EPA-822-R-03-032 Technical Summary of Information Available on the Bioaccumulation of Arsenic in Aquatic Organisms December 2003 Office of Science and Technology Office of Water U.S. Environmental Protection Agency Washington, DC 20460 ------- NOTICE This document has been reviewed by the Health and Ecological Criteria Division, Office of Science and Technology, U.S. Environmental Protection Agency, and is approved for publication. Mention of trade names or commercial products does not constitute endorsement or recommendation for use. This document is available on EPA's web site: http://www.epa.gov/waterscience/humanhealth/. ------- ACKNOWLEDGMENTS Tyler K. Linton Great Lakes Environmental Center Columbus, OH William H. Clement Great Lakes Environmental Center Columbus, OH Dennis Mclntyre Great Lakes Environmental Center Columbus, OH Document Coordinator Tala R. Henry U.S. EPA Health and Ecological Criteria Division Office of Water Washington, DC in ------- CONTENTS Section Notice ii Acknowledgments ni Contents iv Glossary of Arsenic Abbreviations vii 1.0 INTRODUCTION 1 1.1 Important Bioaccumulation Concepts 2 1.2 Bioaccumulation of Arsenic 2 1.3 Overview of Document 3_ 2.0 LITERATURE SEARCH AND CALCULATION METHODS 5 2.1 Literature Search 5_ 2.2 Methods for Estimating Bioaccumulation Factors 6 3.0 BAFs FOR ARSENIC IN FRESHWATER AND SALTWATER ECOSYSTEMS 8 3.1 Estimation of BAFs Using Laboratory-measured BCFs £ 3.2 Estimation of BAFs Using Field Data - Freshwater Lentic Ecosystems K) 3.2.1 BAFs for Trophic Level 2 Organisms K) 3.2.2 BAFs for Trophic Level 3 Organisms 13. 3.2.3 BAFs for Trophic Level 4 Organisms j/7 3.3 Estimation of BAFs Using Field Data - Freshwater Lotic Ecosystems j/7 3.3.1 BAFs for Trophic Level 2 Organisms j/7 3.3.2 BAFs for Trophic Level 3 Organisms \9_ 3.3.3 BAFs for Trophic Level 4 Organisms 20 3.4 Estimation of BAFs for Arsenic Using Field Data - Saltwater Ecosystems . ... 21 3.4.1 BAFs for Trophic Level 2 Organisms 2J_ 3.5 Summary of BAFs for Arsenic in Freshwater and Saltwater Ecosystems 23_ 4.0 CHEMICAL TRANSLATOR FOR ARSENIC IN SURFACE WATERS 25 4.1 Introduction to Chemical Translators 25 4.2 Objective 25 4.3 Results and Discussion 26 4.4 Application of the Chemical Translator for BAF Calculations 27 5.0 ARSENIC SPECIATION IN TISSUES OF AQUATIC ORGANISMS 28 5.1 Freshwater Aquatic Organisms 2J5 5.1.1 Trophic Level 2 28 iv ------- 5.1.2 Trophic Levels 3 and 4 30 5.2 S altwater Aquati c Organ! sm s 32 6.0 SUMMARY OF ARSENIC BAFs AND SUPPORTING INFORMATION 34 6.1 Freshwater and Saltwater Arsenic BAFs 34 6.2 BAFs Based on Total Arsenic versus Other Forms of Arsenic 34 6.3 Arsenic in Tissues of Freshwater and Saltwater Aquatic Organisms 3j5 7.0 CONCLUSIONS 37 8.0 REFERENCES 38 ------- APPENDICES APPENDIX A: BAF LITERATURE SEARCH STRATEGY APPENDIX B: SUMMARY OF ARSENIC BIO ACCUMULATION STUDIES REVIEWED APPENDIX C: BCF STUDIES: RAW DATA AND CALCUATIONS APPENDIX D: BAF STUDIES: RAW DATA AND CALCULATIONS APPENDIX E: ARSENIC TOTAL: DISSOLVED CHEMICAL TRANSLATOR APPENDIX F: TISSUE ARSENIC SPECIATION DATA LIST OF TABLES TABLE 3-1: BAFs for Arsenic in Aquatic Organisms Predicted from Laboratory-measured BCFs 9 TABLE 3-2: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Lentic Ecosystems 11 TABLE 3-3: BAFs for Arsenic in Trophic Level 3 Aquatic Organisms from Lentic Ecosystems H TABLE 3-4: BAFs for Arsenic in Trophic Level 4 Fish from Lentic Ecosystems j/7 TABLE 3-5: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Lotic Ecosystems 18 TABLE 3-6: BAFs for Arsenic in Trophic Level 3 Aquatic Organisms from Lotic Ecosystems 19 TABLE 3-7: BAFs for Arsenic in Trophic Level 4 Fish from Lotic Ecosystems 2J_ TABLE 3-8: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Saltwater Ecosystems 23_ TABLE 3-9: Summary of BAFs for Arsenic by Trophic Level for Freshwater and Saltwater Ecosystems 24 TABLE 4-1: Dissolved Arsenic as a Fraction of Total Arsenic in Surface Waters 27 TABLE 5-1: Arsenic Speciation in Freshwater Trophic Level 2 Aquatic Organisms 29 TABLE 5-2: Arsenic Speciation in Freshwater Trophic Levels 3 and 4 Aquatic Organisms . 3J_ VI ------- Glossary of Arsenic Abbreviations As= Arsenic As(III)= Arsenite As(V)= Arsenate AsB= Arsenobetaine AsC= Arsenocholine TMA= Trimethylarsine DMA= Dimethylarsenic acid MMA= Monomethylarsonic acid TMAO= Trimethylarsine oxide vn ------- 1.0 INTRODUCTION In 2000, the U.S. Environmental Protection Agency (EPA) published the Methodology for Deriving Ambient Water Quality Criteria for the Protection of Human Health (USEPA, 2000). That document (hereafter referred to as the 2000 Human Health Methodology) presents technical guidance and the procedure that EPA will follow when deriving new and revised national recommended ambient water quality criteria (AWQC) for the protection of human health under Section 304(a) of the Clean Water Act. The 2000 Human Health Methodology incorporates a number of scientific advancements made over the past two decades. One of these advancements is in the assessment of chemical exposure to humans through the aquatic food web pathway. For certain chemicals, exposure via the aquatic food web is more important than exposure from ingestion of water. One method for incorporating chemical exposure to humans through the aquatic food web involves estimating the amount of a chemical expected to bioaccumulate in fish and shellfish that are commonly consumed by populations in the United States. Previously, EPA primarily used bioconcentration factors (BCF) to estimate accumulation of waterborne chemicals by aquatic organisms. The BCF reflects contaminant accumulation by fish and shellfish only through the water column. Over the past two decades, however, science has shown that all the routes (e.g., food, sediment, and water) by which fish and shellfish are exposed to highly bioaccumulative chemicals may be important in determining the chemical accumulation in the organism's body, and that these chemicals can be transferred to humans when they consume contaminated fish and shellfish. The EPA's approach to estimating uptake into fish and shellfish now emphasizes the use of bioaccumulation factors (BAFs), which account for chemical accumulation from all potential exposure routes (USEPA 2000). The trophic level offish and shellfish consumed by humans can be important in predicting human exposure through the consumption of contaminated fish and shellfish. Therefore, in EPA's 2000 Human Health Methodology national BAFs are estimated for trophic levels 2, 3, and 4 (BAF2, BAF3, and BAF4, respectively), and are calculated as the geometric mean BAF of all species- specific BAFs calculated for a given trophic level (USEPA 2000). This document contains a summary of information currently available on the bioaccumulation potential of arsenic in aquatic organisms. This information was gathered as a first step in assessing the quantity and quality of data available to derive national BAFs for updating the existing 304(a) human health ambient water quality criteria for arsenic. The Office of Science and Technology (OST) is performing this data review for arsenic because new scientific information has been developed regarding its bioaccumulation since the 304(a) criteria for arsenic was published in 1985 (USEPA 1985). Information available that may be useful for determining bioaccumulation factors for arsenic is compiled in this document. National trophic-level specific BAFs are not included in this document because OST is in the process of determining if the data identified is sufficient to derive national BAFs. In the interim, we are making the results of the literature search available to States and authorized Tribes so that they have access to a current compilation and review of available data as they develop State and Tribal Water Quality Standards. ------- 1.1 Important Bioaccumulation Concepts Aquatic organisms accumulate and retain certain chemicals when exposed to these chemicals through water, their diet and other sources. The magnitude of accumulation can vary widely depending on the chemical and its properties. For chemicals that are persistent and hydrophobic, chemical concentrations in contaminated fish and shellfish may be several orders of magnitude higher than their concentrations in water. These chemicals may also biomagnify in aquatic food webs, a process whereby chemical concentrations increase in aquatic organisms of each successive trophic level due to increasing dietary exposures (e.g., increasing concentrations from algae, to zooplankton, to forage fish, to predator fish). For chemicals that biomagnify, consumption of contaminated fish and shellfish may pose unacceptable human health risks even when concentrations in water do not pose unacceptable health risks from consumption of water alone. The term "bioaccumulation" refers to the net accumulation of a chemical by an aquatic organism as a result of uptake from all environmental sources (e.g., water, food, sediment). Bioaccumulation can be viewed as the result of competing rates of chemical uptake and elimination (chemical loss) by aquatic organisms. When the rates of chemical uptake and elimination achieve balance, the distribution of the chemical between the organism and its source(s) is said to be at steady-state. Under steady-state conditions, a BAF is the ratio (in L/kg) of the concentration of a chemical in the tissue of an aquatic organism to its concentration in water, in situations where both the organism and its food are exposed. (USEPA 2000). The BAF is calculated as: Ct BAF = — (Equation 1) where: Ct = concentration of the chemical in wet tissue (either whole organism or specified tissue) CL = concentration of chemical in water -'w 1.2 Bioaccumulation of Arsenic Arsenic, and/or its metabolites, is a chemical that bioaccumulates in tissues of aquatic organisms but does not biomagnify in the aquatic food chain (Chen and Folt 2000, Maeda et al. 1990, Mason et al. 2000, Spehar et al. 1980, Wagemann et al. 1978, Woolson 1975). Arsenic BAFs for upper trophic level freshwater and estuarine fish and shellfish typically consumed by humans generally range between 5 L/kg and 5,000 L/kg (Baker and King 1994, Cooper and Gillespie 2001, Chen et al. 2000, Chen and Folt 2000, Giusti and Zhang 2002, Langston 1984, Mason et al. 2000). Despite the recent attention focused on arsenic uptake and accumulation in aquatic biota, much uncertainty in the mechanisms and bioaccumulation potential of the various forms of arsenic in the environment still exists. The consensus in the literature is that upwards of 85% to >90% of arsenic found in edible portions of marine fish and shellfish is organic arsenic [arsenobetaine (AsB), arsenocholine (AsC), dimethylarsinic acid (DMA)] and that approximately 10% is inorganic arsenic (De Gieter et al. 2002, Goessler et al. 1997, Johnson and Roose 2002, Ochsenkuhn-Petropulu et al. 1997). Less is known about the forms of arsenic in ------- freshwater fish, but there is evidence that organic arsenic may be as prevalent (Kaise et al. 1987; field-based study) or considerably less (Maeda et al. 1990, 1992, 1993; Suhendrayatna et al. 2001, 2002a,b; laboratory-based studies). Knowledge about the uptake and methylation of arsenic by aquatic biota is important for estimating human health risk because it is becoming increasingly evident that methylation of arsenic is critical in controlling its biological fate and effects (Thomas et al. 2001). Inorganic arsenic was previously implicated as the primary toxic form to both aquatic life and humans (Spehar et al. 1980, USEPA 1985). More recent research indicates that when compared to arsenite, trivalent methylated arsenic metabolites1 exert a number of unique biological effects, are more cytotoxic and genotoxic, and are more potent inhibitors of the activities of some enzymes (Kitchin and Ahmad 2003; Thomas et al. 2001). Because each arsenic species (e.g., As(III), As(V), AsB, MMAV, MMAm) exhibits different toxicities, it may be important to take into account the fraction of total arsenic present in the inorganic and organic forms when estimating the potential risk posed to human health through the consumption of arsenic- contaminated fish and shellfish. Ideally, the most appropriate BAFs for the protection of human health would incorporate the most bioavailable and toxic form(s). Although this may not be possible at this time, recent advances in analytical methodologies should eventually permit such assessment. Although very little organic arsenic is present in surface waters, and most arsenic found in groundwater and surface waters is inorganic in nature, the need still exists for information on as many relevant species of arsenic as possible. Specifically, for the derivation of AWQC, more data is needed on the chemical form and relative amounts of the various forms of arsenic in the tissues of aquatic organisms and in surface waters. 1.3 Overview of Document This document is organized into three primary sections. Section 2.0 presents an overview of the literature search strategy, a discussion of data sources, the data quality parameters used to determine if data identified were appropriate for deriving BAFs, and the methods used to calculate BAFs from data found in the literature. The procedures for calculating the BAFs are those described in detail in the 2000 Human Health Methodology (USEPA 2000) and the Technical Support Document Volume 3: Development of National Bioaccumulation Factors (referred to hereafter as the Bioaccumulation TSD; USEPA, 2003). Section 3.0 contains summaries of experiments identified as having data acceptable and appropriate for deriving BAFs. Section 4.0 presents the data used to calculate an arsenic total/dissolved chemical translator. The chemical translator is used to convert arsenic BAFs from water concentration data reported as total arsenic. The translators are also necessary in the implementation of dissolved water quality standards where monitoring data are reported as total arsenic. Section 5.0 contains information regarding the relative fractions of inorganic and organic arsenic (e.g., As(III), As(V), AsB, AsC, DMA) in freshwater and estuarine/marine fishes and shellfish. A basic understanding of the relative fractions of the various arsenic forms in freshwater and saltwater organisms is useful for considering the representativeness and application of arsenic BAFs based on total arsenic. Finally, Section 6.0 contains a summary of BAFs for arsenic and the supporting chemical translator and tissue speciation data. All pertinent references are 'Primarily in the form of (mono)methylarsonous acid (MMA111) and dimethylarsinous acid (DMA111). ------- provided in Section 7.0. Appendix A contains the literature search strategy and data requirements. Appendix B contains an abbreviated summary of all the studies reviewed. Appendices C and D contain tables with the raw data calculations for each acceptable BCF (Appendix C) and BAF (Appendix D) study determined to be acceptable using the criteria outlined in Appendix A. Appendix E and F contain tables with the chemical translator and arsenic tissue speciation data, respectively, provided by ecosystem type and trophic level. Footnotes are provided in the tables where appropriate for clarification of data quality and data use in the BAF calculations. ------- 2.0 LITERATURE SEARCH AND CALCULATION METHODS 2.1 Literature Search A literature search strategy was designed to identify, to the extent possible, all data meeting the criteria for calculating BAFs using field or laboratory measurements. Preference was given to data published in the peer-reviewed literature. Data from publically available reports (e.g., State, Federal, or trade/industry group reports; dissertations; proceedings from professional meetings) were included if appropriate analytical techniques and quality assurance/quality control measures were provided. Studies identified in the literature search were reviewed within the context of deriving a national B AF and therefore the general data quality considerations described in EPA 2003 were used to judge the suitability of the data. Criteria used to determine the acceptability of field-measured BAFs and laboratory-measured BCFs are discussed in Section 5 of the 2000 Human Health Methodology (USEPA, 2000) and in Section 5 of the Bioaccumulation TSD (USEPA, 2003). The literature search strategy and data acceptability criteria are presented in Appendix A. Every attempt was made to facilitate comparisons between studies. For example, arithmetic and geometric means were estimated, even if the original authors did not do so. Trophic levels for fishes were determined using EPA Guidance (USEPA 1995) and the information provided in the specific papers. When more than one BAF was estimated for a given species, a species-mean BAF (SBAF; calculated as the geometric mean) was calculated. There were, however, some exceptions to this general calculation procedure. In some cases where zooplankton data were available, each individual BAF was used to calculate the overall SBAF. This was done because a zooplankton sample consists of multiple species, with the composition varying from waterbody to waterbody. Also, in cases where species-mean BAFs were reported relative to fish age or size, each species mean age or size-specific BAF (e.g., caddis fly larva versus caddis fly pupa) is reported separately. In these instances, the age and size of the fish or shellfish species were taken into account for each trophic level designation. Log normal distributions were assumed in this evaluation, partly for convenience, but primarily because the underlying process and factors that contribute to variability are likely to be multiplicative rather than additive. All species-mean BAFs reported in the summary tables have been rounded to two significant digits. For comparison purposes, BAFs reported in text discussions may be reported as calculated in the appendices. Because this compilation of data includes studies that used a variety of methods for measuring arsenic, statistical comparisons were not performed. ------- 2.2 Methods for Estimating Bioaccumulation Factors In the 2000 Human Health Methodology, EPA presents a framework for deriving BAFs for various types of chemicals (USEPA, 2000). For inorganics and organometallics, the national BAF methodology relies on field-measured BAFs and lab-measured BCFs without adjustments for site-specific factors that affect bioaccumulation (i.e., conversion to baseline BAF using lipid content of aquatic organisms and organic carbon concentrations in water is not necessary). The data provided in this report are provided on an individual study and species-mean basis and have not been translated into national trophic-level values at this time. Therefore the data provided may be applicable for derivation of BAFs for specific waterbodies, ecosystems, or regions. The applicability of the bioaccumulation presented in this report for site-specific use should be judged on a case-by-case basis. For inorganic and organometallic chemicals, BAFs are calculated by one of two procedures, depending on whether or not the chemical undergoes biomagnification in aquatic food webs. Procedure 5 is recommended for inorganic and organometallic chemicals that do not biomagnify and Procedure 6 is recommended for chemicals that do biomagnify. For arsenic, biomagnification does not occur, therefore Procedure 5 is the recommended for deriving BAFs for arsenic. In Procedure 5, BAFs may be developed by two different methods, either from field- measured BAFs or from laboratory-measured BCFs. Because Procedure 5 applies only to chemicals that do not biomagnify, under this procedure BAFs and BCFs are considered to be of equal value in predicting BAFs and the use of food chain multipliers with BCF measurements is not required. A detailed discussion of the scientific basis for the BAF derivation methods and procedures used in the 2000 Human Health Methodology can be found in the Bioaccumulation TSD (2003). BAFs estimated using data available from the field are calculated using the ratio of tissue and water arsenic data as shown in Equation 1 above. In Procedure #5, when appropriate field data does not exist, or if it is considered unreliable, BAFs for arsenic may be predicted from acceptable laboratory-measured BCFs. The general minimum criteria for overall data acceptability were as follows: • measured levels of arsenic (or arsenical species) in whole body or edible tissue of aquatic organisms and in water; • good analytical accuracy (standard recovery) and precision (reproducibility); and • indication that steady-state was achieved (in the case of laboratory BCF studies). The BAFs contained herein are all expressed on a wet-weight basis. BAFs reported or derived using measurements of arsenic on a dry-weight basis were converted using factors that were either measured or reliably estimated from the tissue used in the determination of the BAF. If no measured or reliable conversion factor was reported, zooplankton, shellfish, and other macroinvertebrates were assumed to be comprised of 80 percent water (multiplication factor = 0.2), and fish were assumed to be 75 percent water (multiplication factor = 0.25), in accordance with the Mercury Report to Congress (USEPA 1997). According to the 2000 Human Health Methodology, data for total arsenic in edible tissue (i.e., muscle tissue) offish and shellfish are preferred over whole body data since the general U.S. population doe not typically ingest the entire organism. The exception was for ------- measurements of whole body arsenic in bivalves, aquatic insects and zooplankton. Although the general U.S. population does not commonly consume aquatic insects or zooplankton, available information on bioaccumulation of arsenic in these organism classes have been included in this report for comparison and for completeness. In the few cases where it was possible (Baker and King 1994), and where the water exposure concentrations of arsenic were similar, total arsenic