Report 601779002/2009 E.A.J. Bleeker | E.M.J. Verbruggen Bioaccumulation of polycyclic aromatic hydrocarbons in aquatic organisms RIVM report 601779002/2009 Bioaccumulation of polycyclic aromatic hydrocarbons in aquatic organisms E.A.J. Bleeker E.M.J. Verbruggen Contact: E.A.J. Bleeker Expertise Centre for Substances [email protected] This investigation has been performed by order and for the account of the Ministry of Housing, Spatial Planning and the Environment (VROM), within the framework of the project ‘Strategic research for REACH’ (M/601779) RIVM, P.O. Box 1, 3720 BA Bilthoven, the Netherlands Tel +31 30 274 91 11 www.rivm.nl © RIVM 2009 Parts of this publication may be reproduced, provided acknowledgement is given to the 'National Institute for Public Health and the Environment', along with the title and year of publication. 2 RIVM report 601779002 Abstract Bioaccumulation of polycyclic aromatic hydrocarbons in aquatic organisms RIVM has evaluated the available data on bioaccumulation of polycyclic aromatic hydrocarbons (PAHs) in aquatic organisms. As a result the categorisation of PAHs regarding their bioaccumulation potential was adapted. Phenanthrene and fluoranthene are now no longer considered ‘very bioaccumulative’ in fish, but ‘bioaccumulative’. The level of accumulation of compounds in organisms (bioaccumulation) is an important criterion in chemicals regulation. It gives an indication that higher in the food chain higher concentrations of a compound are found that may become harmful. Data on individual PAHs, including data on bioaccumulation, are used in risk assessment of (mixtures of) compounds in which PAHs are major components, e.g. oil and oil compounds. As measure for accumulation the bioconcentration factor (BCF) of a compound is used. This is defined as the ratio between the uptake rate of a compound from water into the organism and its elimination rate to water. In the European REACH legislation compounds are divided over three BCF categories: not bioaccumulative (BCF is below 2000), bioaccumulative (BCF is between 2000 and 5000) and very bioaccumulative (BCF is above 5000). Fish are capable of transforming PAHs into compounds that are better soluble in water, which facilitates elimination. This results in lower measured BCF values in fish. Mussels and other invertebrates are much less capable of PAH transformation, which results in higher accumulation of PAHs in these organisms. Key words: bioaccumulation, polycyclic aromatic hydrocarbons (PAHs), risk assessment RIVM report 601779002 3 Rapport in het kort Bioaccumulatie van polycyclische aromatische koolwaterstoffen in waterorganismen Het RIVM heeft beschikbare gegevens over ophopingen van polycyclische aromatische koolwaterstoffen (PAK’s) in waterorganismen geëvalueerd. Naar aanleiding hiervan is de indeling van deze stoffen voor regelgeving aangepast. Fenantreen en fluoranteen worden nu niet meer als ‘zeer bioaccumulerend’ beschouwd in vis, maar als ‘bioaccumulerend’. De mate waarin stoffen in organismen ophopen (bioaccumulatie) is een belangrijk criterium voor regelgeving. Het is een indicatie dat hoger in de voedselketen hogere concentraties van de stof worden aangetroffen die schadelijk kunnen zijn. Gegevens van individuele PAK’s, waaronder bioaccumulatiegegevens, worden gebruikt voor de risicobeoordeling van stoffen(mengsels) waarin PAK’s een belangrijk bestanddeel zijn, zoals bijvoorbeeld olie en olieachtige stoffen. Als maat voor de ophoping wordt de bioconcentratiefactor (BCF) van een stof gebruikt. Dat is de ratio tussen de snelheid waarmee het organisme de stof vanuit water opneemt en de snelheid waarmee het naar water wordt uitgescheiden. Op grond hiervan worden stoffen in de Europese REACH-regelgeving ingedeeld in drie categorieën: niet bioaccumulerend (de BCF is kleiner dan 2000), bioaccumulerend (de BCF ligt tussen 2000 en 5000) en zeer bioaccumulerend (de BCF is hoger dan 5000). Vissen zijn in staat om PAK’s om te zetten in stoffen die beter in water oplosbaar zijn waardoor ze makkelijker kunnen worden uitgescheiden. Hierdoor worden in vissen vaak lagere BCF-waarden gemeten. Mosselen en andere ongewervelden kunnen PAK’s veel minder goed omzetten waardoor PAK’s in deze organismen meer ophopen. Trefwoorden: bioaccumulatie, polycyclische aromatische koolwaterstoffen (PAK’s), risicobeoordeling 4 RIVM report 601779002 Contents Summary 7 1 Introduction 9 2 Methods 11 3 Results 13 3.1 3.2 3.3 Reliability of reported BCF values Additional data Evaluation of reliable BCF values 13 13 15 4 Discussion 21 4.1 4.2 4.3 4.4 Evaluating the bioaccumulation assessment by Lampi and Parkerton Evaluating the bioaccumulation assessment in the RAR Dietary bioaccumulation studies Using bioaccumulation data for regulatory purposes 21 23 24 25 References 29 Annex I Overview of BCF values from studies that were rated as not reliable (validity 3) 37 Annex II Overview of BCF values from studies for which validity was not assignable (validity 4) 47 RIVM report 601779002 5 6 RIVM report 601779002 Summary In risk assessment the potential of a substance to accumulate in a food web is an important criterion. Bioaccumulation may result in increasing internal concentrations in organisms higher in the food chain and then it is called biomagnification. Whether this process of biomagnification actually takes place depends on the properties of the compound itself (e.g. stability, lipophilicity) and on the organisms in the food chain (ability to metabolize and/or excrete the compound). This may result in situations where at lower trophic levels bioaccumulation and biomagnification take place, while higher in the food chain organisms are capable of handling the compound and efficiently excreting it. In the present report and in agreement with regulatory frameworks, therefore, bioaccumulation data on fish (higher in the food chain) and other aquatic organisms (lower in the food chain) are evaluated. These organisms include, but are not restricted to molluscs, crustaceans, insects, oligochaetes and polychaetes. As a measure for bioaccumulation usually the bioconcentration factor (BCF) is used as a trigger. The BCF is defined as the ratio between uptake and depuration rates, which in a steady state situation equals the ratio between the internal concentration in an organism and the concentration in water. Since this ratio not only depends on compound properties and test organisms, but also on the test setup used, quality criteria for testing and reporting bioconcentration have been debated. Using such criteria in the present report reliabilities of reported BCF values for polycyclic aromatic hydrocarbons (PAHs) in aquatic organisms are evaluated, focussing on the 16 PAHs defined as priority substances by the United States Environmental Protection Agency (naphthalene, acenaphthene, acenaphthylene, 9H-fluorene, anthracene, phenanthrene, fluoranthene, pyrene, benz[a]anthracene, chrysene, benzo[a]pyrene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[ghi]perylene, dibenz[a,h]anthracene, and indeno[1,2,3-cd]pyrene). Based on existing databases and reviews, as well as a search in the recent literature, 133 original papers were examined to evaluate the reliability of 855 BCF values. Only about 34% of these values were deemed reliable (in many cases with restrictions), but another 40% were deemed not assignable (due to lack of information in the report). As part of the present study the (re-)evaluated BCFs are compared with previous evaluations of BCF studies and differences in opinion are discussed. Also the role of dietary uptake is discussed but it is concluded that at present not enough data are available to use and compare bioaccumulation data from dietary studies with those from aqueous tests. Finally the evaluation is summarized and conclusions on bioaccumulation potential for each of the 16 PAHs are given, applying the triggers as used in the EU-legislation REACH: compounds are considered as bioaccumulative (B) when their BCF is between 2000 and 5000 and very bioaccumulative (vB) when the BCF is >5000. Naphthalene, acenaphthene, acenaphthylene and 9Hfluorene are considered not bioaccumulative. Anthracene, phenanthrene and fluoranthene are considered B for fish, but they are vB at lower trophic levels (molluscs, crustaceans). Pyrene, benz[a]anthracene and benzo[a]pyrene do not accumulate in fish (due to biotransformation), but are vB at lower trophic levels. For chrysene, benzo[k]fluoranthene, benzo[ghi]perylene, and dibenz[a,h]anthracene only reliable data on daphnids are available which deem these compounds as vB. For benzo[b]fluoranthene and indeno[1,2,3-cd]pyrene no reliable data are available at all, so bioaccumulative potential could not be established. RIVM report 601779002 7 8 RIVM report 601779002 1 Introduction In risk assessment the degree of bioaccumulation of a compound is an important criterion. This is based on the assumption that compounds that accumulate in organisms can accumulate in a food web, resulting in higher internal concentrations in organisms higher in the food chain. This process is known as biomagnification. Whether biomagnification will actually take place depends on the physicochemical properties of the compound (e.g. stability, lipophilicity) and on the organism(s) that take up the compound (ability to metabolize and/or excrete the compound) (Gobas et al., 2009). This may result in situations where at lower trophic levels bioaccumulation and biomagnification takes place, while higher in the food chain organisms are capable of handling the compound and efficiently excreting it (e.g. Wang and Wang, 2006; Wan et al., 2007; Nfon et al., 2008; Takeuchi et al., 2009). Nevertheless, specifically this metabolization may activate the toxicity of some compounds. For regulatory purposes the process of biomagnification is often simplified by assessing the bioaccumulation, especially in fish. According to the European REACH 1 legislation, however, ‘the assessment of bioaccumulation shall be based on measured data on bioconcentration in aquatic species’ (EU, 2007). Also in other frameworks (e.g. Stockholm Convention, 2001) assessment of bioaccumulation is not restricted to fish, so in this report bioaccumulation data on other aquatic organisms are evaluated as well. In aquatic tests the degree of bioaccumulation is usually expressed as a bioconcentration factor (BCF), defined as the ratio between uptake from water into an organism and elimination from an organism to water. In a steady state situation this ratio is independent of time and then it equals the ratio between the concentration in the organism and the concentration in water. The BCF is used as a trigger for bioaccumulation in several regulatory frameworks (e.g. REACH, OSPAR 2 , GHS 3 ), but the trigger values in these frameworks may differ. In this report we focus on the triggers defined in REACH: a compound is defined as bioaccumulative (B) when the wet-weight BCF value (normalized to lipid content) is higher than 2000 and as very bioaccumulative (vB) if this value is higher than 5000. Lipid normalization is applied when bioaccumulating compounds tend to accumulate in the lipids of organisms (ECHA, 2008), resulting in higher BCF values for organisms with higher lipid content. To enable comparison between species BCF values are normalized to an organism that contains 5% lipids, the average value for the small fish species used in OECD guideline 305 (OECD, 1996; Tolls et al., 2000). The degree of bioaccumulation of compounds depends on several factors. First of all, it depends on the compound tested and its properties as well as the test species used, but in addition several test conditions have an influence, e.g. the time of exposure, the type of exposure (static vs. continuous flow), etc. To minimize variation between tests guidelines were developed in which test conditions were described (e.g. OECD, 1996). Still comparisons between bioaccumulation studies are difficult, because quite a few data were generated before guidelines were established. In addition, in some cases not all relevant details on the test setup are described. This has lead to a debate to come to quality criteria for BCF values (e.g. Parkerton et al., 2008), as this is seen as essential in getting a clearer picture on the possibility of predicting BCF values from physicochemical properties of compounds. The present report gives an evaluation of reported BCF values for polycyclic aromatic hydrocarbons (PAHs) in aquatic organisms. By examining the studies in detail the reliability of reported values is 1 2 3 REACH: Registration, Evaluation, Authorisation and restriction of CHemicals. OSPAR: OSlo and PARis conventions (OSPAR, 1992). GHS: Global Harmonizing System of classification and labelling of chemicals. RIVM report 601779002 9 examined. The study was limited to the 16 PAHs defined as priority substances by the United States Environmental Protection Agency (US EPA; http://www.epa.gov/waterscience/methods/pollutants.htm; further indicated as EPA-PAHs, Figure 1 naphthalene acenaphthene acenaphthylene 9H-fluorene anthracene phenanthrene fluoranthene pyrene benz[a]anthracene chrysene benzo[a]pyrene benzo[b]fluoranthene benzo[k]fluoranthene benzo[ghi]perylene dibenz[a,h]anthracene indeno[1,2,3-cd]pyrene Figure 1: Structural formulae of the 16 polycyclic aromatic hydrocarbons defined as priority substances by the United States Environmental Protection Agency. 10 RIVM report 601779002 2 Methods In collecting reported BCF values the following sources were used to create an overview. − The Ecotoxicology Database (ECOTOX) of the US EPA. This database is a source for locating single chemical toxicity data for aquatic life, terrestrial plants and wildlife. ECOTOX was created and is maintained by the US EPA, Office of Research and Development (ORD), and the National Health and Environmental Effects Research Laboratory’s (NHEERL’s) Mid-Continent Ecology Division (MED). It is publicly available at the internet (http://cfpub.epa.gov/ecotox/). − The bioconcentration Gold Standard Database of (EURAS). This database was established in 2006 Research Initiative. Cefic is de European Chemical chemical industry. The database is linked to http://ambit.acad.bg. the European Academy of Standardization in the framework of the Cefic Long-range Industry Council, representing the European the AMBIT database and available at − The database of the Japanese National Institute of Technology and Evaluation. The Chemical Management Field of this institute aims at collecting and transmitting information required for total risk assessment and management of chemical substances. Their Biodegradation and Bioconcentration database is available in English at http://www.safe.nite.go.jp/english/kizon/ KIZON_start_hazkizon.html. Test details are published in the Official Bulletin of Economy, Trade and Industry (in Japanese only). − The EU risk assessment report (RAR) that was produced in the framework of EU regulation EEC/793/93 (EU, 1993) for coal-tar pitch and copied into an Annex XV Transitional Dossier under REACH (The Netherlands, 2008). The risk assessment of coal-tar pitch is based on data for the 16 EPA-PAHs (Figure 1). This report includes an overview of bioconcentration factors for fish and mussels, as well as for oligochaetes, polychaetes, crustaceans and insects. − The database of 1535 data points for 702 chemicals in fish as summarized in the supplementary information for the paper by Arnot et al. (2008). In this paper measured bioconcentration values are compared with values estimated by several quantitative structure-activity relationships (QSARs). − An assessment of the bioaccumulation data of the 16 EPA-PAHs for fish by Lampi and Parkerton (2008). This document complements the review in the EU risk assessment for coal-tar pitch and identifies preferred values for the PBT 4 Working Group of the Technical Committee New and Existing Substances. In 2009 an update of this document (Lampi and Parkerton, 2009) was provided to the European Chemicals Agency (ECHA) in a reaction to their proposal to include coal-tar pitch high temperature on the list of compounds for which authorisation is needed. − Finally recent or additional literature was scanned in Scopus (http://www.scopus.com) for each individual PAH (identified by substance name or CAS registration number) using the following keywords: bioconcentrat*, bioaccumulat*, uptake, depuration, food-web, trophic, biomagnificat*, BCF*, BAF*, FWMF*, TMF*, BMF*, or BSAF*. Information from these sources showed considerable overlap, but eventually the data collection resulted in a list of 855 BCF values, reported in 133 references. With a few exceptions (see below), each of these references were consulted individually and the reliability of reported BCF values was examined by using similar criteria as those formulated by Parkerton et al. (2008). These criteria are: 1. 