PAH Sediment Screening for the Protection of Fish: A Proposed Framework Lyndal Johnson, NOAA Fisheries and Jeremy Buck, US Fish and Wildlife Service SMARM Meeting May 6, 2015 Are we aware of both the physical and chemical habitat requirements of Pacific salmon, such that
Beth Horness Laura Inouye John Incardona Dan Lomax Jim Meador Mark Myers Rob Neely Sandie O Neill Jennifer Peers Contributors Jim West Gina Ylitalo and NWFSC Environmental Assessment Program
Sediment Evaluation Framework (SEF 2009)) SEF Guidelines or Benchmarks: Sediment Screening Levels (SLs) Target Tissue Levels (TTLs) for Invertebrates and Fish, Wildlife, and Humans
Fish TTLs for Contaminants! The Target Tissue Value approach has been applied for some major classes of contaminants, e.g.! PCBs for salmon (Meador et al. 2002)! DDTs for fish (Beckvar et al. 2005)! Methyl mercury for fish (Beckvar et al. 2005)! Translating to sediment value site specific BSAFs! Many contaminants of concern for which values aren t available, but at least a viable approach! Revised criteria based on human health concerns (e.g., new Ecology sediment standards) would protect fish for most compounds (lead, mercury, selenium, TBT, PCP pyrene, phenanthrene possible exceptions)
PAH SLs & TTLs for Fish: Problems and limitations! Current SLs are based on synoptic field data combining chemistry with invertebrate bioassay and/or benthic data! May be protective of fish prey base, but not direct effects on fish! TTL approach proposed as alternative for protection of fish for bioaccumulative compounds! Fish metabolize PAHs, so TTLs won t work; something different needed
Exposure Pathway/Assessment! Direct correlation of sediment PAH levels with biological effects! Alternatives to TTLs! Dietary effects thresholds! Metabolites of PAHs in bile of fish
Exposure Pathway/Assessment! Direct correlation of sediment PAH levels with biological effects! Alternatives to TTLs! Metabolites of PAHs in bile of fish! Dietary effects thresholds
English sole injury vs. sediment PAH concentrations Proportion affected 0.8 0.6 0.4 0.2 DNA adducts Liver lesions Inhibited gonadal growth Inhibited spawning Infertile eggs 100 80 60 40 20 DNA adducts (adduct/mol nucleotides) 0 10 100 1000 10000 100000 1000000 Sediment aromatic hydrocarbons (ppb dry wt)
Sediment ΣPAH concentration vs. biological effects in English sole Biological Effect Liver Gonad Inhib. Infertile DNA Reduced PAH Lesions Dev spawn eggs damage Growth (ppb dry wt) (%) (%) (%) (% eggs) (nmol adducts (%change in per mol bases) wt per day) 50 0 15 12 38 5 1.1-1.2 100 0 15 12 38 5 -- 1000 9 15 17 42 25 -- 2000 18 15 25 48 36 -- 3000 24 15 30 51 43 0.05-0.10 5000 31 18 35 55 51 -- 10000 40 27 43 61 63 -- 100000 71 58 69 80 100 --
Liver Lesions In Other Species Winter flounder Threshold for degenerative lesions 300 ng/g total PAHs Starry flounder HydVac Prevalence 0. 7 0. 6 0. 5 0. 4 0. 3 0. 2 0. 1 0. 0-0. 1 threshold = 300 ng/g 1 2 3 4 5 Log sediment TAH (ng/g dry wt) Threshold = 1,950 ng/g Threshold = 1,950 ng/g SDN prevalence Threshold = 2.9 ug/g dry wt Threshold for degenerative lesions 1950 ng/g Total PAHs 0 10 100 1000 10000 Sediment PAHs (ng/g dry wt)