concentrations in whole body and edible tissues of the same species were compared. The results of this very preliminary assessment were inconclusive. Since no apparent differences were found in whole body versus edible tissue arsenic concentration, the species-mean BAF calculations were made using the tissue from which the majority of the BAFs were estimated for that ecosystem type and trophic level designation. In this summary, only concentrations of total dissolved arsenic in water below levels that acutely affect aquatic organisms were used to derive BAFs. Acute arsenic (as As III) toxicity ranges from approximately 1,000 to 3,000 |ig/L for amphipods and cladocerans to greater than 10,000 |ig/L for most freshwater fishes. In saltwater, it ranges from approximately 250 |ig/L for crabs and copepods to greater than 1,500 |ig/L for bivalve molluscs, shrimps and fishes (USEPA 1985). Using the methods outlined above, BAFs were calculated or predicted initially by trophic level for lakes (i.e., lentic aquatic systems), rivers (i.e., lotic aquatic systems), and estuaries. An ecosystem-approach to deriving BAFs was used because differences in general bioaccumulation trends would be expected among the aquatic ecosystems due to inherent differences in food web dynamics, arsenic loadings, and watershed interactions, among other factors. No clear differences in bioaccumulation trends were observed between lentic and lotic ecosystems based on qualitative and semi-quantitative comparisons of the data (see Section 3.5). The limited estuarine and marine data, however, do appear to indicate a possible need for deriving separate BAFs for saltwater systems. ------- 3.0 BAFs FOR ARSENIC IN FRESHWATER AND SALTWATER ECOSYSTEMS 3.1 Estimation of BAFs Using Laboratory-measured BCFs In this analysis, BAFs for trophic levels 2, 3, and 4 were predicted using the concentration of total arsenic in whole animal or muscle tissue and the concentration of arsenic in filtered (dissolved) laboratory water. Ten studies were identified as potentially useful for the derivation of a BAF from a laboratory-based BCF value. Five of the studies used saltwater (estuarine/marine) organisms, including three bivalve molluscs and a crustacean (Table 3-1). BCF determinations from the remaining five studies were conducted using several freshwater fish and invertebrate species. Studies by Gailer et al. (1995), Franseconi et al. (1999), Maeda et al. (1990, 1992, 1993), and Langston (1984) contain only one time period (• 10 days) for which arsenic was measured in the organism (Table 3-1). Because steady-state conditions could not be confirmed in these studies, they were not considered acceptable for BAF determination. The study completed by Hunter et al. (1998) was not acceptable because the concentration of arsenic in exposure water was not measured. The study by Zaroogian and Hoffman (1982) using the eastern oyster, though it involved a 16 week flow-through exposure, was excluded because arsenic uptake by the oyster increased in the first 5 weeks, decreased with spawning, and increased again following spawing indicating that steady-state was never achieved. Perhaps more importantly, at least in the case of this latter study, statistical analysis showed arsenic uptake by oysters was not correlated with arsenic in seawater at the concentration range tested (3,000 to 5,000 |ig/L), but was correlated with the arsenic concentration in the phytoplankton growing in the exposure tanks. Spehar et al. (1980) report BCFs for four freshwater invertebrate species and for rainbow trout parr exposed for 28-days to arsenic [As(III)], arsenic [As(V)], sodium dimethyl arsenate (DMA), or disodium methyl arsenate (MMA). Although only total arsenic was measured in the test water, the turnover rates (100% water replacement in 9 hrs) were sufficiently high to maintain concentrations of the arsenical species provided (in the form of a salt). Target test concentrations for all experiments were 100 and 1,000 |ig/L. Stoneflies, snails, and daphnids accumulated greater amounts of arsenic than fish. Arsenic tissue concentrations in treated rainbow trout were generally the same as those in control fish (approximately 0.75 |ig/g wet weight). Amphipods did not accumulate arsenic above the detection limit of 5 jig/g when exposed to any of the arsenical compounds for 28 days. Arsenic accumulation in stoneflies and snails was generally higher (note: this is opposite of what is observed with field-measured BAFs, see Sections 3.2 and 3.3) when animals were exposed to higher concentrations and appeared to reach steady-state after 14 days. Total arsenic accumulation in stoneflies and snails exposed to 1,000 |ig/L of the various arsenicals did not appear to be greatly affected by the form of arsenic in water, although some animals exposed to inorganic forms did exhibit higher tissue concentrations. Mean BCFs for freshwater invertebrates (trophic level 2 species) ranged from 2 to 22 L/kg. For freshwater fish, mean BCFs ranged from 0.048 L/kg to 14 L/kg. These values are lower than those obtained for aquatic organisms from field studies (see Sections 3.2 and 3.3). No arsenic BCFs are available for saltwater fish species. BAFs predicted from laboratory BCF studies with saltwater invertebrates ranged from 12 L/kg to 1,390 L/kg. These too were generally lower on average than BAFs obtained for these species in field studies (Section 3.4). ------- Based on these data, it does not appear that water-only arsenic exposure fully represents environmental arsenic exposure. Therefore, the accuracy of using laboratory-measured BCFs to represent BAFs for arsenic should be carefully considered. TABLE 3-1: BAFs for Arsenic in Aquatic Organisms Predicted from Laboratory- measured BCFs BCF Species Duration Method3 Arsenical Exposure Reference Freshwater 9.0 22 10 5.0 14 4.0 2.0 14 7.0 10 8.0 12 4.0 0.048 7.0 7.0 5.0 3.0 6.0 9.0 5.0 2.0 Stonefly Cladoceran Snail Snail Rainbow trout Bluegill sunfish Zooplankter Stonefly Cladoceran Snail Snail Red cherry shrimp Guppy Common carp Stonefly Cladoceran Snail Snail Stonefly Cladoceran Snail Snail 28-d 28-d 28-d 28-d 28-d 28-d 7-d 28-d 28-d 28-d 28-d 7-d 7-d 7-d 28-d 28-d 28-d 28-d 28-d 28-d 28-d 28-d FT, M FT,M FT,M FT, M FT,M FT, M S,U FT,M FT, M FT,M FT,M S,U s,u s,u FT, M FT,M FT, M FT,M FT,M FT, M FT,M FT, M As(III) As(III) As(III) As(III) As(III) As(III) As(V) As(V) As(V) As(V) As(V) As(V) As(V) As(V) MMA MMA MMA MMA DMA DMA DMA DMA Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Barrows etal. 1980 Maedaetal. 1990 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Maedaetal. 1992 Maedaetal. 1990 Maedaetal. 1993 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 Speharetal. 1980 ------- BCF Species Duration Method3 Arsenical Exposure Reference Saltwater 863 12 1,390 1,300 35 454 151 Eastern oyster Peppery furrow shell Blue mussel Blue mussel Common shrimp Blue mussel Blue mussel 16 wk 10-d 10-d 10-d 24-d 10-d 10-d FT, M R,M R,U R,U R,M R,U R,U As(III) As(V) AsB AsB AsB AsC TMAO Zaroogian and Hoffman 1982 Langston 1984 Gaileretal. 1995 Franseconi et al. 1999 Hunter and Goessler 1998 Gaileretal. 1995 Gaileretal. 1995 a S= Static; FT = Flow-through; M = Measured; U = Unmeasured 3.2 Estimation of BAFs Using Field Data - Freshwater Lentic Ecosystems 3.2.1 BAFs for Trophic Level 2 Organisms Wagemann et al. (1978) measured arsenic concentrations in several aquatic invertebrate species and in the ambient surface waters of lakes in the vicinity of Yellowknife, Northwest Territories, Canada. One of the lakes (Kam Lake) in the study received untreated sewage from the City of Yellowknife. This lake previously received seepages from two mine tailing ponds. A second lake for which data were available to calculate BAFs was Grace Lake. Grace Lake was chosen as a reference lake for the study because it was subject only to arsenic in the rock formations surrounding the Yellowknife District. Measured dissolved arsenic concentrations in the water of the two lakes for the year when the invertebrates were collected (1975) ranged from approximately 1.7 x 10"2 to 4.0 x 10"2 mg/L for Grace Lake (mean = 2.7 x 10"2 mg/L), and from 2.29 to 2.93 mg/L (mean = 2.58 mg/L) for Kam Lake. The invertebrates were collected in the littoral zone of each lake once every month during the summer (May to September 1975). The BAFs estimated for the various invertebrates sampled from Grace Lake (the designated reference lake) were consistently higher than the BAFs calculated for the same species in Kam Lake (the designated contaminated lake), see Table 3-2. The BAFs calculated for the invertebrates in Grace Lake were generally in the hundreds (range: 28.3 to 377.8 L/kg), while in Kam Lake, they were in the tens (range: 3.4 to 63.6 L/kg). In a more recent study, Chen et al. (2000) examined the accumulation and fate of arsenic in numerous lakes and large and small zooplankton in the northeastern United States. Data were collected during August through October of 1995 and 1996. Each lake was sampled once for arsenic in water and plankton. Trace metal clean techniques were used for the collection and measurement of dissolved (0.45 |im filtration) arsenic in water. Plankton were collected with vertical tows in the deepest part of the lakes from 0.5 m above bottom to the surface using a cone net for macrozooplankton (> 202 jim size fraction; primarily adult copepods and cladocerans) and a Wisconsin net (45-202 jim size fraction) for large phytoplankton and small zooplankton. None of the lakes sampled were in watersheds with known point sources of metal pollution. The arsenic BAFs calculated for small zooplankton and large phytoplankton (range: 369 to 19,487 10 ------- L/kg) were significantly higher than those calculated for larger zooplankton (range: 154 to 2,748 L/kg). Concentrations of total dissolved arsenic in the lakes ranged from 2.2 x 10"5 to 5.8 x 10"4 mg/L, whereas total arsenic in small and large zooplankton ranged from 0.0258 to 1.98 mg/kg, and from 0.0218 to 0.598 mg/kg, respectively. The authors determined that although the arsenic concentrations of the larger zooplankton were positively correlated with the dissolved arsenic concentration in water, they were best predicted by the arsenic levels in their diet (small zooplankton). In a related study, Chen and Folt (2000) examined the trophic transfer of arsenic in a metal-contaminated lake on a seasonal basis. Using measurement and collection techniques similar to their earlier study (Chen et al. 2000), arsenic concentrations in water, particulates (phytoplankton; 0.4 to 0.45 jim), and the two different size fractions of zooplankton were measured in Upper Mystic Lake, New York in June, August and October 1997. Concentrations of dissolved arsenic in water peaked in August at approximately 1.11 x 10"3 mg/L, and were similar at around 6.0 x 10"4 mg/L in June and October (geometric mean of the three measurements = 7.81 x 10"4 mg/L). The arsenic concentrations in small zooplankton mirrored the fluctuating arsenic concentrations in water, while arsenic in larger zooplankton progressively increased from June through October, again indicating the potentially greater influence of dietary arsenic on the larger size class. The mean BAF for arsenic in small zooplankton from Upper Mystic Lake, NY was calculated as 4,391 L/kg; for large zooplankton, it was 2,747 L/kg (Table 3-2). TABLE 3-2: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Lentic Ecosystems SBAF 9,400 560 770 3,100 19,000 390 5,000 1,300 630 500 2,400 BAF 9412 560.9 768.4 3084 19,490 385.0 5008 1285 630.6 503.7 2,382 Snecies Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Location Canobie Lake, NY Clear Pond, NY Community Lake, NY Gregg Lake, NY Horseshoe Pond, NY Ingham Pond, NY Island Pond, NY Lake Placid, NY Lower Kohanza Res., NY Mirror Lake, NY Palmer Pond, NY Reference Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 11 ------- SBAF 370 1,700 7,800 7,600 4,400 2,900 2,200 190 1,200 150 830 1,300 700 590 390 270 730 570 580 2,300 2,700 960 200 55 BAF 369.2 1731 7,825 7,623 4,392 2,938 2,181 192.9 1,174 153.7 826.3 1,344 701.9 590.2 390.6 274.3 728.5 573.8 578.9 2,300 2,748 962.5 197.8 55.0 Species Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Small zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Large zooplankton Zooplankton Zooplankton Location Post Pond, NY Queen Lake, NY Tewksbury Pond, NY Turkey Pond, NY Upper Mystic Lake Williams Lake, NY Canobie Lake, NY Chaffin Pond, NY Clear Pond, NY Community Lake, NY Gregg Lake, NY Horseshoe Pond, NY Ingham Pond, NY Lake Placid, NY Lower Kohanza Res., NY Mirror Lake, NY Post Pond, NY Queen Lake, NY Tewksbury Pond, NY Turkey Pond, NY Upper Mystic Lake Williams Lake, NY Grace Lake, NW Territories Kam Lake, NW Territories Reference Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen and Folt 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen et al. 2000 Chen and Folt 2000 Chen et al. 2000 Wagemann et al. 1978 Wagemann et al. 1978 12 ------- SBAF 64 34 170 110 380 21 10 47 BAF 63.6 109.6 10.3 171.9 107.4 377.8 105.9 4.3 28.3 3.4 229.6 9.7 Species Oligochaeta Snail Snail Bivalve mollusc Amphipoda Ephemeroptera Trichoptera Trichoptera Corixidae Corixidae Chironomidae Chironomidae Location Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Grace Lake, NW Territories Grace Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Reference Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 3.2.2 BAFs for Trophic Level 3 Organisms The arsenic concentrations measured in aquatic invertebrates in Kam and Grace Lakes in the vicinity of Yellowknife, Northwest Territories, Canada by Wagemann et al. (1978) also included several predatory insects. As is noted above for the herbivorous insects, BAFs estimated for the predatory insects from Grace Lake (reference lake) were consistently higher than BAFs for the same species in the contaminated lake (Kam Lake). This is especially true for damselfly, where the difference between BAF estimates is greater than 250 fold (Table 3-3). In general, the difference in BAFs calculated for predatory insects and for sculpin fish exceeded 10 between the two lakes. Chen and Folt (2000), in their examination of the trophic transfer of arsenic in Upper Mystic Lake, New York, also measured whole body arsenic accumulation in five different forage fish species: alewife, black crappie, bluegill sunfish, killifish, and yellow perch. Their objective was to compare the arsenic body burdens in fish with different feeding strategies and to determine whether arsenic burdens biodiminished2 with respect to the various size classes of zooplankton. The fish were collected in October 1997 at multiple sites in the littoral zone of the lake using seines, fyke nets and minnow traps. Five individuals were obtained of each of the species for total arsenic analysis. The arsenic burdens for all fish in Upper Mystic Lake, NY ' Biodiminution is the trend of decreased chemical concentration in tissues of organisms as trophic level increases. 13 ------- were 30 to 100 times lower than the burdens in zooplankton. Although the average concentrations in the various forage fish species differed by less than a factor of 2.5 (range from 0.031 mg/kg for black crappie to approximately 0.075 mg/kg for alewife), alewife and killifish (predominantly planktivorous fish species) had higher burdens than the bluegill sunfish, black crappie, yellow perch, which are higher on the trophic scale. Corresponding arsenic BAFs only ranged from 39.7 (black crappie) to 95.4 L/kg (alewife) - Table 3-3. In a study to survey the upper Gila River, Arizona to determine if waters from mining and agricultural drainages had the potential to cause significant harmful effects on fish and wildlife, Baker and King (1994) measured the total arsenic concentrations in water and fish from San Carlos Reservoir and Talkalai Lake. Three unfiltered water samples were collected from each site from June to August 1990 for measurement of total recoverable arsenic, along with five-specimen whole-body or edible portion composites of near equal weight or length of each forage fish species that was collected (i.e., channel catfish and common carp). The total recoverable arsenic concentrations in water were the same for both the San Carlos Reservoir and Talkalai Lake at 8.0 x 10"3 mg/L. This is equivalent to 6.7 x 10"3 mg/L dissolved arsenic using the default chemical translator of 0.84 to convert to a dissolved arsenic value as described in Section 4.0 of this document. Whole body and fillet samples contained similar levels of arsenic for each fish species at approximately 1.0 to 2.0 x 10"1 mg/kg. Corresponding BAFs based on the estimated concentration of arsenic dissolved in San Carlos Reservoir and in whole body samples of channel catfish and carp were 29.76 and 14.88 L/kg, respectively (Table 3-3). The BAF calculated for carp in Talkalai Lake was 29.76 L/kg. Skinner (1985) conducted a preliminary study at several electric utility wastewater treatment basins to determine if fish caught from these treatment basins presented a risk to human health through their consumption. Nine basins were sampled October 6-9, 1983 using shore zone electroshocking and seining and open-water trawling at various depths. Fish species common to the basins and representing bottom feeders and predators were targeted. Edible portions (fillets) of specimens of legal or recreationally sought sizes were prepared and analyzed for total arsenic concentration. Corresponding water samples from near mid-basin and from approximately 25 cm below the surface were also collected from each basin from where fish were taken. Concentrations of total arsenic in water from the various basins ranged from 3.0 x 10"3 to 3.0 x 10"2 mg/L total arsenic, or from 2.52 x 10"3 to 2.5 x 10"2 mg/L dissolved arsenic using the default arsenic chemical translator of 0.84 (see Section 4.0). Arsenic in muscle tissue from opportunistic bottom feeders in the basins (brown bullhead, common carp, channel catfish) ranged from <0.04 to 0.18 mg/kg wet weight (assuming a water content of 80% as used by the author in the article), and from <0.04 to <0.10 mg/kg wet weight for other forage fish species (e.g., black crappie, pumpkinseed). Since most of the arsenic in fish tissue was below the level of detection, only BAFs for carp collected from the various basins could be calculated. Arsenic accumulation in carp muscle tissue did not appear to be related to the concentration of total arsenic in water. For example, whole body arsenic in carp from Brunner Island Wastewater Treatment Pond #6 (6.0 x 10"2 mg/kg) was quite low despite the relatively high dissolved arsenic concentration in water estimated for that basin (2.5 x 10"2 mg/L). BAFs for carp from the electric utility wastewater treatment basins ranged from 2.38 to 71.4 L/kg (Table 3-3). To summarize, species- mean BAFs (SBAFs) for eight species of forage fish and 10 14 ------- different predatory insects and a carnivorous leech (Hirudinea) were available from four different studies (Baker and King 1994, Chen and Folt 2000, Skinner 1985, Wagemann et al. 1978). In general, those fish species that are lower on the trophic scale (alewife, killifish) had higher BAFs than those species that are slightly higher on the trophic scale (perch, crappie, catfish, carp, sunfishes). In contrast, data from Moon Lake, Mississippi reported in Cooper and Gillespie (2001) show the average concentration of total arsenic in omnivorous fish species (BAF = 6.0 L/kg) to be twice as high as in benthivorous fishes (BAF = 2.7 L/kg), and nearly 20 times higher than planktivorous fishes (BAF = 0.2 L/kg). The species-mean BAFs for trophic level 3 fish in lakes only range by a factor of 5, from approximately 19 to 96 L/kg. By comparison, the species-mean BAFs for trophic level 3 aquatic insects range from approximately 1 to 26 L/kg. TABLE 3-3: BAFs for Arsenic in Trophic Level 3 Aquatic Organisms from Lentic Ecosystems SBAF 17 17 31 4.7 13 7.4 11 4.0 4.9 3.1 BAF 20.1 14.7 68.3 4.5 40.9 0.2 19.2 1.1 13.3 23.6 2.3 48.1 2.5 4.0 25.9 0.9 3.1 Species leech leech dragonfly dragonfly damselfly damselfly whirligig beetles whirligig beetles water strider back swimmer back swimmer diving beetle diving beetle water mite ceraptogonid ceraptogonid tanypodinae Location Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Kam Lake, NW Territories Grace Lake, NW Territories Kam Lake, NW Territories Kam Lake, NW Territories Reference Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 Wagemann et al. 1978 15 ------- SBAF 19 95 30 86 40 48 59 29 BAF 2.38a 19.84a 27.78a 19.84a 71.43a 63.49a 15.87a 15.87a 10.42a 14.88a 29.76a 95.4 29.76a'b 14.88a'c 85.8 39.7 47.7 58.6 70.6 11.8 Species midge common carp common carp common carp common carp common carp common carp common carp common carp common carp common carp common carp alewife channel catfish channel catfish killifish black crappie bluegill sunfish yellow perch sculpin sculpin Location Brunner Is. WTB #6 Martins Cr. IWTB Martins Cr. IWTB Martins Cr. IWTB Montour Detention Basin Montour Detention Basin Montour Stormwater Basin Montour Stormwater Basin Montour Fly Ash Basin San Carlos Reservoir, AZ Talkalai Lake, AZ Upper Mystic Lake San Carlos Reservoir, AZ San Carlos Reservoir, AZ Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Grace Lake, NW Territories Kam Lake, NW Territories Reference Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Skinner 1985 Baker and King 1994 Baker and King 1994 Chen and Folt 2000 Baker and King 1994 Baker and King 1994 Chen and Folt 2000 Chen and Folt 2000 Chen and Folt 2000 Chen et al. 2000 Wagemann et al. 1978 Wagemann et al. 1978 aValue adjusted using arsenic chemical translator of 0.84 to normalize to a BAF based on dissolved arsenic in water. bBased on whole body value; only this value was used in the calculation to determine the SBAF for the species. °Based on edible tissue. 