2. 3. 4. 4 (details of) test compound and test organism are clearly described the compound is analysed both in water and in the organism no significant adverse effects are reported the reported BCF reflects steady-state conditions with unambiguous units Persistent, Bioaccumulating and Toxic compounds. RIVM report 601779002 11 However, due to different interpretation of the results, the assessment of the studies is not necessarily the same as in the assessment recently submitted to ECHA (Lampi and Parkerton, 2009). Based on this analysis Klimisch scores (Klimisch et al., 1997) were assigned to each BCF value to indicate the reliability. Data that are generated from studies that comply with or are comparable to published guidelines or are conducted with accepted methods that are described in sufficient detail are rated reliable (validity = 1). Studies that include adequate documentation details, but lack specific details or deviate from guideline requirements are deemed reliable with restrictions (validity = 2). Data are rated as unreliable if key information is lacking or when documentation details reveal unacceptable test performance or methodological flaws (validity = 3). The most common reasons for unreliability are exposure concentrations above water solubility and a clear absence of steady state while steady state BCFs are reported. When insufficient details are provided on critical study aspects data are defined as not assignable (validity = 4). Reasons for assigning a validity of 4 include BCF values being based on total radioactivity (which deems it impossible to distinguish between the concentration of the parent compound and that of its transformation products), uncertainty about the exposure concentration (e.g. exposure concentration reported in graphs only, nominal concentration reported only, exposure via sediment or diet, exposure to oil) or (pre-)exposure duration (e.g. for field collected animals). In addition, two studies (Dunn and Stich, 1976; Rantamäki, 1997) that reported depuration half-lives were scored as not assignable, because information was lacking to calculate BCF values from these half-lives (validity = 4). In addition to these 4 scores to indicate reliability we added the score 5 for BCF values that were reported in one of our sources (see above), but for which the original publication could not be evaluated. For instance, a small number of references (US-EPA, 1976; Linder, 1982; Hall, 1993) could not be traced and BCF values from these references (as reported in the ECOTOX-database) were assigned a validity of 5 (not evaluated). In addition Veith et al. (1979) refer to unpublished data by Call and Brook (1977). As such data are by definition untraceable this reference was also assigned a validity of 5. It is, however, possible that (part of) these unevaluated data were reported in public literature as well. In the assessment by Lampi and Parkerton (2009) several references are made to reports by EMBSI (EMBSI, 2001; 2005; 2006; 2007c; 2007b; 2007a; 2008a; 2008b; 2009). These reports are not publicly available and thus the BCF values of these references were also assigned a validity of 5. 12 RIVM report 601779002 3 Results 3.1 Reliability of reported BCF values For almost 40% of the reported BCF values reliability could not be assigned (validity = 4; see Annex II). The main reason for assigning this validity is given for each BCF value as a reliability remark in Annex II. For the majority of unassignable BCF values this was the result of the BCF being based on total radioactivity. Those BCF values that were assigned not reliable (invalid due to experimental flaws or design limitations; validity 3) are summarized in Annex I. This was about 25 % of the BCF values. The main reasons for deeming the study unreliable are given as reliability remark in Annex I. Only 293 BCF values (circa 34 %) were deemed reliable, although in many cases (264) with restrictions (i.e. non-guideline studies, but documented and defensible, validity = 2), because many of these studies were performed before guidelines were established. These 293 BCF values were derived for different types of organisms and are summarized in Table 1. The remaining few BCF values were not evaluated. 3.2 Additional data Most of the data (re-)evaluated in the present study were already described in the RAR 5 (The Netherlands, 2008). Additional studies are briefly described here. Landrum and Poore (1988) determined the role of lipid content and temperature in the bioaccumulation of phenanthrene and benzo[a]pyrene by mayfly (Hexagenia limbata). The values for benzo[a]pyrene were reported already in the RAR, but those for phenanthrene were not. The study report includes enough details to rate this study reliable with restrictions (validity = 2). In Table 1 the range of BCF values given from this study is based on fresh weight. When lipid normalization (to 5% lipid content) is applied the range for phenanthrene yields 666 – 2600 L/kg and for benzo[a]pyrene this range yields 3400 – 7800 L/kg. Hall and Oris (1991) determined BCFs for male and female fathead minnows and for eggs of this species exposed to a concentration series of anthracene for 21 d. Steady water concentrations were maintained, but lipid content was not presented. BCFs were calculated for male and female carcasses individually, and is rated reliable with restrictions (validity = 2). Weinstein (2001) exposed glochidia of Utterbackia imbecillis to fluoranthene in a flow-through system. Both a steady state (1735) and a kinetic BCF value (1813) is given, which are very similar. This is in agreement with the observed steady state. Also further details provided in the study report are sufficient to rate this study as valid with restrictions (validity = 2). Schuler et al. (2004) exposed crustacean species (Diporeia spec. and Hyalella azteca) and insect larvae (3rd instar Chironomus tentans) to fluoranthene to determine the influence of exposure concentration on bioaccumulation and compare species specific differences. The study report provides sufficient detail to 5 RAR: Risk Assessment Report, produced in the framework of EU regulation EEC/793/93 (EU, 1993). RIVM report 601779002 13 rate this study as valid with restrictions (validity = 2). The exposure concentration appears not to have a big influence, but in contrast to Diporeia spec. the other species are able to metabolise fluoranthene, resulting in higher elimination rates and lower BCF values. Richardson et al. (2005) conducted semi-batch seawater experiments to follow the uptake and release of anthracene, fluoranthene, pyrene and benzo[a]pyrene, as well as 4 organochlorine pesticides, in semi-permeable membrane devices and green-lipped mussels (Perna viridis). This study was well conducted and appears to yield reliable BCF values based on lipid weight (anthracene: 380000; fluoranthene: 245000; pyrene: 891000; benzo[a]pyrene: 170000). Normalised to a 5% lipid content (ECHA, 2008), these BCF are 19000, 12250, 44550, and 8500, respectively. Lipid weight itself was not given in the study. This study is rated as reliable with restriction (validity = 2). Wang and Wang (2006) studied the bioaccumulation and transfer of benzo[a]pyrene in a simplified marine food chain. Both dietary and aqueous exposure to benzo[a]pyrene were examined in copepods (Acartia erythraea) and fish (Lutjanus argentimaculatus), but details are not always clear deeming this study unassignable (validity = 4). Yakata et al. (2006) tested seven organic compounds including acenaphthylene in carp (Cyprinus carpio). The tests were conducted according to OECD Guideline 305 (OECD, 1996), resulting in a BCF for acenaphthylene of 271 L/kg (560 after lipid normalization). Sufficient details were provide to rate this guideline study as reliable (validity = 1). Jonker and Van der Heijden (2007) determined BCF values for Lumbriculus variegatus in several different test setups. These studies were, however, deemed unreliable (validity = 3), because sediment was present in the test (adding uncertainties to the exposure route) and BCF values were given in graphs only. In a study by Cheikyula et al. (2008) fish (Paralichthys olivaceus, Pagrus major and Oryzias javanicus) were exposed for ten days to a mixture of 4 PAHs (phenanthrene, pyrene, chrysene and benzo[a]pyrene). The exposure concentration of chrysene in this study appeared to be above the water solubility of this compound, and consequently the mixture as a whole must be oversaturated. So BCF values from this study are not reliable (validity = 3). Bioavailability of benzo[k]fluoranthene was reported for Oryzias latipes by Chen et al. (2008). From this study a BCF value could only be estimated from concentrations in water and fish that were reported in graphs. In addition the reported exposure concentrations appear to be nominal concentrations (validity = 3). Grass shrimp larvae were exposed to fluoranthene and benzo[a]pyrene by Weinstein and Garner (2008). The reported BCF values were averages for several exposure concentrations, but information is lacking to examine the validity of this procedure. In addition, BCF values appear to be based on dry weight and the exposure concentration for benzo[a]pyrene appears to be above water solubility (validity = 3). A rather reliable study in estuarine copepods (Cailleaud et al., 2009), reports dry weight based BCF values for phenanthrene (550), pyrene (900), chrysene (950), benzo(b+k)fluoranthene (1300), and benzo[a]pyrene (1750). These values are only reported in a graph deeming this study as reliable with restrictions (validity = 2). Since no distinction was made between benzo[b]fluoranthene and benzo[k]fluoranthene the value for benzo(b+k)fluoranthene is rated as unassignable (validity 4). In a study by Takeuchi et al. (2009) biomagnification profiles were elucidated for a range of PAHs, alkylphenols and polychlorinated biphenyls. The molluscs, crustaceans and fish that were examined were collected in the Tokyo Bay, which makes the actual exposure concentrations uncertain (although measured water concentrations were given). However, the reported concentrations in seawater and the 14 RIVM report 601779002 organisms can be used to calculate bioaccumulation values (BAFs) and thus this study is rated reliable with restrictions (validity = 2). In general 5% lipid normalized BAF values for all species tested are >5000 L/kg for anthracene, fluoranthene, pyrene, benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo(j+k)fluoranthene, benzo[a]pyrene, indeno[1,2,3-cd]pyrene, and benzo[ghi]perylene, with a few exceptions: in the fish (Acanthogobius flavimanus) BAF values are lower for anthracene (4527), fluoranthene (629), pyrene (1010), and indeno[1,2,3-cd]pyrene (4167), and in the crustacean (Hemigrapsus penicillatus) BAF values are lower for anthracene (4026) and fluoranthene (1713). For phenanthrene the values fall within the 2000 – 5000 L/kg range, with the mollusc Mytilopsis sallei (BAF: 1781), the crustacean (BAF: 776) and the fish (BAF: 1019) as exceptions. Because these values cannot be directly compared with BCF values, the BAF values are not included in Table 1. 3.3 Evaluation of reliable BCF values From Table 1 it can be concluded that BCF values are low for naphthalene (in fish: 66 – 999 L/kg; in crustaceans: 131 – 736 L/kg), acenaphthene (in fish: 735 – 760 L/kg), acenaphthylene (in fish: 271 – 387 L/kg) and 9H-fluorene (in fish: 590 – 1467 L/kg; in Daphnia magna: 506 L/kg; in Lumbriculus variegatus: 400 L/kg). In aquatic plants (Lemna gibba) this holds for all PAHs tested (anthracene: 4 – 28 L/kg; phenanthrene: 11 – 92 L/kg; benzo[a]pyrene: 7 – 910 L/kg). Also polychaetes (Nereis virens) do not highly accumulate the PAHs tested (BCF values for phenanthrene, fluoranthene and pyrene are all below 1000 L/kg). Anthracene is clearly accumulated. Both for carp (Cyprinus caprio) and for fathead minnows (Pimephales promelas) BCF values are reported above 2000 L/kg. For female fathead minnows, the highest BCF (4973 L/kg) is even close to the very bioaccumulative (vB) limit of 5000 L/kg. Hall and Oris (1991) argue that this may be due to a higher lipid content in females, but unfortunately they did not measure lipid content in the fish. The only study that reports lipid content in Pimephales promelas (Carlson et al., 1979) does not distinguish between males and females, but their highest reported lipid content value is 4.8 ± 1.5 % (average ± SD). Assuming that the females are in the higher region of this range (i.e. around 6%), the lipid normalized BCF value will be around 4100. For the amphipod Pontoporeia hoyi the BCF is (far) above this limit (16800 – 40000 L/kg) and also the polychaete Stylodrilus heringianus show a high BCF value for anthracene (5206 L/kg). For phenanthrene BCF values are reported above 2000 L/kg for sheepshead minnows (Cyprinodon variegatus; 2229 L/kg) and fathead minnows (Pimephales promelas; BCFK: 3611 L/kg). For both species also values below 2000 L/kg are reported, but for fathead minnows also a final BCF value of 5100 L/kg is reported on day 28, although concentrations in fish appear to decrease over the period from day 18 to 28 of the uptake phase. In molluscs phenanthrene is accumulating, but BCF levels remain well below 2000 L/kg (maximum: 1280 L/kg). In crustaceans BCF values are generally very high (cf. Diporeia spp. and Pontoporeia hoyi >5000 L/kg), but low values are also reported (cf. Daphnia sp. and Crangon septemspinosa: 210 – 325 L/kg). Whether these differences are due to differences between species is difficult to judge, since other experimental settings (e.g. exposure time) also differ. For insects (Hexagenia limbata) BCFs clearly depend on lipid content of the organism, but on average values are above 2000 L/kg. For oligochaetes (Stylodrilus heringianus) the BCF for phenanthrene is 5222 L/kg. Fluoranthene does accumulate in fish (Pimephales promelas; kinetic BCF calculated from the presented data: 2439). The uptake curve does not fit well to a first order kinetic model. This is mainly because the concentrations in fish are remarkably lower at 28 days than at 4, 7, 14, and 21 days. Static RIVM report 601779002 15 BCF values at these time intervals are 2275, 3265, 2962, and 3443, respectively. In contrast, the static BCF at 28 days is only 1507 – 1884. In juvenile fish, fluoranthene accumulation may be significant, e.g. Cho et al. (2003) reported a kinetic BCF of 14839, although exposure in this experiment was very short (24 h, followed by 24 h depuration phase) and the value may be based on dry weight (study validity = 4). In molluscs (Mya arenaria and Mytilus edulis) fluoranthene is clearly accumulating and also in some crustaceans (Diporeia spp. and Hyalella azteca) fluoranthene shows very high BCF values. The low BCF value for Crangon septemspinosa is likely species