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.

A national probabilistic study of polybrominated diphenyl ethers in fish from US lakes and reservoirs.

Polybrominated diphenyl ethers (PBDEs) are persistent, bioaccumulative, and toxic chemicals that are present in air, water, soil, sediment, and biota (including fish). Most previous studies of PBDEs in fish were spatially focused on targeted waterbodies. National estimates were developed for PBDEs in fish from lakes and reservoirs of the conterminous US (excluding the Laurentian Great Lakes) using an unequal probability design. Predator (fillet) and bottom-dweller (whole-body) composites were collected during 2003 from 166 lakes selected randomly from the target population of 147,343 lakes. Both composite types comprised nationally representative samples that were extrapolated to the sampled population of 76,559 and 46,190 lakes for predators and bottom dwellers, respectively. Fish were analyzed for 34 individual PBDE congeners and six co-eluting congener pairs representing a total of 46 PBDEs. All samples contained detectable levels of PBDEs, and BDE-47 predominated. The maximum aggregated sums of congeners ranged from 38.3 ng/g (predators) to 125 ng/g (bottom dwellers). Maximum concentrations in fish from this national probabilistic study exceeded those reported from recent targeted studies of US inland lakes, but were lower than those from Great Lakes studies. The probabilistic design allowed the development of cumulative distribution functions to quantify PBDE concentrations versus the cumulative number of US lakes from the sampled population.

Occurrence of pharmaceuticals and personal care products in fish: results of a national pilot study in the United States.

Pharmaceuticals and personal care products are being increasingly reported in a variety of biological matrices, including fish tissue; however, screening studies have presently not encompassed broad geographical areas. A national pilot study was initiated in the United States to assess the accumulation of pharmaceuticals and personal care products in fish sampled from five effluent-dominated rivers that receive direct discharge from wastewater treatment facilities in Chicago, Illinois; Dallas, Texas; Orlando, Florida; Phoenix, Arizona; and West Chester, Pennsylvania, USA. Fish were also collected from the Gila River, New Mexico, USA, as a reference condition expected to be minimally impacted by anthropogenic influence. High performance liquid chromatography-tandem mass spectrometry analysis of pharmaceuticals revealed the presence of norfluoxetine, sertraline, diphenhydramine, diltiazem, and carbamazepine at nanogram-per-gram concentrations in fillet composites from effluent-dominated sampling locations; the additional presence of fluoxetine and gemfibrozil was confirmed in liver tissue. Sertraline was detected at concentrations as high as 19 and 545 ng/g in fillet and liver tissue, respectively. Gas chromatography-tandem mass spectrometry analysis of personal care products in fillet composites revealed the presence of galaxolide and tonalide at maximum concentrations of 2,100 and 290 ng/g, respectively, and trace levels of triclosan. In general, more pharmaceuticals were detected at higher concentrations and with greater frequency in liver than in fillet tissues. Higher lipid content in liver tissue could not account for this discrepancy as no significant positive correlations were found between accumulated pharmaceutical concentrations and lipid content for either tissue type from any sampling site. In contrast, accumulation of the personal care products galaxolide and tonalide was significantly related to lipid content. Results suggest that the detection of pharmaceuticals and personal care products was dependent on the degree of wastewater treatment employed.

Survey design for lakes and reservoirs in the United States to assess contaminants in fish tissue.

The National Lake Fish Tissue Study (NLFTS) was the first survey of fish contamination in lakes and reservoirs in the 48 conterminous states based on a probability survey design. This study included the largest set (268) of persistent, bioaccumulative, and toxic (PBT) chemicals ever studied in predator and bottom-dwelling fish species. The U.S. Environmental Protection Agency (USEPA) implemented the study in cooperation with states, tribal nations, and other federal agencies, with field collection occurring at 500 lakes and reservoirs over a four-year period (2000-2003). The sampled lakes and reservoirs were selected using a spatially balanced unequal probability survey design from 270,761 lake objects in USEPA's River Reach File Version 3 (RF3). The survey design selected 900 lake objects, with a reserve sample of 900, equally distributed across six lake area categories. A total of 1,001 lake objects were evaluated to identify 500 lake objects that met the study's definition of a lake and could be accessed for sampling. Based on the 1,001 evaluated lakes, it was estimated that a target population of 147,343 (+/-7% with 95% confidence) lakes and reservoirs met the NLFTS definition of a lake. Of the estimated 147,343 target lakes, 47% were estimated not to be sampleable either due to landowner access denial (35%) or due to physical barriers (12%). It was estimated that a sampled population of 78,664 (+/-12% with 95% confidence) lakes met the NLFTS lake definition, had either predator or bottom-dwelling fish present, and could be sampled.

Contaminants in fish tissue from US lakes and reservoirs: a national probabilistic study.

An unequal probability design was used to develop national estimates for 268 persistent, bioaccumulative, and toxic chemicals in fish tissue from lakes and reservoirs of the conterminous United States (excluding the Laurentian Great Lakes and Great Salt Lake). Predator (fillet) and bottom-dweller (whole body) composites were collected from 500 lakes selected randomly from the target population of 147,343 lakes in the lower 48 states. Each of these composite types comprised nationally representative samples whose results were extrapolated to the sampled population of an estimated 76,559 lakes for predators and 46,190 lakes for bottom dwellers. Mercury and PCBs were detected in all fish samples. Dioxins and furans were detected in 81% and 99% of predator and bottom-dweller samples, respectively. Cumulative frequency distributions showed that mercury concentrations exceeded the EPA 300 ppb mercury fish tissue criterion at nearly half of the lakes in the sampled population. Total PCB concentrations exceeded a 12 ppb human health risk-based consumption limit at nearly 17% of lakes, and dioxins and furans exceeded a 0.15 ppt (toxic equivalent or TEQ) risk-based threshold at nearly 8% of lakes in the sampled population. In contrast, 43 target chemicals were not detected in any samples. No detections were reported for nine organophosphate pesticides, one PCB congener, 16 polycyclic aromatic hydrocarbons, or 17 other semivolatile organic chemicals.

Scientific and societal considerations in selecting assessment endpoints for environmental decision making.

It is sometimes argued that, from an ecological point of view, population-, community-, and ecosystem-level endpoints are more relevant than individual-level endpoints for assessing the risks posed by human activities to the sustainability of natural resources. Yet society values amenities provided by natural resources that are not necessarily evaluated or protected by assessment tools that focus on higher levels of biological organization. For example, human-caused stressors can adversely affect recreational opportunities that are valued by society even in the absence of detectable population-level reductions in biota. If protective measures are not initiated until effects at higher levels of biological organization are apparent, natural resources that are ecologically important or highly valued by the public may not be adequately protected. Thus, environmental decision makers should consider both scientific and societal factors in selecting endpoints for ecological risk assessments. At the same time, it is important to clearly distinguish the role of scientists, which is to evaluate ecological effects, from the role of policy makers, which is to determine how to address the uncertainty in scientific assessment in making environmental decisions and to judge what effects are adverse based on societal values and policy goals.