3.2.3 BAFs for Trophic Level 4 Organisms 16 ------- In addition to the several forage fishes which were examined to assess the trophic transfer of arsenic in metal-contaminated Upper Mystic Lake, New York, Chen and Folt (2000) also measured whole body arsenic accumulation in the largemouth bass. Five individuals were obtained for total arsenic analysis in October 1997. The mean concentration of dissolved arsenic in water measured in June, August and October 1997 was 7.81 x 10"4 mg/L. The average arsenic burden for largemouth bass in Upper Mystic Lake, NY (3.6 x 10"2 mg/kg) was approximately 60 to 95 times lower than the burdens in large and small zooplankton, respectively. The average arsenic concentrations in largemouth bass differed by less than a factor of 2 from the various forage fishes it preys upon, and had an arsenic BAF of 46.1 L/kg (Table 3-4). In the study of the Upper Gila River, Arizona reported by Baker and King (1994), the BAF for largemouth bass based on whole-body tissue was very similar to the value derived for this species by Chen and Folt (2000). The BAF for largemouth bass in San Carlos Reservoir, AZ (in the Upper Gila River Watershed), was based on the estimated dissolved arsenic concentration in the reservoir (0.84 x 8.0 x 10"3 mg/L or 6.72 x 10"3 mg/L) and the total arsenic concentration in a composite of 5 individuals. Analysis of whole body and fillet samples of these bass indicated slightly different levels of total arsenic: 3.0 x 10"1 and 1.0 x 10"1 mg/kg, respectively. As a result, the corresponding BAFs for whole body and edible tissue were 44.64 and 14.88 L/kg, respectively (Table 3-4). Only the BAF based on the whole body arsenic concentration was used to calculate the BAFs for this species because too few BAFs based on edible fish tissue for these and other fish species exist to warrant otherwise. TABLE 3-4: BAFs for Arsenic in Trophic Level 4 Fish from Lentic Ecosystems SBAF 45 BAF 44.64a'b 14.88a'c 46.1 Species largemouth bass largemouth bass largemouth bass Location San Carlos Reservoir, AZ San Carlos Reservoir, AZ Upper Mystic Lake Reference Baker and King 1994 Baker and King 1994 Chen and Folt 2000 aValue adjusted using arsenic chemical translator of 0.84 to normalize to a BAF based on dissolved arsenic in water. bBased on whole body value; only this value was used in the calculation to determine the SBAF for the species. °Based on edible tissue. 3.3 Estimation of BAFs Using Field Data - Freshwater Lotic Ecosystems 3.3.1 BAFs for Trophic Level 2 Organisms Only two studies were found for calculating BAFs for trophic level 2 aquatic organisms in lotic ecosystems. Mason et al. (2000) sampled herbivorous insects and other aquatic organisms in October 1997, April 1998, and July 1998 from two sites in western Maryland: Harrington Creek Tributary and Blacklick Run. Water samples (filtered in situ at 0.8 jim) were collected monthly in both of the streams using clean techniques. The average dissolved arsenic concentrations in water were 6.7 x 10"4 and 3.7 x 10"4 mg/L for Harrington Creek and Blacklick Run, respectively. Despite the difference in dissolved arsenic concentrations, there was no concomitant variation in insect arsenic burdens between the two sites. BAFs for herbivorous aquatic insects were consistently highest in Blacklick Run (Table 3-5). The authors also noted a 17 ------- trend of increasing arsenic body burden with decreasing average size of the animal, which they ascribed to the dependence of arsenic accumulation in small insects on the surface/volume ratio during the process of adsorption directly from water. A similar phenomenon was observed in studies by Hare et al. (1991) and Cain et al. (1992). In addition to the BAF data available from Herrington Creek and Blacklick Run, arsenic levels present in arsenic-rich river water and biota collected from the Haya-kawa River at hot springs in Hakone, Kanagawa, Japan are available in Kaise et al. (1997). In this study, the aquatic herbivorous insects collected included a freshwater snail (Semisulcospira libertind) and the larvae and pupae of a caddisfly (Stenopsyche marmoratd). The river water at the site where the insects were collected contained 3.0 x 10"2 mg/L total arsenic, 93% of which was inorganic and the remaining 7% trimethylated arsenic. The concentration of total arsenic in caddisfly pupae was substantially higher (2.05 mg/kg) than in the larvae of this species (2.36 x 10"1 mg/kg) and in the marsh snails (1.86 x 10"1 mg/kg). BAFs based on estimated concentration of dissolved arsenic in Haya-kawa River water (0.84 x 3.0 x 10"2 mg/L or 2.52 x 10"2 mg/L) were less than 10 L/kg for caddisfly larvae and marsh snails, and approximately 81 L/kg for caddifly pupa (Table 3-5). TABLE 3-5: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Lotic Ecosystems SBAF 7.4 3,800 600 2,300 9.4 81 970 BAF 7.38a 5,619 2,543 604.6 2,810 1,846 9.37a'b 81.35a'b 2,401 392.8 Snecies snail (marsh) mayfly mayfly shredder stonefly caddisfly caddisfly caddisfly (larva) caddisfly (pupa) cranefly cranefly Location Hayakawa River, Japan Blacklick Run, MD Herrington Creek, MD Blacklick Run, MD Blacklick Run, MD Herrington Creek, MD Hayakawa River, Japan Hayakawa River, Japan Blacklick Run, MD Herrington Creek, MD Reference Kaise etal. 1997 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Kaise et al. 1997 Kaise et al. 1997 Mason et al. 2000 Mason et al. 2000 aValue adjusted using arsenic chemical translator of 0.84 to normalize to a BAF based on dissolved arsenic in water. bValues shown to indicate the gross differences in bioaccumulation between the various life stages of this species. Most data for aquatic insects in this document are for larvae of the species; pupa were rarely measured. 3.3.2 BAFs for Trophic Level 3 Organisms 18 ------- Both Mason et al. (2000) and Kaise et al. (1997) included several other aquatic organisms in their studies, including a number of forage fishes, freshwater crustaceans, and some predatory aquatic insects (Table 3-6). Added to this compilation are BAFs for channel catfish, flathead catfish, and common carp from numerous sites along the Gila and San Francisco Rivers, AZ (Baker and King 1994). BAFs for trophic level 3 organisms from the more polluted Haya-kawa, Gila, and San Francisco Rivers are consistently lower, generally by more than an order of magnitude or more, compared to like organisms in the western Maryland streams, Harrington Creek and Blacklick Run, respectively (Table 3-6). The highest BAFs were for dobsonflies, dragonflies and predatory stoneflies (Family: Perlidae), and the lowest for several of the forage fishes, particularly the sweet fish, Japanese dace, and mottled sculpin. TABLE 3-6: BAFs for Arsenic in Trophic Level 3 Aquatic Organisms from Lotic Ecosystems SBAF 32 560 1,000 500 690 110 420 2.0 8.5 11 BAF 32.42a 489.2 646.4 1,333.5 824.8 195.7 1257 1102 432.1 114.1a 571.1 308.2 2.02a 10.82a 11.90a 4.76a 10.60a Species prawn crayfish crayfish predatory stonefly predatory stonefly dragonfly dragonfly dobsonfly dobsonfly dobsonfly larva brook trout (small) brook trout (small) sweet fish common carp common carp common carp downstream Location Hayakawa River, Japan Blacklick Run, MD Herrington Creek, MD Blacklick Run, MD Herrington Creek, MD Blacklick Run, MD Herrington Creek, MD Blacklick Run, MD Herrington Creek, MD Hayakawa River, Japan Blacklick Run, MD Herrington Creek, MD Hayakawa River, Japan Gila River, AZ Gila River, AZ Gila River, AZ Hayakawa River, Japan Reference Kaise etal. 1997 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Mason et al. 2000 Kaise et al. 1997 Mason et al. 2000 Mason et al. 2000 Kaise et al. 1997 Baker and King 1994 Baker and King 1994 Baker and King 1994 Kaise et al. 1997 19 ------- SBAF 510 280 4.0 380 280 5.3 6.5 15 13 800 BAF 512.7 281.5 3.97 376.1 283.9 7.00a 3.50a 5.95a 3.50a 7.00a 11.90a 11.90a'b 5.95a 14.68a 13.21 798.1 Species fatminnow blacknose dace creek chub Japanese dace white sucker brown bullhead channel catfish channel catfish channel catfish flathead catfish flathead catfish flathead catfish flathead catfish flathead catfish amphidromous goby goby Mottled Sculpin Location Blacklick Run, MD Herrington Creek, MD Hayakawa River, Japan Herrington Creek, MD Herrington Creek, MD Gila River, AZ Gila River, AZ San Francisco River, AZ Gila River, AZ Gila River, AZ Gila River, AZ Gila River, AZ San Francisco River, AZ Hayakawa River, Japan Hayakawa River, Japan Blacklick Run, MD Reference Mason et al. 2000 Mason et al. 2000 Kaiseetal. 1997 Mason et al. 2000 Mason et al. 2000 Baker and King 1994 Baker and King 1994 Baker and King 1994 Baker and King. 1994 Baker and King. 1994 Baker and King. 1994 Baker and King. 1994 Baker and King 1994 Kaise et al. 1997 Kaiseetal. 1997 Mason et al. 2000 aValue adjusted using arsenic chemical translator of 0.84 to normalize to a BAF based on dissolved arsenic in water. bValue was based on edible tissue, and therefore, was not used in calculation of the SBAF in lieu of several based on whole body values. 3.3.3 BAFs for Trophic Level 4 Organisms BAFs are only available for two coldwater trophic level 4 fish species in lotic ecosystems, large brook trout (from Mason et al. 2000) and masu salmon (Kaise et al. 1997). As noted above, BAFs for brook trout from the less arsenic contaminated streams in western Maryland (Herrington Creek and Blacklick Run) were substantially higher than the BAF estimated for masu salmon collected from the arsenic-rich Haya-kawa River, Japan (Table 3-7). The SBAF for brook trout was calculated to be 270 L/kg, while for masu salmon it was 45 times lower at 5.8 L/kg (Table 3-7). Compared to the BAFs estimated for forage fishes and other trophic level 3 aquatic organisms from the same locations (refer to Table 3-6 above), the BAFs 20 ------- for the trophic level 4 fishes were approximately the same. TABLE 3-7: BAFs for Arsenic in Trophic Level 4 Fish from Lotic Ecosystems SBAF 270 5.8 BAF 304.6 237.8 5.79a Species brook trout (large) brook trout (large) masu salmon Location Blacklick Run, MD Herrington Creek, MD Hayakawa River, Japan Reference Mason et al. 2000 Mason et al. 2000 Kaiseetal. 1997 aValue adjusted using arsenic chemical translator of 0.84 to normalize to a BAF based on dissolved arsenic in water. 3.4 Estimation of BAFs for Arsenic Using Field Data - Saltwater Ecosystems 3.4.1 BAFs for Trophic Level 2 Organisms Three studies contain information useful for calculating BAFs for trophic level 2 saltwater organisms (Giusti and Zhang 2002, Langston 1984, and Valette-Silver et al. 1999). All three studies examined the arsenic burdens in edible tissues of bivalve molluscs, and included the measured dissolved arsenic concentration in the exposure water. A fourth study by Hung et al. (2001) reportedly contains information on the arsenic burdens in over 30 different marine molluscs at over 12 different coastal sites in Taiwan, but the species-specific values for arsenic in tissue were not provided in the condensed summary of information included in the published article. Giusti and Zhang (2002) examined the level of trace element contamination in water, sediment and the marine mussel Mytilus galloprovincialis in a section of the Venice Lagoon near Murano Island, Italy. The dissolved, labile arsenic concentration in the water of the lagoon was measured by means of a recently developed trace metal speciation technique referred to as DGT (diffusive gradients in thin-films). The DGT technique allows trace metal speciation measurements to be made in situ in marine and fresh waters. In this study, two DGT devices were deployed together at each site to determine the arsenic concentrations representative of the dissolved fraction of arsenic in water available to the mussels. Mussels from about 3-7 cm long were collected from wooden pillars at the four sites where they were most common. They were depurated for 24-h in water from a reference site prior to separating soft tissue from the shells. The soft tissues from all organisms from a site were pooled prior to measuring the total arsenic concentration. Arsenic burdens in the mussels ranged from 2.4 to 3.6 mg/kg. Dissolved, labile arsenic in water from the corresponding sites ranged from 1.90 x 10"3 mg/L to 4.73 x 10"3 mg/L. BAFs were from 762 to 1263 L/kg (Table 3-7). Valette-Silver et al. (1999) examined the arsenic concentrations in bivalve samples collected under the National Status and Trends Program (NS&T), Mussel Watch Project (MWP) from the southeast coasts of the U.S. Compared to the rest of the U.S., the oysters collected from sites located along the southeastern coasts, from North Carolina to the Florida panhandle, displayed high concentrations of arsenic in their soft tissues. As part of their examination of this phenomenon in oysters, samples of two species of bivalves (the eastern oyster and a marine mussel species -Isognomon sp.), water, sediment, and particulates, were collected in 1993 in 21 ------- Biscayne Bay, Florida in addition to the samples collected in the NS&T MWP. In the brackish waters collected from the mouth of the Miami River feeding into Biscayne Bay, total dissolved arsenic concentrations averaged 8.9 x 10"4 mg/L. Most of the arsenic in the water was present as inorganic arsenate (As(V) = 6.9 x 10"4 mg/L versus As(III) = 1.0 x 10"4 mg/L), with only very small concentrations of organic arsenic present (MMA = 3.0 x 10"5 mg/L and DMA = 6.0 x 10"5 mg/L). The average total arsenic concentration in eight individual mussels was high at 7.46 mg/kg, while the total arsenic in small oysters averaged 4.72 mg/kg. The corresponding BAFs calculated for the two bivalve species are 8,382 L/kg and 5,303 L/kg, respectively (Table 3-7). Langston et al. (1984) carried out a field and laboratory evaluation of the availability of arsenic to estuarine and marine organisms. The field study area focused primarily on Restronguet Creek, a branch of the Fal estuary system. Restronguet Creek has historically been contaminated by metalliferous mining in southwest England. Water, sediment, and selected organisms were collected from Restrognuet Creek between 1978 and 1981, and for comparison, from the Tamar and Torridge estuaries. The accumulation of arsenic in the field was studied by transplanting the bivalve mollusc Scrobiculariaplana from the Tamar estuary to sites in Restrognuet Creek and recovering subsamples (usually 6 individuals were pooled for analysis) at intervals between February 1980 and March 1981. The effect of dissolved arsenic concentration on uptake rate in the laboratory was also determined in Tamar S. plana (3 cm shell length) using 74As as arsenic acid. Arsenic concentrations in S. plana transferred from the Tamar estuary to site S in Restrognuet Creek (4.9 x 10"3 mg/L measured dissolved arsenic concentration taken at high-water, 4 September 1980) had more than doubled in 1 month and after 4 months were similar to levels in native individuals (approximately 32 mg/kg, whole bivalve). The arsenic concentrations in native and transplanted populations remained constant for the remainder of the experiment (up to 12 months). The total arsenic in tissue remained stable despite a seasonal increase in concentrations of dissolved arsenic entering the creek during the summer. This observation suggested to the authors a particulate (dietary) rather than waterborne source of arsenic for this mollusc species, which was confirmed through laboratory studies where concentration factors determined for this species in experimental exposures to dissolved arsenic were two orders of magnitude less than the estimated values in natural populations. The B AF for transplanted S. plana in Restroguet Creek was estimated to be 6,490 L/kg (Table 3-7). Additional BAFs for native populations of this species in Restrognuet Creek and the Tamar Estuary based on measured interstitial water arsenic concentrations and tissue concentrations back-calculated from the reported concentration factors at the sites are 776.8 L/kg and 623.9 L/kg, respectively (Table 3-7). The latter values were not included in the calculation of the SBAF for the species. TABLE 3-8: BAFs for Arsenic in Trophic Level 2 Aquatic Organisms from Saltwater Ecosystems SBAF 6,500 BAF 6,490 776.8a 623. 9a Species bivalve bivalve bivalve Location Restronguet Cr, Fal Estuary, U.K. Restronguet Cr., Fal Estuary, U.K. Tamar Estuary, U.K. Reference Langston 1984 Langston 1984 Langston 1984 22 ------- 880 8,400 5,300 1,263 680.8 923.1 761.6 8,382 5303 mussel mussel mussel mussel mussel oysters Is. of Murano, Italy - Site G Is. of Murano, Italy - Site E Is. of Murano, Italy - Site B Is. of Murano, Italy - Site F Biscayne Bay, FL Biscayne Bay, FL Giusti and Zhang 2002 Giusti and Zhang 2002 Giusti and Zhang 2002 Giusti and Zhang 2002 Valette-Silver et al. 1999 Valette-Silver et al. 1999 aValue was based on measurements of arsenic in interstitial water, and therefore, was not used in calculation of the SB AF in lieu of a value based on measurements of total dissolved arsenic in the water column. 3.5 Summary of BAFs for Arsenic in Freshwater and Saltwater Ecosystems Preliminary assessment of BAFs estimated from laboratory-measured BCFs indicate that the estimated values are lower than those derived using data from the field BAFs. Much of the BCF data failed to meet the requirement that steady-state conditions be achieved during the exposure. The majority of the BAFs estimated for trophic level 2 organisms in lentic ecosystems come from a single comprehensive study of arsenic accumulation in northeastern lakes (Chen et al. 2000). Although the lakes are free from any known point sources of arsenic, the range in species-mean BAFs is quite large, and highest for the smaller size class of zooplankton collected. Other values were estimated from trophic level 2 aquatic insects from the Northwest Territories, Canada (Wagemann et al. 1978). The species-mean BAFs estimated for these species are substantially lower on the average than for the zooplankters, though mostly higher than those estimated for organisms comprising the higher trophic levels (3 and 4, respectively). Only one species-mean BAF is available for trophic level 4 organisms. The BAFs estimated for trophic level 2 organisms in lotic ecosystems are all for herbivorous aquatic insects from one of three river systems, Haya-kawa River, Japan (Kaise et al. 1997), and Harrington Creek and Blacklick Run tributaries in northwest Maryland ( Mason et al. 2000). Trophic level 3 and 4 species-mean BAFs for lotic ecosystems were more variable than those for lentic ecosystems (Table 3-8). There is no clear explanation for this finding. The number and diversity of aquatic organisms represented at these higher trophic levels were about the same. Moreover, the concentrations of total and dissolved arsenic in water from the various lakes represented were more variable than for rivers and streams. An observation that does seem to hold for both lentic and lotic ecosystems is that BAFs estimated for aquatic animals in the most arsenic contaminated waters were consistently lowest. This phenomenon has been noted for other trace elements, most recently for selenium (Mclntyre et al. 2002). However, unlike arsenic, selenium is considered an essential trace metal. 23 ------- The concentrations of arsenic in the edible soft tissues of marine and estuarine bivalve mollusks are substantially higher than for their freshwater counterparts. Species-mean BAFs were calculated for four saltwater species, from three different studies. In one study (Lin, 2001) arsenic BAF data for the herbivorous marine fish species the mullet, Liza macrolepis, was over several hundred times lower than the lowest BAF estimated for a saltwater species. TABLE 3-9: Summary of BAFs for Arsenic by Trophic Level for Freshwater and Saltwater Ecosystems Trophic Level 2 3 4 Freshwater Species-Mean BAFs Range (number) Lentic 9.8- 19,000 (n = 43) 4.0-95 (n=18) 45-46 (n=l) Lotic 7.4-3,800 (n = 7) (2.0 - 1,000) (n = 20) 5.8-270 (n=2) Saltwater Species- Mean BAFs Range (number) 880 - 8,400 (n = 4) - - 24 ------- 4.0 CHEMICAL TRANSLATOR FOR ARSENIC IN SURFACE WATERS 4.1 Introduction to Chemical Translators Dissolved forms of a chemical are more readily bioaccumulated by organisms than are corresponding particulate forms. Dissolved metal more closely approximates the bioavailable fraction of metal in the water column than does total recoverable metal (USEPA 1993). This does not necessarily mean that particulate metal is nontoxic, only that particulate metal uptake into aquatic organisms is limited (USEPA 1996). Dissolved metal is operationally defined as that which passes through a 0.45 jim or a 0.40 jim filter and particulate metal is operationally defined as total recoverable metal minus dissolved metal. A part of what is measured as dissolved metal is particulate metal that is small enough to pass through the filter, or that is adsorbed to or complexed with organic colloids and ligands. Some or all of this may be biologically unavailable. EPA defines the chemical translator (fd) as the fraction (f) of the total recoverable metal in the surface water that is dissolved (d). The translator can be used to estimate the concentration of dissolved metal from measured total metal values, or vice versa. The most reliable translators are produced from site-specific data. Two procedures can be used to develop site-specific translators. Complete guidance for determining a site-specific translator is provided by EPA (USEPA 1996). The most straightforward approach is to analyze directly the dissolved and total recoverable fractions. In this approach, a number of samples are taken over time and an fd value is determined Cd (Equation 2) for each sample, where: where: Cd = the dissolved (operationally-defined) concentration of chemical in water Ct = the total concentration of chemical in water The translator is then calculated as the geometric mean (GM) of the dissolved fractions (fds). The second approach is to derive fd from the use of a partition coefficient, Kd, where usually the coefficient is determined as a function of total suspended solids (TSS) (although some other basis such a humic substances or particulate organic carbon may be used). 