specific, since this species generally shows lower BCF values in comparison with other invertebrates (cf. McLeese and Burridge, 1987). For insects (Chironomus tentans larvae) BCF values for fluoranthene are around 2000 L/kg. Fluoranthene is also the only PAH tested on an amphibian (Rana pipiens), but for this species BCF values are (far) below 2000 L/kg. Based on Table 1 BCF values for pyrene in fish are lower than 2000, most likely because it is metabolized and subsequently excreted. For a study with fathead minnows (Carlson et al., 1979) the BCFK was estimated as 1279 L/kg. As with fluoranthene, however, these data appear to deviate from first order kinetics. The concentrations in fish after 28 d are much lower than those after 14 or 21 days, resulting a much lower BCFss after 28 d (785 L/kg) than the ones reported after 14 and 21 days (2300 and 2600 L/kg respectively). Yet, in a recent field study (Takeuchi et al., 2009) pyrene was not highly accumulating (BAF: 1010), supporting the non-bioaccumulative behaviour of pyrene in fish. Also insects (Chironomus riparius larvae) do not highly accumulate pyrene (Wildi et al., 1994). In molluscs, however, BCF values are generally (far) above 5000 L/kg, which is only partly due to their relatively high lipid content (cf. Bruner et al., 1994; Baussant et al., 2001a). In crustaceans (Diporeia spp., Pontoporeia hoyi) BCF values are also very high. Only Cragon septemspinosa shows again a low BCF value (see also the results for fluoranthene). The oligochaete Stylodrilus heringianus shows a very high BCF for pyrene (6688), but for Lumbriculus variegatus the BCF is much lower (1720). Benz[a]anthracene hardly accumulates in fish (Pimephales promelas) but in crustaceans BCF values are very high (>10000). Benzo[a]pyrene shows similar patterns with fish hardly accumulating and invertebrates that do so significantly, with the exception of Chironomus riparius that is capable of metabolizing benzo[a]pyrene (Leversee et al., 1981; 1982). For chrysene, benzo[k]fluoranthene, benzo[ghi]perylene and dibenz[a,h]anthracene only for Daphnia magna valid data are available, showing very high BCF values for all compounds. For benzo[b]fluoranthene and indeno[1,2,3-cd]pyrene no reliable data are available at all, although these compounds appear to accumulate in molluscs in the field (Takeuchi et al., 2009). Table 1. Overview of reliable BCF values. Species Test Systema) Chem. analysisb) BCF (L/kg) c) Type Vd) Ref.e) Naphthalene 16 Pisces Cyprinodon variegatus Cyprinus carpio Lepomis macrochirus FT FT FT GCMS GC 14 C 895, 999 1) 66, 76 1) 300 Kin. Equi. Kin. 1 2 2 [12] [26] [20] Crustacea Daphnia pulex Diporeia spp. S SR Flu.Spec. 14 C 131 311, 459, 736 1) Equi. Kin. 2 2 [31] [15] RIVM report 601779002 Species Test Systema) Chem. analysisb) BCF (L/kg) c) Type Vd) Ref.e) Acenaphthene Pisces Cyprinus carpio FT HPLC 735, 760 1) Equi. 2 [27] FT FT HPLC HPLC 385, 387 1) 271 Equi. Equi. 2 1 [28] [34] Pisces Cyprinus carpio Pimephales promelas FT FT GCMS HPLC 590, 637 1) 1112, 1459 1) Equi. Kin. 2 2 [29] [4] Crustacea Daphnia magna SR HPLC 506 Equi. 2 [23] Oligochaeta Lumbriculus variegatus SR HPLC 400 Equi. 2 [1] FT GCMS [25] HPLC HPLC HPLC Equi. Kin. Equi. Equi. Equi. 2 FT FT FT 1890, 2225 1) 2545, 1960 2) 563 – 966 1) 1126, 2476 1) 3581, 4973 1) 2 2 2 [10] [10] [10] SR GC 19000 3) Equi. 2 [24] SR S FT FT FT HPLC Flu.Spec. 14 C 14 C 14 C 970 917 1800 16800 39727 Equi. Equi. Equi. Kin. Kin. 2 2 2 2 1 [23] [31] [14] [16] [17] Oligochaeta Lumbriculus variegatus Stylodrilus heringianus SR FT HPLC 14 C 1370 5206 Equi. Kin. 2 2 [1] [8] Magnoliophyta Lemna gibba S 14 4 – 28 1) Kin. 2 [6] Pisces Cyprinodon variegatus Pimephales promelas FT FT GCMS HPLC 810, 2229 1) 2050 – 5100 1) 4) 2086 – 3611 Kin. Equi. Kin. 1 2 2 [12] [4] Mollusca Mya arenaria Mytilus edulis FT FT HPLC HPLC 1280 1240 Kin. Kin. 1 1 [21] [21] Acenaphthylene Pisces Cyprinus carpio 9H-fluorene Anthracene Pisces Cyprinus carpio Pimephales promelas (eggs) Pimephales promelas (male) Pimephales promelas (female) Mollusca Perna viridis Crustacea Daphnia magna Daphnia pulex Hyalella azteca Pontoporeia hoyi C Phenanthrene RIVM report 601779002 17 Species Crustacea Crangon septemspinosa Daphnia magna Daphnia pulex Diporeia spp. Eurytemora affinis Pontoporeia hoyi Test Systema) FT SR S SR FT Chem. analysisb) BCF (L/kg) c) Type Vd) Ref.e) HPLC HPLC Flu.Spec. 14 C GCMS 14 C 210 324 325 5513 – 11440 1) 550 5) 28043 Kin. Equi. Equi. Kin. Equi. Kin. 1 2 2 2 2 1 [21] [23] [31] [15] [3] [17] Insecta Hexagenia limbata FT 14 C 493 – 5697 6) Kin. 2 [13] Oligochaeta Stylodrilus heringianus FT 14 C 5222 Kin. 2 [8] Polychaeta Nereis virens FT HPLC 500 Kin. 1 [21] Magnoliophyta Lemna gibba S 14 11 – 92 1) Kin. 2 [6] Pisces Pimephales promelas FT HPLC 2439 Equi. 2 [4] Mollusca Mya arenaria Mytilus edulis Perna viridis Utterbackia imbecillis (glochidia) FT FT SR FT HPLC HPLC GC HPLC 4120 5920 12250 3) 1735, 1813 Kin. Kin. Equi. Equi., Kin. 1 1 2 2 [21] [21] [24] [32] Crustacea Crangon septemspinosa Daphnia magna Diporeia spp. Hyalella azteca FT SR SR SR HPLC HPLC 14 C 14 C 180 1742 15136 – 58884 1) 1202 – 5370 1) Kin. Equi. Kin. Kin. 1 2 2 2 [21] [23] [30] [30] SR 14 891 – 2512 1) Kin. 2 [30] Polychaeta Nereis virens FT HPLC 720 Kin. 1 [21] Amphibia Rana pipiens FT HPLC 611 – 1659 1) Equi. 1 [22] FT FT GCMS HPLC 97, 145 1) 1297 Kin. Kin. 1 2 [12] [4] S S FT FT SR 3 13000 – 35000 6) 22000 – 77000 7) 6430 4430 44550 3) Kin. Kin. Kin. Kin. Equi. 2 2 1 1 2 [2] [9] [21] [21] [24] C Fluoranthene Insecta Chironomus tentans rd (3 instar larvae) C Pyrene Pisces Cyprinodon variegatus Pimephales promelas Mollusca Dreissena polymorpha Mya arenaria Mytilus edulis Perna viridis 18 H H HPLC HPLC GC 3 RIVM report 601779002 Species Crustacea Crangon septemspinosa Daphnia magna Daphnia pulex Diporeia spp. Eurytemora affinis Pontoporeia hoyi Test Systema) FT SR S SR FT Chem. analysisb) BCF (L/kg) c) Type Vd) Ref.e) HPLC HPLC Flu.Spec. 14 C GCMS 3 H 225 2702 2702 12300 – 36333 1) 900 5) 166000 Kin. Equi. Equi. Kin. Equi. Kin. 1 2 2 2 2 1 [21] [23] [31] [15] [3] [17] 713 – 1227 8) Equi. 2 [33] Insecta Chironomus riparius (larvae) S 14 Oligochaeta Lumbriculus variegatus Stylodrilus heringianus SR FT HPLC 3 H 1720 6688 Equi. Kin. 2 2 [1] [8] Polychaeta Nereis virens FT HPLC 700 Kin. 1 [21] Pisces Pimephales promelas FT HPLC 260 Equi. 2 [5] Crustacea Daphnia magna Daphnia pulex Pontoporeia hoyi SR S FT HPLC Flu.Spec. 14 C 10226 10109 63000 Equi. Equi. Kin. 2 2 1 [23] [31] [17] SR HPLC GCMS 6088 950 5) Equi. Equi. 2 2 [23] [3] FT FT 14 367 – 608 9) 30 Kin. Kin. 2 2 [11] [20] S S SR 3 3 H H GC 41000 – 84000 6) 24000 – 273000 7) 8500 3) Kin. Kin. Equi. 2 2 2 [2] [9] [24] SR S HPLC 14 C GCMS 3 H 14 C 3 H 12761 2837 1750 5) 8496 73000 48582 Equi. Equi. Equi. Kin. Kin. Kin. 2 2 2 2 1 2 [23] [18] [3] [7] [17] [7] S 14 650 Equi. 2 [19] S FT 14 166 2725 – 11167 6) Equi. Kin. 2 2 [18] [13] C Benz[a]anthracene Chrysene Crustacea Daphnia magna Eurytemora affinis Benzo[a]pyrene Pisces Lepomis macrochirus Mollusca Dreissena polymorpha Perna viridis Crustacea Daphnia magna Eurytemora affinis Mysis relicta Pontoporeia hoyi Insecta Chironomus riparius th (4 instar larvae) Hexagenia limbata RIVM report 601779002 FT FT FT 14 3 C C C C H 19 Species Test Systema) Chem. analysisb) Oligochaeta Stylodrilus heringianus FT 3 Magnoliophyta Lemna gibba S 14 SR H BCF (L/kg) c) Type Vd) Ref.e) 7317 Kin. 2 [8] 7 – 910 1) Kin. 2 [6] HPLC 13225 Equi. 2 [23] SR HPLC 28288 Equi. 2 [23] SR HPLC 50119 Equi. 2 [23] C Benzo[k]fluoranthene Crustacea Daphnia magna Benzo[ghi]perylene Crustacea Daphnia magna Dibenz[a,h]anthracene Crustacea Daphnia magna a) b) 14 FT: flow-through system; S: static; SR: static renewal. C: radioactive carbon in the parent compound; GC: Gas chro3 matography; GCMS: Gas chromatography with mass spectrometry; Flu.Spec.: fluorescence spectrometry; H: radioactive c) hydrogen in the parent compound; HPLC: high pressure liquid chromatography. Kin.: Kinetic BCF, i.e. k1/k2; Equi.: BCF at d) e) (assumed) equilibrium, i.e. Corganism/Cwater. V: validity; 1: valid without restrictions; 2: valid with restrictions. References: [1] (Ankley et al., 1997); [2] (Bruner et al., 1994); [3] (Cailleaud et al., 2009); [4] (Carlson et al., 1979); [5] (De Maagd et al., 1998); [6] (Duxbury et al., 1997); [7] (Evans and Landrum, 1989); [8] (Frank et al., 1986); [9] (Gossiaux et al., 1996); [10] (Hall and Oris, 1991); [11] (Jimenez et al., 1987); [12] (Jonsson et al., 2004); [13] (Landrum and Poore, 1988); [14] (Landrum and Scavia, 1983); [15] (Landrum et al., 2003); [16] (Landrum, 1982); [17] (Landrum, 1988); [18] (Leversee et al., 1981); [19] (Leversee et al., 1982); [20] (McCarthy and Jimenez, 1985); [21] (McLeese and Burridge, 1987); [22] (Monson et al., 1999); [23] (Newsted and Giesy, 1987); [24] (Richardson et al., 2005); [25] (RIITI, 1977); [26] (RIITI, 1979); [27] (RIITI, 1990a); [28] (RIITI, 1990b); [29] (RIITI, 1990c); [30] (Schuler et al., 2004); [31] (Southworth et al., 1978); [32] (Weinstein, 2001); [33] (Wildi et al., 1994); [34] (Yakata et al., 2006) 1) 2) Values represent (a range of) BCF values from (a range of) different exposure concentrations. Kinetic model with 3) estimated uptake rate constant based on fish size applied to the data, high and low concentration, respectively. In this 4) study BCF values are based on lipid weight, values given in this table are normalized to 5% lipid content. Kinetic value based on the presented data. However, the uptake curve for phenanthrene does not show the regular levelling off in time. 5) 6) Therefore, static BCF values at the end of 28 d do exceed 5000. BCFs are based on dry weight. BCFs were determined 7) 8) with test animals that differ in lipid content. BCFs were determined at different exposure temperatures. BCFs were 9) determined at different exposure pHs. BCFs were determined at different feeding regimes, i.e. fed both during uptake and depuration, not fed during uptake but fed during depuration. 20 RIVM report 601779002 4 Discussion In the Risk Assessment Report (RAR) on coal-tar pitch, high temperature (The Netherlands, 2008) and in the assessment by Lampi and Parkerton (2009) validity was also assigned to the different BCF studies. In the present report the re-evaluation of the studies resulted in different validity scores in comparison to these references which are discussed below. 4.1 Evaluating the bioaccumulation assessment by Lampi and Parkerton In a study by De Voogt et al. (1991) BCFs were calculated for 9H-fluorene, anthracene and pyrene, based on 7-day semi-static renewal bioaccumulation tests with guppy (Poecilia reticulata). In the RAR (The Netherlands, 2008) these BCF were assigned a validity of 2 (valid with restrictions), but Lampi and Parkerton (2009) argue that many details on test set-up and results (e.g. whether fish are fed or not, measured water concentrations) are lacking from the paper, so they rate these values not assignable (validity = 4). De Voogt et al. (1991) also report BCF values from 48-hour static exposures. Our reevaluation of this source showed some inconsistencies within the study and thus reliability of the reported BCF could not be assigned (validity 4). First, the static renewal study with renewal every 12 h showed a steady state BCF for pyrene at 48 h of 11300 L/kg, which is extraordinarily high, even considering the high lipid content of 9%. However, in the static Banerjee method during 48 h, with correction for loss due to volatilisation and sorption in controls, the BCF was 4810 L/kg. Analysis of the fish was only performed at the end of this 48 h period. The amount of pyrene in fish was only 62% of that estimated from the loss of the water phase. The remaining 38% might be attributed to metabolism, which would yield a BCF value of circa 3000 L/kg. The elimination of pyrene from fish was followed as well during 6 days after the static exposure had ended. This yielded an elimination rate constant of 0.66 d-1. With the estimated rate constant from the static uptake phase this would yield a BCF value of 4863 L/kg. However, the uptake rate constant estimated by the Banerjee method is remarkably high, even considering the small size of the fish (135 mg). If the uptake rate constant would be estimated from the fish size (ECHA, 2008), similar to what is done in the dietary bioaccumulation tests (see section 4.3), the BCF would only be 1485 L/kg. The results from this study are therefore rather inconclusive (validity 4). For similar reasons the short-term BCF values as reported in De Maagd (1996) were rated as unreliable (validity = 3) by Lampi and Parkerton (2009). However, the BCF values from De Maagd (1996) were derived kinetically with the adjusted Banerjee method, in which not only the decrease in the water concentration is monitored but the increase in the concentration in fish as well. Additional measurements were done with piperonyl butoxide added to the water to stop metabolism in the fish by inhibiting the cytochrome P450 isoenzymes. The test duration is very short and induction of metabolization may occur if fish are exposed for a prolonged period. Yet, for benz[a]anthracene De Maagd et al. (1998) found that the exposure time did not influence the metabolic rate. This substance, however, is metabolized to a large extent by fish and for the PAHs that are less easily metabolised, induction may still be an important process. The BCF values from De Maagd (1996) for anthracene, phenanthrene and fluoranthene are indeed higher than values obtain from studies with the same species but a longer exposure time, with constant exposure over time (Carlson et al., 1979; Hall and Oris, 1991), but still within a factor of 1 to 3. Therefore, the results from De Maagd (1996) should be considered with care, but are still important as circumstantial evidence in a weight of evidence approach to decide on the bioaccumulation potential of the studies PAHs. RIVM report 601779002 21 Further, Lampi and Parkerton (2009) state that the water concentrations of several PAHs as used by De Maagd (1996) approach the LC50. However, such LC50 values can only be obtained by irradiation with ultraviolet light, such that the PAHs exert phototoxic effects. Under normal laboratory conditions with gold or cool white fluorescent lighting or similar, under which BCF studies are performed, such phototoxic effects will not occur. Most PAHs are not acutely toxic to fish up to their limit of solubility under such conditions. Values for benz[a]anthracene as reported by De Maagd et al. (1998) were rated as unassignable by Lampi and Parkerton (2009), in contrast with the rating in the RAR (validity = 2). This appears to be based on the absence of lipid data only, which in our opinion is not sufficient for rating a study as unassignable. We therefore still support the rating from the RAR (validity = 2). A study by Weinstein and Oris (1999) with larval fathead minnows reports a BCF for fluoranthene of 9054. This value, however, is based on dry weight, which makes it difficult to compare with BCF values based on wet weight. Lampi and Parkerton (2009) assigned the study as unassignable (validity = 4), which we consider justified given the uncertainties regarding the expression of the concentration. Assuming a water content of 75 – 85%, which is not uncommon in fish, the BCF will be 1358 – 2264 based on wet weight. In addition, it might be assumed that this value is an overestimation for the larger fish regularly used in bioconcentration tests, because biotransformation systems in larvae are not yet fully developed, although for the same species a BCF of 2439 was derived from a 28-day study with fish that were 5 to 6 weeks old (Carlson et al., 1979). Another study with larval fathead minnows (Cho et al., 2003) was rated reliable (validity = 1) in the RAR. Lampi and Parkerton (2009) rated the same study as unreliable (validity = 