Liver Lesions in Other Species Brown Bullhead Neoplasm prevalence Threshold = 3.4 µg/g dry wt Threshold = 3,400 ng/g Threshold for neoplasms 3400 ng/g total PAHs 100 1000 10000 100000 Sediment PAHs (ng/g dry wt) Threshold for FCA and neoplasms 2900 ng/g total PAHs Neoplasm/FCA prevalence Threshold = 2.9 µg/g dry wt Threshold = 2,900 ng/g 100 1000 10000 100000 Sediment PAHs (ng/g dry wt)
Additional Studies of ΣPAH concentration in sediments vs. biological effects Species Compound Endpoint Concentration Reference Pink salmon eggs PAHs in weathered oil Embryo mortality 2800 ng/g dry wt (LOEC) Murphy et al. 1999 Pink salmon embryos PAHs in weathered oil Embryo mortality 2800-4600 ng/g dry wt (LOEC) Heinz et al. 1999 Senegalese sole PAHs in sediment Degenerative liver lesions Turbot PAHs in sediment Reduced growth; lipid depletion 1100 ng/g dry wt Costa et al. 2009 2000-3000 ng/g dry wt (LOEC) Kerambrum et al. 2012 White perch PAHs in sediment Altered stress response 3000-4000 ng/g dry wt (LOEC) Hontela et al. 1995 Mummichog PAHs in sediment (BaP only) EROD activity in the intestine 3500 ng/g dry wt (LOEC) Couillard et al. 2009 Mummichog PAHs in sediment Liver neoplasms 16000 ng/g dry wt (NOEC) White paper Zebrafish PAHs in sediment Developmental abnormalities 28000 ng/g dry wt (LOEC) Raimudo et al. 2014 Zebrafish PAHs in sediment Mortality 78000 ng/g dry wt (LOEC) Raimudo et al. 2014
Cumulative Distribution for Sediment PAH studies 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% 0 10 20 30 40 50 60 70 80 90 Sediment PAH concentration (ug/g dry wt) 10% percentile: 0.9 ug/g dry wt 25% percentile: 1.9 ug/g dry wt For liver lesion thresholds, PAH concentration where prevalence was 2x the background was used
Sediment PAH guidelines and concentrations associated with effects in fish Sediment Total PAHs (ug/g dry wt) 100 10 1 0.1 Prolif lesopms - ES DNA damage - ES HydVac- WF SDN - ES 1+ liver lesions - ES inhibited spawning - ES infertile eggs - ES SDN - ES_NBSP Degen lesions - SS Consensus TEC SDN - SF reduced growth - ET Fish neoplasms - ES egg mortality - PS Neo and FCA - BB stress response - WP Neo only -BB embryo mortaliy - PS LEL ERL inhibited gonad growth-es reduced growth - CS immunotoxicity - CS Consensus MEC Neo-M Consencus PEC PEL FW SL1 FW SL2
Exposure Pathway/Assessment! Alternatives to TTLs! Dietary effects thresholds! Metabolites of PAHs in bile of fish Might be used to derive sediment guidelines to support SLs; or used for Level 2B testing
Exposure Pathway/Assessment! Alternatives to TRVs! Dietary effects thresholds! Metabolites of PAHs in bile of fish Might be used to derive sediment guidelines to support SLs; or used for Level 2B testing
PAHs in sole stomach contents vs. lesions Threshold value of 0.2 mg/ kg wet wt for specific degenerative necrosis (SDN) Threshold value of 0.6 mg/ kg wet wt for neoplasms
Dietary ΣPAH concentrations vs. biological effects Species Endpoint Dose (ug/g fish wt/ day) Concentration in food (ug/g ww) Reference English sole Degenerative lesions - 0.2 2014 white paper English sole Neoplasms - 0.6 2014 white paper Pink salmon Reduced growth rate 0.14 0.9 Carls et al. 1996 English sole Reduced growth rate 0.12 2.3 Rice et al. 2000 Chinook salmon Rainbow trout Chinook salmon Increased growth variability Decreased disease resistance Changes in enzymes related to lipid metabolism 0.7 3.8 Meador et al. 2006 0.66 4.1 Bravo et al. 2010 2.3 12 Meador et al. 2006 Chinook salmon Changes in lipid content 6.1 32 Meador et al. 2006 Chinook salmon Reduced weight 18 95 Meador et al. 2006
