CHAPTER 3 National Distribution and Trends This chapter provides an overview of pesticide occurrence, geographic distribution, and trends in bed sediment and aquatic biota in the nation's rivers and estuaries, synthesized from existing studies and review articles and books as described in Chapter 2. General patterns of pesticide occurrence in bed sediment and aquatic biota (Section 3.1) are discussed, followed by national patterns of pesticide use (Section 3.2). Then, the geographic distribution (Section 3.3) and long-term trends (Section 3.4) of individual pesticides in bed sediment and aquatic biota are evaluated in relation to pesticide use. As is clear from the discussion in this chapter, pesticides in aquatic biota from United States rivers have been studied more extensively than in bed sediment, especially at the national scale. 3.1 PESTICIDE OCCURRENCE Existing studies can be used as the basis for a preliminary assessment of pesticide occurrence in sediment and aquatic biota in the United States. Process and matrix distribution studies generally investigate the environmental fate and persistence of a single pesticide applied in known quantities or measure pesticide residues in artificial media (such as semipermeable membrane devices). Because these types of studies do not address ambient conditions, they do not provide much information on the occurrence and distribution of pesticides in bed sediment and aquatic biota in the nation's rivers. Monitoring studies (regardless of scale) assess ambient conditions, but the results depend largely on study design characteristics. To assess pesticide occurrence, monitoring data from all national, multistate, state, and local studies were combined and aggregate detection frequencies were calculated. These aggregate detection frequencies provide an indication of how often individual pesticides have been detected in monitoring studies in the United States. Computing detection frequencies from the combined data set offers two benefits: (1) the combined data set is bigger and more extensive over space and time than that provided by any individual study; and (2) any biases in design of individual studies may be averaged out. On the other hand, these calculations are simplistic in that for a given analyte, the bias caused by quantity of data and differences among the designs of the studies combined is unknown. In contrast, detection frequencies can be used from a single © 1999 by CRC Press LLC study, in which case the results can be considered in the context of study design and sampling location. Thus, aggregate detection frequencies presented below (Section 3.1.1) are followed by a discussion of the results of the individual national programs that monitored pesticides in sediment or aquatic biota (Section 3.1.2). Each national program comprises a data set large enough to provide nationwide perspective on pesticide occurrence and distribution in bed sediment or aquatic biota in United States rivers. Although state and local monitoring studies also provide considerable information on the occurrence and distribution of pesticides, the results of these studies are difficult to compare because of the large variability in site selection strategy, sampling methods, time of sampling, analytical methods, and detection limits. For each national program discussed in Section 3.1.2, important study characteristics and highlights of the results provide a synopsis of that program's contribution to our understanding of pesticide occurrence in bed sediment and aquatic biota in United States rivers on a national scale. Finally, comparison of results from the major national programs (Section 3.1.3) provides an overview of pesticide occurrence in sediment and aquatic biota in United States rivers and streams. 