3), based on the absence of reported units for BCF, the absence of reported lipid content, the test concentration being close to LC50, and uncertainty about whether the BCF is based on dry weight or wet weight. In our opinion these reasons just rate this value as unassignable due to a lack of information provided (validity = 4). Moreover, given the fact that an earlier publication from this group (Weinstein and Oris, 1999) are based on dry weight and for the analysis a reference is made to this publication, it seems plausible to assume that BCF values are on a dry weight basis. With the same assumptions as above for the dry weight content, BCF values on wet weight basis of 2225 – 3709 are calculated, in the presence of 40 µg/L methyl-tert-butyl ether the range is 4381 – 7302. With respect to toxicity, it should be noted that fluoranthene is only acutely toxic to fish at the used concentrations in the presence of UV-lighting and certainly not under laboratory lighting. From a study by Finger et al. (1985) in which bluegills are exposed to 9H-fluorene for 30 days exposure concentrations and internal fish concentrations could be derived. These values were based on dry weight and Lampi and Parkerton (2009) rated the study as unassignable (validity = 4), which is agreed upon. Using the highest reported value (1800) and assuming a water content of 75 – 85%, the BCF will be 270 – 450 based on wet weight. Baussant et al. (2001a; 2001b) reported BCF values for several PAHs based on studies in which turbots were exposed to crude oil. Due to the absence of reported fish and water concentrations these BCF values were rated as unassignable by Lampi and Parkerton (2009). Exposure concentrations, are however given in a figure, and although these values did not exceed water solubility, the test was performed using a dispersed crude oil. Consequently, the solution is oversaturated and BCF values are rated unreliable (validity = 3) instead of unassignable. A depuration phase was also reported in these studies. The half-lives for naphthalene, fluorene, phenanthrene and chrysene were remarkably constant, varying only between 14 and 29 hours. With the uptake rate constant estimated from fish size (see section 4.3), BCF values of 196 to 407 are calculated for these compounds. However, the lack of differentiation in the BCF values for the studied PAHs is not in accordance with other studies. Possibly, the use of saturated concentrations leads to high fish concentrations of total PAH, such that interference 22 RIVM report 601779002 of the different single PAHs can not be excluded. Therefore, these results should be considered as unassignable (validity =4). A study by Carlson et al. (1979) reports BCF results for fathead minnows exposed to a series of PAHs via flow-through conditions for 28 d, followed by a 5 d depuration phase. Although this is not a guideline study, enough details are provided to rate this study as reliable with restrictions (validity = 2). Instead of using the reported BCF values for day 28 we calculated kinetic BCF values based on the reported fish and water concentrations to minimize variability. Lampi and Parkerton (2009) indicated that phenanthrene exposures in one exposure (experiment 2, tank #1) are unreliable, because of declining water concentrations during the 28 d exposure. In addition they assign the results from another exposure (experiment 2, tank#2) reliable only up to 10 days (averaging reported BCFss values for days 7 and 10), considering data later in the experiment as unreliable ‘due to lack of steady state, and fluctuating test concentrations’. We agree that in this experiment a steady state is lacking, but in our opinion the test concentrations in this study do not fluctuate too much. Using the average BCFss value of the last three reported values (day 18, 25 and 28; resulting in a BCF value of 4300) appears more reasonable than the approach by Lampi and Parkerton. 4.2 Evaluating the bioaccumulation assessment in the RAR Freitag et al. (1982; 1985) report steady state BCF values for golden ide (Leuciscus idus melanotus) exposed to different PAHs for 3 d. In the RAR these studies are rated unassignable (validity = 4). The exposure, however, is static for 3 days, which deems it unlikely that a steady state has been established. In addition, no aeration of the water column was provided, suggesting additional stress for the fish and deeming these studies unreliable (validity = 3). Barrows et al. (1980) report a reliable study on the accumulation of acenaphthene in bluegill sunfish (Lepomis macrochirus) (RAR: validity = 2). Unfortunately, concentrations were based on total radioactivity and since biotransformation can be expected this study is rated unassignable (validity = 4). Also the study by Weinstein and Polk (2001), which reports BCF values for Utterbackia imbecillis glochidia exposed to anthracene and pyrene is a very good study (RAR: validity = 2) with one major flaw: BCF values are based on dry weight, resulting in very high values and complicating comparisons with BCF values based on wet weight (validity = 4). In general, however, BCFs in this study are low. Assuming a water content of 75 – 85% the highest value for anthracene (420) would result in a wet weight BCF of 63 – 105, and for pyrene this value (1229) would result in a wet weight BCF of 184 – 307. McCarthy and Jimenez (1985) report both a kinetic and a steady state BCF for bluegill sunfish (Lepomis macrochirus) after a 2 d benzo[a]pyrene exposure, followed by a 4 d depuration phase In the RAR these values are rated valid with restrictions (validity = 2). In this re-assessment, the short exposure time and the presence of humic material in some of the tests, and the high fish loading should rate these values as unreliable (validity = 3), especially since these values are based on total radioactivity. A correction for parent substance in fish between 16 and 32 hours of the uptake phase is not accurate but would indicate a BCF value well below 100 for benzo[a]pyrene. The results for naphthalene, without added humic material, can be considered as more reliable as it was shown that naphthalene was not metabolized to a significant degree. RIVM report 601779002 23 4.3 Dietary bioaccumulation studies Lampi and Parkerton (2009) underline the importance of dietary exposure scenarios, especially for the more lipophilic PAHs. Although we agree with their views in this respect, the available data that could be evaluated were restricted to two studies (Niimi and Palazzo, 1986; Niimi and Dookhran, 1989). Other dietary studies only appear to be done by EMBSI (EMBSI, 2001; 2005; 2006; 2007c; 2007b; 2007a; 2008a; 2008b), which could not be evaluated for this study (validity = 5). For the dietary studies that could be evaluated, Lampi and Parkerton (2009) give half-lives (t0.5) and normalized BCF values. These BCF values are calculated based on the following two equations (ECHA, 2008): BCF = k1 ⋅ t 0.5 k = 1 ln(2) k 2 and k1 = (520) ⋅ W −0.32 in which: k1 = uptake rate (ml/gwet weight/day); k2 = elimination rate (/day); W = fish wet weight (g); t0.5 = growth-corrected half-life in fish (days). With the weight of the fish at the beginning of the depuration phase (estimated from the values presented during the depuration phase) of 658 g (Niimi and Palazzo, 1986), BCF values were estimated to be 645 for fluorene, 847 for phenanthrene, 672 for anthracene, 582 for fluoranthene, 286 for benzo[a]pyrene, and 356 for benz[a]anthracene. Values for phenanthrene, anthracene and fluoranthene are remarkably lower than from studies with aqueous exposure (Table 1). For the study with acenaphthylene (Niimi and Dookhran, 1989) a weight of 250 g is reported and a BCF of 139 can be calculated from the presented data. These values differ from the values reported by Lampi and Parkerton (2009) and the reason for these differences could not be produced, even if other weight assumptions were applied. For instance, for phenanthrene Niimi and Palazzo reported a growth corrected depuration rate (k2 = t0.5/0.693) of 0.077 (d-1), resulting in a t0.5 of 9 d (in agreement with Lampi and Parkerton). The calculated k1 depends on the fish weight. Niimi and Palazzo reported a weight range of 651 ± 132 to 875 ± 141 g, resulting in a k1 range of 57 – 70 (using 1016 and 519 g as weights). These values would result in a BCF range of 738 – 915. When these values are normalized to a fish with 5% lipid content (using the lipid content of 8% as reported in Lampi and Parkerton, although no lipid content is indicated in the Niimi and Palazzo study) this results in a range for the normalized BCF of 461 – 572, while a normalized BCF of 407 is reported by Lampi and Parkerton (2009). Similar differences were found for the other compounds from the Niimi and Palazzo study, which suggests that the calculations in Lampi and Parkerton (2009) are not as straightforward as indicated in that report. Further, very low BCF values are reported by Lampi and Parkerton (2009) for chrysene and pyrene based on the study by Niimi and Palazzo (1986). This was based on the fact that these compounds were not detected at all in fish tissues and the assumption that this could be attributed to low half-lives of less than 2 days. However, this assumption could be incorrect, because the absence of the compounds in the fish tissue may be fully attributable to a very low absorption efficiency. This is also indicated in a subsequent paper (Niimi and Dookhran, 1989), where the same was observed for the PAHs dibenz[a,h]anthracene and benzo[ghi]perylene. 24 RIVM report 601779002 In addition, the reported BCF values from dietary studies in Lampi and Parkerton (2009) show other oddities, e.g. the data for benz[a]anthracene, pyrene and benzo[a]pyrene from the EMBSI 2005 study show the same BCF value for all compounds, which is highly unlikely. Due to the uncertainties in calculating BCF values from the evaluated dietary studies (Niimi and Palazzo, 1986; Niimi and Dookhran, 1989) and the fact that the study reports from EMBSI could not be evaluated at all, in the present report BCF values based on dietary studies were not considered in the assessment of bioaccumulation of PAHs. 4.4 Using bioaccumulation data for regulatory purposes In regulatory frameworks BCFs values are usually considered as a measure for the biomagnification potential of a certain compound. As stated before in the introduction, several factors influence the level of biomagnification of a compound, which may result in situations where at lower trophic levels bioaccumulation and biomagnification takes place, while higher in the food chain organisms are capable of handling the compound and efficiently excreting it (e.g. Wang and Wang, 2006; Wan et al., 2007; Nfon et al., 2008; Takeuchi et al., 2009). According to the European REACH legislation, ‘the assessment of bioaccumulation shall be based on measured data on bioconcentration in aquatic species’ (EU, 2007). When data are available for several aquatic species (preferably from several levels within a food chain) all these data should be taken into account. It might be argued that in this case it appears to make sense to take a weight-of-evidence approach in which (reliable) information from fish (which are higher in the food chain and serve as food for mammals, including humans, and birds) add more weight to an assessment of biomagnification than information on e.g. daphnids (lower in the food chain), although it cannot be excluded that bioaccumulation in the lower food chain may result in effects higher up in the food chain that are not directly related to internal concentrations. In addition, although mussels are relatively low in the food chain, (reliable) results from mussel studies, may add more weight to a biomagnification assessment than data on daphnids, because mussels serve as food for mammals and birds as well. Recently the European Chemicals Agency (ECHA) published an Annex XV Report proposing coal-tar pitch, high temperature, for identification of a substance as a CMR, PBT, vPvB or substance of equivalent level of concern. Part of this report is an assessment of the aquatic bioaccumulation of this substance, which is based on the bioaccumulation potential of the 16 EPA-PAHs. This assessment is solely based on data that were published in the RAR (The Netherlands, 2008). As argued above (see sections 4.1 and 4.2), the present re-evaluation of bioaccumulation data resulted in conflicts with the conclusions from the RAR, which may result in a different conclusion on the PBT/vPvB assessment for the individual PAHs, but not for coal-tar pitch, high temperature as a substance and other substances for which such an assessment is based on PAHs, considering the fact that at least some of the substances that can regarded as PBT and/or vPvB are present in amounts amply exceeding 0.1%. ECHA did not assess the bioaccumulation potential of naphthalene, acenaphthene, acenaphthylene, and 9H-fluorene, as these were not detected in coal-tar pitch high temperature in concentrations exceeding 0.1%. Anthracene was deemed bioaccumulative (B: BCF 2000 – 5000) and each of the other EPAPAHs were deemed very bioaccumulative (vB: BCF >5000), although only for fluoranthene and pyrene this was based on fish data. For the other PAHs the vB status was based on invertebrates. RIVM report 601779002 25 Table 2. Summary of highest reliable BCF values for the 16 EPA-PAHs. Substance BCF value (WW) Type b) BCF value Species (5% lipid norm.) a) Reference c) Naphthalene1) 999 515 Cyprinodon variegatus (Fish) Kin. [6] Acenaphthene1) 760 1000 Cyprinus carpio (Fish) Equi. [10] Acenaphthylene1) 387 509 Cyprinus carpio (Fish) Equi. [11] 9H-fluorene1) 1459 1658 Pimephales promelas (Fish) Kin. [1] 2) Anthracene 4973 –3) 39727 – 19000 210984) Pimephales promelas (Fish) Perna viridis (Mollusc) Pontoporeia hoyi (Crustacean) Equi. Equi. Kin. [4] [9] [7] Phenanthrene 3611 28043 4751 148934) Pimephales promelas (Fish) Pontoporeia hoyi (Crustacean) Kin. Kin. [1] [7] Fluoranthene 2439 –3) 58884 2772 12250 –5) Pimephales promelas (Fish) Perna viridis (Mollusc) Diporeia spec. (Crustacean) Kin. Equi. Kin. [1] [9] [12] Pyrene 1297 –3) 166000 1474 44550 881574) Pimephales promelas (Fish) Perna viridis (Mollusc) Pontoporeia hoyi (Crustacean) Kin. Equi. Kin. [1] [9] [7] Benz[a]anthracene 260 63000 –6) 334574) Pimephales promelas (Fish) Pontoporeia hoyi (Crustacean) Equi. Kin. [2] [7] Chrysene 6088 – Daphnia magna (Crustacean) Equi. [8] 608 1910009) 73000 –8) 119375 387684) Lepomis macrochirus (Fish) Dreissena polymorpha (Mollusc) Pontoporeia hoyi (Crustacean) Kin. Kin. Kin. [5] [3] [7] – – No experimental data available – – 10) Daphnia magna (Crustacean) Equi. [8] Daphnia magna (Crustacean) Equi. [8] Equi. [8] – – Benzo[a]pyrene Benzo[b]fluoranthene 7) Benzo[k]fluoranthene 13225 – Benzo[ghi]perylene 28288 –11) Dibenz[a,h]anthracene 50119 12) Daphnia magna (Crustacean) Indeno[1,2,3-cd]pyrene – – No experimental data available a) – b) BCF values are normalized to organisms with a lipid content of 5%. Kin.: kinetic BCF value (k1/k2); Equi. BCF value at c) (assumed) equilibrium (Corganism/Cwater). [1] (Carlson et al., 1979); [2] (De Maagd et al., 1998); [3] (Gossiaux et al., 1996); [4] (Hall and Oris, 1991); [5] (Jimenez et al., 1987); [6] (Jonsson et al., 2004); [7] (Landrum, 1988); [8] (Newsted and Giesy, 1987); [9] (Richardson et al., 2005); [10] (RIITI, 1990a); [11] (RIITI, 1990b); [12] (Schuler et al., 2004). 1) 2 For these compounds invertebrates showed lower BCF values than fish, so only fish data are given. In this study no lipid content was given, but based on lipid contents in fathead minnows reported by Carlson et al. (1979) lipid content is 3) expected to be 5 – 6 %, which would result in lipid normalized values ranging from 4100 – 5000. In this study only lipid4) based BCF values were given, but lipid content itself was not reported. In this study lipid content was expressed only as percentage of dry weight (35%). In addition the ratio between total wet weight and dry weight was given (0.269). For lipid normalization it was assumed that the same ratio holds for lipids, resulting in a lipid content of 9.4% based on wet weight. 