4.2 Objective To expand the BAF database for arsenic, a chemical translator was required to derive BAFs from water concentration data reported as total arsenic. Translators and/or related Kd values can be generated from an acceptable existing literature-derived data base. To gather this 25 ------- data base, peer-reviewed literature papers from 1985 to present were searched and reviewed. All data identified in the literature were required to meet the following criteria in order to be used it in developing the translator: Appropriate techniques were used in sampling and analysis. Adequate QA/QC procedures were used. Analytical methods used provided sufficiently low detection level. Given the available data it was possible to determine the relative fractions of total and dissolved arsenic in ambient surface waters, and hence generate a translator for total arsenic, but it is not possible to determine the total and dissolved fractions of inorganic arsenic, AsB, AsC, and DMA. 4.3 Results and Discussion The results of the literature review are presented in Table 4-1. Due to the paucity of data found, these fd results are presented for combined lake, river and estuarine systems. The data represent four lotic, two lentic, one estuarine, and one lotic-lentic combined systems. Clearly, insufficient data were obtained to provide reliable fd (translator) values for arsenic for individual systems. The translator for total dissolved arsenic derived from the recent literature data base (Table 4-1) is 0.84. Little information that would allow for development of translator values for individual dissolved arsenic species was found. Only two articles (Anderson and Bruland, 1991; Michel et al., 2001) contained adequate data for use in calculating arsenic species translators. In addition, the dynamic inter-conversion that occurs between arsenic species all but precludes use of arsenic species translators. Thermodynamically predicted As(V)/As(III) ratios are rarely observed in natural surface waters, and experimental evidence clearly indicates that a multiplicity of factors influences the relative concentrations of these species (Cullen and Reimer 1989; Smedley and Kinniburg 2002). The interconversion of arsenite and arsenate by algal/bacteria transformations prevents achievement of thermodynamic equilibrium. A recent survey of surface drinking water sources in the U.S. found that about two thirds of the soluble arsenic was As(V) arsenate, and about one third was in the As(III) arsenite form (Chen et al. 1999). Concentrations and relative proportions of As(V) and As(III) vary according to changes in input sources, redox conditions, pH, and biological activity. The presence of As(III) may be maintained in oxygenated waters by biological reduction of As(V), particularly during summer months. Proportions of As(III) and As(V) are particularly variable in stratified lakes where redox gradients and biological activity can be large and seasonally variable. For example, Anderson and Bruland (1991) found an fd value of 0.34 for As(V) in Davis Reservoir, CA surface water in October, 1988, but an fd value of 0.87 was measured in February, 1989. Similarly, an fd value determined for dimethyarsenic acid (DMA) was 0.419 in October but was found to be <0.01 in February, showing the large seasonal variability of the arsenic species fds. Variability was encountered with depth of sample also (an fd of 0.42 for DMA on the surface but an fd of 0.01 at 17.7 m depth in the reservoir in October, 1988). Therefore, because of the dynamic transformations and variability of species, no attempt has been made to present species specific arsenic translators. 26 ------- 4.4 Application of the Chemical Translator for BAF Calculations Application of the arsenic translator to the saltwater BAF data set was not required because all values for arsenic in water were already provided in the desired form (total dissolved arsenic). The translator was used for two lotic studies and one lentic study in the freshwater dataset. The BAF data to which the translator was applied was primarily for trophic level 3 and 4 freshwater organisms. Because the BAFs estimated for these organisms were generally very low, the use of the translator did not greatly alter the original BAF estimate. The use of the translator permitted the calculation of additional BAFs in 12 instances for freshwater fish species and 5 instances for freshwater invertebrate species. TABLE 4-1: Dissolved Arsenic as a Fraction of Total Arsenic in Surface Waters fd Value 0.62 0.74 0.81 0.87 0.88 0.92 0.94 0.94 Location Surface Drinking Water Sources, U.S. Ogeechec River, GA Los Angeles Aquaduct Channel, CA Tanagawa and Saganigawa Rivers, Japan Upper Mystic Lake, MA Davis Creek Reservoir, CA Seine River, France Thames Estuary, England Reference Chenetal. 1999 Waslenchuk 1979 Hering and Kneebone 2002 Tanzakietal. 1992 Chen and Folt 2000 Anderson and Brulandl991 Michel etal. 2001 Millward et al. 1997 GM= 0.84 Range 0.62 - 0.94 27 ------- 5.0 ARSENIC SPECIATION IN TISSUES OF AQUATIC ORGANISMS As indicated in the Introduction to this document, there exists in the literature a general consensus that from 85% to >90% of arsenic found in edible portions of marine fish and shellfish is in an organic form [(arsenobetaine (AsB), arsenocholine (AsC), dimethyl arsinic acid (DMA)] and that approximately 10% is inorganic arsenic species [As(III), As(V)]. Less is known about the forms of arsenic in freshwater fish, but the available evidence suggests inorganic forms predominate over organic forms (AsB, AsC). Marine algae accumulate inorganic arsenic from seawater and incorporate it into an array of carbohydrate compounds known as arsenosugars. Arsenosugars are precursors in the metabolic pathway to AsB and AsC which may explain the source of these latter forms in marine animals (Hansen et al. 2003). Currently, there is no similar information on freshwater phytoplankton. This section includes a compilation of the available information regarding the relative fractions of inorganic and organic (e.g, AsB, AsC, DMA) arsenic in freshwater and marine aquatic organisms by trophic level. These data are useful for understanding the transformation of arsenic in tissues of organisms within the aquatic food web, and for considering and approximating possible BAFs based on the various forms of arsenic present in animal tissue. 5.1 Freshwater Aquatic Organisms 5.1.1 Trophic Level 2 Very little field data exists to determine the relative fractions of the various arsenic forms in tissues of trophic level 2 organisms in freshwater systems. For example, no data were found for trophic level 2 organisms in lentic ecosystems, and only a single study contains this type of information in lotic ecosystems. Kaise et al. (1997) reported the arsenic species present in arsenic-rich river water and the corresponding arsenic body burden in aquatic invertebrates from the Haya-kawa River in Hakone, Kanagawa, Japan. The river water at the site where the organisms were collected contained 3.0 x 10"2 mg/L total arsenic, 93% of which was inorganic and the remaining 7% trimethylated arsenic. The corresponding chemical speciation of arsenic in whole body tissue of trophic level 2 organisms varied greatly between species. Caddisfly larvae and pupae were composed mostly of dimethylarsenic (DMA) compounds, 86% and 56%, respectively, while the marsh snail contained only about 27% (Table 5-1). The remainder of the total arsenic burden in the whole body of these organisms was identified as trimethylarsenic compounds, which is commonly distinguished as AsB or AsC in marine fish. Very little inorganic arsenic was detected in these organisms. These findings are meaningful in that nearly all of the arsenic accumulated naturally by these particular freshwater organisms in the Haya- kawa River was biomethylated. Substantially more data are available on the various forms of arsenic present in tropic level 2 organisms exposed to arsenic as either arsenate [As(V)] or arsenite [As(III)] in laboratory experiments. Modified Detmer medium was used as the laboratory dilution water in all of the laboratory studies. The experimental designs were such that water-only and dietary (2 or 3 step laboratory food-chain model) arsenic exposure was included. 28 ------- Suhendrayatna et al. (2001,2002a, 2002b) investigated the bioaccumulation and biotransformation of arsenite [As(III)] by the waterflea, Daphnia magna, and red cherry shrimp, Neocaridina denticulata. Waterfleas exposed for 7 days to arsenite under static conditions at concentrations ranging from 0.05 to 1.5 mg/L contained from 63% to 75% As(III) and from 24% to 36% As(V), with geometric means of approximately 70 and 28%, respectively (Table 5-1). The relative fraction of DMA measured in their whole body tissues was less than 2%. Shrimp exposed under similar conditions to water containing from 0.1 to 1.5 mg/L arsenic as arsenite contained from 37% to 48% As(III) and from 22% to 56% As(V), with geometric means of approximately 43 and 35%, respectively (Table 5-1). The relative fraction of DMA in whole body was markedly higher for shrimp ranging from 7% to 32%. In contrast, for waterfleas fed a diet of arsenite-dosed alga (Chlorella vulgaris) which contained approximately 83% As(V), 9% As(III), and only 6% DMA, the fraction of As(III) and As(V) in their tissues was nearly 50:50, while in shrimp, a much greater percentage existed as As(V) (80 to 90%), the remainder in the form of As(III) (Table 5-1). In both cases, regardless of exposure type (water-only or dietary), inorganic arsenic was accumulated as the predominant arsenic species in these organisms, with relatively little indication of biomethylation. Similar observations were made for the red cherry shrimp exposed to arsenic as arsenate in the medium (Maeda et al. 1992, 1993), whereas the relative fraction of organic arsenic (measured as DMA) in the zooplankterMo/'wa macrocopa exposed to arsenic as arsenite in the medium was much higher, approximately 55% (Maeda et al. 1990). In general, for trophic level 2 organisms exposed to arsenic as either arsenite or arsenate in laboratory water, approximately 80% of their tissue body burden remains in the inorganic forms, while less than 10% to 20% is biomethylated. The same appears to be true when these organisms are exposed to arsenic via their diet. The observations differ substantially from those reported by Kaise et al. (1997) who examined trophic level 2 organisms in field studies. TABLE 5-1: Arsenic Speciation in Freshwater Trophic Level 2 Aquatic Organisms Species marsh snail caddisfly larva caddisfly pupa zooplank. grazer waterflea Test type Field Field Field Lab; As(III) (water) Lab; As(III) (water) Fraction of Total Arsenic3 Inorganic NM NM NM 0.45 - As(III) - - - NM 0.70 As(V) - - - NM 0.28 Organic 0.89 0.95 0.99 0.55 0.012 Reference Kaise etal. (1987) Kaise etal. (1987) Kaise etal. (1987) Maeda etal. (1990) Suhendrayatna et al. (2001) 29 ------- red cherry shrimp red cherry shrimp zooplank. grazer waterflea red cherry shrimp red cherry shrimp Lab; As(III) (water) Lab; As(V) (water) Lab; As(III) (diet) Lab; As(III) (diet) Lab; As(III) (diet) Lab; As(V) (diet) - 0.83 0.81 - - 0.88 0.43 NM NM 0.44 0.13 NM 0.35 NM NM 0.56 0.86 NM 0.16 0.15 0.24 - 0.016 0.056 Suhendrayatna et al. (2001) Maedaetal. (1992, 1993) Maedaetal. (1990) Suhendrayatna et al. (2001, 2002a) Suhendrayatna et al. (2001, 2002b) Maedaetal. (1993) aValues represent geometric mean; calculations based on data compiled in Appendix X. 5.1.2 Trophic Levels 3 and 4 The field study by Kaise et al. (1997) provides data on the proportion of organic arsenic (di- and trimethyl arsenic species) in several forage fishes, a piscivorous fish, a freshwater prawn, and dobsonfly larvae. In addition to these data, the relative fractions of inorganic arsenic and AsB in the tissues of crayfish caught in an area affected by a toxic mine-tailing spill near Seville, southern Spain were analyzed and reported by Devesa et al. (2002). In the former study, the range in percent dimethylarsenic compounds identified in trophic levels 3 and 4 species from Haya-kawa River in Hakone, Kanagawa, Japan, was quite large with Japanese dace, prawn, and dobsonfly larva each containing 76, 75, and 96% dimethylarsenic compounds, respectively, whereas other species including goby, downstream fatminnow, and sweet fish contained less than 25% of these dimethylated arsenic compounds, but a much greater percentage of trimethylarsenic. The single trophic level 4 fish represented in the dataset from this study, the masu salmon, contained about 43% dimethylarsenic compound and 55% trimethylarsenic compounds. Thus, although there appears to be very large differences in the form of biomethylated arsenic species present in tissues of aquatic organisms within each of the respective trophic levels, very little inorganic arsenic in tissues is present (Table 5-2). By contrast, in the recent study by Devesa et al. (2002), crayfish from the River Guadiamar and Puente de los Vaqueros and Aguas Minimas Canal, Seville, Spain contained from 21% to 92% inorganic arsenic based on whole body analysis. The mean (geometric) fraction of inorganic arsenic in crayfish whole body tissue was about 54% (Table 5-2). The fraction of AsB in this species ranged from a mere 2% to less than 16% (geometric mean = 4%). Crayfish from experimental ponds raised near the contaminated study area contained similar mean fractions of the arsenicals (Table 5-2), 29% and 4%, respectively. The findings of the various laboratory exposures of higher trophic level organisms, i.e., 30 ------- carp, tilapia, Japanese medaka, and guppy, exposed to arsenite and arsenate via the water in the Suhendrayatna and Maeda studies indicated that inorganic arsenic comprised a large portion of the total arsenic present in these animals, except for tilapia (Table 5-2). One observation from the Suhendrayatna et al. (2002b) experiment, however, is the fact that tilapia fish exposed to dimethylarsinic acid in water (nominal concentrations ranging from 1 to 50 mg/L) carried a body burden of approximately 94% organic arsenic (one third DMA related compounds and two thirds TMA related compounds), which is approximately two to three times higher than in tilapia exposed to any other form of arsenic from the same study (Table 5-2). These data imply that the amount of dimethylated arsenic chemical species in ambient surface waters may result in a greater proportion of total arsenic in aquatic biota existing in the organic form. The importance of the amount of organic arsenic in ambient surface water is further supported by the observation that very little of this form of arsenic was found in the whole bodies of tilapia and Japanese medaka exposed to arsenic as arsenite through a simulated 3-step food chain model (Suhendrayatna et al. 2002b, Table 5-2). In this particular study, arsenic residues in tilapia and Japenese medaka exposed to arsenite in water were actually higher than when they accumulated it via the food chain. The same was not true for guppies exposed via a simulated food chain where the arsenic in water was originally provided as arsenate (Maeda et al. 1990). Mean fractions of inorganic and organic arsenic in dorsal muscle of carp exposed to arsenic as arsenate in water do not differ substantially from the corresponding whole body concentrations measured for other fishes (Maeda et al. 1993). TABLE 5-2: Arsenic Speciation in Freshwater Trophic Levels 3 and 4 Aquatic Organisms Species dobsonfly larvae freshwater prawn amphidromous goby Japanese dace downstream fatminnow goby sweet fish masu salmon Test type Field Field Field Field Field Field Field Field Fraction of Total Arsenic3 Inorganic NM NM NM NM NM NM NM NM As(III) - - - - - - - - As(V) - - - - - - - - Organic 0.96 0.75 0.97 0.96 0.97 0.95 0.88 0.99 Reference Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) Kaiseetal. (1997) 31 ------- crayfish crayfish tilapia tilapia tilapia tilapia tilapia Japanese medaka guppy carp tilapia tilapia Japanese medaka guppy Field Field Lab; As(III) (water) Lab; As(V) (water) Lab; As(III) (water) Lab; MMA (water) Lab; DMA (water) Lab; As(III) (water) Lab; As(V) (water) Lab; As(V) (water) Lab; As(III) (diet) Lab; As(III) (diet) Lab; As(III) (diet) Lab; As(V) (diet) 0.54 0.29 - - - - - - 0.78 0.76 - - - 0.15 NM NM 0.25 0.36 0.37 0.40 - 0.45 NM NM 0.41 0.41 0.26 NM NM NM 0.14 0.36 0.24 0.31 - 0.38 NM NM 0.56 0.44 0.74 NM 0.04 0.04 0.50 0.25 0.37 0.27 0.94 0.06 0.21 0.19 0.023 0.037 0.0 0.84 Devesa et al. (2002) Devesa et al. (2002) Suhendrayatna et al. (2001) Suhendrayatna et al. (2002b) Suhendrayatna et al. (2002b) Suhendrayatna et al. (2002b) Suhendrayatna et al. (2002b) Suhendrayatna et al. (2002a) Maedaetal. (1990) Maedaetal. (1993) Suhendrayatna et al. (2001) Suhendrayatna et al. (2002b) Suhendrayatna et al. (2002a) Maedaetal. (1990) aValues represent geometric mean; calculations based on data compiled in Appendix X. 5.2 Saltwater Aquatic Organisms Most of the available arsenic speciation data in tissues of saltwater organisms are from field studies. The majority of these data pertain to marine bivalve molluscs, and all of it from soft or edible tissues. Clearly, only a very small percentage of inorganic arsenic exists in the soft tissues of these organisms (most often less than 1%), the bulk of it being in the form of AsB. The studies by De Gieter et al. (2002), Goessler et al. (1997), and Ochsenkuhn-Petropulu et al. (1997), 32 ------- confirm the general assertion that from 85% to >90% of arsenic found in edible portions of marine fish and shellfish is organic arsenic (primarily AsB). Geizinger et al. (2002) recently showed that the total arsenic concentration in marine polychaetes Nereis diversicolor and N. virens (Geizinger et al. 2002) was about 70% water- soluble and consisted of approximately 60% AsB and 20 to 30% tetramethylarsonium ion. Tetramethylarsoniopropionate and arsenosugars were also present as minor constituents. When the polychaetes were exposed in the laboratory to different concentrations of arsenate in seawater (0.010, 0.050, 0.100, 0.500, and 1.0 mg/L arsenic), the arsenic taken up by the polychaetes was readily methylated with the major metabolite as tetramethylarsonium ion (up to 85% of the accumulated arsenic). Methylation is assumed to be a process of detoxification, and the authors note the fact that tetramethylarsonium ion is a common compound in marine organisms, which suggests that this methylating ability is not restricted to Nereis sp. 33 ------- 6.0 SUMMARY OF ARSENIC BAFs AND SUPPORTING INFORMATION 6.1 Freshwater and Saltwater Arsenic BAFs The present data compilation indicates that insufficient data are available to determine if distinguishing separate BAFs for freshwater lotic and lentic ecosystems is warranted, and the only data available for estimating field-derived arsenic BAFs for estuarine and marine ecosystems is for trophic level 2 organisms. The species-mean BAFs for saltwater organisms are on average several times higher than for the majority of trophic level 2 organisms in the two freshwater ecosystem types. This apparent difference in arsenic BAFs calculated for freshwater and saltwater trophic level 2 organisms indicates the possible need to derive separate BAF values for arsenic in the two water types. 