3.1.1 AGGREGATE DETECTION FREQUENCIES OF PESTICIDES To examine general patterns of pesticide occurrence in sediment and aquatic biota, results from national and multistate monitoring studies (listed in Table 2.1) were combined with those from state and local monitoring studies (listed in Table 2.2). Two types of aggregate detection frequencies were calculated for individual pesticides: the percentage of total sites where a pesticide was detected in at least one sample, and the percentage of total samples with detectable residues of that pesticide. Because many of the pesticides targeted in sediment and aquatic biota have not been used in agriculture in the United States since the 1970s, it is possible that detection frequencies have declined over time. Therefore, aggregate detection frequencies were calculated for each decade of sampling. As noted above, these calculations are necessarily simplistic because they do not consider differences in analytical detection limits, sample volumes, or quantitation methods, all of which may affect the sensitivity of the analytical method, and therefore the probability of detection. The individual monitoring studies that were combined had different study designs and collected data for different durations of time. For site detection frequencies, each study is weighted according to the number of sites, not the number of samples or years of sampling. For example, a single Fish and Wildlife Service’s (FWS) National Contaminant Biomonitoring Program (NCBP) site, which may have been sampled 10–12 times between 1967 and 1986, would be weighted equally with a site from a local study that was sampled only once. For the sample detection frequencies, however, each study is weighted according to the total number of samples collected. To continue with the above example, the NCBP study, which collected hundreds of samples, would be weighted more heavily than a local study that collected only a few samples. For some multicomponent residues, different studies reported data for different analytes. For example, some studies reported chlordane results as total chlordane, whereas others reported results for individual components of technical chlordane. Because these data could not be combined, aggregate detection frequencies were calculated for each individual analyte as reported. Therefore, cis -chlordane represents the detection frequency only for studies that © 1999 by CRC Press LLC reported that analyte and does not include studies that reported the detection frequency only for total chlordane. If a study reported data for individual chlordane components (such as cis - chlordane, trans -nonachlor) as well as for total chlordane, data from this study were included in the calculations for all of these analytes. Target analytes for bed sediment and aquatic biota are listed in Tables 3.1 and 3.2, respectively, along with the total number of sites and samples in the combined data set and the corresponding aggregate detection frequencies, by decade of sampling. Data in Table 3.2 are combined for whole fish, fish muscle, and mollusk tissue. Sample detection frequencies for each of these three types of tissue are presented separately in Table 3.3, also by sampling decade. For Tables 3.1–3.3, each study was assigned to the most appropriate decade based on the years of sampling. For long-term national studies that reported data in a series of sequential reports, data from each report were assigned to the appropriate decade. Aggregate detection frequencies for individual pesticide analytes that were analyzed at 15 or more sites in the combined data set are shown graphically in Figures 3.1 (bed sediment) and 3.2 (aquatic biota). The aggregate detection frequencies in Figures 3.1 and 3.2 do not take into account sampling