5) In this study no lipid content was given, but for a lipid normalized value to fall below the trigger value of 5000 the lipid 6) content needs to be 59%, which seems to be unrealistically high. In this study no lipid content was given, but for a lipid normalized value to exceed the trigger value of 2000 the lipid content needs to be 0.65%, which seems to be unrealistically 7) low. In this study no lipid content was given, but Liu et al. (1996) report lipid contents in Daphnia magna ranging from 4 – 6%, suggesting that a lipid normalized BCF value will be similar to the wet weight value. If the lipid content is higher than 8) 6.1%, the normalized BCF value will be below 5000. In this study no lipid content was given, but for a lipid normalized value to exceed the trigger value of 2000 the lipid content needs to be 1.5%, which seems to be unrealistically low. 9) 10) Higher BCF values were reported, but this is the highest value for which lipid normalization could be applied. In this study no lipid content was given, but for a lipid normalized value to fall below the trigger value of 5000 the lipid content 11) needs to be 13%, which seems to be unrealistically high. In this study no lipid content was given, but for a lipid normalized value to fall below the trigger value of 5000 the lipid content needs to be 28%, which seems to be unrealistically 12) high. In this study no lipid content was given, but for a lipid normalized value to fall below the trigger value of 5000 the lipid content needs to be 50%, which seems to be unrealistically high. 26 RIVM report 601779002 The results from the present evaluation of BCF values are summarized in Table 2. This table shows that for most PAHs the same conclusions are reached for their bioaccumulative properties, i.e. naphthalene, acenaphthene, acenaphthylene and 9H-fluorene are considered not bioaccumulative, and chrysene, benzo[k]fluoranthene, benzo[ghi]perylene, and dibenz[a,h]anthracene are considered vB (based on invertebrates). Anthracene is still considered B for fish, but additional data show that it is vB in molluscs and crustaceans. For phenanthrene and fluoranthene, however, re-evaluation of data deemed these compounds B instead of vB when based on fish. Based on invertebrates (crustaceans for phenanthrene; mussels and crustaceans for fluoranthene) both compounds are considered vB. Similarly pyrene, benz[a]anthracene and benzo[a]pyrene do not accumulate in fish (due to biotransformation), but are very bioaccumulative at lower trophic levels (molluscs and crustaceans). RIVM report 601779002 27 28 RIVM report 601779002 References Ahrens MJ, Nieuwenhuis R and Hickey CW, 2002. Sensitivity of juvenile Macomona liliana (bivalvia) to UV-photoactivated fluoranthene toxicity. Environ. Toxicol. 17: 567-577. Anderson JW, Neff JM, Cox BA, Tatem HE and Hightower GM, 1974. The effects of oil on estuarine animals: toxicity, uptake and depuration, respiration. In: Vernberg FJ and Vernberg WB, eds. Pollution and Physiology of Marine Organisms. Academic Press, New York, NY, USA, pp. 367379. Ankley GT, Erickson RJ, Sheedy BR, Kosian PA, Mattson VR and Cox JS, 1997. Evaluation of models for predicting the phototoxic potency of polycyclic aromatic hydrocarbons. Aquat. Toxicol. 37: 37-50. Arnot JA, Mackay D, Parkerton TF and Bonnell M, 2008. A database of fish biotransformation rates for organic chemicals. Environ. Toxicol. Chem. 27: 2263-2270. Barrows ME, Petrocelli SR, Macek KJ and Carroll JJ, 1980. Bioconcentration and elimination of selected water pollutants by bluegill sunfish Lepomis macrochirus. In: Hague R, ed. Dynamic Exposure Hazard Assessment of Toxic Chemicals. Ann Arbor Science Publishers, Ann Arbor, Michigan, USA, pp. 379-392. Baussant T, Sanni S, Jonsson G, Skadsheim A and Børseth JF, 2001a. Bioaccumulation of polycyclic aromatic compounds: 1. Bioconcentration in two marine species and in semipermeable membrane devices during chronic exposure to dispersed crude oil. Environ. Toxicol. Chem. 20: 1175-1184. Baussant T, Sanni S, Skadsheim A, Jonsson G, Børseth JF and Gaudebert B, 2001b. Bioaccumulation of polycyclic aromatic compounds: 2. Modeling bioaccumulation in marine organisms chronically exposed to dispersed oil. Environ. Toxicol. Chem. 20: 1185-1195. Bayona JM, Fernandez P, Porte C, Tolosa I, Valls M and Albaiges J, 1991. Partitioning of urban wastewater organic microcontaminants among coastal compartments. Chemosphere 23: 313-326. Black MC, Burton W, McCarthy JF, Peterson MJ and Southworth GR, 1993. Bioaccumulation studies. In: Hinzman RL, ed. Second Report on the Oak Ridge Y-12 Plant Biological Monitoring and Abatement Program for East Fork Poplar Creek. Publication Nr 3859. Oak Ridge National Laboratory, Environmental Sciences Division, Oak Ridge, TN, USA, pp. 109-172. Boese BL, Ozretich RJ, Lamberson JO, Swartz RC, Cole FA, Pelletier J and Jones J, 1999. Toxicity and phototoxicity of mixtures of highly lipophilic PAH compounds in marine sediment: Can the ΣPAH model be extrapolated? Arch. Environ. Con. Tox. 36: 270-280. Bruner KA, Fisher SW and Landrum PF, 1994. The role of the zebra mussel, Dreissena polymorpha, in contaminant cycling: I. The effect of body size and lipid content on the bioconcentration of PCBs and PAHs. J. Great Lakes Res. 20: 725-734. Cailleaud K, Budzinski H, Le Menach K, Souissi S and Forget-Leray J, 2009. Uptake and elimination of hydrophobic organic contaminants in estuarine copepods: An experimental study. Environ. Toxicol. Chem. 28: 239-246. Carls MG and Rice SD, 1988. Sensitivity differences between eggs and larvae of walleye pollock (Theragra chalcogramma) to hydrocarbons. Mar. Environ. Res. 26: 285-297. Carlson RM, Oyler AR, Gerhart EH, Caple R, Welch KJ, Kopperman HL, Bodenner D and Swanson D, 1979. Implications to the aquatic environment of polynuclear aromatic hydrocarbons liberated from Northern Great Plains coal. US EPA report EPA-600/3-79-093, U.S. Environmental Protection Agency (US EPA), Duluth, MN. Casserly DM, Davis EM, Downs TD and Guthrie RK, 1983. Sorption of organics by Selenastrum capricornutum. Wat. Res. 17: 1591-1594. Cheikyula JO, Koyama J and Uno S, 2008. Comparative study of bioconcentration and EROD activity induction in the Japanese flounder, red sea bream, and Java medaka exposed to polycyclic aromatic hydrocarbons. Environ. Toxicol. 23: 354-362. Chen S, Ke R, Zha J, Wang Z and Khan SU, 2008. Influence of humic acid on bioavailability and toxicity of benzo[k]fluoranthene to Japanese medaka. Environ. Sci. Technol. 42: 9431-9436. Cho EA, Bailer AJ and Oris JT, 2003. Effect of methyl tert-butyl ether on the bioconcentration and photoinduced toxicity of fluoranthene in fathead minnow larvae (Pimephales promelas). Environ. Sci. Technol. 37: 1306-1310. RIVM report 601779002 29 Clements WH, Oris JT and Wissing TE, 1994. Accumulation and food chain transfer of fluoranthene and benzo[a]pyrene in Chironomus riparius and Lepomis macrochirus. Arch. Environ. Con. Tox. 26: 261-266. Correa M and Coler R, 1983. Enhanced oxygen uptake rates in dragonfly nymphs (Somatochlora cingulata) as an indication of stress from naphthalene. Bull. Environ. Contam. Toxicol. 30: 269-276. Correa M and Venables BJ, 1985. Bioconcentration of naphthalene in tissues of the white mullet (Mugil curema). Environ. Toxicol. Chem. 4: 227-231. Couch JA, Courtney LA, Winstead JT and Foss SS, 1979. American oyster (Crassostrea virginica) as an indicator of carcinogens in the aquatic environment. In: Animals as Monitors of Environmental Pollutants. National Academy of Sciences, Washington, DC, USA, pp. 65-84. De Maagd PG-J, 1996. Polycyclic aromatic hydrocarbons: fate and effects in aquatic environment. Ph.D. thesis. Utrecht University, Utrecht, The Netherlands. De Maagd PG-J, de Poorte J, Opperhuizen A and Sijm DTHM, 1998. No influence after various exposure times on the biotransformation rate constants of benzo(a)anthracene in fathead minnow (Pimephales promelas). Aquat. Toxicol. 40: 157-169. De Voogt P, van Hattum B, Leonards P, Klamer JC and Govers H, 1991. Bioconcentration of polycyclic heteroaromatic hydrocarbons in the guppy (Poecilia reticulata). Aquat. Toxicol. 20: 169-194. DiMichele L and Taylor MH, 1978. Histopathological and physiological responses of Fundulus heteroclitus to naphthalene exposure. J. Fish. Res. Board Can. 35: 1060-1066. Djomo JE, Garrigues P and Narbonne JF, 1996. Uptake and depuration of polycyclic aromatic hydrocarbons from sediment by the zebrafish (Brachydanio rerio). Environ. Toxicol. Chem. 15: 1177-1181. Dunn BP and Stich HF, 1976. Release of the carcinogen benzo(a)pyrene from environmentally contaminated mussels. Bull. Environ. Contam. Toxicol. 15: 398-401. Duxbury CL, Dixon DG and Greenberg BM, 1997. Effects of simulated solar radiation on the bioaccumulation of polycyclic aromatic hydrocarbons by the duckweed Lemna gibba. Environ. Toxicol. Chem. 16: 1739-1748. Eastmond DA, Booth GM and Lee ML, 1984. Toxicity, accumulation, and elimination of polycyclic aromatic sulfur heterocycles in Daphnia magna. Arch. Environ. Con. Tox. 13: 105-111. ECHA, 2008. Guidance on information requirements and chemical safety assessment, Chapter R.11: PBT Assessment. Guidance for the implementation of REACH. European Chemicals Agency (ECHA), Helsinki, Finland. EMBSI, 2001. Fish, dietary bioaccumulation test, study no. 100047AB. Report 01MRL61, ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2005. Fish, dietary bioaccumulation test, study no. 100047P. Report 05MRL127, ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2006. Fish, dietary bioaccumulation test, study no. 0681647. Report 06EMBSI506, ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2007a. Fish, dietary bioaccumulation study, study no. 0711047. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2007b. Fish, dietary bioaccumulation study, study no. 0796347C. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2007c. Fish, dietary bioaccumulation study, study no. 0796347T. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2008a. Fish, dietary bioaccumulation study, study no. 0818447. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2008b. Fish, dietary bioaccumulation study, study no. 0821047. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EMBSI, 2009. Fish, aqueous bioaccumulation study, study no. 0829644. ExxonMobil Biomedical Sciences Inc. (EMBSI), Annandale, NJ, USA. EU, 1993. Council Regulation (EEC) No 793/93 of 23 March 1993 on the evaluation and control of the risks of existing substances. O. J. L 84: 1-75. EU, 2007. Corrigendum to Regulation (EC) No 1907/2006 of the European Parliament and of the Council of 18 December 2006 concerning the Registration, Evaluation, Authorisation and Restriction of Chemicals (REACH), establishing a European Chemicals Agency, amending Directive 1999/45/EC and repealing Council Regulation (EEC) No 793/93 and Commission Regulation (EC) No 1488/94 30 RIVM report 601779002 as well as Council Directive 76/769/EEC and Commission Directives 91/155/EEC, 93/67/EEC, 93/105/EC and 2000/21/EC. O. J. L 136: 3-280. Evans MS and Landrum PF, 1989. Toxicokinetics of DDE, benzo(a)pyrene, and 2,4,5,2',4',5'hexachlorobiphenyl in Pontoporeia hoyi and Mysis relicta. J. Great Lakes Res. 15: 589-600. Fan CW and Reinfelder JR, 2003. Phenanthrene accumulation kinetics in marine diatoms. Environ. Sci. Technol. 37: 3405-3412. Finger SE, Little EF, Henry MG, Fairchild JF and Boyle TP, 1985. Comparison of laboratory and field assessment of fluorene - Part I: Effects of fluorene on the survival, growth, reproduction, and behavior of aquatic organisms in laboratory tests. In: Boyle TP, ed. Validation and Predictability of Laboratory Methods for Assessing the Fate and Effects of Contaminants in Aquatic Ecosystems. American Society for Testing and Materials, Philadelphia, PA, USA Frank AP, Landrum PF and Eadie BJ, 1986. Polycyclic aromatic hydrocarbon rates of uptake, depuration, and biotransformation by Lake Michigan Stylodrilus heringianus. Chemosphere 15: 317-330. Freitag D, Ballhorn L, Geyer H and Korte F, 1985. Environmental hazard profile of organic chemicals. An experimental method for the assessment of the behaviour of organic chemicals in the ecosphere by means of simple laboratory tests with 14C labelled chemicals. Chemosphere 14: 1589-1616. Freitag D, Geyer H and Kraus A, 1982. Ecotoxicological profile analysis. VII. Screening chemicals for their environmental behavior by comparative evaluation. Ecotox. Environ. Saf. 6: 60-81. Gerould S, Landrum P and Giesy JP, 1983. Anthracene bioconcentration and biotransformation in chironomids: Effects of temperature and concentration. Environ. Pollut. Ser. A 30: 175-188. Geyer H, Politzki G and Freitag D, 1984. Prediction of ecotoxicological behaviour of chemicals: Relationship between n-octanol/water partition coefficient and bioaccumulation of organic chemicals by alga Chlorella. Chemosphere 13: 269-284. Gharrett JA and Rice SD, 1987. Influence of simulated tidal cycles on aromatic hydrocarbon uptake and elimination by the shore crab Hemigrapsus nudus. Mar. Biol. 95: 365-370. Gobas FAPC, de Wolf W, Burkhard LP, Verbruggen E and Plotzke K, 2009. Revisiting bioaccumulation criteria for POPs and PBT assessments. Integr. Environ. Assess. Manag. 5: 624-637. Gossiaux DC, Landrum PF and Fisher SW, 1996. Effect of temperature on the accumulation kinetics of PAHs and PCBs in the zebra mussel, Dreissena polymorpha. J. Great Lakes Res. 22: 379-388. Granier LK, Lafrance P and Campbell PGC, 1999. An experimental design to probe the interactions of dissolved organic matter and xenobiotics: Bioavailability of pyrene and 2,2',5,5'-tetrachlorobiphenyl to Daphnia magna. Chemosphere 38: 335-350. Haitzer M, Abbt-Braun G, Traunspurger W and Steinberg CEW, 1999a. Effects of humic substances on the bioconcentration of polycyclic aromatic hydrocarbons: Correlations with spectroscopic and chemical properties of humic substances. Environ. Toxicol. Chem. 18: 2782-2788. Haitzer M, Höss S, Traunspurger W and Steinberg C, 1999b. Relationship between concentration of dissolved organic matter (DOM) and the effect of DOM on the bioconcentration of benzo[a]pyrene. Aquat. Toxicol. 45: 147-158. Hall AT, 1993. Reproductive and behavioral toxicity of anthracene in the fathead minnow (Pimephales promelas). PhD Thesis. Miami University, Oxford, OH, USA. Hall AT and Oris JT, 1991. Anthracene reduces reproductive potential and is maternally transferred during long-term exposure in fathead minnows. Aquat. Toxicol. 19: 249-264. Halling-Sørensen B, Nyholm N, Kusk KO and Jacobsson E, 2000. Influence of nitrogen status on the bioconcentration of hydrophobic organic compounds to Selenastrum capricornutum. Ecotox. Environ. Saf. 45: 33-42. Herbes SE, 1976. Transport and bioaccumulation of polycyclic aromatic hydrocarbons (PAH) in aquatic systems. In: Coal Technology Program Quarterly Progress Report for the Period Ending December 31, 1975. Oak Ridge National Laboratory, Oak Ridge, TN, USA, pp. 65-71. Herbes SE and Risi GF, 1978. Metabolic alteration and excretion of anthracene by Daphnia pulex. Bull. Environ. Contam. Toxicol. 19: 147-155. Jimenez BD, Cirmo CP and McCarthy JF, 1987. Effects of feeding and temperature on uptake, elimination and metabolism of benzo[a]pyrene in the bluegill sunfish (Lepomis macrochirus). Aquat. Toxicol. 10: 41-57. Johnsen S, Kukkonen J and Grande M, 1989. Influence of natural aquatic humic substances on the bioavailability of benzo(a)pyrene to Atlantic Salmon. Sci. Total Environ. 