6.2 BAFs Based on Total Arsenic versus Other Forms of Arsenic The hypothesis that BAFs based on total arsenic may not be representative of all freshwater ecosystems, and especially saltwater ecosystems, due to variation in the various forms of arsenic present in the water and tissues of organisms from those systems remains an issue requiring further consideration. Average concentrations of arsenic in ambient freshwater are generally <1 to 10 |ig/L, and arsenic in seawater is present at a fairly uniform concentration of 2 |ig/L (Smedley and Kinniburgh 2002). Concentrations of As in lake waters are typically close to or lower than those found in river waters. Some polluted rivers and lakes show levels of arsenic in the hundreds of ppb. The environmental behavior of arsenic is dependent on the physical and chemical properties, toxicity, mobility, and biotransformation of individual arsenic compounds. Arsenic can occur in the environment in several oxidation states (0, +3 and +5), but in natural waters is mostly found in inorganic form as oxyanions of trivalent arsenite [As(III)] or pentavalent arsenate [As(V)]. Naturally occurring organo-arsenic compounds are described as having either As(III) or As(V) oxidation numbers. For example, the designated oxidation states in (CH3)3As is As(+III) and in (CH3)3AsO is As(+V) (Cullen and Reimer 1989). In oxygenated waters, inorganic arsenic acid (As(V)) species-H3AsO4, H2As(V ,»HAsO42» ,»andAsO43» *-are stable. Under slightly reducing conditions and/or lower pH arsenous (As(III)) acid becomes stable, mainly as neutral H3AsO3 (Cullen and Reimer 1989). The range of arsenic species is more restricted when the pH domain of natural water is considered. Freshwater systems rarely exceed a pH range of 5-9 and the maximum pH distribution in seawater is 7.5-8.3. Thus As(V) should dominate over As(III) in oxygenated waters-at least on thermodynamic grounds. For examples, As(V)/As(III) ratios of 1015-1026 have been calculated for seawater. Furthermore, As(V) should mainly consist of HAsO42> in oxygenated seawater (calculations show 98% HAsO42> «and 1% each of H2AsO4» *and AsO43> ). In fresh water of pH 6, H2AsO4» •becomes dominant (89% versus 11% HAsO42> ). Inorganic As(III) species should mainly be neutral, as H3AsO3. The solution properties of arsenic acid 34 ------- (H3AsO4) closely resemble those of phosphoric acid (H3PO4) and the ionization behavior of As(OH)3 more closely resembles that of boric acid. Thermodynamically predicted As(V)/As(III) ratios are rarely observed, and experimental evidence clearly indicates that a multiplicity of factors influences the relative concentrations of these species. Paramount among these are biologically mediated redox reactions. The interconversion of arsenite and arsenate by algal/bacteria transformations prevents achievement of thermodynamic equilibrium. Concentrations and relative proportions of As(V) and As(III) vary according to changes in input sources, redox conditions and biological activity. The presence of As(III) may be maintained in oxic waters by biological reduction of As(V), particularly during summer months. Proportions of As(III) and As(V) are particularly variable in stratified lakes where redox gradients and biological activity can be large and seasonally variable. Organoarsenic compounds are widely distributed in the environment. The origin of essentially all organoarsenicals starts with biomethylation of inorganic arsenic species. The principal biomethylation products are: Monomethylarsonate (MMA) CH3AsO2OH» • Dimethylarsenate (DMA) (CH3)2AsOO • Trimethylarsine (TMA) (CH3)3As Trimethylarsine oxide (TMAO) (CH3)3AsO Arsenobetaine (AsB) (CH3)3As« CH2COOH Arsenocholine (AsC) (CH3)3As« (CH2)2OH also, arsenoribosides and arsenophospholipids are formed. MMA and DMA are the organoarsenics usually encountered in surface waters and usually do not exceed 10% of the total dissolved arsenic. However, some seasonally anoxic lakes have shown methylated forms to be the dominate temporal species( >50%) of dissolved arsenic within the surface photic zone as a result of phytoplankton activity. Clearly, the speciation of arsenic in natural surface waters depends upon pH, DO (dissolved oxygen) and corresponding oxidation potential (Eh), and biological activity. The only field data identified in our literature search for which concentrations of corresponding inorganic and organic arsenic in both the water and tissues of aquatic organisms are from Kaise et al. (1997). In their study of the arsenic species present in arsenic-rich river water from the Haya-kawa River at hot springs in Hakone, Kanagawa, Japan, the authors showed that the river water at the site where the organisms were collected contained 3.0 x 10"2 mg/L total arsenic, 93% of which was inorganic and the remaining 7% trimethylated arsenic. The corresponding chemical speciation of arsenic in whole body tissue of the various organisms collected there varied greatly between species, but were composed mostly of dimethylarsenic (DMA) and trimethylarsenic (TMA) compounds, which are commonly distinguished as AsB or AsC in marine fish. The corresponding BAFs based on the organic fraction of arsenic in water and tissues of these organisms ranged from 26 to 1,590 L/kg, compared to 2.0 to 114.1 L/kg based on total arsenic; an increase of a factor often. In contrast, in the laboratory studies composed by Spehar et al. (1980), there was no difference in BCFs for several freshwater invertebrate species exposed to inorganic arsenic either as As(III) or As(V), or organic arsenic as DMA or MMA (see Table 3-1). Much more field data are required to adequately compare and support the derivation of separate BAFs for the various forms of arsenic in ambient surface waters. 35 ------- 6.3 Arsenic in Tissues of Freshwater and Saltwater Aquatic Organisms The tissue data collected from this literature search for bioaccumulation of arsenic appear to confirm earlier assumptions that the majority of arsenic in saltwater organisms is arsenobetaine (AsB), with only a relatively small fraction of the total arsenic in these organisms existing in the inorganic form. However, these observations are based on data for relatively few saltwater species. A finding for freshwater organisms is that a very high percentage of organic arsenic in the tissues of animals collected from the arsenic-rich (containing approximately 93% inorganic arsenic) Haya-kawa River, Japan (Kaise et al. 1997). These observations run counter to those observed for like animals exposed to arsenic (delivered as inorganic arsenic) in laboratory water- only and food-chain experiments (Suhendrayatna et al. 2001, 2002a,b; Meada et al. 1990, 1992, 1993). The reason for this apparent discrepancy in results cannot be easily explained. It would appear that rates of biomethylation for aquatic organisms in the field may greatly exceed those for like organisms exposed to arsenic in a laboratory setting. In general, the concentrations of total arsenic in marine and estuarine bivalve molluscs (data from the National Oceanic and Atmospheric Administration's Mussel Watch Program, National Status and Trends) and saltwater fish (data for flounder from EPA's Mid-Atlantic Integrated Assessment Program) greatly exceed those in freshwater fishes (Lowe et al. 1985; Schmitt and Brumbaugh 1990). Typical background total arsenic levels in the respective organisms (marine bivalves, flounder, freshwater fish) are in the range of 1 to 2 mg/kg, 0.75 to 2.5 mg/kg, and 0.10 to 0.25 mg/kg wet weight, respectively. Clearly, more field studies are needed regarding the biogeochemical cycling of arsenic in aquatic environments and the biological fate and disposition of arsenic in both freshwater and saltwater organisms. 36 ------- 7.0 CONCLUSIONS This document presents the information and methodologies used to support EPA's current effort to update the existing 304(a) human health ambient water quality criteria (AWQC) for arsenic. The BAF values calculated from raw data of appropriate studies are summarized in Appendices B through D and appear in various tables throughout the text. Only those total dissolved arsenic BAFs estimated directly from field-measured data were included in the summary tables and used to calculate species-mean BAFs. Insufficient data were available to support the derivation of BAFs for other forms of arsenic (i.e., organic, inorganic; see Section 6.2). BAFs estimated from laboratory BCF experiments are presented, but are not considered robust for estimating BAFs because the majority of the values generated from these studies did not meet data acceptability criteria and because the estimated BCFs were lower than BAFs calculated using field-data. Data on the uptake and accumulation of arsenic in estuarine and marine shellfish representative of those regularly consumed by humans were very limited. Species-mean BAFs were calculated for four saltwater species, all of which were trophic level 2 organisms. Chemical speciation data for arsenic in fresh and salt surface water was limited. Insufficient data were obtained to provide reliable fd (translator: dissolved/total) values for arsenic for the individual systems specified in this document. An interim default chemical translator value of 0.84 (range 0.62 to 0.94) based on four lotic, two lentic, one estuarine, and one lotic- lentic combined systems was generated for arsenic in this document. Information available that may be useful for determining bioaccumulation factors for arsenic is compiled in this document. National trophic-level specific BAFs are not included in this document because OST is in the process of determining if the data identified in our literature search is sufficient to derive national BAFs. In the interim, we are making the results of the literature search available to States and authorized Tribes so that they have access to a current compilation and review of available data as they develop State and Tribal Water Quality Standards. 37 ------- 8.0 REFERENCES Anderson, L.C.D., and K.W. Bruland. 1991. Biogeochemistry of arsenic in natural waters: he importance of methylated species. Environ. Sci. Technol. 25:420-427. Baker, D.L. and K.A. King. 1994. 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Uptake of arsenate, trimethylarsine oxide, and arsenobetaine by the shrimp Crangon crangon. Mar. Biol. 131:543-552. Johnson, A. and M. Roose. 2002. Inorganic arsenic levels in puget sound fish and shellfish from 303 (d) listed waterbodies and other areas. Washington State Department of Ecology. Environmental Assessment Program Olympia Washington. Publication no. 02-03-057. Kaise, T., M. Ogura, T. Nozaki, K. Saithoh, T. Sakurai, C. Matsubara, C. Watanabe, and K. Hanaoka. 1997. Biomethylation of arsenic in an arsenic-rich freshwater environment. Appl. Organom. Chem. 11:297-3 04. Kitchin, K.T. and S. Ahmad. 2003. Oxidative stress as a possible mode of action for arsenic carcinogenesis. Toxicology Letters. 137:3-13. 39 ------- Langston, WJ. 1984. Availability of arsenic to estuarine and marine organisms: a field and laboratory evaluation. Marine biology. 80:143-154. Lin, M.-C., C.-M. Liao, C.-W. Liu, S. Singh. 2001. Bioaccumulation of arsenic in aquacultural large-scale mullet Liza macrolepis from Blackfoot Disease area in Taiwan. Bull. Environ. Contam. Toxicol. 67: 91-97. Lowe, T.P., T.W. May, W.G. Brumbaugh, and D.A. Kane. 1985. National contaminant biomonitoring program: Concentrations of seven elements in freshwater fish, 1978-1981. Arch. Environ. Contam. Toxicol. 14:363-388. Maeda, S., K. Mawatari, A. Ohki, and K. Naka. 1993. Arsenic metabolism in a freshwater food chain: Blue-green alga (Nostoc sp.)» •shrimp (Neocardina denticulatd)* «carp (Cyprinus carpio). Appl. Organom. Chem. 7:467-476. Maeda, S., A. Ohki, K. Kusadome, T. Kuroiwa, I. Yoshifuku, and K. Naka. 1992. Bioaccumulation of arsenic and its fate in a freshwater food chain. Appl. Organom. Chem. 6:213-219. Maeda, S., A. Ohki, T. Tokuda and M. Ohmine. 1990. Transformation of arsenic compounds in a freshwater food chain. Appl. Organom. Chem. 4:251-254. Mason, R.P., J.-M. Laporte, and S. Andres. 2000. Factors controlling the bioaccumulation of mercury, methylmercury, arsenic, selenium, and cadmium by freshwater invertebrates and fish. Arch. Environ. Contam. Toxicol. 38:283-297. Mclntyre, D.O., C.G. Delos, W.H. Clement and T.K. Linton. 2002. BAFs for selenium: Implications for implementation of a tissue-based chronic criterion. Abstract Book. SET AC 23rd Annual Meeting in North America, Salt Lake City, UT 16-20 November, 2002. Society of Toxicology and Chemistry. Abstract No. 042. p. 13. MDEQ (Michigan Department of Environmental Quality). 1996. Michigan default metals translator. MI/DEQ/SWQ-95/085. Lansing, MI. Michel, P., B. Averty, J.-F. Chiffoleau, and L.-A. Romana. 2001. Biogeochemical behavior of arsenic species in the seine estuary in relation of successive high-amplitude primary production, anoxia, turbidity, and salinity events. Estuaries. 24:1066-1073. Millward, G.E., HJ. Kitts, L. Ebdon, J.I. Allen and A.W. Morris. 1997. Arsenic in the Thames Plume, UK. Marine Environmental Research. 44:51-67. Ochsenkuhn-Petropulu, J. Varsamis, and G. Parissakis. 1997. Speciation of arsenobetaine in marine organisms using a selective leaching/digestion procedure and hydride generation atomic absorption spectrometry. Analytica Chimica Acta. 337:323-327. 40 ------- Schmitt, CJ. and W.G. Brumbaugh. 1990. National contaminant biomonitoring program: Concentrations of arsenic, cadmium, copper, lead, mercury, selenium, and zinc in U.S. freshwater fish, 1976-1984. Arch. Environ. Contam. Toxicol. 19:731-747. Skinner, W.F. 1985. Trace element concentrations in wastewater treatment basin-reared fishes: Results of a pilot study. Proceedings of the Pennsylvania Academy of Science. 59:155-161. Smedley, P.L., and D.G. Kinniburgh. 2002. A review of the source, behaviour and distribution of arsenic in natural waters. Applied Geochemistry 17:517-568. Spehar, R.L., J.T. Fiandt, R.L. Anderson, and D.L. DeFoe. 1980. Comparative toxicity of arsenic compounds and their accumulation in invertebrates and fish. Arch. Environm. Contam. Toxicol. 9:53-63. Suhendrayatna, A.O., T. Nakajima, and S. Maeda. 2002a. Studies on the accumulation and transformation fo arsenic in freshwater organisms I. Accumulation, transformation and toxicity of arsenic compounds to the Japenese medaka, Oryzias latipes. Chemosphere. 46:319-324. Suhendrayatna, A.O., T. Nakajima, and S. Maeda. 2002b. Studies on the accumulation and transformation fo arsenic in freshwater organisms II. Accumulation and transforamtion of arsenic compounds by Tilapia mossambica. Chemosphere. 46:325-331. Suhendrayatna, A.O., and S. Maeda. 2001. Biotransformation of arsenite in freshwater food-chain models. Applied Organometallic Chemistry. 15:277-284. Tanizaki, Y., T. Shimokawa, andM. Nakamura. 1992. Physicochemical speciation of trace elements in river waters by size fractionation. Environ. Sci. Technol. 26:1433-1443. Thomas, D.J., M. Styblo, and S. Lin. 2001. The cellular metabolism and systemic toxicity of arsenic. Toxicol. Appl. Pharm. 176: 127-144. USEPA (United States Environmental Protection Agency). 2000. Methodology for deriving ambient water quality criteria for the protection of human health (2000). Office of Water, Washington, DC. EPA-822-B-00-004. USEPA (United States Environmental Protection Agency). 1996. The metals translator: Guidance for calculating a total recoverable permit limit from a dissolved criteria, Washington, DC. USEPA (United States Environmental Protection Agency). 1995. Trophic level and exposure analyses for selected piscivorous birds and mammals. Volume II: Analyses of species in the conterminous United States. Draft. Office of Water, Washington, DC. USEPA (United States Environmental Protection Agency). 1993. Memo from Martha G. Prothro, Acting Assistant Administrator for Water, to Water Management Division Directors and 41 ------- Environmental Services Division Directors, titled "Office of Water Policy and Technical Guidance on Interpretation and Implementation of Aquatic Life Metals Criteria, Office of Water, Washington, DC. USEPA (United States Environmental Protection Agency). 1985. Ambient aquatic life water quality criteria for arsenic - 1984. PB85-227445. National Technical Information Service, Springfield, VA. Valette-Silver, N.J., G.F. Riedel, E.A. Crecelius, H. Windom, R.G. Smith, and S.S. Dolvin. 1999. Elevated arsenic concentrations in bivalves from the southeast coasts of the USA. Marine Environ. Research. 48:311-333. Wagemann, R., N.B. Snow, D.M. Rosenberg, and A. Lutz. 1978. Arsenic in sediments, water and aquatic biota from lakes in the vicinity of Yellowknife, Northwest territories, Canada. Arch. Environm. Contam. Toxicol. 7:169-191. Waslenchuk, D.G. 1979. The geochemical controls on arsenic concentrations in Southeastern United States River. Chemical Geology. 24:315-325. Woolson, E.A. 1975. Bioaccumulation of arsenicals. In: Arsenical pesticides. E.A. Woolson (ed.). ACS Symposium Series 7. American Chemical Society, Washington, D.C. Zaroogian, G.E., and G.L Hoffman. 1982. Arsenic Uptake and Loss in the American Oyster, Crassostrea Virginica. Environmental Monitoring and Assessment. 1:345-358. 42 ------- APPENDIX A BAF LITERATURE SEARCH STRATEGY ------- Literature Search Strategy for Data on Arsenic Bioaccumulation in Aquatic Organisms The literature search strategy is designed to obtain all relevant information for the calculation (if data are available of bioaccumulation factors (BAFs) for total arsenic, total inorganic arsenic, dissolved inorganic arsenic, arsenobetaine (AsB), arsenocholine (AsC) and dimethyl aresinic acid (DMA). A 'bioaccumulation' search was conducted with the objective of retrieving relevant information for arsenic in lotic, lentic and estuarine ecosystems. A 'translator' search was conducted to obtain additional information relevant to establishing chemical translators for arsenic. This search used a set of search terms different than those used in the primary search, and therefore eliminated the hits obtained in the primary search. Elements of the searches: • Major Database: Chemical Abstracts Time Period for the Literature Search: 1980 through 2002 Bioaccumulation Search Objective: To obtain information relevant for determining BAFs from acceptable field bioaccumulation or laboratory bioconcentration studies. The search used the following sets of search terms to obtain information relevant to deriving bioaccumulation factors for lotic, lentic, and marine/estuarine ecosystems: arsenic, arsenite, arsenate, arsine, arsenobetaine, arsenocholine, dimethyl arsinic acid (search included chemical name and/or CAS number) • all the organisms listed in Attachment A-l • bioaccumulat, or bioconcentrat, or accumulat, or biomagnif, or uptake, or depurat, or eliminat, or BAF, or BCF, or AF, or residue, or tissue, or food chain, or food web, or predator/prey, or PPF, or pharmacokinetic, or toxicokinetic The titles and abstracts of those references that contained the three sets of search terms shown above (e.g., arsenic and walleye and bioaccumulat) were printed and reviewed by senior scientists/specialists. The titles and abstracts were reviewed for indication that the references contained the following information necessary for deriving bioaccumulation factors: • the concentration of arsenic (or forms of interest) in the tissue of an aquatic organism (fish and invertebrates; mammal data were excluded) the concentration of the arsenic (or forms of interest) in water, and any indication that a predator-prey factor could be determined. Articles containing the above information were retrieved, reviewed and data extracted and recorded in tables/spreadsheets for use in deriving BAFs. A-2 ------- Translator Search Objective: To obtain information relevant for development of arsenic translators for lotic, lentic , and marine/estuarine ecosystems. The search used the following sets of search terms to obtain relevant: arsenic, arsenite, arsenate, arsine, arsenobetaine, arsenocholine, dimethyl arsinic acid (search included chemical name and/or CAS number) lotic, or river, or stream, or creek, or brook, or spring, or trib, or canal, or lentic, or lake, or pond, or water, or loch, or saltwater, or ocean, or marine, or sea, or delta, or harb, or waterway, or estuar, or bay, or inlet, or sound, or firth, or fjord, or mouth, or coast • distribu, or speciation, or partition, or Kd, or dissolv, or fraction, or translat, or filter The titles and abstracts of those references that contained the three sets of search terms shown above (e.g., arsenic and walleye and bioaccumulat) were printed and reviewed by senior scientists/specialists. Articles containing information on (1) the total and dissolved concentration of arsenic or forms of interest, or (2) the concentration of particulate arsenic and total suspended solids, or (3) arsenic partition coefficients were were retrieved, reviewed and data extracted and recorded in tables/spreadsheets for use in deriving BAFs. A-3 ------- ATTACHMENT A-l abalone acartia aeolosoma* agnatha alevin alewife alga ambystoma* amoeb* amphipod * anchov* annelid* aquaculture archannelid * artemi* aufwuchs backswimmer barnacle bass benth* beetle bivalv* blackfl* blenny bluegill boatman bream bryophyt* bryozoa* bullhead caddisfl * carassius carp catfish centrarch * ceriodaphni * chaetognatha chaetonotid* char charphyt* chinook chironom * chlamydomonas chlorophyt* chrysophyt* chub ciliat* cisco cladocera* clup* cnidaria coho coleoptera* conchostracan copepod* corbicula coregon* crab cranefl* crangon crappie crayfish* crassostrea croaker Crustacea* cryptophyt* ctenophor* cyanophyt* cyprini * cyprinodon* dab dace damself 1 * daphni * darter diptera* dobsonfl* dolphin dragonfl* drum duckweed ecihno* eel ephemer* esoc* esox etheostoma euglen* fmgerling fish fishes flounder fundulus gambusia gammar* gar gastropod * gastrotrich* goby goldfish grunlon guppy gupples haddock hemiptera herring hexagenia hirudin * hyallela hydra hydridae hydroid hydrozoa hyla ictalur* isopod* jordanella kelp killifish lamprey lancelet leech lemna lepomis lobster lymnaea macoma mayfl* medaka A-4 ------- menhaden menidia mlcropogon micropterus midge minnow mollus* molly morone mosquito * mudminnow mullet mummichog muskellunge mussel mysid* mytilus naupli* neanthes nereis notropis odonata oligochaet* oncorhynchus osmerid* osteichthyes ostracod ostre* oyster palaemon* paramec* parr pelecypod* penae* perch perci* periphyt* phaeophyt* philodin* physa phytoplankton * pike pimephaeles pinfish pipefish plaice planari* plankton* platyfish plecoptera polychaet* pompano porifera porpoise prawn protozo* puffer pyrrophyt* quahog rhinichthy* rhodophyt* roach roccus rockfish rotifer* salmo* salvelinus sanddab sauger scallop sciaenid* scud sculpin seagrass seaweed selnastrum shad shellfish sheep shead shiner shrimp silverside skeletonema smelt smolt snail sockeye sole spong* spot squid squawfish starfish steelhead stickleback stonefl* sturgeon sucker sunfish surfclam tench tilapia toad* trematod * trichoptera trout tubificid* tubifex tuna turbellar* urchin walleye whitefish wonn wrasse zooplankton* A-5 ------- APPENDIX B SUMMARY OF ARSENIC BIO ACCUMULATION STUDIES REVIEWED ------- APPENDIX B: Summary of Arsenic Bioaccumulation Studies Reviewed Article # 1 1 1 1 1 2 2 2 3 3 3 4 4 4 5 6 7 7 8 8 9 10 10 10 Field or Lab Lab Lab Lab Lab Lab Field Field Field Lab Lab Lab Lab Lab Lab Field Lab Field Field Field Field Field Field Field Field Water or Waterbody Type Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Rock pool at Rosedale NSW Rock pool at Rosedale NSW Rock pool at Rosedale NSW Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Red River of the North, North Dakota Lab Water Coal fly ash basin at US DOE Fire Pond (unaffected by fly ash effluent) Elevsis bay near Athens Greece Elevsis bay near Athens Greece 12 Coastal sites in western Taiwan 6 Sites along the Lower Gila 6 Sites along the Lower Gila 6 Sites along the Lower Gila Habitat Type NA NA NA NA NA Marine Marine Marine NA NA NA NA NA NA Lentic NA Lentic Lentic Marine Marine Marine Lotic Lotic Lotic Species Chlorella vulgaris Daphnia magna Neocardina denticulata Tilapia mossambica Zacco playtypus Hormosira banksii Austrocochlea Morula marginalba Chlorella vulgaris Daphnia magna Oryzias latipes Tilapia mossambica Tilapia mossambica Tilapia mossambica Cyprinus carpio Lepomis macrochirus Micropterus salmoides Micropterus salmoides Mytilus edulis Murex trunculus Cyprinus carpio Micropterus salmoides Ictalurus punctatus Common Name green