year, the percentage of samples in which a given analyte was detected, or the number of years in which it was detected. Because detection frequencies in Tables 3.1, 3.2, and 3.3 are presented for each decade of sampling, they represent only studies that reported the sampling year. However, the calculations for the corresponding Figures 3.1 and 3.2 also included data from studies that did not report the sampling year. The national, multistate, state, and local monitoring studies, taken together, show that a large number of pesticide analytes have been detected in sediment and aquatic biota at some time over the last 35 years. The term “pesticide analytes” encompasses pesticides, individual components of technical mixtures, and pesticide transformation products. Altogether, 109 pesticide analytes were measured in sediment, and 129 pesticide analytes were measured in the most commonly sampled types of aquatic biota tissues (whole fish, fish muscle, or mollusk tissue). Some studies did not report the data necessary to calculate aggregate detection frequencies (i.e., the total number of sites, the number of sites with detections, the total number of samples, and number of samples with detections). However, for studies that did report sufficient data, 41 of 93 pesticide analytes (44 percent) were detected in bed sediment in at least one study, and 68 of 106 pesticide analytes (64 percent) in aquatic biota. Most of the pesticides detected are organochlorine insecticides or their transformation products, despite the fact that most of the organochlorine insecticides were banned or severely restricted during the 1970s. The prevalence of organochlorine insecticides in sediment and biota samples across the United States reflects both the extreme hydrophobicity and persistence of these compounds and the bias in the target analyte list (discussed below). The most commonly detected compounds in both sediment and aquatic biota were DDT and its metabolites, chlordane compounds, and dieldrin. A few compounds in pesticide classes other than the organochlorine insecticides had fairly high detection frequencies in sediment or biota. In sediment, the herbicide diuron was detected at 100 percent of sites at which it was targeted, although diuron was targeted at only 15 sites nationwide. Additional pesticides from other classes were detected at 10–30 percent of sites: the organophosphate insecticide zytron; the herbicides ametryn, dacthal, 2,4-DB, and dicamba; and the wood preservative pentachlorophenol. All of these compounds except ametryn contain two or more chlorines. Trifluralin, which contains fluorine, was detected at 8 percent of sites. Many of © 1999 by CRC Press LLC Target Analytes Total Number of Sites Sampled for Sediment Percentage of Sites with Detectable Residues in Sediment Total Number of Sediment Samples Percentage of Sediment Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Acephate 3030 Alachlor nr nr 15 nr nr 0 28 nr 15 0 nr 0 Aldicarb 3030 Aldrin 70 792 839 83 9 5 5 7 555 2,346 1,505 84 6 2 6 7 Ametryn 15 20 38 16 Atrazine 141 12 15 0 0 0 413 14 15 0 0 0 Azinphosmethyl nr 3 nr 0 nr 3 nr 0 Butylate 15 0 15 0 Carbaryl nr 3 nr 0 nr 3 nr 0 Carbofuran nr 15 15 nr 0 0 28 17 15 0 0 0 Carbofuran, 3-hydroxy nr nr nr nr Carbophenothion nr nr nr nr nr nr nr nr Chlorbenside nr nr nr nr Chlordane, α - 25 184 46 56 36 0 25 672 46 56 53 0 Chlordane, γ - 25 225 46 48 28 0 52 275 46 35 19 0 Chlordane, total 58 818 894 35 12 41 41 77 551 2,736 2,328 36 5 20 43 75 Chlordene nr nr nr nr nr nr nr nr Chlordene, hydroxy- nr nr nr nr nr nr nr nr Chlordene, α - 4 nr 75 nr 4 nr 75 nr Chlordene, γ - 4 nr 25 nr 4 nr 25 nr Chlorobenzilate 28 0 28 0 Chlorpyrifos 5 15 20 0 5 15 20 0 Coumaphos 3030 Cyanazine nr 15 nr 0 nr 15 nr 0 D, 2,4- (or ester) 247 102 64 2 3 9 636 125 64 1 2 9 Dacthal (DCPA) 2 58 nr 50 16 nr 72 63 nr 1 16 nr DB, 2,4- 20 15 20 15 DBP nr nr nr nr Table 3.1. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in bed sediment from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2 [Data include some estuarine sites and samples for some national studies. Results are listed by decade of sampling. Blank cell indicates that no samples were collected in studies from the noted decade. Abbreviations: nr, not reported; PCNB, pentachloronitrobenzene] © 1999 by CRC Press LLC © 1999 by CRC Press LLC DDD, o , p ′ - 54 21 255 46 28 76 36 0 530 34 768 46 6 56 39 0 DDD, p , p ′ - or total 76 884 892 145 53 57 44 41 578 2,597 1,607 146 18 37 46 41 DDE, o , p ′ - 21 255 46 81 35 0 35 768 46 60 20 0 DDE, p , p ′ - or total 76 880 903 145 46 54 49 38 578 2,900 1,618 146 12 35 54 38 DDMS, p , p ′ - 11 nr 0 nr 11 nr 0 nr DDMU, p , p ′ - or total nr 16 nr nr 88 nr nr 11 nr nr 82 nr DDT, o , p ′ - 54 106 326 46 4 57 34 0 530 144 825 46 1 54 25 0 DDT, p , p ′ - or ( o , p ′ + p , p ′ )- 88 882 862 145 39 40 26 27 578 2,879 1,653 146 7 26 34 27 DDT, total nr 142 647 14 nr 79 72 100 nr 243 1,689 14 nr 77 75 100 DEF nr nr nr nr Demeton nr 3 nr 0 nr 3 nr 0 Diazinon 584 118 nr 1 9 nr 1,648 123 nr 1 10 nr Dicamba 20 9 20 0 44 9 9 0 Dichlorvos 3030 Dicofol nr 2 nr nr 0 nr nr 2 nr nr 0 nr Dieldrin 82 850 1,272 125 26 48 37 20 584 3,105 3,105 126 8 27 37 20 Dimethoate 3030 Disulfoton nr 3 nr 0 nr 3 nr 0 Diuron 15 100 38 97 DP, 2,4- 49 38 20 2 0 0 75 55 20 1 0 0 Endosulfan, total 127 315 35 2 6 9 254 363 36 4 5 8 Endosulfan I 23 260 64 30 8 11 23 288 64 30 9 11 Endosulfan II 23 282 64 26 11 3 23 296 64 26 10 3 Endosulfan sulfate 186 64 9 22 198 64 8 22 Endosulfan sulfate I nr nr nr nr Endothal 19 0 19 0 Endrin 68 798 827 145 6 9 4 3 570 2,798 1,047 146 4 3 2 3 Endrin aldehyde 19 79 64 0 0 14 19 81 64 0 0 14 Endrin ketone 54 63 2 0 530 72 2 0 EPN 3030 Target Analytes Total Number of Sites Sampled for Sediment Percentage of Sites with Detectable Residues in Sediment Total Number of Sediment Samples Percentage of Sediment Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Table 3.1. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in bed sediment from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2— Continued © 1999 by CRC Press LLC © 1999 by CRC Press LLC Ethion 493 113 0 0 1,419 118 0 0 Ethoprop 3 15 0 0 3 15 0 0 Famphur 3030 Fenthion 3030 Fenvalerate nr nr 20 0 Fonofos 15 0 15 0 Glyphosate 19 0 19 0 HCH, α - nr 42 479 46 nr 14 10 0 nr 42 646 46 nr 14 2 0 HCH, β 42 359 46 0 10 0 69 527 46 29 4 0 HCH, δ - 196 110 0 1 249 110 0 1 HCH, total 54 10 49 nr 13 0 10 nr 530 20 46 nr 3 0 11 nr Heptachlor 64 636 847 103 3 4 5 19 549 1,732 1,547 104 2 2 3 19 Heptachlor epoxide 72 768 904 145 7 12 5 6 557 2,516 1,569 146 1 5 4 5 Heptachlor, total nr nr nr nr nr nr nr nr Hexachlor 8090 Hexachlorobenzene 65 845 46 57 46 0 59 2,526 46 53 37 0 Isodrin 54 28 17 0 530 28 6 0 Isopropalin nr nr nr nr Kepone nr 28 nr 0 nr 28 nr 0 Lindane 22 798 1,065 81 0 3 17 0 48 2,753 2,823 82 0 1 19 0 Linuron 22 0 79 0 Malathion 575 116 0 0 1,642 121 0 0 Methamidophos 3030 Methiocarb 3030 Methomyl 3030 Methoxychlor nr 323 647 79 nr 6 6 1 nr 1,261 730 80 nr 1 6 1 Methyl parathion 567 116 nr 0 0 nr 1,606 141 nr 0 2 nr Methyl trithion 474 113 0 0 1,397 118 0 0 Metolachlor 15 0 15 0 Metribuzin 15 0 15 0 Mevinphos 3030 Target Analytes Total Number of Sites Sampled for Sediment Percentage of Sites with Detectable Residues in Sediment Total Number of Sediment Samples Percentage of Sediment Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Table 3.1. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in bed sediment from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2— Continued © 1999 by CRC Press LLC © 1999 by CRC Press LLC Mirex 237 298 847 81 35 7 16 0 241 381 2,580 82 36 6 18 0 Molinate Monocrotophos 3030 Nitrofen Nonachlor, cis - nr 117 46 nr 3 0 nr 163 46 nr 2 0 Nonachlor, trans - nr1746 nr120 nr046 nrnr0 Nonachlor, total 134 19 623 52 Oxadiazon 3 nr 100 nr 3 nr 100 nr Oxamyl 3030 Oxychlordane nr nr 177 46 nr nr 4 0 nr nr 323 46 nr nr 2 0 Parathion 569 299 nr 2 3 nr 1,605 450 nr 1 2 nr PCNB Pentachloroanisole nr nr nr nr Pentachlorophenol 19 146 12 0 21 33 19 189 12 0 16 33 Permethrin nr 20 15 Perthane 107 264 35 0 1 0 201 300 36 0 1 0 Phorate nr 3 15 nr 0 0 nr 3 15 nr 0 0 Photomirex nr nr nr nr Picloram 20 9 5 0 44 9 2 0 Silvex 253 48 20 3 2 0 702 67 20 1 1 0 T, 2,4,5- 239 45 20 1 4 10 647 61 20 0 3 10 Terbufos 3 15 0 0 3 15 0 0 Tetrachlorvinphos Tetradifon 36 3 37 3 Thiobencarb Toxaphene 54 682 565 65 11 4 2 0 530 2,197 694 66 2 1 3 0 Trichlorfon 3 0 3 35 0 3 Trifluralin nr 48 35 nr 13 3 nr 52 nr 12 Trithion 455 113 0 0 1,351 118 0 0 Zytron (Xytron) 48 29 52 31 Target Analytes Total Number of Sites Sampled for Sediment Percentage of Sites with Detectable Residues in Sediment Total Number of Sediment Samples Percentage of Sediment Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Table 3.1. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in bed sediment from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2— Continued © 1999 by CRC Press LLC © 1999 by CRC Press LLC Target Analytes Total Number of Sites Sampled for Aquatic Biota Percentage of Sites with Detectable Residues in Aquatic Biota Total Number of Aquatic Biota Samples Percentage of Aquatic Biota Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Acephate 3 0 3 0 Alachlor 5 2 nr 0 0 nr 215 20 nr 0 0 nr Aldicarb 3 0 3 0 Aldrin 306 154 413 65 11 3 6 0 12,146 2,047 2,073 70 1130 Ametryn nr nr nr nr Atrazine 3 2 nr 0 0 nr 209 20 nr 0 0 nr Azinphosmethyl 110 5 0 0 1,702 97 0 0 Butylate nr nr nr nr Carbaryl nr 3 nr 0 24 3 13 0 Carbofuran nr 5 nr nr 20 nr 36 98 nr 0 2 nr Carbofuran, 3- hydroxy- 2 100 69 6 Carbophenothion 110 nr 2 nr 1,702 nr 0 nr Chlorbenside nr nr nr nr Chlordane, α - 235 877 108 74 63 52 744 2,709 150 79 58 57 Chlordane, γ - 227 835 103 78 54 43 744 2,263 141 59 43 51 Chlordane, total 109 329 1,075 276 78 46 81 40 1,575 2,734 3,836 71 10 24 69 45 Chlordene 28 31 7 0 28 39 7 0 Chlordene, hydroxy- nr 31 nr 0 75 39 17 0 Chlordene, α - nr 61 nr 3 nr 66 nr 3 Chlordene, γ - nr 61 nr 5 nr 66 nr 5 Chlorobenzilate nr nr nr nr Chlorpyrifos 571 61 21 15 1,226 66 15 17 Coumaphos 3 0 3 0 Cyanazine 3 nr 0 nr 173 nr 0 nr D, 2,4- (or ester) 2 3 nr 0 0 nr 30 14 nr 7 0 nr Dacthal (DCPA) 123 431 61 33 67 23 450 1,484 66 18 26 24 Table 3.2. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in aquatic biota from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2 [Data are for whole fish, fish muscle, and mollusk tissue, combined. Data include some estuarine sites and samples for some national studies. Results are listed by decade of sampling. Blank cell indicates that no samples were collected in the noted decade by the studies reviewed. Abbreviations: nr, not reported; PCNB, pentachloronitrobenzene] © 1999 by CRC Press LLC © 1999 by CRC Press LLC DB, 2,4- nr nr nr nr DBP 5 60 6 67 DCA nr nr nr nr DDD, o , p ′ - nr 32 259 108 nr 13 28 24 nr 69 1,202 150 nr 16 51 31 DDD, p , p ′ - or total 264 392 647 114 95 60 66 59 3,334 3,591 2,607 151 51 77 70 63 DDE, o , p ′ - 4 254 108 75 22 21 52 1,190 150 58 27 29 DDE, p , p ′ - or total 277 479 1,174 121 97 77 92 86 4,198 3,988 3,185 167 68 85 90 86 DDMS, p , p ′ - nr 61 nr 0 nr 66 nr 0 DDMU, p , p ′ - or total 28 9 61 4 100 18 28 nr 66 4 nr 17 DDT, o , p ′ - 23 80 262 101 96 23 29 15 285 182 1,171 127 2 37 36 13 DDT, p , p ′ or ( o , p ′ + p , p ′) - 394 375 629 114 95 66 55 39 4,759 3,654 2,786 156 57 58 57 38 DDT, total 412 