81-82: 691-702. RIVM report 601779002 31 Jonker MTO and Van der Heijden SA, 2007. Bioconcentration factor hydrophobicity cutoff: An artificial phenomenon reconstructed. Environ. Sci. Technol. 41: 7363-7369. Jonsson G, Bechmann RK, Bamber SD and Baussant T, 2004. Bioconcentration, biotransformation, and elimination of polycyclic aromatic hydrocarbons in sheepshead minnows (Cyprinodon variegatus) exposed to contaminated seawater. Environ. Toxicol. Chem. 23: 1538-1548. Kane Driscoll S, Landrum PF and Tigue E, 1997. Accumulation and toxicokinetics of fluoranthene in wateronly exposures with freshwater amphipods. Environ. Toxicol. Chem. 16: 754-761. Kira S, Nogami Y, Taketa K and Hayatsu H, 1996. Comparison of techniques for monitoring water-borne polycyclic mutagens: Efficiency of blue rayon, sep-pak C18, and a biota, Corbicula, in concentrating benzo(a)pyrene in a model water system. Bull. Environ. Contam. Toxicol. 57: 278283. Klimisch HJ, Andreae M and Tillmann U, 1997. A systematic approach for evaluating the quality of experimental toxicological and ecotoxicological data. Regul. Toxicol. Pharmacol. 25: 1-5. Kuhnhold WW and Busch F, 1978. On the uptake of three different types of hydrocarbons by salmon eggs (Salmo salar L.). Meeresforschung 26: 50-59. Kukkonen J, McCarthy JF and Oikari A, 1990. Effects of XAD-8 fractions of dissolved organic carbon on the sorption and bioavailability of organic micropollutants. Arch. Environ. Con. Tox. 19: 551-557. Lampi M and Parkerton T, 2008. Bioaccumulation Assessment of PAHs - Draft. ExxonMobil Biomedical Sciences, Inc. Lampi M and Parkerton T, 2009. Bioaccumulation Assessment of PAHs - Draft. ExxonMobil Biomedical Sciences, Inc. (EMBSI). Landrum PF, 1982. Uptake, depuration and biotransformation of anthracene by the scud Pontoporeia hoyi. Chemosphere 11: 1049-1057. Landrum PF, 1988. Toxicokinetics of organic xenobiotics in the amphipod, Pontoporeia hoyi: Role of physiological and environmental variables. Aquat. Toxicol. 12: 245-271. Landrum PF, Lotufo GR, Gossiaux DC, Gedeon ML and Lee JH, 2003. Bioaccumulation and critical body residue of PAHs in the amphipod, Diporeia spp.: Additional evidence to support toxicity additivity for PAH mixtures. Chemosphere 51: 481-489. Landrum PF and Poore R, 1988. Toxicokinetics of selected xenobiotics in Hexagenia limbata. J. Great Lakes Res. 14: 427-437. Landrum PF and Scavia D, 1983. Influence of sediment on anthracene uptake, depuration, and biotransformation by the amphipod Hyalella azteca. Can. J. Fish. Aquat. Sci. 40: 298-305. Laurén DJ and Rice S, 1985. Significance of active and passive depuration in the clearance of naphthalene from the tissues of Hemigrapsus nudus (Crustacea: Decapoda). Mar. Biol. 88: 135-142. Lee JH, Landrum PF and Koh CH, 2002. Toxicokinetics and time-dependent PAH toxicity in the amphipod Hyalella azteca. Environ. Sci. Technol. 36: 3124-3130. Lee RF, Sauerheber R and Dobbs GH, 1972. Uptake, metabolism and discharge of polycyclic aromatic hydrocarbons by marine fish. Mar. Biol. 17: 201-208. Leversee GJ, Giesy JP, Landrum PF, Bartell S, Gerould S, Bruno M, Spacie A, Bonling J, Haddock J and Fannin T, 1981. Disposition of benzo(a)pyrene in aquatic system components: periphyton, chironomids, daphnia, fish. In: Cooke M and Dennis AJ, eds. Analysis and Biological Fate: Polynuclear Aromatic HydroCarbons. Batelle Press, Columbus, OH, USA, pp. 357-366. Leversee GJ, Giesy JP, Landrum PF, Gerould S, Bowling JW, Fannin TE, Haddock JD and Bartell SM, 1982. Kinetics and biotransformation of benzo(a)pyrene in Chironomus riparius. Arch. Environ. Con. Tox. 11: 25-31. Leversee GJ, Landrum PF, Giesy JP and Fannin T, 1983. Humic acids reduce bioaccumulation of some polycyclic aromatic hydrocarbons. Can. J. Fish. Aquat. Sci. 40: s63–s69. Levine SL, Czosnyka H and Oris JT, 1997. Effect of the fungicide clotrimazole on the bioconcentration of benzo[a]pyrene in Gizzard shad (Dorosoma cepedianum): In vivo and in vitro inhibition of cytochrome P4501A activity. Environ. Toxicol. Chem. 16: 306-311. Linder G, 1982. Anthracene bioconcentration in rainbow trout in single-compound and complex chemical mixture exposures. PhD Thesis. University of Wyoming, Laramie, WY, USA. Linder G and Bergman HL, 1984. Periodic depuration of anthracene metabolites by rainbow trout. T. Am. Fish. Soc. 113: 513-520. 32 RIVM report 601779002 Linder G, Bergman HL and Meyer JS, 1985. Anthracene bioconcentration in rainbow trout during singlecompound and complex-mixture exposures. Environ. Toxicol. Chem. 4: 549-558. Liu ZT, Kong ZM, Zhou F and Wang LS, 1996. Bioconcentration and toxicity effect on lipid content of aquatic organisms. Bull. Environ. Contam. Toxicol. 56: 135-142. Lockhart WL, Metner DA, Billeck BN, Rawn GP and Muir DCG, 1983. Bioaccumulation of some forestry pesticides in fish and aquatic plants. In: Chemical and Biological Controls in Forestry. ACS Symposium Series. 238. American Chemical Society, Washington, D.C., pp. 297-318. Lu PY, Metcalf RL, Plummer N and Mandel D, 1977. The environmental fate of three carcinogens: Benzo(α)-pyrene, benzidine, and vinyl chloride evaluated in laboratory model ecosystems. Arch. Environ. Con. Tox. 6: 129-142. Mailhot H, 1987. Prediction of algal bioaccumulation and uptake rate of nine organic compounds by ten physicochemical properties. Environ. Sci. Technol. 21: 1009-1013. McCarthy JF, 1983. Role of particulate organic matter in decreasing accumulation of polynuclear aromatic hydrocarbons by Daphnia magna. Arch. Environ. Con. Tox. 12: 559-568. McCarthy JF and Jimenez BD, 1985. Reduction in bioavailability to bluegills of polycyclic aromatic hydrocarbons bound to dissolved humic material. Environ. Toxicol. Chem. 4: 511-521. McCarthy JF, Jimenez BD and Barbee T, 1985. Effect of dissolved humic material on accumulation of polycyclic aromatic hydrocarbons: Structure-activity relationships. Aquat. Toxicol. 7: 15-24. McLeese DW and Burridge LE, 1987. Comparative accumulation of PAHs in four marine invertebrates. In: Capuzzo JM and Kester DR, eds. Biological Processes and Wastes in the Ocean. Oceanic Processes in Marine Pollution. 1. Robert E Krieger, Malabar, FL, USA, pp. 109-118. Melancon Jr MJ and Lech JJ, 1978. Distribution and elimination of naphthalene and 2-methylnaphthalene in rainbow trout during short- and long-term exposures. Arch. Environ. Con. Tox. 7: 207-220. Monson PD, Call DJ, Cox DA, Liber K and Ankley GT, 1999. Photoinduced toxicity of fluoranthene to northern leopard frogs (Rana pipiens). Environ. Toxicol. Chem. 18: 308-312. Moy FE and Walday M, 1997. Accumulation and depuration of organic micro-pollutants in marine hard bottom organisms. Mar. Pollut. Bull. 33: 56-63. Murray AP, Richardson BJ and Gibbs CF, 1991. Bioconcentration factors for petroleum hydrocarbons, PAHs, LABs and biogenic hydrocarbons in the blue mussel. Mar. Pollut. Bull. 22: 595-603. Neff JM and Anderson JW, 1975. Accumulation, release and distribution of benzo[a]pyrene-C14 in the clam Rangia cuncata. In: Proceedings of the Conference on Prevention and Control of Oil Pollution, March 25-27, 1975. American Petroleum Institute, Washington, DC, USA, pp. 469-471. Neff JM, Anderson JW, Cox BA, Laughlin Jr. RB, Rossi SS and Tatem HE, 1976a. Effects of petroleum on survival, respiration and growth of marine animals. In: Sources, Effects and Sinks of Hydrocarbons in the Aquatic Environment. American Institute of Biological Sciences, Arlington, VA, USA, pp. 515-539. Neff JM, Cox BA, Anderson JW and Dixit D, 1976b. Accumulation and release of petroleum derived aromatic hydrocarbons by four species of marine animals. Mar. Biol. 38: 279-289. Netherlands, 2008. Coal Tar Pitch High Temperature. Documentation of the work done under the Existing Substance Regulation (EEC) No 793/93 and submitted to the European Chemicals Agency according to Article 136(3) of Regulation (EC) No 1907/2006. Annex XV Transitional Dossier, Rapporteur: the Netherlands. European Chemicals Agency, Helsinki, Finland. Newsted JL and Giesy JP, 1987. Predictive models for photoinduced acute toxicity of polycyclic aromatic hydrocarbons to Daphnia magna, Strauss (Cladocera, Crustacea). Environ. Toxicol. Chem. 6: 445461. Nfon E, Cousins IT and Broman D, 2008. Biomagnification of organic pollutants in benthic and pelagic marine food chains from the Baltic Sea. Sci. Total Environ. 397: 190-204. Niimi AJ and Dookhran GP, 1989. Dietary absorption efficiencies and elimination rates of polycyclic aromatic hydrocarbons (PAHs) in rainbow trout (Salmo gairdneri). Environ. Toxicol. Chem. 8: 719-722. Niimi AJ and Palazzo V, 1986. Biological half-lives of eight polycyclic aromatic hydrocarbons (PAHs) in rainbow trout (Salmo gairdneri). Wat. Res. 20: 503-507. OECD, 1996. OECD Guideline for Testing of Chemicals 305: Bioconcentration: Flow-through Fish Test. Organisation for Econonomic Co-operation and Development (OECD), Paris, France. RIVM report 601779002 33 Ogata M, Fujisawa K, Ogino Y and Mano E, 1984. Partition coefficients as a measure of bioconcentration potential of crude oil compounds in fish and shellfish. Bull. Environ. Contam. Toxicol. 33: 561567. Oris JT, Hall AT and Tylka JD, 1990. Humic acids reduce the photo-induced toxicity of anthracene to fish and daphnia. Environ. Toxicol. Chem. 9: 575-583. OSPAR. 1992. OSPAR Convention. http://www.ospar.org. Palmork KH and Solbakken JE, 1981. Distribution and elimination of [9-14C]phenanthrene in the horse mussel (Modiola modiolus). Bull. Environ. Contam. Toxicol. 26: 196-201. Parkerton TF, Arnot JA, Weisbrod AV, Russom C, Hoke RA, Woodburn K, Traas T, Bonnell M, Burkhard LP and Lampi MA, 2008. Guidance for evaluating in vivo fish bioaccumulation data. Integr. Environ. Assess. Manag. 4: 139-155. Petersen GI and Kristensen P, 1998. Bioaccumulation of lipophilic substances in fish early life stages. Environ. Toxicol. Chem. 17: 1385-1395. Rantamäki P, 1997. Release and retention of selected polycyclic aromatic hydrocarbons (PAH) and their methylated derivatives by the common mussel (Mytilus edulis) in the brackish water of the Baltic Sea. Chemosphere 35: 487-502. Richardson BJ, Tse ES-C, De Luca-Abbott SB, Martin M and Lam PKS, 2005. Uptake and depuration of PAHs and chlorinated pesticides by semi-permeable membrane devices (SPMDs) and green-lipped mussels (Perna viridis). Mar. Pollut. Bull. 51: 975-993. RIITI, 1977. Anthracene. The Official Bulletin of the Ministry of International Trade and Industry. Research Insititute of International Trade and Industry (RIITI), Tokyo, Japan. RIITI, 1979. Naphthalene. The Official Bulletin of the Ministry of International Trade and Industry. Research Insititute of International Trade and Industry (RIITI), Tokyo, Japan. RIITI, 1990a. Acenaphthene. The Official Bulletin of the Ministry of International Trade and Industry. Research Insititute of International Trade and Industry (RIITI), Tokyo, Japan. RIITI, 1990b. Acenaphthylene. The Official Bulletin of the Ministry of International Trade and Industry. Research Insititute of International Trade and Industry (RIITI), Tokyo, Japan. RIITI, 1990c. Fluorene. The Official Bulletin of the Ministry of International Trade and Industry. Research Insititute of International Trade and Industry (RIITI), Tokyo, Japan. Riley RT, Mix MC, Schaffer RL and Bunting DL, 1981. Uptake and accumulation of naphthalene by the oyster Ostrea edulis, in a flow-through system. Mar. Biol. 61: 267-276. Roubal WT, Stranahan SI and Malins DC, 1978. The accumulation of low molecular weight aromatic hydrocarbons of crude oil by Coho salmon (Oncorhynchus kisutch) and starry flounder (Platichthys stellatus). Arch. Environ. Con. Tox. 7: 237-244. Schuler LJ, Landrum PF and Lydy MJ, 2004. Time-dependent toxicity of fluoranthene to freshwater invertebrates and the role of biotransformation on lethal body residues. Environ. Sci. Technol. 38: 6247-6255. Seaton CL and Tjeerdema RS, 1996. Tissue disposition and biotransformation of naphthalene in striped bass (Morone saxatilis). Mar. Environ. Res. 42: 345-348. Sheedy BR, Mattson VR, Cox JS, Kosian PA, Phipps GL and Ankley GT, 1998. Bioconcentration of polycyclic aromatic hydrocarbons by the freshwater oligochaete Lumbriculus variegatus. Chemosphere 36: 3061-3070. Skarphéðinsdóttir H, Ericson G, Dalla Zuanna L and Gilek M, 2003. Tissue differences, dose-response relationship and persistence of DNA adducts in blue mussels (Mytilus edulis L.) exposed to benzo[a]pyrene. Aquat. Toxicol. 62: 165-177. Southworth GR, Beauchamp JJ and Schmieder PK, 1978. Bioaccumulation potential of polycyclic aromatic hydrocarbons in Daphnia pulex. Wat. Res. 12: 973-977. Spacie A, Landrum PF and Leversee GJ, 1983. Uptake, depuration, and biotransformation of anthracene and benzo[a]pyrene in bluegill sunfish. Ecotox. Environ. Saf. 7: 330-341. Stockholm Convention. 2001. Stockholm Convention on Persistent Organic Pollutants (POPs). http://www.pops.int/. Takeuchi I, Miyoshi N, Mizukawa K, Takada H, Ikemoto T, Omori K and Tsuchiya K, 2009. Biomagnification profiles of polycyclic aromatic hydrocarbons, alkylphenols and polychlorinated biphenyls in Tokyo Bay elucidated by δ13C and δ15N isotope ratios as guides to trophic web structure. Mar. Pollut. Bull. 58: 663-671. 34 RIVM report 601779002 Tolls J, Haller M, Labee E, Verweij M and Sijm DTHM, 2000. Experimental determination of bioconcentration of the nonionic surfactant alcohol ethoxylate. Environ. Toxicol. Chem. 19: 646653. Trucco RG, Engelhardt FR and Stacey B, 1983. Toxicity, accumulation and clearance of aromatic hydrocarbons in Daphnia pulex. Environ. Pollut. Ser. A 31: 191-202. US-EPA, 1976. Semi-Annual Report. April-September 1976. U.S. Environmental Protection Agency (US EPA), Gulf Breeze, FL, USA. Van Hattum B and Cid Montañes JF, 1999. Toxicokinetics and bioconcentration of polycyclic aromatic hydrocarbons in freshwater isopods. Environ. Sci. Technol. 33: 2409-2417. Veith GD, DeFoe DL and Bergstedt BV, 1979. Measuring and estimating the bioconcentration factor of chemicals in fish. J. Fish. Res. Board Can. 36: 1040-1048. Veith GD, Macek KJ, Petrocelli SR and Carroll J, 1980. An evaluation of using partition coefficients and water solubility to estimate bioconcentration factors for organic chemicals in fish. In: Eaton JG, Parrish PR, and Hendricks AC, eds. Aquatic Toxicology. ASTM STP 707. American Society for Testing and Materials, Philadelphia, PA, USA, pp. 116-129. Wan Y, Jin X, Hu J and Jin F, 2007. Trophic dilution of polycyclic aromatic hydrocarbons (PAHs) in a marine food web from Bohai Bay, North China. Environ. Sci. Technol. 41: 3109-3114. Wang X and Wang WX, 2006. Bioaccumulation and transfer of benzo(a)pyrene in a simplified marine food chain. Mar. Ecol. Prog. Ser. 312: 101-111. Weinstein JE, 2001. Characterization of the acute toxicity of photoactivated fluoranthene to glochidia of the freshwater mussel, Utterbackia imbecillis. Environ. Toxicol. Chem. 20: 412-419. Weinstein JE, 2002. Photoperiod effects on the UV-induced toxicity of fluoranthene to freshwater mussel glochidia: Absence of repair during dark periods. Aquat. Toxicol. 59: 153-161. Weinstein JE and Garner TR, 2008. Piperonyl butoxide enhances the bioconcentration and photoinduced toxicity of fluoranthene and benzo[a]pyrene to larvae of the grass shrimp (Palaemonetes pugio). Aquat. Toxicol. 