20th Anniversary Report The State of U.S. Coastal Environmental Quality, 1990