Cumulative Distribution for Dietary PAH studies 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% 0 20 40 60 80 100 120 Dietary PAH concentration (ug/g wet wt) 10% percentile: 0.825 ug/g dry wt 25% percentile: 1.95 ug/g dry wt For liver lesion thresholds, PAH concentration where prevalence was 2x the background was used
PAHs in salmon stomach contents (ug/g wet wt) 40 35 30 25 20 15 10 5 0
Exposure Pathway/Assessment! Alternatives to TRVs! Dietary effects thresholds! Metabolites of PAHs in bile of fish
Salmonid bile metabolites vs. PAHs in diet Strong correlation between bile metabolites and dietary dose Dietary PAH concentrations of 2-6 ug/g fish/day correspond to bile metabolite levels of 3-8 ug PHN-FACs/mg bile protein Dietary dose of 18-22 ug/g fish/ day correspond to PHN FACs of 20-35 ug/mg bile protein (See Meador et al. 2008)
Dose, PHN FACs and Toxicity Estimated no effect level of ~2 ug FACs-PHN/mg protein (Meador et al. 2008)
PAH metabolites in bile vs. biological effects Species Endpoint Dose (ug/g fish wt/ day) FACs-PHN (ug/g bile protein) Reference English sole Increased liver lesions prevalence (2-4 x) - 5 PSAT 2007 English sole Reduced growth rate 0.12 4.7 Rice et al. 2000 Pink salmon Reduced growth rate 0.14 4.8 Carls et al. 1996 Rainbow trout Decreased disease resistance 0.66 5.5 Bravo et al. 2010 Chinook salmon Increased growth variability 0.7 3.5 Meador et al. 2006 Dolly varden trout Reduced reproductive hormones - 5 Sol et al. 2000 Chinook salmon Changes in enzymes related to lipid metabolism 2.3 6.3 Meador et al. 2006 Chinook salmon DNA damage in gill tissue - 11 Kelley et al. 2011 Chinook salmon Changes in lipid content 6.1 12 Meador et al. 2006 Chinook salmon Reduced weight 18 36 Meador et al. 2006
Cumulative Distribution for Bile Metabolite Studies 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% 0 5 10 15 20 25 30 35 40 FACs-PHN (ug/mg protein) 10% percentile: 3.5 ug/mg protein 25% percentile: 4.7 ug/mg protein
Bile metabolite concentrations in juvenile salmon 30 25 FACs-PHN (ug/mg protein) 20 15 10 5 0
Other bile metabolite benchmarks! White sucker bile metabolite levels from EMAP (Cormier 2000)! Upper 5%: 0.4 ug FACs-BaP/mg protein 60 ug FACs-NPH/mg protein! Lower 25%: 0.12 ug FACs-BaP/mg protein 23 ug FACs-NPH/mg protein
Bile metabolite concentrations in juvenile salmon 0.4 0.3 FACs-BaP (ug/mg protein) 0.2 0.1 0
Summary of Findings 10 th and 25 th percentile values for PAHs or metabolites in sediment, diet and bile! Sediment PAHs: 0.9-1.9 ug/g dry wt! Dietary PAHs: 0.83 1.95 ug/g wet wt! Bile FACs-PHN: 3.5-4.8 ug/mg protein
Next Steps? Review sediment, diet, and bile data to determine appropriate screening guidelines Consider Conceptual Site Model to determine whether PAHs are an issue (e.g., compare with existing data to see if field caught fish from project area have biliary FACs above thresholds) Identify appropriate test-out options (e.g., bioassays, bioaccumulation tests, field risk assessments) when guidelines are exceeded Develop evaluation framework and incorporate recommendations into the SEF/DMMP