87: 28-36. Weinstein JE and Oris JT, 1999. Humic acids reduce the bioaccumulation and photoinduced toxicity of fluoranthene to fish. Environ. Toxicol. Chem. 18: 2087-2094. Weinstein JE and Polk KD, 2001. Phototoxicity of anthracene and pyrene to glochidia of the freshwater mussel Utterbackia imbecillis. Environ. Toxicol. Chem. 20: 2021-2028. Weinstein JE, Sanger DM and Holland AF, 2003. Bioaccumulation and toxicity of fluoranthene in the estuarine oligochaete Monopylephorus rubroniveus. Ecotox. Environ. Saf. 55: 278-286. Weston DP, 1990. Hydrocarbon bioaccumulation from contaminated sediment by the deposit-feeding polychaete Abarenicola pacifica. Mar. Biol. 107: 159-169. Widdows J, Moore SL, Clarke KR and Donkin P, 1983. Uptake, tissue distribution and elimination of [114 C] naphthalene in the mussel Mytilus edulis. Mar. Biol. 76: 109-114. Wilcoxen SE, Meier PG and Landrum PF, 2003. The toxicity of fluoranthene to Hyalella azteca in sediment and water-only exposures under varying light spectra. Ecotox. Environ. Saf. 54: 105-117. Wildi E, Nagel R and Steinberg CEW, 1994. Effects of pH on the bioconcentration of pyrene in the larval midge, Chironomus riparius. Wat. Res. 28: 2553-2559. Yakata N, Sudo Y and Tadokoro H, 2006. Influence of dispersants on bioconcentration factors of seven organic compounds with different lipophilicities and structures. Chemosphere 64: 1885-1891. RIVM report 601779002 35 36 RIVM report 601779002 Annex I Overview of BCF values from studies that were rated as not reliable (validity 3) Total Exp. Test Parent Type Reliability remark f) a) b) c) d) e) BCF (ww) BCF (ww) type Ref. SR UD 1778 – Equi. Value based on dry weight [47] SR UD 1820 – Equi. Value based on dry weight [47] S UD nr nr – S U – 30 Equi. U U U – – 71.5, 4153) 245.5 283.7 – Equi. Equi. Equi. FT UD 13000 – Equi. FT U – Equi. S U 25, 25, 1754) – 302 Equi. S UD – 6.1 Equi. S UD – 51.3 Equi. Short, static exposure; steady state unlikely [5] Mollusca Rangia cuneata NR UD 9.30 6.1 Equi. No steady state [44] Crustacea Daphnia magna S U – 57 – 745) S U – 19 UD – 1270 Equi. Static exposure, only nominal [30] exposure concentration reported Kin. Short, static exposure; constant [38] exposure unlikely Kin. BCF calculated based on con[27] centrations at beginning and end of depuration phase and nominal water concentrations S U – 24.9 – 6) 1548 Equi. Static exposure, no monitoring of [10] water concentrations S U – 130 S U – 6965 Equi. Static exposure, steady state unlikely Equi. Static exposure, steady state unlikely Species g) Naphthalene Pisces Brachydanio rerio (larvae) Brachydanio rerio (eggs) Cyprinodon variegatus Leuciscus idus melanotus Morone saxatilis Oncorhynchus mykiss2) Pimephales promelas Theragra chalcogramma (eggs) Theragra chalcogramma (larvae) FT FT S Hemigrapsus nudus S Insecta Somatochlora cingulata Algae Chlorella fusca Selenastrum capricornutum RIVM report 601779002 1) Short exposure to oil; concentrations only in graphs; steady state unlikely 3-day static exposure, no aeration Exposure less than 96h Exposure less than 96h Static exposure, biotransformation reported, BCF in bile Biotransformation reported, BCF in bile Biotransformation reported, BCF in different tissues No constant exposure, exposure less than 96h Short, static exposure; steady state unlikely [1] [17 [48] [48] [40] [40] [40] [12] [5] [18] [6] 37 Species Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) Ref. S S UD UD [13] [34] FT Short, static exposure Short, static exposure; decrease in exposure concentration Exposed to oil, PAH concentration > water solubility; BCF based on lipid weight Kin. Exposed to oil, PAH concentration > water solubility; BCF based on lipid weight g) 9H-Fluorene Pisces Poecilia reticulata Oncorhynchus 2) mykiss (larvae) Scophthalmus maximus 2230 – UD – 422, 512 – FT UD – 1451 SR U – 405, 5003) Equi. Exposure too short to reach steady state [49] NR UD 88, 105 nr Kin. Based on total radioactivity of Equi. initial concentration [34] S UD 9500 – [14] Carassius auratus NR U – 162 Lepomis macrochirus Leuciscus idus melanotus Oncorhynchus 2) mykiss S U – 675 Kin. Sediment exposure, less than 96h; parent compound not distinguished Equi. Exposure concentration and test system unknown Equi. Juveniles exposed for 4h only S U – 910 S UD – 190, 270 SR UD – 5400 SR UD – 9100 Pimephales promelas Poecilia reticulata S U – 6760 S UD – 7260 Scophthalmus maximus FT UD – 17200 S UD – 560 Oligochaeta Lumbriculus variegatus Magnoliophyta Lemna minor 33100 Equi Kin. Equi. Equi [2] [3] Anthracene Pisces Brachydanio rerio Crustacea Asellus aquaticus 38 Equi. 3-day static exposure, no aeration, no food Equi. Decreasing exposure concentration, no steady state Equi. Exposure concentration above water solubility; exposure to a mixture Equi. Exposure concentration above water solubility Kin. Decreasing exposure concentration, exposure less than 96h Equi. Static exposure, steady state unlikely Equi. Animals exposed to oil; PAH concentration > water solubility; BCF based on lipid weight Equi. Short, static exposure; steady state unlikely [45] [51] [16; 17] [32] [33] [33] [12] [13] [2] [52] RIVM report 601779002 Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) NR UD – 200 Equi. Exposure system and concentration unknown 5) S U – 319 – 607 Equi. DOC present, only initial water concentration used; static exposure 5) Equi. Static exposure; also yeast S U – 230, 370 present in system (as DOC), steady state unlikely S U – 500 Equi. Static exposure; steady state unlikely S U – 512 Kin. Static exposure; constant exposure unlikely FT UD – 1419 Kin. Biotransformation reported, but not corrected for FT UD 947 Kin. Exposure via sediment; author indicates this BCF to be misleading FT UD 10985 9096 Equi. Exposure via sediment; author indicates this BCF to be misleading Ref. Insecta Hexagenia sp. (nymph) NR U Oligochaeta Lumbriculus variegatus S U SR Species Daphnia magna Hyalella azteca g) [21] [30] [39] [39] [38] [26] [26] [26] 3500 Equi. Exposure system and concentration unknown; also yeast present in system (as DOC), steady state unlikely [21] – 40700 [24] U – 1010, 14103) Equi. Static exposure; sediment present; steady state unlikely Equi. Steady state unlikely; exposure concentration above water solubility S U – 7800 [16] S U – 7770 S U 7800 – Equi. Static exposure; steady state unlikely; exposure concentration above water solubility Equi. Static exposure; steady state unlikely; exposure concentration above water solubility Equi. Static exposure; steady state unlikely; little details on setup reported S UD 11446 – [14] SR UD – Clupea harengus SR UD 7943 – 91203) 20893 Gadus morhua SR UD 10715 – Kin. Exposure via sediment for less than 96h Equi. BCF values based on dry weight; early life stages used Equi. BCF values based on dry weight; early life stages used Equi. BCF values based on dry weight; early life stages used Algae Chlorella fusca Selenastrum capricornutum [49] [18] [36] Phenanthrene Pisces Brachydanio rerio RIVM report 601779002 – [47] [47] [47] 39 Species Leuciscus idus melanotus Oryzias javanicus Pagrus major Parlychthys olivaceus Pimephales promelas Scophthalmus maximus Mollusca Modiola modiolus FT UD – 10300 FT UD – 936 SR UD 11220 – S UD 3.1 – NR UD 240 32 S UD – S U S Equi. Exposure to oil, PAH concen[2] tration appears to be above water solubility Kin. Exposure to oil, PAH concen[3] tration appears to be above water solubility Equi. BCF values based on dry weight; [47] early life stages used Equi. Low on experimental detail, exposure concentration unclear. Kin. Low on experimental detail, exposure type not reported; steady state not reached [46] 1300 Equi. Short, static exposure; steady state unlikely [52] – 34700 Equi. Static exposure; sediment present; steady state unlikely [24] U – 1760 [18] S U – 10620 S U 4.22 – 4.477) – Thalassiosira pseudonana S U 17 – Thalassiosira weissfloggii S U 38.3 – Equi. Short, static exposure; steady state unlikely Equi. Short, static exposure; steady state unlikely Equi. Static exposure; steady state unlikely; BCF value based on dry weight and total radioactivity Equi. Static exposure; steady state unlikely; BCF value based on dry weight and total radioactivity Equi. Static exposure; steady state unlikely; BCF value based on dry weight and total radioactivity Rangia cuneata Crustacea Asellus aquaticus Oligochaeta Lumbriculus variegatus Algae Chlorella fusca Selenastrum capricornutum 40 Exp. Test Parent Type Reliability remark f) Ref. Total a) b) c) d) e) g) type BCF (ww) BCF (ww) S U – 1760 Equi. No air or food was provided; [17] exposure for 72h FT U – 150 Equi. Exposed to oversaturated PAH [7] mixture FT U – 180 Equi. Exposed to oversaturated PAH [7] mixture FT U – 173, 7372) Equi. Exposed to oversaturated PAH [7] mixture ;BCF values in different tissues FT U – 75 Equi. Exposed to oversaturated PAH [7] mixture 2) Equi. Exposed to oversaturated PAH [7] FT U – 10, 181 mixture; BCF values in different tissues S U – 6760 Kin. Static exposure for less than 96h [12] [44] [6] [20] [15] [15] RIVM report 601779002 Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) Ref. S U – 3388 [12] FT UD – >10000 Mollusca Utterbackia imbecillis (glochidia) SR U – 2147 Equi. BCF averaged for 5 different ex- [56] posure concentrations; individual exposure concentrations uncertain Crustacea Palaemonetes pugio (larvae) SR U – 142 Equi. BCF averaged for different ex[54] posure concentrations; individual exposure concentrations uncertain Oligochaeta Lumbriculus variegatus S U – 27500 FT U – SR U – 1510 – 30803) 10893 Equi. Static exposure; sediment [24] present; steady state unlikely Equi. Short exposure; steady state [49] unlikely Equi. BCF averaged for different ex[55] posure concentrations; individual exposure concentrations uncetain S UD 4333 – SR UD – Carassius auratus NR U 10000 – 549543) – Clupea harengus SR UD 97724 – Gadus morhua SR UD 60256 – Oryzias javanicus FT U – 15 Pagrus major FT U – 10 FT U – 9, 572) FT U – 5 FT U – 4, 52 Species g) Fluoranthene Pisces Pimephales promelas Scophthalmus maximus Monopylephorus rubroniveus Kin. Decreasing exposure concentration Equi. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight [2] Pyrene Pisces Brachydanio rerio Parlychthys olivaceus RIVM report 601779002 457 2) Kin. Exposure via sediment for less than 96h Equi. BCF values based on dry weight; early life stages used Equi. Exposure concentration above water solubility Equi. BCF values based on dry weight; early life stages used Equi. BCF values based on dry weight; early life stages used Equi. Exposed to oversaturated PAH mixture Equi. Exposed to oversaturated PAH mixture Equi. Exposed to oversaturated PAH mixture ; BCF values in different tissues Equi. Exposed to oversaturated PAH mixture Equi. Exposed to oversaturated PAH mixture ; BCF values in different tissues [14] [47] [45] [47] [47] [7] [7] [7] [7] [7] 41 Species Poecilia reticulata Scophthalmus maximus Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) S UD – 4810 Equi. Short, static exposure; steady state unlikely FT UD – <5000 Equi. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight Ref. g) [13] [2] Mollusca Mytilus edulis FT UD – 334300 Equi. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight [2] Crustacea Asellus aquaticus S UD – 2050 Equi. Short, static exposure; steady state unlikely [52] S U – 380000 [24] SR U – 1480 – 3) 2370 Equi. Static exposure; sediment present; steady state unlikely Equi. Short exposure; steady state unlikely S U – 16760 Equi. Static exposure; steady state unlikely [6] S U – 350 [17] FT UD – >10000 Equi. No food, no aeration; exposure concentration above water solubility Equi. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight S U – 2920 Kin. Static exposure; constant exposure unlikely [38] S U – 3090000 Equi. Static exposure; sediment present; steady state unlikely [24] S U – 3180 Equi. Static exposure; steady state unlikely [17] FT U – 10 [7] Pagrus major FT U – 15 Scophthalmus maximus FT UD – >10000 FT UD – 54 Equi. Exposure concentration above water solubility Equi. Exposure concentration above water solubility Equi. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight Kin. Exposure to oil, PAH concentration above water solubility; BCF based on lipid weight Oligochaeta Lumbriculus variegatus Algae Selenastrum capricornutum [49] Benz[a]anthracene Pisces Leuciscus idus melanotus Scophthalmus maximus Crustacea Daphnia magna Oligochaeta Lumbriculus variegatus Algae Chlorella fusca [2] Chrysene Pisces Oryzias javanicus 42 [7] [2] [3] RIVM report 601779002 Parent Type Reliability remark f) Total Exp. Test a) b) c) d) e) BCF (ww) BCF (ww) type Ref. NR UD 31.56 8.2 Equi. Exposure type not reported; steady state unlikely [44] Crustacea Rhepoxynius abronius SD U – 1141 Equi. Exposure via sediment; exposure [4] concentration above water solubility Oligochaeta Lumbriculus variegatus S U – 3020000 Equi. Static exposure; sediment present; steady state unlikely [24] S UD 3600 – [14] SR UD – FT U 20893 – 3311313) – D U – 30 – 1403) Gillichthys mirabilis S U 20 – 3,4) 7400 S U – 490 FT FT UD UD – – 3208 225 FT UD – 301 Kin. Exposure via sediment for less than 96h Equi. BCF values based on dry weight; early life stages used Equi. Short exposure; steady state unlikely Equi. Exposure in model ecosystem; exposure concentration appears to be above water solubility Equi. Based on total radioactivity; based on several organs; short exposure concentration, steady state unlikely Equi. Very short static exposure; steady state unlikely Kin. Not fed; short exposure Kin. Humic material present; short exposure Equi. Humic material present; short exposure; steady state unlikely Equi. Short, static exposure; steady state unlikely Equi. Exposed to oversaturated PAH mixture Kin. Short exposure; uncertain exposure concentration; based on total radioactivity Species Mollusca Rangia cuneata g) Benzo[a]pyrene Pisces Brachydanio rerio Dorosoma cepedianum Gambusia affinis Lepomis macrochirus 3.2, 3.7 Leuciscus idus melanotus Oryzias javanicus S U – 480 FT U – 5 Salmo salar FT UD 1160 – 23101) – FT U – 4 – 416) FT U – 236 – 244 Mollusca Corbicula japonica Crassostrea virginica RIVM report 601779002 6) Equi. Short exposure; no constant exposure concentration Equi. Initial concentration above water solubility; steady state unlikely; BCF values based on dry weight [47] [31] [35] [28] [51] [22] [37] [37] [17] [7] [23] [25] [11] 43 Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) FT UD 255 – Equi. Based on total radioactivity but metabolism reported; no steady state SR U 6294 – – Equi. BCF based on dry weight and 152783,6) nominal exposure concentrations; photolytic breakdown possible FD U – 100000 Equi. Field collected animals; BCF based on dry weight; exposure unclear FD U – 1400000 Equi. Field collected animals; BCF based on lipid weight; exposure unclear Equi. Exposed in model ecosystem; FT U – 4860 – 3) exposure concentrations appears 7520 to be above water solubility S UD 187, 236 – Equi. No measured water concentrations reported; nominal exposure concentration > water solubility NR UD 55.63 8.7 Equi. Short exposure to oil; no steady state; exposure type not reported Ref. Crustacea Acartia erythraea S UD 5500000 24000 [53] Asellus aquaticus S UD – 32400 Daphnia magna S U – 838 – 27453,5) S U – 1000 – 25005) S U – 8250 S U – 5771 SR U – 289 U – 250 UD – 200 Species Mytilus edulis Physa spp. Rangia cuneata Palaemonetes pugio (larvae) Insecta Chironomus riparius S th (4 instar larvae) S 44 Kin. Short, static exposure; also uptake via food Equi. Short, static exposure; steady state unlikely Equi. Short, static exposure; DOC present; only initial exposure concentration used; steady state unlikely Equi. Short, static exposure; yeast present, resulting in dietary uptake as well; steady state unlikely Equi. Short, static exposure; biotransformation reported; no constant exposure; steady state unlikely Kin. Short, static exposure; constant exposure unlikely Equi. BCF averaged for different exposure concentrations; individual exposure concentrations uncertain g) [41] [50] [42] [42] [35] [43] [44] [52] [30] [39] [39] [38] [54] Equi. Exposure concentration reported [9] in graphs only and above water solubility; sediment present Equi. Short, static exposure; reported [29] BCF is average for several exposure concentrations; steady state unlikely RIVM report 601779002 Parent Type Reliability remark f) Total Exp. Test a) b) c) d) e) BCF (ww) BCF (ww) type Equi. Exposed in model ecosystem; D U – 2093 – 3) exposure concentration appears 2120 to be above water solubility Ref. Oligochaeta Lumbriculus variegatus