543 1,159 83 98 78 96 89 9,064 6,078 4,002 105 67 80 95 90 DEF 110 0 1,702 0 Demeton 110 3 0 0 1,702 3 0 0 Diazinon 111 203 61 0 2 3 1,703 646 66 0 1 3 Dicamba nr nr nr nr nr nr nr nr Dichlorvos 3 0 3 0 Dicofol 2 595 61 0 12 0 6 1,363 66 0 8 0 Dieldrin 454 540 1,784 108 75 66 58 39 12,774 5,955 6,378 145 24 50 57 46 Dimethoate 3 0 3 0 Disulfoton 2 3 0 0 6 3 0 0 Diuron nr nr nr nr DMDT methoxychlor nr nr nr nr DP, 2,4- nr nr nr nr nr nr nr nr nr nr nr nr Endosulfan, total 112 210 61 0 13 25 1,717 766 66 0 12 24 Endosulfan I nr 41 68 nr 61 31 nr 122 89 nr 24 37 Endosulfan II nr 43 45 nr 56 2 nr 157 49 nr 25 4 Endosulfan sulfate 18 45 0 4 103 49 1 6 Endosulfan sulfate I 14 0 28 0 Target Analytes Total Number of Sites Sampled for Aquatic Biota Percentage of Sites with Detectable Residues in Aquatic Biota Total Number of Aquatic Biota Samples Percentage of Aquatic Biota Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Table 3.2. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in aquatic biota from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2— Continued © 1999 by CRC Press LLC © 1999 by CRC Press LLC Endotetrasulfuron I 16 0 21 0 Endothal nr nr nr nr Endrin 294 321 1,300 108 13 41 12 9 12,125 3,331 3,628 150 2 21 10 12 Endrin aldehyde 6 30 nr 0 23 nr 6 112 nr 0 15 nr Endrin ketone nr 16 nr 0 nr 21 nr 0 EPN 3 0 3 0 Ethion 111 nr 2 nr 1,703 nr 1 nr Ethoprop 3 nr 0 nr 3 nr 0 nr Famphur 3 0 3 0 Fenthion 3 0 3 0 Fenvalerate 2 0 109 2 Fonofos nr nr nr nr Glyphosate nr nr nr nr HCH, α - 50 137 1,029 101 98 85 42 7 147 657 3,139 127 90 51 27 8 HCH, β - 9 406 101 0 7 5 24 1,468 127 0 10 6 HCH, δ - 356 96 4 0 1,244 118 2 0 HCH, total nr 92 243 61 nr 16 23 8 2,150 150 725 66 8 45 14 9 Heptachlor 295 216 841 72 11 6 9 6 12,200 2,072 2,626 93 1188 Heptachlor epoxide 307 127 1,056 108 17 26 22 19 12,214 1,984 3,212 150 3 6 14 27 Heptachlor, total 177 365 46 21 2,726 841 9 11 Hexachlor 5 60 14 64 Hexachlorobenzene 288 1,509 101 53 38 15 912 4,535 127 26 25 14 Hexachlorobutadiene 7 57 31 19 Isodrin nr nr nr nr nr nr nr nr Isophorone nr nr nr nr Isopropalin 362 4 560 3 Kepone 6 63 67 10 nr 85 nr 7 Lindane 15 300 1,395 108 7 13 37 19 46 2,743 4,533 150 2 3 32 27 Linuron nr nr nr nr Target Analytes Total Number of Sites Sampled for Aquatic Biota Percentage of Sites with Detectable Residues in Aquatic Biota Total Number of Aquatic Biota Samples Percentage of Aquatic Biota Samples with Detectable Residues 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s 1960s 1970s 1980s 1990s Table 3.2. Total number of sites and samples, and corresponding aggregate detection frequencies (in percent) of pesticides in aquatic biota from United States rivers, calculated by combining data from the monitoring studies in Tables 2.1 and 2.2— Continued © 1999 by CRC Press LLC © 1999 by CRC Press LLC [...]... 31 3 261 235 nr 181 119 54 34 6 110 3 1,288 2 3 362 7 93 881 38 9 3 3 800 182 36 2 506 52 nr 36 8 3 nr 1990s 0 1970s 1980s 0 68 61 1960s 0 0 0 0 8 0 nr 0 1 5 nr nr nr 40 5 96 108 12 66 69 61 108 61 nr 30 3 nr 35 3 nr nr 0 0 0 33 100 0 3 37 71 87 33 100 0 30 2 1 60 40 nr 1 0 nr Percentage of Aquatic Biota Samples with Detectable Residues Total Number of Aquatic Biota Samples 1990s 8,1 13 1970s 1980s 1, 738 ... sampling may result in a geographic bias as well In the monitoring studies reviewed, 42 organochlorine insecticides (including components of technical mixtures and pesticide transformation products) were targeted in sediment, and 47 organochlorine insecticides were targeted in aquatic biota Of pesticides in other classes, 58 were analyzed in sediment and 53 in aquatic biota However, pesticides in other... 