algae waterflea shrimp fish fish seaweed gastropod gastropod green algae waterflea Japanese medaka fish fish fish common carp bluegill sunfish largemouth bass largemouth bass blue mussel marine snail 30 different marine molluscs common carp largemouth bass channel catfish Trophic Level 1 2 2 3 3 1 2 4 1 2 3 3 3 3 3 3 4 4 2 2 2 3 4 3 Chemical Form Water Arsenite Arsenite Arsenite Arsenite Arsenite NM NM NM Arsenite Arsenite Arsenite Arsenite MMA DMA NM Arsenite NM NM NM NM NM NM NM NM Chemical Form Reject Tissue or Accept Total, Inorganic, Reject Organic Total, Inorganic, Organic Total, Inorganic, Organic Total, Inorganic, Organic Total, Inorganic Inorganic, Organic Reject Inorganic, Organic Inorganic, Organic Total, Inorganic, Reject Organic Total, Inorganic Total, Inorganic Total, Inorganic, Reject Organic Total, Inorganic, Organic Total, Inorganic, Organic Total Reject Total Reject Total Reject Total Total, AsB Reject Total, AsB Total Uncertain Total Reject Total Total BAF/BCF Reason for Rejection provided in paper? Y=Yes N=No N No indication that steady-state was achieved. Water concentrations not measured. N Water concentrations not measured. N No indication that steady-state was achieved. Water concentrations not measured. N No indication that steady-state was achieved. Water concentrations not measured. N Water concentrations were not measured. Y Article states that steady-state conditions in bluegills did not appear to be reached during this period. N Water concentrations were not measured. N Water concentrations were not measured. N Concentrations of arsenic in water and sediment were measured, but not N Water concentrations were not measured. Water Tissue Notes Speciation Speciation Data? Data? N Y 7-day exposure (static). Includes speciation in tissue from wateborne and dietary exposure (lab food chain study). Dietary exposure of greater significance in lower trophic levels. No indication of bioamagnification. N Y Tissue speciation useful for indicating differences in As species in the Marine food chain, but the arsenic species in tissues are not quantified. N Y 7-day exposure (static). Does include speciation in tissue from wateborne and dietary exposure (lab food chain study). No indication of biomagnification in lab food chain. Y Y 7-day exposure (static). N N Specimens collected at 4 sites. Study includes Total Arsenic in whole body, muscle, and liver tissue. N N BCF of 4 reported for 28-day exposure period. N N Study includes Total Arsenic in gill, gonad, liver, and muscle tissue. [As] is highest in liver tissue. Further analysis of gill and liver extracts from bass indicated that AB was not present. N Y N N N N B-2 ------- APPENDIX B: Summary of Arsenic Bioaccumulation Studies Reviewed Article # 11 11 11 11 12 12 12 13 13 13 13 13 14 15 15 16 16 17 18 Field or Lab Field Field Field Field Field Field Field Field Field Field Field Field Field Lab Lab Field Field Lab Field Water or Waterbody Type 7 Sites along the Santa Cruz 7 Sites along the Santa Cruz 7 Sites along the Santa Cruz 7 Sites along the Santa Cruz 1 1 Sites along the Middle Gila 1 1 Sites along the Middle Gila 1 1 Sites along the Middle Gila Campaign Creek, OH Ohio River, OH Singy Run, OH Singy Run, OH Little Scary Creek, OH 20 Coastal States Simulated Irrigation Drainwater Simulated Irrigation Drainwater 18 Sites in Lake Xolotlan, Managua, Nicaragua 18 Sites in Lake Xolotlan, Managua, Nicaragua Lab water Los Angeles Harbor (Sediment) Habitat Type Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Marine NA NA Lentic Lentic NA Marine Species Aeshnidae Belostoma sp. Physa virgata Pantosteous clarki Cyprinus carpio Ictalurus punctatus Pantosteous clarki Lepomis macrochirus Lepomis macrochirus Lepomis macrochirus Lepomis cyanellus Lepomis macrochirus Xyrauchen texanus Gila elegans C. citrinellum C. managuense Oncorhynchus mykiss Genyonemus lineatus Common Name dragonfly larvae giant water bug snail desert sucker common carp channel catfish desert sucker bluegill sunfish bluegill sunfish bluegill sunfish green sunfish bluegill sunfish shellfish razorback bonytail fish fish rainbow trout feral fish Trophic Level 3 3 2 3 3 3 3 3 3 3 3 3 2 3 3 Uncertai n Uncertai n 4 Uncertai n Chemical Form Water NM NM NM NM NM NM NM Total Total Total Total Total NM Total Total Total Total NA NM Chemical Form Tissue Total Total Total Total Total Total Total Total Total Total Total Total Total NM NM Total Total Total Total Reject BAF/BCF Reason for Rejection or provided Accept in paper? Y=Yes N=No Reject N Water concentrations were not measured. Reject N Water concentrations were not measured. Reject N The only applicable data is for arsenic in liver tissue, which is not an edible tissue. Reject N Water concentrations were not provided. Reject N Tissue concentrations were not provided. Reject N Tissue concentrations were given as a range from less than detect (<0.01 ug/g w/v) to 0.2 to 0.4 ug/g wet Reject N Dietary exposure only. Reject N Tissue concentrations not measured. Water Tissue Notes Speciation Speciation Data? Data? N N Sediment As concentrations reported. N N Sediment As concentrations reported. N N N N N N N N N N Arsenic measured in muscle, gills, liver and skin. Concentrations were highest in the liver. N N B-3 ------- APPENDIX B: Summary of Arsenic Bioaccumulation Studies Reviewed Article # 19 19 19 19 19 19 19 19 19 19 19 20 20 21 21 21 22 22 22 22 22 22 23 24 Field or Lab Field Field Field Field Field Field Field Field Field Field Field Lab Lab Field Field Field Lab Lab Lab Lab Lab Lab Field Field Water or Waterbody Type Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Savannah River, South Carolina Natural seawater Natural seawater Ponds at Horsethief Canyon Adobe Creek, CO North Pond near Fruita, CO Filtered Air River water Filtered Air River water Filtered Air River water Filtered Air River water Filtered Air River water Filtered Air River water 3 sites along Thane Creek, India Coastal waters of Yoshimi, Shimonoseki, Japan Habitat Type Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic NA NA Lentic Lotic Lentic NA NA NA NA NA NA Lotic Marine Species Amia calva Micropterus salmoides Ictalurus punctatus Esox niger Perca fluvescens Pomoxis Anguilla rostrata Lepomis microlophus Lepomis macrochirus Lepomis auritus Minytrema melanops Nereis virens Nereis diversicolor Physa fontinalis Asellus aquaticus Gammarus fossarum Niphargus Hydropsiche pellucidula Hepatgenia sulphurea Common Name bowfin bass channel catfish chain pickerel yellow perch black crappie american eel shellcracker bluegill redbreast spotted sucker marine polychaetes marine polychaetes cladocerans and cladocerans and cladocerans and snail isopod amphipod amphipod caddisfly mayfly phytoplankton (algae, diatoms) mixed marine organisms Trophic Level 4 4 3 3 3 3 3 3 3 3 2 2 2 2 2 2 2 2 2 2 2 1 1 thru 4 Chemical Form Water NM NM NM NM NM NM NM NM NM NM NM Arsenate Arsenate NM NM NM Arsenite Arsenite Arsenite Arsenite Arsenite Arsenite Total Arsenic NM Chemical Form Tissue Total Total Total Total Total Total Total Total Total Total Total Total, Inorganic, Organic Total, Inorganic, Organic Total Total Total Total Total Total Total Total Total Total Total Reject BAF/BCF Reason for Rejection or provided Accept in paper? Y=Yes N=No Reject N Water concentrations were not measured. Reject N No indication that steady-state was achieved. Water concentrations measured as dissolved Total Arsenic. Reject N Water concentrations were not provided. Reject N No indication that steady-state was achieved. Uncertain Y BCF is suspect. High Total Arsenic concentrations (mean of 527 ug/L) were measured in water, but arsenic was not detected in macroinvertebrates and fish. Reject N Water concentrations were not measured. Water Tissue Notes Speciation Speciation Data? Data? N N N Y 12-day exposure (static). Includes Speciation data in tissues. N N Arsenic in zooplankton measured as part of dietary exposure treatment for the razorback sucker. N N 10-day exposure (flow-through) N N N N Tissue Speciation useful for indicating differences in As species in the Marine food chain, but the arsenic species in tissues are not quantified. B-4 ------- APPENDIX B: Summary of Arsenic Bioaccumulation Studies Reviewed Article # 25 26 27 27 27 27 27 27 27 28 29 29 30 30 30 31 31 31 31 32 33 34 34 Field or Lab Field Field Field Field Field Field Field Field Field Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Water or Waterbody Type Sites in the North Sea and English Channel from Venice Lagoon Mine-affected and adjacent areas at Aznalcollar (Seville, Spain) Puget Sound, WA Puget Sound, WA Puget Sound, WA Puget Sound, WA Puget Sound, WA Puget Sound, WA Puget Sound, WA City of Winnipeg tap water Synthetic softwater Synthetic softwater Sea water Sea water Sea water Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Modified Detmer medium Sand filtered sea water Sand filtered sea water Habitat Type Marine Lotic Marine Marine Marine Marine Marine Marine Marine NA NA NA Species Procambarus clarkii Monoraphidium Chlorella sp. Crangon crangon Crangon crangon Crangon crangon Chlorella vulgaris Phormidium sp. Moina macrocopa Poecila reticulata Cyprinus carpio Neocaridina denticulata Mytilus edulis Mytilus edulis Common Name fish (25 species); shellfish freshwater crayfish English sole quillback Dungeness crab coho salmon Pacific herring clams graceful crabs lake whitefish freshwater freshwater shrimp shrimp shrimp freshwater algae freshwater algae zooplankton guppy fish carp shrimp mussels mussels Trophic Level 2 thru 4 3 3 3 3 4 2 2 3 3 1 1 2 2 2 1 1 2 3 3 2 2 2 Chemical Form Water NM NM NM NM NM NM NM NM NM NA Arsenate Arsenate Arsenate TMAO AB Arsenate Arsenate Arsenate Arsenate Arsenate Arsenate AsB 1,2,3 AsB 1,2,3 Chemical Form Reject Tissue or Accept primarily Total Reject Total, Inorganic, Reject Organic Total, Inorganic Reject Total, Inorganic Total, Inorganic Total, Inorganic Total, Inorganic Total, Inorganic Total, Inorganic Total Reject Inorganic, Organic Reject Inorganic, Organic Total Reject Total Total Total, Inorganic, Reject Organic Total, Inorganic, Organic Total, Inorganic, Organic Total, Inorganic, Organic Total, Inorganic, Reject Organic Total, Inorganic, Reject Organic Total Reject AsB BAF/BCF Reason for Rejection provided in paper? Y=Yes N=No N Water concentrations were not measured. N Water concentrations were not measured. N Water concentrations were not measured. N Exposure was via diet only. N No indication that steady-state was achieved. N Data did indicate that steady-state was achieved after 8 days. Concentrations of As species in water were not measured. N No indication that steady-state was achieved. N No indication that steady-state was achieved. Water Arsenate concentrations not measured. N No indication that steady-state was achieved. concentrations not measured. N No indication that steady-state was achieved. Water Tissue Notes Speciation Speciation Data? Data? N Y Some tissue speciation data provided, divided into toxic (inorganic, MMA, DMA) and non-toxic fractions (AsB, AsC, TMAO), but the individual arsenic species are not quantified separately. N Y Tissue speciation useful for indicating differences in As species in freshwater crayfish. Arsenic species in tissues are quantified. N Y Tissue speciation useful for indicating differences in As species in Marine fish, clams and crabs. Combined inorganic As species in tissues are quantified. N N Arsenic measured in muscle and non-edible tissue. Concentrations were highest in pyloric caeca, intestine, liver, and scales. N Y 72-h exposure (static). Tissue As speciation measured at IC50 concentrations (high). Y N 10-day static renewal exposure. N Y 7-day exposure (static). Does include speciation in tissue from wateborne and dietary exposure (lab food chain study). No indication of biomagnification. N Y 7-day exposure (static). Does include speciation in tissue from wateborne and dietary exposure (lab food chain study). No indication of biomagnification. Arsenic species measured in muscle, gut, and skin. Total As concentrations were highest in the gut. N Y 7-day exposure (static). Does include speciation in tissue from wateborne and dietary exposure (lab food chain study). No indication of biomagnification. Biomethylation increases with trophic level. N Y 10-day exposure (static). Water AsB concentrations were confirmed with measurement. Order of AsB uptake efficieny is the following AsB1 >AsB2>AsB3. B-5 ------- APPENDIX B Article Field * or Lab 35 35 36 37 37 38 38 39 40 41 42 43 44 44 44 44 45 45 45 45 Field Field Field Field Field Field Field Field Field Lab Field Lab Field Field Field Field Field Field Field Field Water or Waterbody Type Mouth of Miami River, Biscayne Mouth of Miami River, Biscayne Electric utility wastewater Restronguet Creek in Fal Estuary, Tamar Estuary, SW England Devil's Swamp, lower Mississippi Tunica Swamp, lower Mississippi Hypersaline evaporation ponds, CA Hayakawa River, Japan Sea water Venetian Lagoon, Island of Narragansett Bay seawater Grace Lake, NW Territories, Grace Lake, NW Territories, Kam Lake, NW Territories, Kam Lake, NW Territories, San Francisco and Upper Gila San Francisco and Upper Gila Upper Gila River, AZ Upper Gila River, AZ Habitat Species Type Estuarine Isognomon sp. - Estuarine Crassostrea virginica Lentic Cyprinus carpio Estuarine Scrobicularia plana Estuarine Scrobicularia plana Lotic / 33 species Lotic / 28 species Saltwater Artemia franciscana Lotic 1 3 FW species NA Mytilus edulis Marine Mytilus galloprovincialis NA Crassostrea virginica Lotic Lotic Cottus cognatus Lotic Lotic Cottus cognatus Lotic Ictalurus punctatus Lotic Pilodictis olivaris Lotic Cyprinus carpio Lotic Micropterus salmoides Summary of Arsenic Bioaccumulation Studies Reviewed Common Name Trophic Chemical Level Form Water mussels oysters common carp bivalve bivalve freshwater fish freshwater fish brine shrimp an alga, diatom, invertebrates and fishes blue mussel mussell eastern oyster zooplankton & sculpin zooplankton & sculpin channel catfish flathead catfish common carp largemouth bass 2 2 3 2 2 3-4 3-4 2 1-4 2 2 2 2 3 2 3 3 3 2 4 Dissolved Dissolved Total Dissolved Dissolved Total Total Total Arsenic Total Arsenic Dissolved Total Dissolved Dissolved Dissolved Dissolved Total Total Total Total Chemical Form Tissue Total, Inorganic, Total, Inorganic, Total Total Total Total Total Total Total, Inorganic, Organic Total, Organic Total Total Total Total Total Total Total Total Total Total Reject or Accept Accept Accept Accept Accept Accept Accept Reject Accept Reject Accept Reject Accept Accept Accept Accept Accept Accept Accept Accept BAF/BCF Reason for Rejection Water provided Speciation in paper? Data? Y=Yes N=No N N Y (3882) Y(3110) N N N Data are for brine shrimp. Water [As] was measured in samples collected December 1995, but corresponding [As] in adult brine shrimp weren't collected for analysis until August 1996. N N N N Y Y Y Y N N N N Y N N N N N N N N N N Tissue Notes Speciation Data? N N N N N N N N N N N B-6 ------- APPENDIX B Article Field * or Lab 46 46 46 46 46 46 46 46 47 48 48 49 49 49 50 50 50 50 50 50 50 Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Field Water or Waterbody Type Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Blacklick Run and Herrington Fish ponds, southwest coast of 20 Lakes in NW U.S. 20 Lakes in NW U.S. Moon lake, Mississippi Moon lake, Mississippi Moon lake, Mississippi Upper Mystic Lake, MA Upper Mystic Lake, MA Upper Mystic Lake, MA Upper Mystic Lake, MA Upper Mystic Lake, MA Upper Mystic Lake, MA Upper Mystic Lake, MA Habitat Type Lotic Lotic Lotic Lotic Lotic Lotic Lotic Lotic Estuarine Lentic Lentic Lentic Lentic Lentic Lentic Lentic Lentic Lentic Lentic Lentic Lentic Species Crustacea cranefly, caddisfly, Ameirus nebulosus Catostomus Cottus bairdi Rhinichthys atratulus Semotilus Salvelinusfontinalis Liza macrolepis Pomoxis Lepomis macrochirus Micropterus salmoides Perca flavescens Summary of Arsenic Bioaccumulation Studies Reviewed Common Name Trophic Chemical Level Form Water crayfish invertebrates brown bullhead white sucker mottled sculpin blacknose dace creek chub brook trout mullet zooplankton piscivorous and omnivorous fish benthivorous omnivorous fish planktivorous zooplankton alewife Killifish black crappie bluegill sunfish largemouth bass yellow perch 3 2-3 3 3 3 3 4 4 2 3-4 3 3 2 2 3 3 3 3 4 3 Dissolved Dissolved Dissolved Dissolved Dissolved Dissolved Dissolved Dissolved Total Dissolved Dissolved Arsenic Total Total Total Dissolved Dissolved Dissolved Dissolved Dissolved Dissolved Dissolved Chemical Form Reject Tissue or Accept Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept BAF/BCF Reason for Rejection Water Tissue Notes provided Speciation Speciation in paper? Data? Data? Y=Yes N=No N N N N N N N Y N N Y N N N N N N N N N N N N N N N N N N N N N N B-7 ------- APPENDIX B: Summary of Arsenic Bioaccumulation Studies Reviewed Article # 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 51 52 Field or Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Lab Water or Waterbody Type Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Filtered Lake Superior water Well water Habitat Type NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA NA Species Pteronarcys dorsata Pteronarcys dorsata Pteronarcys dorsata Pteronarcys dorsata Helisoma campanulata Helisoma campanulata Helisoma campanulata Helisoma campanulata Stagnicola emarginata Stagnicola emarginata Stagnicola emarginata Stagnicola emarginata Daphnia magna Daphnia magna Daphnia magna Daphnia magna Gammarus Gammarus Gammarus Gammarus Oncorhynchus mykiss Oncorhynchus mykiss Oncorhynchus mykiss Oncorhynchus mykiss Lepomis macrochirus Common Name stonefly stonefly stonefly stonefly snail snail snail snail snail snail snail snail cladoceran cladoceran cladoceran cladoceran amphipod amphipod amphipod amphipod rainbow trout rainbow trout rainbow trout rainbow trout bluegill sunfish Trophic Level 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 4 4 4 4 3 Chemical Form Water Arsenite Arsenate DMA MMA Arsenite Arsenate DMA MMA Arsenite Arsenate DMA MMA Arsenite Arsenate DMA MMA Arsenite Arsenate DMA MMA Arsenite Arsenate DMA MMA Arsenite Chemical Form Tissue Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Total Reject or Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept Accept BAF/BCF Reason for Rejection provided in paper? Y=Yes N=No N N N N N N N N N N N N N N N N N N N N N N N N Y Authors state that it appeared that steady-state was not achieved over the 4 wk exposure period; This data was used in the 1985 Arsenic AWQC document, so it was included for comparison. Water Speciation Data? N N N N N N N N N N N N N N N N N N N N N N N N N Tissue Notes Speciation Data? N N N N N N N N N N N N N N N N N N N N N N N N N B-l ------- APPENDIX B: Articles Reviewed Article Authors # Year Reference 1 Suhendrayatna et al. 2 Goessler et al. 3 Suhendrayatna et. al. 4 Suhendrayatna et. al. 5 Goldstein and DeWeese. 6 Barrows et al. 7 Jackson et al. 8 Ochsenkuhn-Petropulu et al. 9 Hung et al. 10 King et al. 11 King et al. 12 King and Baker. 13 Lohneretal. 14 United States Food and Drug Administration. 15 Hamilton et al. 16 Lacayo et al. 17 Oladimejei etal. 18 Anderson et al. 19 Burger etal. 20 Geiszinger et al. 21 Hamilton et al. 2001 Applied Organometallic Chemistry 15:277-284. 1997 Fresenius Journal of Analytical Chemistry 359:434-437. 2002 Chemosphere 46:319-324. 2002 Chemosphere 46:325-331. 1999 Journal of the American Water Resources Association 35(5):1133-1140. 1980 In: Dynamics, Exposure and Hazard Assessment of Toxic Chemicals. Ann Arbor Science Pub., Inc., Ann Arbor, MI 2002 Analytical and Bioanalytical Chemistry 374:203-211. 1997 Analytica Chimica Acta 337:323-327. 2001 Chemosphere 44:833-841. 1997 Environmental contaminants in fish and wildlife of the lower Gila River, Arizona. US Fish & Wildlife Service, pp. 1-70. 1999 Contaminants as a limiting factor of fish and wildlife populatios in the Santa Cruz River, Arizona. US Fish & Wildlife Service, pp. 1-56 1995 Contaminants in fish and wildlife of the Middle Gila River, Arizona. US Fish & Wildlife Service, pp 1-17. 2001 Ecotoxicology and Environmental Safety 50:203-216. 1993 Guidance Document for Arsenic in Shellfish, pp. 1-27. 2000 Environmental Toxicology 15:48-64 1992 Bulletin of Environmental Contamination and Toxicology 49:463-470. 1984 Bulletin of Environmental Contamination and Toxicology 32:732-741. 2002 Environmental Toxicology and Chemistry 20(2):359-370. 2002 Environmental Research Section A 89:85-97. 2002 Environmental Science and Technology 36:2905-2910. 2002 Aquatic Toxicology 59:253-281. B-9 ------- APPENDIX B: Articles Reviewed Article Authors # Year Reference 22 Canivet et al. 23 Athalye et al. 24 Hanaoka et. al. 25 De Gieter et al. 26 Devesa et al. 27 Johnson and Roose. 28 Pedlar and Klaverkamp. 29 Strauber et al. 30 Hunter and Goessler. 31 Maeda et al. 32 Maeda et al. 33 Maeda et al. 34 Francesconi et al. 35 Valette-Silver et al. 36 Skinner 37 Langston 38 Bart et al. 39 Tanner et al. 40 Kaise et al. 41 Gaileretal. 42 Giusti and Zhang. 43 Zaroogian and Hoffman. 44 Wagemann et al. 2001 Archives of Environmental Contamination and Toxicology 40:345-354. 2001 Ecology, Environment and Conservation 7(3):319-325. 1988 Applied Organometallic Chemistry 2:371-376. 2002 Archives of Environmental Contamination and Toxicology 43:406-417. 2002 Applied Organometallic Chemistry 16:123-132. 2002 Report for the Environmental Assessment Program, Olympia, Washington. Pub. No. 02-03-057 2002 Aquatic Toxicology 57:153-166. 2002 23rd Annual Meeting of the Society of Environmental Toxicology and Chemistry, Poster and Absract No. P296. 1998 Marine Biology 131:543-552. 1990 Applied Organometallic Chemistry 4:251-254. 1993 Applied Organometallic Chemistry 7:467-476. 1992 Applied Organometallic Chemistry 6:213-219. 1999 Comparative Biochemistry and Physiology Part C 122:131-137. 1999 Marine Environmental Research 48:311-333. 1985 Proceedings of the Pennsylvania Academy of Science 59:155-161. 