S U – 18200000 Equi. Static exposure; sediment present; steady state unlikely [24] Nematoda Caenorhabiditis elegans S U >25000 – Equi. Short exposure above water solubility; BCF reported in graphs only; steady state unlikely [19] S U – 3300 [17] Fucus vesiculosus FT UD 55.4 – Oedogonium cardiacum D U – 3610, 41053) Equi. Short, static exposure; steady state unlikely Equi. Based on total radioactivity, but metabolism observed; steady state unlikely Equi. Exposed in model ecosystem; exposure concentration appears to be above water solubility FD U – 430000 [42] FD U – 2800000 Equi. Field collected animals; BCF based on dry weight; exposure unclear Equi. Field collected animals; BCF based on lipid weight; exposure unclear S U – 13800000 Equi. Static exposure; sediment present; steady state unlikely [24] Species Culex pipiens quinquefasciatus Algae Chlorella fusca g) [35] [41] [35] Benzo[b]fluoranthene Mollusca Mytilus edulis Oligochaeta Lumbriculus variegatus [42] Benzo[k]fluoranthene Pisces Oryzias latipes nr U – 17 Equi. Only nominal exposure concentration reported, concentration in fish only reported in graphs [8] Mollusca Mytilus edulis FD U – 300000 [42] FD U – 1700000 Equi. Field collected animals; BCF based on dry weight; exposure unclear Equi. Field collected animals; BCF based on lipid weight; exposure unclear S U – 15100000 Equi. Static exposure; sediment present; steady state unlikely [24] S UD – 16000 Equi. Short, static exposure; steady state unlikely [52] Oligochaeta Lumbriculus variegatus [42] Benzo[ghi]perylene Crustacea Asellus aquaticus RIVM report 601779002 45 Species Exp. Test Parent Type Reliability remark f) Total a) b) c) d) e) type BCF (ww) BCF (ww) Ref. Oligochaeta Lumbriculus variegatus S g) U – 33100000 Equi. Static exposure; sediment present; steady state unlikely [24] S U – 10 Equi. Short, static exposure; steady state unlikely [17] S U – 666 – 9685) Equi. Short, static exposure; DOC pre- [30] sent; only initial exposure concentration used; steady state unlikely S U – 20000000 Equi. Static exposure; sediment present; steady state unlikely [24] S U – 2380 Equi. Short, static exposure; steady state unlikely [17] U – 39800000 Equi. Static exposure; sediment present; steady state unlikely [24] Dibenz[a,h]anthracene Pisces Leuciscus idus melanotus Crustacea Daphnia magna Oligochaeta Lumbriculus variegatus Algae Chlorella fusca Indeno[1,2,3-cd]pyrene Oligochaeta Lumbriculus variegatus a) S b) FD: organisms collected from the field; FT: flow-through system; S: static; SR: static renewal; NR: not reported. Test c) d) phases: U: uptake phase only; UD: both uptake and depuration phase. nr: not reported; –: only parent BCF available. nr: e) not reported; –: only total BCF available. Kin.: Kinetic BCF, i.e. k1/k2; Equi.: BCF at (assumed) equilibrium, i.e. f) f) Corganism/Cwater. Main reason(s) for rating the specific BCF value(s) as unreliable. References: [1] (Anderson et al., 1974); [2] (Baussant et al., 2001a); [3] (Baussant et al., 2001b); [4] (Boese et al., 1999); [5] (Carls and Rice, 1988); [6] (Casserly et al., 1983); [7] (Cheikyula et al., 2008); [8] (Chen et al., 2008); [9] (Clements et al., 1994); [10] (Correa and Coler, 1983); [11] (Couch et al., 1979); [12] (De Maagd, 1996); [13] (De Voogt et al., 1991); [14] (Djomo et al., 1996); [15] (Fan and Reinfelder, 2003); [16] (Freitag et al., 1982); [17] (Freitag et al., 1985); [18] (Geyer et al., 1984); [19] (Haitzer et al., 1999a; 1999b); [20] (Halling-Sørensen et al., 2000); [21] (Herbes, 1976); [22] (Jimenez et al., 1987); [23] (Johnsen et al., 1989); [24] (Jonker and Van der Heijden, 2007); [25] (Kira et al., 1996); [26] (Landrum and Scavia, 1983); [27] (Laurén and Rice, 1985); [28] (Lee et al., 1972); [29] (Leversee et al., 1982); [30] (Leversee et al., 1983); [31] (Levine et al., 1997); [32] (Linder and Bergman, 1984); [33] (Linder et al., 1985); [34] (Lockhart et al., 1983); [35] (Lu et al., 1977); [36] (Mailhot, 1987); [37] (McCarthy and Jimenez, 1985); [38] (McCarthy et al., 1985); [39] (McCarthy, 1983); [40] (Melancon Jr and Lech, 1978); [41] (Moy and Walday, 1997); [42] (Murray et al., 1991); [43] (Neff and Anderson, 1975); [44] (Neff et al., 1976a); [45] (Ogata et al., 1984); [46] (Palmork and Solbakken, 1981); [47] (Petersen and Kristensen, 1998); [48] (Seaton and Tjeerdema, 1996); [49] (Sheedy et al., 1998); [50] (Skarphéðinsdóttir et al., 2003); [51] (Spacie et al., 1983); [52] (Van Hattum and Cid Montañes, 1999); [53] (Wang and Wang, 2006); [54] (Weinstein and Garner, 2008); [55] (Weinstein et al., 2003); [56] (Weinstein, 2002) 1) 2) 3) Exposed in salt water (35 ‰). Formerly known as Salmo gairdneri. Values represent (a range of) BCF values from (a 4) 5) range of) different exposure concentrations. Values represent BCF values for different tissues. BCFs were determined 6) 7) at different DOC concentrations. BCFs were determined at different exposure durations. Values represent (a range of) BCF values for (a range of) different lipid contents. 46 RIVM report 601779002 Annex II Overview of BCF values from studies for which validity was not assignable (validity 4) Species Naphthalene Pisces Fundulus heteroclitus Total Exp. Test Parent Type Reliability remark f) a) c) d) b) e) BCF (ww) BCF (ww) type 1) Ref. g) S U 2.0, 2.2 – Equi. Based on total radioactivity [13] S U 1.0 – 1051,2) – [13] Gillichthys mirabilis S UD S Mugil curema FT Oncorhynchus kisutch Platichthys stellatus FT U U 263 – 37·106 1,2,3) – – Equi. Based on total radioactivity; values for different organs Kin. Based on total radioactivity; values for different organs Kin. Values for different organs Equi. BCF based on dry weight U – FT Salmo salar (eggs) S UD U – – FT UD – 150 – 11002,3) 100 – 7003) 18.5 – 82.51,3) 17800 FT UD – 421 FT UD – 266 NR FT D U nr – nr 48 FT FT U UD – – 24 – 592) 2.3 Equi. Exposed to oil; BCF based on lipid weight – Only half-life reported Equi. Steady state reported, but no exposure concentrations Equi. Values for different organs Equi. Exposed to oil S S NR Daphnia pulex Hemigrapsus nudus FT U UD U U 36.5 50 677, 23371) 325 – – – – Equi. Equi. Equi. Equi. Based on total radioactivity Based on total radioactivity Based on total radioactivity Based on total radioactivity; based on one organ [6] [15] [37] [18] S UD 387 nr Equi. Based on total radioactivity [2] FT FT UD UD 387 – nr 5500 Equi. Based on total radioactivity Equi. Exposure to oil [38] [3] FT UD – 1308 Equi. Exposed to oil [3] Scophthalmus maximus Mollusca Mytilus edulis Ostrea edulis Rangia cuneata Crustacea Daphnia magna 81 – 11582) 3) 20 – 80 [25] [11] [35] Equi. BCF based on dry weight; values [35] for different organs Equi. BCF based on dry weight [35] Equi. Based on total radioactivity; [23] exposure of eggs Equi. Exposed to oil; BCF based on [3] lipid weight Kin. Exposed to oil [4] [3] [33] [43] [34] [33] Acenaphthene Pisces Lepomis macrochirus Scophthalmus maximus Mollusca Mytilus edulis RIVM report 601779002 47 Exp. Test Parent Type Reliability remark f) Total a) c) d) b) e) type BCF (ww) BCF (ww) Ref. D D – 128 Kin. Exposed via diet [30] FT UD – 53300 Equi. Exposure to oil [3] FT UD – 2892 Equi. Exposed to oil [3] FT U – D – Equi. No details on exposure concentration Kin. Exposed via diet [16] D 180 – 1) 1800 589 SR U – 1050 Equi. No details on exposure concentration [12] Mollusca Mytilus edulis FT UD – 1018 Equi. Exposed to oil [3] Crustacea Hyalella azteca SR UD 255 – 3151) – Kin. Based on total radioactivity [26] D D – 773 Kin. Exposed via diet [31] SR U – 1016 SR U – 4550 Equi. Exposure concentration is [32] unclear Equi. Exposure concentration [12] uncertain, based on two fish only Mollusca Utterbackia imbecillis (glochidia) SR U – 247 – 4201) Equi. Value based on dry weight [41] Crustacea Daphnia magna Daphnia pulex Rhepoxynius abronius SR S SD U U U – 760 – 2699 – 3267 – 267861) Equi. Exposure concentration unclear Equi. Based on total radioactivity Equi. Exposure via sediment [32] [21] [7] Insecta Chironomus riparius FT (larvae) U 47 – 1964 – Kin. Based on total radioactivity [17] FD FD nr nr – – 23.6 6.6 Equi. Exposed in the field Equi. Exposed in the field [5] [5] D D – 613 Kin. Exposed via diet [31] Species g) Acenaphthylene Pisces Oncorhynchus 4) mykiss Scophthalmus maximus Mollusca Mytilus edulis 9H-Fluorene Pisces Lepomis macrochirus Oncorhynchus mykiss4) Poecilia reticulata [31] Anthracene Pisces Oncorhynchus mykiss4) Pimephales promelas Poecilia reticulata Polychaeta Capitella capitata Polychaete sp. 1) Phenanthrene Pisces Oncorhynchus mykiss4) 48 RIVM report 601779002 Exp. Test Parent Type Reliability remark f) Total a) c) d) b) e) type BCF (ww) BCF (ww) Ref. FT NR UD D – nr Equi. Exposed to oil – Only half-lives reported [3] [33] Crustacea Daphnia magna Daphnia pulex S NR UD U Equi. Based on total radioactivity Equi. Based on total radioactivity [15] [37] Hyalella azteca SR UD 600 – 1165 – – 14241) 440 – 5041) – Kin. Based on total radioactivity [26] Polychaeta Capitella capitata Polychaete sp. FD FD nr nr – – 30.7 5.7 Equi. Exposed in the field Equi. Exposed in the field [5] [5] D D – 531 Kin. Exposed via diet [31] FT UD – 14836 [10] SR U – 9054 Kin. Short exposure; BCF value maybe based on dry weight Equi. BCF value based on dry weight [40] S FT NR UD UD D 14 – nr – 2932 nr Kin. Based on total radioactivity Equi. Exposed to oil – Only half-lives reported [1] [3] [33] SR UD UD SR U [44] SD U 980 – 1) 4741 – Kin. Based on nominal exposure concentration Equi. Based on nominal exposure concentration Equi. Based on total radioactivity [22] SR 28095 – 1) 56757 1932 – 23351) – 18470 – 1) 50484 Equi. Exposure via sediment [7] FD FD nr nr – – 12 5.7 Equi. Exposed in the field Equi. Exposed in the field [5] [5] FD U – 61 Equi. Exposed in the field [36] SR U – 11300 Equi. Based on 2 fish only; little detail reported [12] NR SR D U nr – nr 830 – 1) 1229 Only half-lives reported Equi. Value based on dry weight [33] [41] S U 1400 – Equi. Based on total radioactivity [18] Species Mollusca Mytilus edulis 2932 nr g) Fluoranthene Pisces Oncorhynchus mykiss4) Pimephales promelas Mollusca Macomona liliana Mytilus edulis Crustacea Diporeia spp. Hyalella azteca Rhepoxynius abronius Polychaeta Capitella capitata Polychaete sp. [22] Pyrene Pisces Acanthogobius flavimanus Poecilia reticulata Mollusca Mytilus edulis Utterbackia imbecillis (glochidia) Crustacea Daphnia magna RIVM report 601779002 49 Species Hyalella azteca Polychaeta Capitella capitata Polychaete sp. Exp. Test Parent Type Reliability remark f) Total a) c) d) b) e) type BCF (ww) BCF (ww) SR UD 2323 – – Kin. Based on total radioactivity 51651) Ref. g) [26] FD FD nr nr – – 13.3 5.2 Equi. Exposed in the field Equi. Exposed in the field [5] [5] S U >11000 – Equi. Values only reported in graph only [20] D D – 325 Kin. Exposed via diet [33] NR U – Equi. Based on total radioactivity [37] SD U 803 – 11061) – 2832 – 1) 25465 Equi. Exposure via sediment [7] FD FD nr nr – – 3.6 9.4 Equi. Exposed in the field Equi. Exposed in the field [5] [5] S FT SD UD U U 5500 – – – 950 1560 – 1) 21080 Equi. Based on total radioactivity [15] Equi. BCF value reported in graph only [8] Equi. Exposure via sediment [7] FD FD nr nr – – 6.2 14.7 Equi. Exposed in the field Equi. Exposed in the field [5] [5] Pisces FT Gambusia affinis Gillichthys mirabilis S U U 22 Equi. Exposed in model ecosystem Kin. Based on total radioactivity; based on several organs Kin. Based on total radioactivity [28] [25] nr Nematoda Caenorhabiditis elegans Benz[a]anthracene Pisces Oncorhynchus 4) mykiss Crustacea Daphnia pulex Rhepoxynius abronius Polychaeta Capitella capitata Polychaete sp. Chrysene Crustacea Daphnia magna Eurytemora affinis Rhepoxynius abronius Polychaeta Capitella capitata Polychaete sp. Benzo[a]pyrene Lepomis macrochirus Lutjanus argentimaculatus Oligocottus maculosus Oncorhynchus mykiss4) Oryzias javanicus Salmo salar (eggs) Mollusca Mytilus edulis Physa spp. 50 S UD – 158 – 57451) 4700 S U 275000 S U 70 – 200 D D – 261 Equi. Exposure in simplified marine food chain Equi. Based on total radioactivity; based on several organs Kin. Exposed via diet FT S U U – 8.2 – 70.71,3) 5 – Equi. BCF value reported in graph only [9] Equi. Based on total radioactivity [23] FD FT D U nr – nr 2177 – Only half-lives reported Equi. Exposed in model ecosystem nr 1) [27] [39] [25] [31] [14] [28] RIVM report 601779002 Species Crustacea Acartia erythraea Daphnia magna Daphnia pulex Insecta Culex pipiens quinquefasciatus Exp. Test Parent Type Reliability remark f) Total a) c) d) b) e) type BCF (ww) BCF (ww) FT U – 3056 Equi. Exposed to mixture in model ecosystem Ref. S UD 5500000 24000 [39] S S NR U U U 5990 5990 1259, 27201) FT U FT [28] – – – Kin. Exposure in simplified marine food chain Equi. Based on total radioactivity Equi. Based on total radioactivity Equi. Based on total radioactivity [6] [24] [37] – 37 Equi. Exposed in model ecosystem [28] U – 453 Equi. Exposed to mixture in model ecosystem [28] U – Equi. Exposed via sediment [42] nr nr – – 4700 – 110001) 0.7 13.8 Equi. Exposed in the field Equi. Exposed in the field [5] [5] FT U – 1300 [8] SD U – 1657 – 167721) Equi. Pooled value for benzo[k]fluoranthene and benzo[b]fluoranthene Equi. Exposure via sediment FD FD nr nr – – 1.7 9.1 Equi. Exposed in the field Equi. Exposed in the field [5] [5] Polychaeta Aberenicola pacifica S Capitella capitata Polychaete sp. g) FD FD Benzo[b]fluoranthene Crustacea Eurytemora affinis Rhepoxynius abronius Polychaeta Capitella capitata Polychaete sp. [7] Benzo[k]fluoranthene Crustacea Eurytemora affinis FT U – 1300 Equi. Pooled value for benzo[k]fluoranthene and benzo[b]fluoranthene [8] Polychaeta Capitella capitata Polychaete sp. FD FD nr nr – – 1.8 14.1 Equi. Exposed in the field Equi. Exposed in the field [5] [5] a b) FD: organisms collected from the field; FT: flow-through system; S: static; SR: static renewal; NR: not reported Test c) d) phases: U: uptake phase only; UD: both uptake and depuration phase. nr: not reported; –: only parent BCF available nr: e) not reported; –: only total BCF available. Kin.: Kinetic BCF, i.e. k1/k2; Equi.: BCF at (assumed) equilibrium, i.e. f) g) Corganism/Cwater. Main reason for rating the specific BCF value(s) not assignable. References: [1] (Ahrens et al., 2002); [2] (Barrows et al., 1980); [3] (Baussant et al., 2001a); [4] (Baussant et al., 2001b); [5] (Bayona et al., 1991); [6] (Black et al., 1993); [7] (Boese et al., 1999); [8] (Cailleaud et al., 2009); [9] (Cheikyula et al., 2008); [10] (Cho et al., 2003); [11] (Correa and Venables, 1985); [12] (De Voogt et al., 1991); [13] (DiMichele and Taylor, 1978); [14] (Dunn and Stich, 1976); [15] (Eastmond et al., 1984); [16] (Finger et al., 1985); [17] (Gerould et al., 1983); [18] (Gharrett and Rice, 1987); [18] (Granier et al., 1999); [20] (Haitzer et al., 1999a); [21] (Herbes and Risi, 1978); [22] (Kane Driscoll et al., 1997); [23] (Kuhnhold and Busch, 1978); [24] (Kukkonen et al., 1990); [25] (Lee et al., 1972); [26] (Lee et al., 2002); [27] (Leversee et al., 1981); [28] (Lu et al., 1977); [29] (Neff et al., 1976b); [30] (Niimi and Dookhran, 1989); [31] (Niimi and Palazzo, 1986); [32] (Oris et al., 1990); [33] (Rantamäki, 1997); [34] (Riley et al., 1981); [35] (Roubal et al., 1978); [36] (Takeuchi et al., 2009); [37] (Trucco et al., 1983); [38] (Veith et al., 1980); [39] (Wang and Wang, 2006); [40] (Weinstein and Oris, 1999); [41] (Weinstein and Polk, 2001); [42] (Weston, 1990); [43] (Widdows et al., 1983); [44] (Wilcoxen et al., 2003). 1) 2) Values represent (a range of) BCF values from (a range of) different exposure concentrations. Values represent BCF 3) 4) values for different tissues. BCFs were determined at different exposure durations. Formerly known as Salmo gairdneri. RIVM report 601779002 51 RIVM National Institute for Public Health and the Environment P.O. Box 1 3720 BA Bilthoven The Netherlands www.rivm.com
© Copyright 2026 Paperzz