Contaminants in fish from U.S. rivers: Probability-based national assessments.

Most fish consumption advisories in the United States (U.S.) are issued for mercury and polychlorinated biphenyls (PCBs), and recently per- and polyfluoroalkyl substances (PFAS) have become a contaminant group that warrants fish consumption advice. An unequal probability survey design was developed to allow a comprehensive characterization of mercury, PCB, and PFAS contamination in fish from U.S. rivers on a national scale. During 2013-14 and 2018-19, fish fillet samples were collected from 353 and 290 river sites, respectively, selected randomly from the target population of rivers (≥5th order in size) in the conterminous U.S. These comprised nationally representative samples, with results extrapolated to chemical-specific sampled populations of 48,826-79,448 river kilometers (km) in 2013-14 and 66,142 river km in 2018-19. National distribution estimates were developed for total mercury, all 209 PCB congeners, and up to 33 PFAS (including perfluorooctane sulfonate or PFOS) in river fish. All fillet tissue samples contained detectable levels of mercury and PCBs. One or more PFAS were detected in 99.7 % and 95.2 % of the fillet samples from fish collected in 2013-14 and 2018-19, respectively. Fish tissue screening levels applied to national contaminant probability distributions allowed an estimation of the percentage of the sampled population of river lengths that contained fish with fillet concentrations above a level protective of human health. Fish tissue screening level exceedances for an average level of fish consumption ranged from 23.5 % to 26.0 % for mercury, 17.3 % to 51.6 % for PCBs, and 0.7 % to 9.1 % for PFOS.

An Evaluation of Fish Tissue Monitoring Alternatives for Mercury and Selenium: Fish Muscle Biopsy Samples Versus Homogenized Whole Fillets.

Fish contaminant studies with human health protection objectives typically focus on muscle tissue, recognizing that fillets are the commonly consumed tissue fraction. Muscle biopsy punch sampling for mercury analysis has recently been used as an alternative to harvesting fish for fillets; however, there is limited information comparing fillet plug results to whole fillet results. This study was conducted to address that data gap and to test the applicability of plugs for monitoring associated with United States Environmental Protection Agency's fish tissue-based mercury and selenium water quality criteria. The mercury phase included 300 fillet homogenates and 300 field-extracted plug samples from 60 fish, and the selenium phase included 120 fillet homogenates and 120 plugs from 30 fish. Both phases showed that there were no statistically significant differences between fillet plug and homogenized fillet results at the community level; however, a selenium plug monitoring alternative must employ a sufficiently sensitive analytical method and consider total solids. Plug and fillet sampling alternatives have inherent advantages and disadvantages. Fillet sampling provides sufficient mass to consider multiple contaminants but requires fish to be harvested. Plug sampling only provides adequate mass for a single analyte but may allow fish survival, although additional research is needed on survival following plug removal.

Perfluorinated compounds in fish from U.S. urban rivers and the Great Lakes.

Perfluorinated compounds (PFCs) have recently received scientific and regulatory attention due to their broad environmental distribution, persistence, bioaccumulative potential, and toxicity. Studies suggest that fish consumption may be a source of human exposure to perfluorooctane sulfonate (PFOS) or long-chain perfluorocarboxylic acids. Most PFC fish tissue literature focuses on marine fish and waters outside of the United States (U.S.). To broaden assessments in U.S. fish, a characterization of PFCs in freshwater fish was initiated on a national scale using an unequal probability design during the U.S. Environmental Protection Agency's (EPA's) 2008-2009 National Rivers and Streams Assessment (NRSA) and the Great Lakes Human Health Fish Tissue Study component of the 2010 EPA National Coastal Condition Assessment (NCCA/GL). Fish were collected from randomly selected locations--164 urban river sites and 157 nearshore Great Lake sites. The probability design allowed extrapolation to the sampled population of 17,059 km in urban rivers and a nearshore area of 11,091 km(2) in the Great Lakes. Fillets were analyzed for 13 PFCs using high-performance liquid chromatography tandem mass spectrometry. Results showed that PFOS dominated in frequency of occurrence, followed by three other longer-chain PFCs (perfluorodecanoic acid, perfluoroundecanoic acid, and perfluorododecanoic acid). Maximum PFOS concentrations were 127 and 80 ng/g in urban river samples and Great Lakes samples, respectively. The range of NRSA PFOS detections was similar to literature accounts from targeted riverine fish sampling. NCCA/GL PFOS levels were lower than those reported by other Great Lakes researchers, but generally higher than values in targeted inland lake studies. The probability design allowed development of cumulative distribution functions (CDFs) to quantify PFOS concentrations versus the sampled population, and the application of fish consumption advisory guidance to the CDFs resulted in an estimation of the proportion of urban rivers and the Great Lakes that exceed human health protection thresholds.