1960s 3 3 3 3 1,8 53 93 nr 20 1,781 1,524 nr nr nr 0 8,095 28 57 2 ,30 4 770 744 11 25 0 nr 36 9 1,715 nr 54 34 nr nr 19 1,702 3 4,508 2 3 560 2,142 2, 734 105 27 5 3 2,128 589 560 1, 235 38 3 90 650 3 nr 1990s 1960s 1970s 1980s 1990s 0 89 66 0 0 0 nr nr nr 61 0 118 145 18 47 60 66 150 66 nr 25 0 nr 35 3 nr nr 0 0 0 0 0 0 4 16 nr 0 0 21 0 0 2 35 61 58 22 100 0 27 1 1 37 13 7 1 0 nr 1 2 nr nr 0 25 62 12 35 0... analyzed in sediment and aquatic biota in fewer studies (see Table 2.4), at fewer sites, and in fewer samples (see Tables 3. 1 and 3. 2) compared with organochlorine insecticides © 1999 by CRC Press LLC Table 3. 3 Total number of sites and corresponding aggregate detection frequencies (in percent) of pesticides in whole fish, fish muscle, and mollusk samples from United States rivers, calculated by combining... Chemical Residues in Fish (NSCRF); 80 percent of the 400 sites sampled in this study were located near potential point or nonpoint sources, including many industrial and urban sites These results are better considered in the context of study design and will be discussed below (Sections 3. 1.2 and 3. 3) Comparison of Bed Sediment and Aquatic Biota The number of pesticides detected in aquatic biota is slightly... Nonagricultural uses of pesticides include use in lawn and garden care, control of nuisance insects (indoor and outdoor), subterranean termite control, landscape maintenance and rights-ofway, control of public-health pests, industrial settings, forestry, roadways and rights-of-way, and direct application to aquatic systems Nonagricultural uses of pesticides were reviewed in more detail by Larson and others (1997)... organophosphate insecticides were more frequently targeted in sediment studies) Aggregate detection frequencies for most organochlorines were higher in aquatic biota than in bed sediment (as shown in Tables 3. 1 and 3. 2, Figures 3. 1 and 3. 2) Moreover, direct comparison between sediment and biota samples collected from the same sites as part of the same study supports this In samples from the National Oceanic and. .. included both freshwater and marine systems The six major national programs in Table 3. 4 differ in their scope, objectives, and study design These differences affect the study results and need to be considered in integrating the results of these studies into a comprehensive picture of pesticides in bed sediment and aquatic biota in the United States Comparison of results within and among these programs... (Aspelin, 1997), as shown in Figures 3. 5 and 3. 6 USEPA divided nonagricultural use into two market sectors: in and around homes and gardens, and on industrial, commercial, and © 1999 by CRC Press LLC EXPLANATION Home and garden sector Industry sector Agriculture sector Estimated use, in lb a.i x 106 30 0 250 200 Total insecticide use 150 100 50 0 1979 1981 19 83 1985 1987 Year 1989 1991 19 93 1995 Figure 3. 8... Estimated annual insecticide use in the United States by market sector from 1979 to 1995 Home and garden sector: homeowner applications (both indoor and outdoor) to homes (both single- and multiple-unit housing), lawns, and gardens Industry sector: applications by business owners and commercial applicators to industrial, commercial, and government facilities, buildings, sites, and land; and by commercial . targeted in sediment, and 47 organochlorine insecticides were targeted in aquatic biota. Of pesticides in other classes, 58 were analyzed in sediment and 53 in aquatic biota. However, pesticides in. nr Isopropalin 36 2 4 560 3 Kepone 6 63 67 10 nr 85 nr 7 Lindane 15 30 0 1 ,39 5 108 7 13 37 19 46 2,7 43 4, 533 150 2 3 32 27 Linuron nr nr nr nr Target Analytes Total Number of Sites Sampled for Aquatic Biota Percentage. 10 Terbufos 3 15 0 0 3 15 0 0 Tetrachlorvinphos Tetradifon 36 3 37 3 Thiobencarb Toxaphene 54 682 565 65 11 4 2 0 530 2,197 694 66 2 1 3 0 Trichlorfon 3 0 3 35 0 3 Trifluralin nr 48 35 nr 13 3 nr 52