1984 Marine Biology 80:143-154. 1998 Ecotoxicology 7:325-334. 1999 Water Environment Research 71(4):494-505. 1997 Applied Organometallic Chemistry 11:297-304. 1995 Applied Organometallic Chemistry 9:341-355. 2002 Environmental Geochemistry and Health 24:47-65. 1982 Environmental Monitoring and Assessement 1:345-358. 1978 Archives of Environmental Contamination and Toxicology 7:169-191. B-10 ------- APPENDIX B: Articles Reviewed Article Authors # Year Reference 45 Baker and King. 46 Mason et al. 47 Lin et al. 48 Chen et al. 49 Cooper and Gillespie. 50 Chen and Folt. 51 Speharetal. 52 Barrows et al. 1994 Environmental contamination investigations of water quality, sediment, and biota of the upper Gila River Basin, Arizona. US Fish & Wildlife Service, 2000 Archives of Environmental Contamination and Toxicology 38:283-297. 2001 Bulletin of Environmental Contamination and Toxicology 67:91-97. 2000 Limnology and Oceanography 45(7): 1525-1536. 2001 Environmental Pollution 111:67-74. 2000 Environmental Science and Technology 34:3878-3884. 1980 Archives of Environmental Contamination and Toxicology 9:53-63 1980 In: R. Hague (ed.) Dyanmics, Exposure, and Hazard Assessment of Toxic Chemicals. Ann Arbor Sci., Ann Arbor, MI B-ll ------- APPENDIX C BCF STUDIES: RAW DATA AND CALCUATIONS ------- APPENDIX C: BCF Studies Gailer et al. 1995. Applied Organometallic Chemistry 9:341-355 10-day static-renewal exposure of different arsenic compounds to Mytilus edulis Note: arsenate, dimethylarsenic acid, dimethyl(2-hydroxyethyl)arsine oxide, trimethylarsine oxide, arsenite and methylarsonic acid were also exposed to Mytilus at 0.1 mg/L, but did not accumulate in tissues more than the control. Arsenic cmpd used in Species Common name Cw Ct BCF exposure mg/L* mg/kg** arsenobetaine trimethylarsonium iodide arsenocholine Mytilus edulis Mytilus edulis Mytilus edulis 0.1 0.1 0.1 * nominal concentration 139 15.1 45.4 ** wet weight whole animal 1390 151 454 Hunter and Goessler 1998. Marine Biology. 131:543-552 24-day static-renewal exposure of different arsenic compounds to the common shrimp, Crangon crangon Note: arsenate and trimethylarsine oxide were also exposed to the shrimp but were not accumulated Arsenic cmpd used exposure arsenobetaine Maeda, etal. 1990 in Species Crangon crangon Common name Cw mg/L* 0.108 * measured concentration Ct mg/kg** 18.8 ** dry weight tail muscle Ct mg/kg*** 3.76 *** converted to wet weight assuming 80% water content BCF dry weight 174.07 BCF wet weight 35 . Applied Organometallic Chemistry. 4:251-254 7-day static exposure (not specified in paper) Note: only one data point on day 7, therefore Nominal concentration Species of Na2HAsO4 used in exposure, mg/L 1 0.5 1 10 Moina Poecilia Poecilia Poecilia of different Na2HAsO4to the zooplankter, Moina macrocopa and the guppy, Poecilia it is not known if steady-state has been Common name Cw mg/L* 0.403 0.2015 0.403 4.03 *conc'n as As, based on 0.403 of 186 MW achieved Total As Ct mg/kg** 4.7 6.8 6.9 40 ** dry weight Total As Ct mg/kg*** 0.94 1.7 1.725 10 *** converted to wet weight assuming 80% water content for Moina, and 75% for Poecilia Inorganic As Ct mg/kg** 2.1 5 5.8 30.6 reticulata Mono-CH3 DI-CH3 Tri-CH3 Total As Ct Ct Ct BCF mg/kg** mg/kg** mg/kg** dry weight trace 2.6 trace 11.66 0.6 0.1 1.1 33.75 0.1 0.2 0.8 17.12 5.9 0.7 2.8 9.93 Geomean Total As BCF wet weight 2 8 4 2 4 C-2 ------- APPENDIX C: BCF Studies Maeda, etal. 1993. Applied Organometallic Chemistry. 7:467-476 7-day static exposure (not specified in paper) of different Na2HAsO4*7H20 (As(V)) to the carp, Cyprinus carpio. Mote: only one data point on day 7, therefore it is not known if steady-state has been achieved MUSCLE Nomina of As(V) 0 10 20 30 40 50 60 GUT Nomina of As(V) 0 10 20 30 40 50 60 concentration Species Common name mg/L Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus concentration Species Common name mg/L Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Total As Ct mg/kg** 2 3.8 6 5.8 7.2 11.4 12 ** dry weight in muscle tissue Total As Ct mg/kg** 7.6 19.7 23.8 40 51.4 60.6 82.8 ** dry weight in gut Total As Ct mg/kg*** 0.4 0.76 1.2 1.16 1.44 2.28 2.4 Total As Ct mg/kg*** 1.52 3.94 4.76 8 10.28 12.12 16.56 Non-methylat edAs Ct mg/kg** 1.8 3.6 5 4.6 6 7 7.1 Non-methylat edAs Ct mg/kg** 7.3 15 16 13 17 20 22 Mono-CH3 Ct mg/kg** trace 0.4 0.2 0.5 3.1 2.5 Mono-CH3 Ct mg/kg** 3.8 4.8 24 29 36 57 DI-CH3 Ct mg/kg** trace 0.2 0.1 0.3 0.6 1 DI-CH3 Ct mg/kg** 0.2 0.6 1.4 1.4 3.4 3.1 1.5 Tri-CH3 Ct mg/kg*** 0.2 0.2 0.4 0.9 0.4 0.7 1.4 Tri-CH3 Ct mg/kg*** 0.1 0.3 1.9 1.6 2 1.5 2.3 Total As BCF dry weight 0.38 0.30 0.19 0.18 0.23 0.20 Geomean Total As BCF dry weight 1.97 1.19 1.33 1.28 1.21 1.38 Geomean Total As BCF wet weight 0.08 0.06 0.04 0.04 0.05 0.04 0.048 Total As BCF wet weight 0.39 0.24 0.27 0.26 0.24 0.28 0.275 CARP REMNANTS (SKIN, SCALE, BONE, FIN) Nomina ofAs(V) 0 10 20 30 40 50 60 concentration Species Common name mg/L Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Cyprinus Total As Ct mg/kg** 5.5 7.5 7.9 6.7 6.8 13.8 12.6 Total As Ct mg/kg*** 1.1 1.5 1.58 1.34 1.36 2.76 2.52 Non-methylat edAs Ct mg/kg** 5.4 6.5 6.7 5.2 5 9.2 9 Mono-CH3 Ct mg/kg** 0.3 0.4 0.5 0.5 2.7 1.8 DI-CH3 Ct mg/kg** 0.1 0.1 0.2 0.2 0.4 0.7 0.5 Tri-CH3 Ct mg/kg*** trace 0.6 0.6 0.8 0.9 1.2 1.3 Total As BCF dry weight 0.75 0.40 0.22 0.17 0.28 0.21 Total As BCF wet weight 0.15 0.08 0.04 0.03 0.06 0.04 C-3 ------- APPENDIX C: BCF Studies "dry weight *** converted to wet weight Geomean 0.059 assuming 80% water content C-4 ------- APPENDIX C: BCF Studies Maeda, etal. 1992. Applied Organometallic Chemistry. 6:213-219 7-day static exposure (not specified in paper) of different Na2HAsO4 (As V) to the shrimp, Neocaridina denticulata Note: only one data point on day 7, therefore it is not known if steady-state has been achieved Nominal concentration Species of Na2HAs04 (as As V) used in exposure, mg/L 0.1 Neocardia 0.2 Neocardia 0.3 Neocardia 0.5 Neocardia 1 Neocardia 1 .5 Neocardia Common name Francesconi et al. 1999. Comparative Biochemistry and Physiology Part C 122 Total As Ct mg/kg** 18.9 18.5 19.8 22.6 33.2 31.6 ** dry weight 131-137 Total As Ct mg/kg*** 3.78 3.7 3.96 4.52 6.64 6.32 *** converted to wet weight assuming 80% water content Inorganic As Ct mg/kg** 15.9 14.9 17.3 15.4 30.2 27.9 Mono-CH3 DI-CH3 Tri-CH3 Total As Ct Ct Ct BCF mg/kg** mg/kg** mg/kg** dry weight 1.9 1.1 189 trace 1.9 1.7 92 1.4 1.1 66 trace 2.6 4.6 45 trace 1.7 1.3 33 trace 2.2 1.5 21 Geomean Total As BCF wet weight 38 18 13 9 7 4 12 10-day static exposure of arsenic-betaines to the mussel, Mytilus edulis Note: only one data point on day 10, therefore it is not known if steady-state has been Nominal concentration Species of As-betaine used in exposure, mg/L* control Mytilus 0.1 C-1 betaine Mytilus 0.1 C-2 betaine Mytilus 0.1 C-3 betaine Mytilus "nominal concentrations were confirmed with measurements - all within 4% Zaroogian and Hoffman. 1982. Environmental Common name achieved Total As Ct mg/kg** 18.3 1740 1220 151 ** dry weight Total As Ct mg/kg*** 3.66 348 244 30.2 *** converted to wet weight assuming 80% water content Total As BCF dry weight NA 17217 12017 1327 Geomean Total As BCF wet weight 3443 2403 265 1300 Monitoring and Assessment 1:345-358 16 week study flow-through exposure of arsenic as arsenite to eastern oysters, Note: uptake initially increased in the first 5 weeks Nominal concentration Species ofNa2HAs04(asAslll) used in exposure, mg/L control Crassostrea 3 Crassostrea 5 Crassostrea Crassostrea virginica then decreased with spawning, followed by a Common name Total As Cw mg/L 0.0012 0.0033 0.0058 Total As Ct mg/kg** 10.3 12.7 14.1 ** dry weight subsequent increase again. Steady-state is never really achieved. Total As Ct mg/kg*** 2.06 2.54 2.82 *** converted to wet weight assuming 80% water content Total As BCF dry weight 8583 3848 2431 Total As BCF wet weight 1717 770 486 C-5 ------- APPENDIX C: BCF Studies Langston. 1984. Marine Biology. 80:143-154 10-day renewal exposure of native Scrobicularia plana (3 cm length) from Restronguet Creek and Tamar Estuary, U.K. Dry Weight Basis Species Scrobicularia plana common name bivalve Dissolved As Cw mg/L* 0.01 * Interstitial water As concentrations Spehar et al. 1980. Archives of Environmental Contamination and Toxicology. Total As Ct mg/kg** 0.784 ** dry weight of total soft parts 9:53-63. Total As Ct mg/kg*** 0.124656 ** converted to wet weight based on a water content of 84.1% Total As BCF dry weight 78 Total As BCF wet weight 12 28-day intermittent flow exposure (1 00% renewal every 9 hrs) of wild-caught invertebrates and hatchery-reared rainbow trout parr Original whole body tissue arsenic concentrations reported on a dry weight basis; converted to wet wt assuming 80% water content for invertebrates, 75% for fish. Nominal concentration of As2O3(As(lll)used in exposure, mg/L 100 1000 100 1000 100 1000 100 1000 100 1000 100 1000 Species Pteronarcys dorsata Pteronarcys dorsata Daphnia magna Daphnia magna Helisoma campanulata Helisoma campanulata Stagnicola emarginata Stagnicola emarginata Gammurus pseudolimnaeus Gammurus pseudolimnaeus Oncorhynchus mykiss Oncorhynchus mykiss Common name stonefly stonefly cladoceran cladoceran snail snail snail snail amphipod amphipod rainbow trout rainbow trout Total As Cw mg/L* 0.088 0.961 0.088 0.961 0.088 0.961 0.088 0.961 0.088 0.961 0.088 0.961 * Measured as total As in water Total As Ct mg/kg* NA 42 21 47 2.5 80 3.3 16 Total As Ct mg/kg wet wt 8.4 4.2 9.4 0.5 16 0.66 3.2 Total As BAF dry weight 44 239 49 28 83 38 17 and Total As Geomean BAF wet weight 9 48 10 6 17 8 3 9 22 10 5 C-6 ------- APPENDIX C: BCF Studies Speharetal. 1980. Archives of Environmental Contamination and Toxicology. 9:53-63. 28-day intermittent flow exposure (100% renewal every 9 hrs) of wild-caught invertebrates and hatchery-reared rainbow trout parr Original whole body tissue arsenic concentrations reported on a dry weight basis; converted to wet wt assuming 80% water content for invertebrates, and 75% for fish. Nominal concentration Species Common name Total As Total As Total As Total As Total As Geomean of 3As205 .5H20 Cw Ct Ct BAF BAF (As(V) used in mg/L* mg/kg* mg/kg wet wt dry weight wet weight exposure, mg/L 100 1000 100 1000 100 1000 100 1000 100 1000 100 1000 Pteronarcys dorsata stonefly Pteronarcys dorsata stonefly Daphnia magna cladoceran Daphnia magna cladoceran Helisoma campanulata snail Helisoma campanulata snail Stagnicola emarginata snail Stagnicola emarginata snail Gammurus pseudolimnaeus amphipod Gammurus pseudolimnaeus amphipod Oncorhynchus mykiss rainbow trout Oncorhynchus mykiss rainbow trout 0.089 0.973 0.089 0.973 0.089 0.973 0.089 0.973 0.089 0.973 0.089 0.973 * Measured as total As in water 12 34 5.2 19 8.8 27 8.2 17 2.4 6.8 1.04 3.8 1.76 5.4 1.64 3.4 135 35 58 20 99 28 92 17 27 7 12 4 20 6 18 3 14 7 10 8 Speharetal. 1980. Archives of Environmental Contamination and Toxicology. 9:53-63. 28-day intermittent flow exposure (100% renewal every 9 hrs) of wild-caught invertebrates and hatchery-reared rainbow trout parr Original whole body tissue arsenic concentrations reported on a dry weight basis; converted to wet wt assuming 80% water content for invertebrates, and 75% for fish. Nominal concentration Species Common name Total As Total As Total As Total As Total As Geomean of (CH3)2AsO(ONa) Cw Ct SDMA used in mg/L* mg/Kg* exposure, mg/L Total As Total As Ct BAF mg/Kg wet wt dry weight Total As BAF wet weight 100 1000 100 1000 100 1000 100 1000 100 1000 100 1000 Pteronarcys dorsata stonefly Pteronarcys dorsata stonefly Daphnia magna cladoceran Daphnia magna cladoceran Helisoma campanulata snail Helisoma campanulata snail Stagnicola emarginata snail Stagnicola emarginata snail Gammurus pseudolimnaeus amphipod Gammurus pseudolimnaeus amphipod Oncorhynchus mykiss rainbow trout Oncorhynchus mykiss rainbow trout 0.086 0.97 0.086 0.97 0.086 0.97 0.086 0.97 0.086 0.97 0.086 0.97 * Measured as total As in water 2.4 29 7.2 23 1.9 23 NA 9.8 0.48 5.8 1.44 4.6 0.38 4.6 1.96 28 30 84 24 22 24 10 6 6 17 5 4 5 C-7 ------- APPENDIX C: BCF Studies Speharetal. 1980. Archives of Environmental Contamination and Toxicology. 9:53-63. 28-day intermittent flow exposure (1 00% renewal every 9 hrs) of wild-caught invertebrates and hatchery-reared rainbow trout parr Original whole body tissue arsenic concentrations reported on a dry weight basis; converted to wet wt assuming 80% water content for invertebrates, and 75% for fish. Nominal concentration Species Common name Total As Total As Total As Total As Total As Geomean of Cw Ct Ct BAF BAF CH32AsO(ONa)2.6H2O mg/L* mg/Kg* mg/Kg wet wt dry weight wet weight DSMA used in exposure, mg/L 100 1000 100 1000 100 1000 100 1000 Pteronarcys dorsata Pteronarcys dorsata Daphnia magna Daphnia magna Helisoma campanulata Helisoma campanulata Stagnicola emarginata Staanicola emarainata stonefly stonefly cladoceran cladoceran snail snail snail snail 0.085 0.846 0.085 0.846 0.085 0.846 0.085 0846 1.8 44 5 17 2.6 18 1 16 0.085 8.8 1 3.4 0.52 3.6 0.2 32 2 52 59 20 31 21 12 19 0 10 12 4 6 4 2 4 7 7 5 3 Co -o ------- APPENDIX D BAF STUDIES: RAW DATA AND CALCULATIONS ------- RAF Studies Skinner. 1985. Proceedings of the Pennsylvania Academy of Science. 59:155-161 Scope: measurements of contaminants in fish and water in fly ash basins (As BAF) Dry Weight Basis DryaWcright Basis Species Bl#6 Mon FA Mon DB Mon DB MonSW MonSW MCIWTB MCIWTB MCIWTB Wet Weight Basis Location Species Bl#6 Mon FA Mon DB Mon DB MonSW MonSW MCIWTB MCIWTB MCIWTB Common Name carp carp carp carp carp carp carp carp carp Common Name carp carp carp carp carp carp carp carp carp Cw mg/L* 0.03 0.016 0.003 0.003 0.003 0.003 0.006 0.006 0.006 "Total As Cw mg/L* 0.03 0.016 0.003 0.003 0.003 0.003 0.006 0.006 0.006 "Total As ct mg/kg** 0.3 0.7 0.9 0.8 0.2 0.2 0.5 0.7 0.5 **Total As, dry weight edible ct mg/kg*** 0.06 0.14 0.18 0.16 0.04 0.04 0.1 0.14 0.1 *** converted to wet weight assuming 80% BAF dry weight 10.0 43.7 300.0 266.7 66.7 66.7 83.3 116.7 83.3 BAF dry weight 2.0 8.7 60.0 53.3 13.3 13.3 16.7 23.3 16.7 log BAF 1.0 1.6 2.5 2.4 1.8 1.8 1.9 2.1 1.9 log BAF 0.3 0.9 1.8 1.7 1.1 1.1 1.2 1.4 1.2 Avg log BAF per Location 1.00 1.64 2.45 1.82 1.97 Avg log BAF per Location 1.00 0.94 1.75 1.12 1.27 Avg BAF per Location 10.0 43.8 282.8 66.7 93.2 Avg BAF per Location 10.0 8.8 56.6 13.3 18.6 D-2 ------- RAF Studies Kaiseetal. 1997. Applied Organometallic Chemistry. 11:297-304 Scope: As species in water, algae, Location Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Hayakawa River (Japan) Bartetal. 1998. Ecotoxicology. macroinvertebrates and fish collected from the Hayakawa Species Clodophora glomerate Diatom Plecoglossus altivelis Onchorhynchus masou masou Rhinogobius sp. Phoxinus steindachneri Trobolodon hakonensis Sicyopterus japonicus Macrobranchiura nipponense Semisulcospira libertina Plotohermes grandis caddisfly larva Stenopsyche marmorata 7:325-334 Common Name green alga FW Diatom sweet fish masu salmon goby downstream fatminnow Japanese dace amphidromous goby prawn marsh snail dobsonfly larva caddisfly larva caddisfly pupa River (Japan) Total As Total As Cw Ct mg/L* mg/kg* 0.03 0.453 0.03 0.124 0.03 0.051 0.03 0.146 0.03 0.333 0.03 0.267 0.03 0.100 0.03 0.370 0.03 0.817 0.03 0.186 0.03 2.875 0.03 0.236 0.03 2.050 *wet weight Inorganic As Ct mg/kg* 0.0 0.0 ND ND ND ND ND ND ND ND ND ND ND Methylarsine Ct mg/kg* ND ND ND ND ND ND ND ND ND ND ND ND ND Diemthylarsine Ct mg/kg* 0.385 0.101 0.005 0.063 0.077 0.061 0.076 0.089 0.614 0.050 2.762 0.202 1.180 Trimethylarsine Ct mg/kg* 0.015 0.003 0.040 0.081 0.238 0.197 0.020 0.269 0.187 0.116 0.043 0.022 0.839 Total As BAF 15.1 4.1 1.7 4.9 11.1 8.9 3.3 12.3 27.2 6.2 95.8 7.9 68.3 Scope: Total As in fish and water from the lower Mississippi River Location Devil's Swamp Tunica Swamp Species mean of numerous spp. mean of numerous spp. Common Name Total As Total As Cw Ct mg/L* mg/kg* 0.147 0.061 0.221 0.035 *assumed to be wet weight (not stated) based on the article's stating of dry wt for sediment samples with no reference to fish Total As BAF 0.4 0.2 D-3 ------- RAF Studies Valette-Silver et al. 1999. Marine Environmental Research. 48:311-333 Scope: As data from National Status and Trends program (1 986-1 995) Dry Weight Basis Location Miami River mouth Miami River mouth Wet Weight Basis Location Miami River mouth Miami River mouth Langston. 1984. Marine Biology. Scope: In field study, measued Total Dry Weight Basis Location Restronguet Creek, Site S Restronguet Creek* Tamar Estuary* Wet Weight Basis Location Restronguet Creek, Site S Restronguet Creek Tamar Estuary Species Isognomon sp.-radiatus? Crassostrea virginica Species Isognomon sp.-radiatus? Crassostrea virginica 80:143-154 As in the bivalve mollusk, Species Scrobicularia plana Scrobicularia plana Scrobicularia plana Species Scrobicularia plana Scrobicularia plana Scrobicularia plana Common Name bivalve bivalve Common Name bivalve bivalve Scrobicularia plana and in Common Name bivalve bivalve bivalve Common Name bivalve bivalve bivalve Total As As(lll) Cw Cw mg/L* mg/L** 0.00089 0.0 0.00089 0.0 * water samples ** dry weight were filtered Total As As(lll) Cw Cw mg/L* mg/L** 0.00089 0.0 0.00089 0.0 * water samples *** converted to were filtered wet weight assuming 80% water content Restronguet Creek Dissolved As Total As Cw Ct mg/L* mg/kg** 0.0049 200.0 0.0551 214.0 0.0109 34.0 * I nterstitial water ** dry weight of As concentrations Total soft parts Dissolved As Total As Cw Ct mg/L* mg/kg** 0.0049 31.8 0.0551 34.0 0.0109 5.4 * I nterstitial water ** converted to wet As concentration weight based on a water content of 84.1% As(V) MMA Cw Cw mg/L** mg/L** 0.00069 0.00003 0.00069 0.00003 As (V) MMA Cw Cw mg/L** mg/L** 0.00069 0.00003 0.00069 0.00003 Total As BAF 40816.3 3883.8 3119.3 Total As BAF 6489.8 617.5 496.0 DMA Total As Total As Cw Ct BAF mg/L** mg/kg** dry weight 0.00006 37.3 41910 0.00006 23.6 26517 DMA Total As Total As Cw Ct BAF mg/L** mg/kg*** wet weight 0.00006 7.46 8382 0.00006 4.72 5303 D-4 ------- BAF Studies Cooper and Gillespie. 2001. Environmental Pollution. 111:67-74 Scope: Study was designed to measure concentrations of As and Hg associated with different components (sediment, water, fish) of a NW Mississippi Dry Weight Basis Location Species Common Name Total As Total As Total As Cw mg/L* Ct mg/kg* BAF Moon Lake Moon Lake Moon Lake Moon Lake Wet Weight Basis Location freshwater fish species benthivorous fish omnivorous fish planktivorous fish Species Common Name 0.00512 0.00512 0.00512 0.00512 * Average of six sites Total As Cw mg/L* 0.0 0.0 0.1 0.0 7.2 8.9 20.3 0.8 * dry weight Total As Ct mg/kg** Total As BAF Moon Lake Moon Lake Moon Lake Moon Lake freshwater fish species benthivorous fish omnivorous fish planktivorous fish 0.00512 0.00512 0.00512 0.00512 0.0 0.0 0.0 0.0 1.8 2.2 5.1 0.2 * Average of six ** converted to wet sites weight assuming 75% water content Giusti and Zhang. Scope: Study of the Dry Weight Basis Location 2002. Environmental Geochemistry and Health 24:47-65. trace metal distribution in sediments, marine water and mussel Mytilus galloprovincialis of the Venetian Lagoon, Island of Murano Species Common Name Dissolved As Cw mg/L Total As Ct mg/kg* Total As BAF B E F H Wet Weight Basis Location Mytilus galloprovincialis Mytilus galloprovincialis Mytilus galloprovincialis Mytilus galloprovincialis Species Mussel Mussel Mussel Mussel Common Name 0.0039 0.00473 0.00323 0.0019 18.0 16.1 12.3 12.0 4615.4 3403.8 3808.0 6315.8 "Edible portion, composite samples (n = 15 to 20 mussels per site) Dissolved As Cw mg/L Total As Ct mg/kg* Total As BAF Mytilus galloprovincialis Mussel Mytilus galloprovincialis Mussel Mytilus galloprovincialis Mussel Mytilus galloprovincialis Mussel 0.0039 0.00473 0.00323 0.0019 3.6 3.2 2.5 2.4 923.1 680.8 761.6 1263.2 D-5 ------- BAF Studies * converted to wet weight assuming 80% water content D-6 ------- RAF Studies Chen and Folt. 2000. Environmental Science & Technology, 34:3878-3884. Scope: Bioaccumulation (and Diminution) of As in Freshwater Food Web Dry Weight Basis Location Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Wet Weight Basis Location Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Upper Mystic Lake Species Common Name zooplankton (small) NA zooplankton (large) NA alewife killifish black crappie bluegill sunfish yellow perch largemouth bass Species Common Name zooplankton (small) NA zooplankton (large) NA alewife killifish black crappie bluegill sunfish yellow perch largemouth bass Dissolved As Cw mg/L* 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 * average of 3 samples (June, August, October) Dissolved As Cw mg/L* 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 0.000781 *average of 3 samples (June, August, October) Total As Ct mg/kg** 17.2 10.7 0.3 0.3 0.1 0.1 0.2 0.1 ** dry weight Total As Ct mg/kg** 3.4 2.1 0.1 0.1 0.0 0.0 0.0 0.0 ** converted to wet weight assuming 75% water content for fish and 80% for zooplankton Total As BAF 21959.0 13738.8 381.6 343.1 158.8 190.8 234.3 184.4 Total As BAF ERR 2747.8 95.4 85.8 39.7 47.7 58.6 46.1 D-7 ------- RAF Studies Chenetal. 2000. Limnology and Oceanography 45:1 525-1 536. Scope: Arsenic in food web across a gradient of lakes Dry Weight Basis Location Species Common Name Canobie Lake Canobie Lake Chaffin Pond Clear Pond Clear Pond Community Lake Community Lake Gregg Lake Gregg Lake Horseshoe Pond Horseshoe Pond Ingham Pond Ingham Pond Island Pond Lake Placid Lake Placid Lower Kohanza Reservoir Lower Kohanza Reservoir Mirror Lake Mirror Lake Palmer pond Post pond Post pond Queen Lake Queen Lake Tewksbury pond Tewksbury pond Turkey pond Turkey pond Williams Lake Williams Lake All lakes Small zooplankton Large zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Piscivores and omnivores freshwater fish Dissolved As Cw mg/L 0.000221 0.000221 0.000113 0.000046 0.000046 0.000367 0.000367 0.00038 0.00038 0.000078 0.000078 0.000587 0.000587 0.00026 0.000123 0.000123 0.000085 0.000085 0.000409 0.000409 0.000022 0.00026 0.00026 0.000107 0.000107 0.000057 0.000057 0.00026 0.00026 0.000096 0.000096 0.000174 Total As Ct mg/kg* 10.4 2.4 0.1 0.1 0.3 1.4 0.3 5.9 1.6 7.6 0.5 1.1 2.1 6.5 0.8 0.4 0.3 0.2 1.0 0.6 0.3 0.5 0.9 0.9 0.3 2.2 0.2 9.9 3.0 1.4 0.5 0.6 *dry weight Total As BAF** 95.4 10905.0 964.6 2804.3 5869.6 3842.0 768.4 15421.1 4131.6 97435.9 6717.9 1925.0 3509.4 25038.5 6422.8 2951.2 3152.9 1952.9 2518.3 1371.6 11909.1 1846.2 3642.3 8654.2 2869.2 39122.8 2894.7 38115.4 11500.0 14687.5 4812.5 3281.6 **BAF for fish was back calculated from the Loa BAF and Cw D-8 ------- RAF Studies Chenetal. 