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Coastal and estuarine regions are important areas of mercury pollution. Therefore, it is important to properly characterize the sources and bioaccumulation processes of mercury in these regions. Here, we present mercury stable isotopic compositions in 18 species of wild marine fish collected from the Pearl River Estuary (PRE), south China. Our results showed variations in mass-independent fractionation (Δ(199)Hg: +0.05 ± 0.10‰ to +0.59 ± 0.30‰) with a Δ(199)Hg/Δ(201)Hg of ∼1.26, suggesting that aqueous MeHg underwent photo-degradation prior to incorporation into the food chain. For the results, we discovered small but significant differences of Δ(199)Hg values among herbivorous, demersal, and carnivorous fish, indicating that different feeding guilds of fish may have incorporated MeHg with various degrees of photo-demethylation. The consistent mercury isotope compositions between fish feeding habitat and mercury sources in the estuary provide potentially important findings on the transformation and bioaccumulation of this toxic metal in subtropical coastal environments., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Between 1932 and 1968, industrial wastewater containing methylmercury (MeHg) and other mercury (Hg) compounds was discharged directly into Minamata Bay, Japan, seriously contaminating the fishery. Thousands of people who consumed tainted fish and shellfish developed a neurological disorder now known as Minamata disease. Concentrations of total mercury (THg) in recent fish and sediment samples from Minamata Bay remain higher than those in other Japanese coastal waters, and elevated concentrations of THg in sediments in the greater Yatsushiro Sea suggest that Hg has moved beyond the bay. We measured stable Hg isotope ratios in sediment cores from Minamata Bay and the southern Yatsushiro Sea and in archived fish from Minamata Bay dating from 1978 to 2013. Values of δ(202)Hg and Δ(199)Hg in Yatsushiro Sea surface sediments were indistinguishable from those in highly contaminated Minamata Bay sediments but distinct from and nonoverlapping with values in background (noncontaminated) sediments. We conclude that stable Hg isotope data can be used to track Minamata Bay Hg as it moves into the greater Yatsushiro Sea. In addition, our data suggest that MeHg is produced in bottom sediments and enters the food web without substantial prior photodegradation, possibly in sediment porewaters or near the sediment-water interface.

Total mercury (Hg) concentrations in hair and urine are often used as biomarkers of exposure to fish-derived methylmercury (MeHg) and gaseous elemental Hg, respectively. We used Hg stable isotopes to assess the validity of these biomarkers among small-scale gold mining populations in Ghana and Indonesia. Urine from Ghanaian miners displayed similar Δ(199)Hg values to Hg derived from ore deposits (mean urine Δ(199)Hg=0.01‰, n=6). This suggests that urine total Hg concentrations accurately reflect exposure to inorganic Hg among this population. Hair samples from Ghanaian miners displayed low positive Δ(199)Hg values (0.23-0.55‰, n=6) and low percentages of total Hg as MeHg (7.6-29%, n=7). These data suggest that the majority of the Hg in these miners' hair samples is exogenously adsorbed inorganic Hg and not fish-derived MeHg. Hair samples from Indonesian gold miners who eat fish daily displayed a wider range of positive Δ(199)Hg values (0.21-1.32‰, n=5) and percentages of total Hg as MeHg (32-72%, n=4). This suggests that total Hg in the hair samples from Indonesian gold miners is likely a mixture of ingested fish MeHg and exogenously adsorbed inorganic Hg. Based on data from both populations, we suggest that total Hg concentrations in hair samples from small-scale gold miners likely overestimate exposure to MeHg from fish consumption., (Copyright © 2014 Elsevier Inc. All rights reserved.)

Identification of sources of biologically accessible Hg is necessary to fully evaluate Hg exposure in aquatic ecosystems. This study assesses the relationship between Hg in forage fish and Hg in surface sediments throughout San Francisco Bay (SF Bay) and evaluates processes influencing the incorporation of Hg into the aquatic food web. We measured the Hg stable isotope compositions of two nearshore fish species and compared them with previously reported analyses of colocated intertidal surface sediments. Fish δ(202)Hg values (mass-dependent fractionation) demonstrated a distinct spatial gradient within SF Bay that ranged from 0.60‰ in the south to -0.25‰ in the north. Fish δ(202)Hg values were consistently higher than sediment δ(202)Hg values by 0.73‰ (±0.16‰, 1SD). Fish and sediment δ(202)Hg values in SF Bay proper were well correlated (r(2) = 0.83), suggesting that sediment is a primary source of Hg to the nearshore aquatic food web. Fish Δ(199)Hg values (mass-independent fractionation) ranged from 0.46‰ to 1.55‰, did not correlate with sediment values, and yielded a Δ(199)Hg/Δ(201)Hg ratio of 1.26 (±0.01, 1SD; r(2) = 0.99). This mass-independent fractionation is consistent with photodegradation of MeHg to varying degrees at each site prior to incorporation into the food web.

This study presents the determination and comparison of isotopic compositions of Hg in sediments, plankton, roach, and perch of two freshwater systems in the Lake Baikal-Angara River aquatic ecosystem: the man-made Bratsk Water Reservoir contaminated by Hg from a chlor-alkali factory and the noncontaminated Lake Baikal. Isotopic ratios of biota exhibit both significant mass-independent fractionation (MIF) (Δ(199)Hg from 0.20 to 1.87‰) and mass-dependent fractionation (MDF) (δ(202)Hg from -0.97 to -0.16‰), whereas sediments exhibit high MDF (δ(202)Hg from -1.99 to -0.83‰) but no MIF. δ(15)N and δ(13)C are correlated with methylmercury in organisms from both sites, indicating bioaccumulation and biomagnification through food webs of both regions. Combining this with isotopic composition of samples shows that δ(202)Hg increases with the trophic level of organisms and also with methylmercury in fish from Lake Baikal. This study demonstrates that MIF in fish samples from Bratsk Water Reservoir allow to trace anthropogenic Hg, since fish with the highest levels of Hg in muscle have the same isotopic composition as the sediment in which anthropogenic Hg was deposited. Less contaminated fish do not exhibit this anthropogenic signature accumulating relatively lower Hg amount from the contaminated sediments. This work reveals that Hg isotopic composition can be used to track the contribution of anthropogenic sources in fish from a contaminated lake.