2000. Limnology and Oceanography 45:1 525-1 536. Scope: Arsenic in food web across a gradient of lakes Wet Weight Basis Location Species Common Name Canobie Lake Canobie Lake Chaffin Pond Clear Pond Clear Pond Community Lake Community Lake Gregg Lake Gregg Lake Horseshoe Pond Horseshoe Pond Ingham Pond Ingham Pond Island Pond Lake Placid Lake Placid Lower Kohanza Reservoir Lower Kohanza Reservoir Mirror Lake Mirror Lake Palmer pond Post pond Post pond Queen Lake Queen Lake Tewksbury pond Tewksbury pond Turkey pond Turkey pond Williams Lake Williams Lake All lakes Small zooplankton Large zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Small zooplankton Large zooplankton Piscivores and omnivores freshwater fish Dissolved As Cw mg/L 0.000221 0.000221 0.000113 0.000046 0.000046 0.000367 0.000367 0.00038 0.00038 0.000078 0.000078 0.000587 0.000587 0.00026 0.000123 0.000123 0.000085 0.000085 0.000409 0.000409 0.000022 0.00026 0.00026 0.000107 0.000107 0.000057 0.000057 0.00026 0.00026 0.000096 0.000096 0.000174 Total As Ct mg/kg* 2.1 0.5 0.0 0.0 0.1 0.3 0.1 1.2 0.3 1.5 0.1 0.2 0.4 1.3 0.2 0.1 0.1 0.0 0.2 0.1 0.1 0.1 0.2 0.2 0.1 0.4 0.0 2.0 0.6 0.3 0.1 0.1 Total As BAF** 2894.7 2181.0 192.9 560.9 1173.9 768.4 153.7 3084.2 826.3 19487.2 1343.6 385.0 701.9 5007.7 1284.6 590.2 630.6 390.6 503.7 274.3 2381.8 369.2 728.5 1730.8 573.8 7824.6 578.9 7623.1 2300.0 2937.5 962.5 361.0 D-9 ------- BAF Studies * converted to wet weight based on 88% water content for fish (as in the article) and 80% forzooplankton D-10 ------- RAF Studies Mason et al. 2002. Archives of Environmental Contamination and Toxicology 38:283-297. Scope: Bioaccumulation of As and other metals by freshwater Inverts and fish Wet Weight Basis Species Common Name Location Dissolved As Total As Total As Cw Ct BAF mg/L mg/kg** Diptera/Tipulidae Diptera/Tipulidae Tricoptera/Hydropsychidae Tricoptera/Hydropsychidae Ephemeroptera/Heptageniidae Ephemeroptera/Heptageniidae Plecoptera/Pteronacidae/Pteronarcy s Plecoptera/Perlidae/Acroneuria Plecoptera/Perlidae/Acroneuria Odonata/Aeshnidae/Aeshna Odonata/Aeshnidae/Aeshna Megaloptera/Corydalidae Megaloptera/Corydalidae Crustacea/Decapoda Crustacea/Decapoda Ameierus nebulosus Catostomus commersoni Cottus bairdi Rhinichthys atratulus Semotilus atromaculatus Salvelinus fontinalis Salvelinus fontinalis Salvelinus fontinalis Salvelinus fontinalis *whole body periphyton periphyton bryophytes bryophytes cranefly cranefly caddisfly caddisfly mayfly mayfly shredder stonefly predatory stonefly predatory stonefly dragonfly dragonfly dobsonfly dobsonfly Crayfish Crayfish Brown Bullhead White Sucker Mottled Sculpin Blacknose Dace Creek Chub Small Brook Trout Small Brook Trout Large Brook Trout Large Brook Trout Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Herrington Creek Blacklick Herrington Creek Herrington Creek Herrington Creek Blacklick Blacklick Harrington Creek Blacklick Harrington Blacklick Harrington Creek 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.00037 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.00067 0.00067 0.00037 0.00037 0.00067 0.00037 0.00067 0.00037 0.00067 0.6 1.4 1.1 1.6 0.9 0.3 1.0 1.2 2.1 1.7 0.2 0.5 0.6 0.1 0.8 0.4 0.3 0.2 0.4 0.2 0.3 0.3 0.2 0.2 0.2 0.2 0.1 0.2 1600.3 2062.1 2915.9 2415.5 2400.5 392.8 2809.5 1846.0 5618.6 2543.1 604.6 1333.5 824.8 195.7 1256.9 1102.4 432.1 489.2 646.4 283.9 376.1 798.1 512.7 281.5 571.1 308.2 304.6 237.8 D-ll ------- RAF Studies Wagemann et al. 1978 Scope: As in water and Dry Weight Basis Location Grace Lake Grace Lake Kam Lake Kam Lake Grace Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Kam Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Grace Lake Kam Lake Archives of Environmental Contamination and Toxicology 7:169-191. Biota from Lakes in N. West Canada Species Common Name Dissolved As Total As Total As Cw Ct BAF mg/L* mg/kg** Pelecypoda Gastropoda Gastropoda Oligochaeta Ephemeroptera Trichoptera Trichoptera Chironomidae Chironomidae zooplankton zooplankton Hemiptera: Notonectidae Hemiptera: Notonectidae Hemiptera: Gerridae Odonata: Anispotera Odonata: Anispotera Odonota: Zygoptera Odonota: Zygoptera Coleoptera: Dytiscidae Coleoptera: Dytiscidae Coleoptera: Gyrinidae Coleoptera: Gyrinidae Diptera: Ceratopogonidae Diptera: Ceratopogonidae Chironomidae: Tanypodinae Hydracarnia Hirudinea Hirudinea Cottus cognatus Cottus cognatus Amphipoda Hemiptera: Corixidae Hemiptera: Corixidae Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Herbivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore', sculpin Carnivore; sculpin Omnivore Omnivore Omnivore 0.027 0.027 2.58 2.58 0.027 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 0.027 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 2.58 2.58 0.027 2.58 0.027 2.58 0.027 0.027 2.58 23.2 14.8 133.0 820.0 51.0 14.3 56.0 31.0 125.0 26.7 710.0 3.2 30.0 1.8 9.2 57.5 5.5 2.0 6.5 32.1 2.6 14.6 3.5 12.0 40.0 51.6 2.7 190.0 7.6 122.0 14.5 3.8 44.1 859.3 548.1 51.6 317.8 1888.9 529.6 21.7 1148.1 48.4 988.9 275.2 118.1 11.6 66.7 341.5 22.3 204.4 0.8 240.4 12.4 95.9 5.7 129.6 4.7 15.5 20.0 100.7 73.6 282.2 47.3 537.0 141.5 17.1 D-12 ------- RAF Studies *Average of 1 975 **Geometric mean of whole body monthly samples samples collfrin summer months 1975 Wagemann et al. 1978 Scope: As in water and Wet Weight Basis Location Archives of Environmental Contamination and Toxicology 7:169-191. Biota from Lakes in N. West Canada Species Common Name Dissolved As Total As Total As Cw Ct BAF mg/L mg/kg** Grace Lake Grace Lake Kam Lake Kam Lake Grace Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Kam Lake Kam Lake Grace Lake Kam Lake Grace Lake Kam Lake Grace Lake Grace Lake Pelecypoda Gastropoda Gastropoda Oligochaeta Ephemeroptera Trichoptera Trichoptera Chironomidae Chironomidae zooplankton zooplankton Hemiptera: Notonectidae Hemiptera: Notonectidae Hemiptera: Gerridae Odonata: Anispotera Odonata: Anispotera Odonota: Zygoptera Odonota: Zygoptera Coleoptera: Dytiscidae Coleoptera: Dytiscidae Coleoptera: Gyrinidae Coleoptera: Gyrinidae Diptera: Ceratopogonidae Diptera: Ceratopogonidae Chironomidae: Tanypodinae Hydracarnia Hirudinea Hirudinea Cottus cognatus Cottus cognatus Amphipoda Hemiptera: Corixidae Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore Carnivore; sculpin Carnivore; sculpin Omnivore Omnivore 0.027 0.027 2.58 2.58 0.027 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 0.027 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 0.027 2.58 2.58 2.58 0.027 2.58 0.027 2.58 0.027 0.027 4.6 3.0 26.6 164.0 10.2 2.9 11.2 6.2 25.0 5.3 142.0 0.6 6.0 0.4 1.8 11.5 1.1 0.4 1.3 6.4 0.5 2.9 0.7 2.4 8.0 10.3 0.5 38.0 1.9 30.5 2.9 0.8 171.9 109.6 10.3 63.6 377.8 105.9 4.3 229.6 9.7 197.8 55.0 23.6 2.3 13.3 68.3 4.5 40.9 0.2 48.1 2.5 19.2 1.1 25.9 0.9 3.1 4.0 20.1 14.7 70.6 11.8 107.4 28.3 D-13 ------- BAF Studies Kam Lake Hemiptera: Corixidae Omnivore 2.58 8.8 3.4 * converted to wet weight assuming 80% water content for invertebrates and 75% for fish D-14 ------- BAF Studies Lin et al. 2001 . Bulletin of Environmental Conamination and Toxicology 67:91 -97. Scope: Bioaccumulation Dry Weight Basis Location Putai 3 Wet Weight Basis Location Putai 3 Baker and King. 1994. of As in Mullet in Fish Ponds using As contaminated groundwater Species Common Name Liza macrolepis Mullet Species Common Name Liza macrolepis mullet Total As Total As Cw Ct mg/L mg/kg* 0.1697 2.2 * value is average As in dorsal muscle of eleven fish Total As Total As Cw Ct mg/L mg/kg* 0.1697 0.6 * Converted to wet weight assuming 75% water content Total As BAF 13.2 Total As BAF 3.3 Environmental contamination investigations of water quality, sediment, and biota of the upper Gila River Basin, Scope: As in water and biota of the San Francisco River (site 2) and Upper Gila River, AZ. Wet Weight Basis Locaton 2 2 4 4 5 5 6 7 7 7 8 9 9 9 9 9 10 Species Common Name Ictalurus punctatus Channel Catfish Pilodictis olivaris FH Catfish* Ictalurus punctatus Channel Catfish Pilodictis olivaris FH Catfish Ictalurus punctatus Channel Catfish Pilodictis olivaris FH Catfish Cyprinis carpio Carp Pilodictis olivaris FH Catfish Cyprinis carpio Carp Pilodictis olivaris FH Catfish* Cyprinis carpio Carp Ictalurus punctatus Channel Catfish Cyprinis carpio Carp Micropterus salmoides LM Bass Ictalurus punctatus Channel Catfish* Micropterus salmoides LM Bass* Cyprinis carpio Carp Total As Total As Cw Ct mg/L** mg/kg 0.02 0.1 0.02 0.1 0.034 0.1 0.034 0.1 0.017 0.1 0.017 0.1 0.025 0.1 0.01 0.1 0.01 0.1 0.01 0.1 0.011 0.1 0.008 0.2 0.008 0.1 0.008 0.3 0.008 0.1 0.008 0.1 0.008 0.2 Total As BAF 5.0 5.0 2.9 2.9 5.9 5.9 4.0 10.0 10.0 10.0 9.1 25.0 12.5 37.5 12.5 12.5 25.0 D-15 ------- 3 0> LJ_ < m *Edible portion ** water sample is average of 3 monthly samples collected June thru Alienist 1990 whpn fig;h WPTP nnllpntpH APPENDIX E ARSENIC TOTAL: DISSOLVED CHEMICAL TRANSLATOR ------- Dissolved Fraction (f-d) of Author/Location Anderson and Bruland (1991)/CA 10/23/88- depth, m= 0 10/23/88- depth, m= 3.7 10/23/88- depth, m= 15.2 10/23/88- depth, m= 17.7 12/20/88- depth, m= 0 12/20/88- depth, m= 3.7 12/20/88- depth, m= 7.6 12/20/88- depth, m= 12.2 12/20/88- depth, m= 16.8 2/13/89-depth, m=0 2/13/89-depth, m=3.7 2/13/89-depth, m=7.6 2/13/89-depth, m=12.2 2/13/89-depth, m=16.8 GM Chen and Folt (2000)/Upper Mystic Lake, Summer, 1997 Fall, 1997 As-D (nM) Davis Creek 24.9 26.8 22.4 19.6 23.9 24.2 23.8 24.8 24.2 17.8 17.4 16.4 16.8 15.6 for the three MA 0.85 0.65 Arsenic (As) for Lentic Systems As-T (nM) As f-d As log (f-d) Reservoir 25.8 25.6 32.4 37.9 22.6 23.2 23.3 23.1 21.9 15.9 16.4 16.5 16.3 16.4 dates: 0.985 0.72 0.965 1.000 0.691 0.517 0.766 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 1.000 0.950 0.987 0.918 0.86 0.9 0.88 -0.015 0.000 -0.161 -0.287 -0.116 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 -0.022 -0.006 -0.066 -0.046 -0.056 E-2 ------- Dissolved Author/Location Tanzaki et al (1992)/ Japan Tamagawa River- S-1 Tamagawa River- S-2 Tamagawa River- S-3 Tamagawa River- S-4 Tamagawa River- S-5 Tamagawa River- S-6 Sagamigawa River- S-7 Sagamigawa River- S-8 Tamagawa and Sagamigawa Rivers Waslenchuk(1979)/GA Ogeechee River Hering and Kneebone (2002)/CA Los Angelos Aqueduct, channel Michel et al./France Seine River* *Average of samples from the 210-280 Kmn to Paris zone of freshwater. Fraction As-D (ug/L) 0.596 0.530 0.785 0.719 0.409 0.535 0.325 0.356 0.265 4.6 1.65 (f-d) of Arsenic (As) for Lotic Systems As-T (ug/L) 0.655 0.578 0.851 0.754 0.898 0.535 0.382 0.380 0.36 5.7 1.76 As f-d 0.910 0.917 0.924 0.954 0.455 1 0.851 0.937 0.862 0.736 0.807 0.938 As log (f-d) -0.041 -0.038 -0.034 -0.020 -0.342 0.000 -0.070 -0.028 -0.076 -0.133 -0.093 -0.028 E-3 ------- Dissolved Author/Location Milward et al. (1997)/England Thames estuary Febuary, 1989 July, 1990 Fraction As-D (ug/L) 3.277 2.292 (f-d) of Arsenic (As) Participate As (ug/L) 0.227 0.133 for Estuarine Systems As-T (ug/L) 3.504 2.425 As f-d 0.935 0.945 0.940 As log (f-d) -0.029 -0.024 -0.027 E-4 ------- Dissolved Fraction (f-d) of Arsenic (As) for Combined Surface Drinking Water Sources Author/Location Relative Sample Contribution Range of As f-d Chen et al. (1999)/ U.S. Surface Drinking Water Sources 6.54 5.05 6.35 5.85 5.61 5.79 5.79 5.99 6.16 5.61 6.36 4.48 6.54 5.43 5.79 6.17 4.67 5.70 0.901-1 0.789-0.901 0.783-0.789 0.756-0.783 0.753-0.756 0.72-0.753 0.693-0.72 0.673-0.693 0.651-0.673 0.589-0.651 0.589-0.589 0.5-0.589 0.497-0.56 0.483-0.497 0.451-0.483 0.441-0.451 0.182-0.441 M id-Rang e of As f-d 0.950 0.845 0.783 0.770 0.754 0.737 0.706 0.683 0.662 0.610 0.589 0.544 0.498 0.490 0.467 0.446 0.312 Weighted Log Dissolved Weighted Sample Log Relative Contributi Contribution* Contribution on 6.210 4.270 4.970 4.500 4.230 4.270 4.090 4.090 4.080 3.420 3.750 2.440 3.260 2.660 2.700 2.750 1.460 3.418 GM f-d: f-d= "relative sample contribution x midrange f-d. 5.74xf-d=3.54 0.60 0.816 0.703 0.803 0.767 0.749 0.763 0.763 0.777 0.790 0.749 0.803 0.651 0.816 0.735 0.763 0.790 0.669 0.756 0.793 0.630 0.696 0.653 0.626 0.630 0.612 0.612 0.611 0.534 0.574 0.387 0.513 0.425 0.431 0.439 0.164 0.534 E-5 ------- APPENDIX F TISSUE ARSENIC SPECIATION DATA ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # whole :reshwater -Field 2 40 body marsh snail whole 2 40 body caddisfly larva whole 2 40 body caddisfly pupa GMEAN whole :reshwater-Lab 2 1 body waterflea whole Water Exposure) 2 1 body waterflea whole 2 1 body waterflea GMEAN whole 2 1 body shrimp whole 2 1 body shrimp whole 2 1 body shrimp GMEAN whole zooplanktonic 2 31 body grazer whole 2 32, 33 body shrimp whole 2 32, 33 body shrimp whole 2 32, 33 body shrimp whole 2 32, 33 body shrimp whole 2 32, 33 body shrimp whole 2 32, 33 body shrimp GMEAN Total As Ct mg/kg 0.186 0.236 2.05 0.4481 18 19.4 35.2 23.07& 1 1.88 2.2 1 .605! 0.94 3.78 3.7 3.96 4.52 6.64 6.32 4.679S Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 13 0.722 4.6 0.256 14.6 0.753 4.6 0.237 22 0.625 12.8 0.364 16.1030 0.6978 6.4701 0.280^ 0.46 0.460 0.2 0.220 0.9 0.479 0.6 0.340 0.82 0.373 1.2 0.555 0.6976 0.4346 0.5559 0.346; 0.42 0.447 3.18 0.841 2.98 0.805 3.46 0.874 3.08 0.681 6.04 0.910 5.58 0.883 3.8784 0.8287 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 1.058 0.05 0.269 0.116 0.624 1.173 0.202 0.856 0.022 0.093 3.004 1.18 0.576 0.839 0.409 0.2284 0.1289 0.060 0.3 0.017 0.020 0.18 0.009 0.020 0.42 0.012 0.0288 0.2831 0.0123 0.32 0.320 0.34 0.181 0.16 0.073 0.2592 0.1615 0.52 0.553 0.759 0.38 0.101 0.22 0.058 0.915 0.38 0.103 0.34 0.092 0.626 0.28 0.071 0.22 0.056 1.759 0.52 0.115 0.92 0.204 0.690 0.34 0.051 0.26 0.039 0.857 0.44 0.070 0.3 0.047 0.8761 0.3828 0.0818 0.3251 0.0695 F-2 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # whole :reshwater-Lab 2 1,3 body waterflea Dietary Exposure - ab foodchain nodel) 2 whole 2 1 body shrimp whole 2 1 body shrimp whole 2 4 body shrimp GMEAN whole zooplanktonic 31 body grazer whole zooplanktonic 31 body grazer whole 33 body shrimp Total As Ct mg/kg 41.8 2.5 6.4 6.4 4.678^ 15.12 22.2 5.12 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 18.4 0.440 23.4 0.560 0.44 0.176 2.0 0.808 0.6 0.094 5.8 0.906 0.6 0.094 5.8 0.906 0.5411 0.1157 4.0807 0.872! 13.24 0.876 16.66 0.750 4.52 0.883 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 0.04 0.016 0.0400 0.0160 1.88 0.124 3.930 1.860 0.084 3.68 0.166 0.286 0.056 F-3 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # whole :reshwater-Field 3 40 body prawn whole 3 40 body dobsonfly larva whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish GMEAN whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish GMEAN whole amphidromous 3 40 body goby whole 3 40 body Japanese dace whole downstream 3 40 body fatminnow whole 3 40 body goby whole 3 40 body sweet fish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish Total As Ct mg/kg 0.817 2.875 0.6 1.26 0.32 0.62 0.76 1 0.4 1.16 1.26 1.02 1.7 0.52 0.52 0.766C 0.26 0.24 0.36 0.32 0.291! 0.37 0.1 0.267 0.333 0.051 0.5 1.44 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.44 0.733 0.15 0.469 0.42 0.677 0.44 0.579 0.174 0.435 0.72 0.621 0.56 0.549 1.08 0.635 0.36 0.692 0.48 0.923 0.4172 0.6179 0.22 0.611 0.068 0.213 0.1223 0.3604 0.146 0.292 0.86 0.597 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 0.614 0.752 0.187 2.762 0.961 0.043 0.054 0.090 0.056 0.044 0.0112 0.035 0.024 0.039 0.034 0.045 0.034 0.034 0.05 0.125 0.022 0.019 0.024 0.019 0.03 0.029 0.028 0.016 0.0118 0.023 0.054 0.104 0.0296 0.0386 0.016 0.062 0.038 0.158 0.0144 0.040 0.026 0.081 0.0218 0.0750 1.326 0.089 0.241 0.269 0.727 1.056 0.076 0.760 0.02 0.200 1.224 0.061 0.228 0.197 0.738 1.261 0.077 0.231 0.238 0.715 0.927 0.005 0.098 0.04 0.784 0.022 0.044 F-4 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish whole 3 26 body freshwater crayfish GMEAN whole rreshwater-Lab 3 1 body tilapia whole Water Expsoure) 3 1 body tilapia whole 3 1 body tilapia GMEAN whole 3 3 body Japanese medaka whole 3 3 body Japanese medaka whole 3 3 body Japanese medaka whole 3 3 body Japanese medaka whole 3 3 body Japanese medaka GMEAN whole 3 4 body tilapia whole 3 4 body tilapia whole 3 4 body tilapia GMEAN whole 3 4 body tilapia whole 3 4 body tilapia whole 3 4 body tilapia GMEAN whole 3 4 body tilapia whole 3 4 body tilapia whole 3 4 body tilapia GMEAN whole 3 4 body tilapia whole 3 4 body tilapia whole 3 4 body tilapia Total As Ct mg/kg 0.44 0.82 0.76 0.722S 0.675 0.8 5.15 1 .406; 5.3 53.25 80.25 77.75 62.5 40.5811 0.85 1.9 2.8 1 .653* 5.15 3 3.075 3.621 1 0.625 2.475 3.025 1 .672* 0.475 1.775 5.25 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.3543 0.4176 0.15 0.222 0.0 0.074 0.15 0.187 0.1 0.094 2.025 0.393 1.8 0.359 0.3572 0.2540 0.1907 0.1 35( 1.375 0.259 1.6 0.292 38.25 0.718 11.5 0.216 41.5 0.517 36.2 0.452 34.25 0.441 41.5 0.534 27 0.432 32.5 0.520 1 8 2390 0 4494 1 5 41 89 0 380C 0.25 0.294 0.2 0.294 0.725 0.382 0.7 0.382 1.125 0.402 1.2 0.429 05886 03559 06014 03637 2.025 0.393 1.8 0.359 0.975 0.325 0.9 0.300 1.25 0.407 1.2 0.374 13514 03731 12418 0 342S 0.25 0.400 0.2 0.280 1.025 0.414 1.0 0.384 1.2 0.397 0.9 0.289 0.6750 0.4035 0.5259 0.314^ 0.95 0.181 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 0.0134 0.030 0.017 0.022 0.0171 0.0311 1.179 0.475 0.704 1.294 0.575 0.719 1.248 0.275 0.053 0.4 0.078 0.6 0.117 1.2391 0.2750 0.0534 0.4000 0.0777 0.5472 0.3891 1.598 1.225 0.231 0.6 0.113 0.55 0.104 1.066 2.500 0.047 1 0.019 0.781 1.750 0.022 0.75 0.009 0.026 2.000 0.026 1.048 2.000 0.032 0.875 0.014 0.125 0.002 05140 18460 00455 07329 00246 04097 00157 0.762 0.35 0.412 0.612 0.075 0.039 0.125 0.066 0.25 0.132 0.570 0.075 0.027 0.175 0.062 0.225 0.080 06427 00750 00325 01479 00641 02700 01633 1.248 0.275 0.053 0.4 0.078 0.6 0.117 1.350 0.150 0.050 0.275 0.092 0.7 0.233 0.870 0.025 0.008 0.25 0.081 0.4 0.130 11356 01010 00279 03018 00833 05518 01524 0.370 0.150 0.240 0.05 0.080 0.377 0.325 0.131 0.175 0.071 0.614 0.650 0.215 0.3 0.099 0.4408 0.3164 0.1892 0.1379 0.0825 1.475 0.15 0.316 0.325 0.684 2.775 0.625 0.352 1.15 0.648 5.119 1.8 0.343 2.5 0.476 F-5 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # GMEAN whole 3 31 body guppy whole 3 31 body guppy whole 3 31 body guppy GMEAN 3 32 muscle carp 3 32 muscle carp 3 32 muscle carp 3 32 muscle carp 3 32 muscle carp 3 32 muscle carp GMEAN whole :reshwater-Lab 3 1 body Tilapia Dietary Exposure - ab foodchain whole tiodel) 3 4 body Tilapia whole 3 1 body freshwater minnow whole 3 1 body freshwater minnow whole 3 3 body Japanese Medaka whole 3 31 body guppy whole 3 31 body guppy whole rreshwater-Field 4 40 body masu salmon Total As Ct mg/kg 1.641S 1.7 1.725 10 3.083S 0.95 1.5 1.45 1.8 2.85 3 1 .779S 6.65 6.75 0.55 0.4 12.5 0.925 1.4 0.146 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.9500 0.1810 1.25 0.735 1.45 0.841 7.65 0.765 0.7791 #NUM! #NUM! 0.9 0.947 1.25 0.833 1.15 0.793 1.5 0.833 1.75 0.614 1.775 0.592 1 .3491 0.7579 2.75 0.414 3.8 0.564 2.75 0.407 3 0.444 0.35 0.636 0.2 0.364 0.25 0.625 0.2 0.375 3.25 0.260 9.2 0.740 0.125 0.135 0.225 0.161 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 2.7569 0.5526 0.3366 0.9776 0.5954 0.565 0.150 0.088 0.025 0.015 0.275 0.162 0.409 0.025 0.014 0.05 0.029 0.2 0.116 1.110 1.480 0.148 0.175 0.017 0.7 0.070 0.6356 0.1771 0.0574 0.0603 0.0195 0.3377 0.1095 0.103 0.05 0.053 0.317 0.100 0.067 0.05 0.033 0.1 0.067 0.457 0.050 0.034 0.025 0.017 0.225 0.155 0.342 0.125 0.069 0.075 0.042 0.1 0.056 0.711 0.775 0.272 0.15 0.053 0.175 0.061 1.008 0.625 0.208 0.25 0.083 0.35 0.117 0.3922 0.1978 0.0980 0.0811 0.0402 0.1379 0.0775 0.173 0.15 0.023 0.25 0.037 0.287 1.665 0.8 0.865 2.014 0.025 0.018 1.15 0.821 1.130 0.063 0.432 0.081 0.555 F-6 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # Saltwater-Field 2 8 edible blue mussel 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam 2 27 edible dam GMEAN 2 27 edible cockle clam 2 27 edible littleneck clam 2 27 edible littleneck clam 2 27 edible littleneck clams 2 8 soft marine snail 2 8 soft marine snail 2 27 edible oyster 2 25 edible oysters whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes whole 2 20 body marine polychaetes Total As Ct mg/kg 1.022 1.9 2.3 2.9 4.2 3.2 8.4 4.2 2.2 12 2.8 2.1 3.4 2.3 3 3.344! 1.1 6.9 2.2 2.4 6.106 5.408 2.1 10 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.025 0.025 0.015 0.007 0.018 0.006 0.018 0.004 0.017 0.005 0.009 0.001 0.021 0.005 0.015 0.007 0.008 0.001 0.022 0.008 0.02 0.010 0.035 0.010 0.022 0.010 0.021 0.007 0.0178 0.0053 0.02 0.018 0.02 0.003 0.02 0.009 0.02 0.008 0.01 0.005 0.010 0.013 0.024 0.022 0.119 0.149 0.051 0.208 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 0.888 0.869 5.984 0.980 5.138 0.950 0.68 0.068 10.4 1.040 0.64 0.70 0.78 0.60 0.53 0.70 0.81 0.0127 1.22 0.0095 0.77 0.0206 0.66 0.0175 0.83 0.0222 F-7 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # whole 2 20 bodv marine polvchaetes Total As Ct mg/kg Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.211 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 0.58 0.0190 F-8 ------- APPENDIX F: TISSUE SPECIATION DATA Study Type Trophic Articl Tissue Common Name Level e # Saltwater-Field 3 27 edible sand dab 3 27 edible rock sole 3 27 edible red rock crab 3 2 edible gastropod Total As Ct mg/kg 4.5 17 3.6 46.6 Inorganilnorgani As (III) As (III) As (V) As (V) cAs c Ct Fraction Ct Fractior Ct As mg/kg mg/kg mg/kg Fraction 0.01 0.002 0.05 0.003 0.03 0.008 Organic MMA MMA DMA DMA TMA TMA AsB AsB AsC AsC As Ct Fraction Ct Fraction Ct Fraction Ct Fraction Ct Fraction Fraction mg/kg mg/kg mg/kg mg/kg mg/kg 44.7 0.959 F-9 ------- |