Dimethylmercury as a Source of Monomethylmercury in a Highly Productive Upwelling System.

Monomethylmercury (MMHg) is a neurotoxicant that biomagnifies in marine food webs, reaching high concentrations in apex predators. To predict changes in oceanic MMHg concentrations, it is important to quantify the sources and sinks of MMHg. Here, we study mercury speciation in the California Current System through cruise sampling and modeling. Previous work in the California Current System has found that upwelling transports mercury-enriched deep waters to productive surface waters. These upwelled waters originate within the California Undercurrent water mass and are subsequently advected as a surface water parcel to the California Current. Between the two major water masses, we find that compared to the California Current, the California Undercurrent contains elevated dissolved total mercury (THg) and dimethylmercury (DMHg) concentrations by 59 and 69%, respectively. We explain that these differences result from losses during advection, specifically scavenging of THg and DMHg demethylation. We calculate a net DMHg demethylation rate of 2.0 ± 1.1% d-1 and build an empirically constrained mass budget model to demonstrate that net DMHg demethylation accounts for 61% of surface MMHg sources. These findings illustrate that DMHg is a significant source of MMHg in this region, challenging the current understanding of the major sources of marine MMHg.

Description of a Dimethylmercury Automatic Analyzer for the High-Resolution Measurement of Dissolved Gaseous Mercury Species in Surface Ocean Waters.

Our understanding of the significance of dimethylmercury (DMHg) to the mercury (Hg) global ocean biogeochemical cycle is unclear because of the lack of detailed DMHg measurements in the water column. To our knowledge, 30 years of published studies have generated no more than 200 DMHg data points in the ocean surface waters and marine boundary layer (MBL). To improve the precision and reduce the uncertainty in determining DMHg in surface seawater, we developed a simple and robust DMHg automatic analyzer (DAA). This DAA system couples the main sampling and analytic steps, including a continuous flow chamber, with dual Carbotrap preconcentration, a gas chromatographic column, a cold vapor atomic fluorescence spectrometry, and a data logger for signal integration. We compared the operation, performance, and reproducibility between our DAA and the traditional manual analytic method. Its advantages include the ease of operation, the high time resolution and precision (30 min sampling and <5% relative variation), and long-term stability (2 weeks). The DAA can determine DMHg in both the MBL and surface seawater. The estimated detection limits for DMHg with the DAA in the atmosphere and in surface seawater are 10 pg/m3 and 0.2 fM, respectively. The successful DAA field measurement in coastal waters indicates that it can help detect the low DMHg concentration in surface seawater, and the time series DMHg data helped our understanding of the DMHg behavior (sources and sinks) and its flux into the MBL. The comparison of DMHg concentration in various oceans also suggests that the coastal region had the lowest averaged DMHg, up to an order of magnitude lower than other ecosystems.

Characterization of the metalloproteome of Pseudoalteromonas (BB2-AT2): biogeochemical underpinnings for zinc, manganese, cobalt, and nickel cycling in a ubiquitous marine heterotroph.

Pseudoalteromonas (BB2-AT2) is a ubiquitous marine heterotroph, often associated with labile organic carbon sources in the ocean (e.g. phytoplankton blooms and sinking particles). Heterotrophs hydrolyze exported photosynthetic materials, components of the biological carbon pump, with the use of diverse metalloenzymes containing zinc (Zn), manganese (Mn), cobalt (Co), and nickel (Ni). Studies on the metal requirements and cytosolic utilization of metals for marine heterotrophs are scarce, despite their relevance to global carbon cycling. Here, we characterized the Zn, Mn, Co, and Ni metallome of BB2-AT2. We found that the Zn metallome is complex and cytosolic Zn is associated with numerous proteins for transcription (47.2% of the metallome, obtained from singular value decomposition of the metalloproteomic data), translation (33.5%), proteolysis (12.8%), and alkaline phosphatase activity (6.4%). Numerous proteolytic enzymes also appear to be putatively associated with Mn, and to a lesser extent, Co. Putative identification of the Ni-associated proteins, phosphoglucomutase and a protein in the cupin superfamily, provides new insights for Ni utilization in marine heterotrophs. BB2-AT2 relies on numerous transition metals for proteolytic and phosphatase activities, inferring an adaptative potential to metal limitation. Our field observations of increased alkaline phosphatase activity upon addition of Zn in field incubations suggest that such metal limitation operates in sinking particulate material collected from sediment traps. Taken together, this study improves our understanding of the Zn, Mn, Co, and Ni metallome of marine heterotrophic bacteria and provides novel and mechanistic frameworks for understanding the influence of nutrient limitation on biogeochemical cycling.

Bluefin tuna reveal global patterns of mercury pollution and bioavailability in the world's oceans.

Bluefin tuna (BFT), highly prized among consumers, accumulate high levels of mercury (Hg) as neurotoxic methylmercury (MeHg). However, how Hg bioaccumulation varies among globally distributed BFT populations is not understood. Here, we show mercury accumulation rates (MARs) in BFT are highest in the Mediterranean Sea and decrease as North Pacific Ocean > Indian Ocean > North Atlantic Ocean. Moreover, MARs increase in proportion to the concentrations of MeHg in regional seawater and zooplankton, linking MeHg accumulation in BFT to MeHg bioavailability at the base of each subbasin's food web. Observed global patterns correspond to levels of Hg in each ocean subbasin; the Mediterranean, North Pacific, and Indian Oceans are subject to geogenic enrichment and anthropogenic contamination, while the North Atlantic Ocean is less so. MAR in BFT as a global pollution index reflects natural and human sources and global thermohaline circulation.

The role of plastic debris in the biogeochemical cycle of mercury in Lake Erie and San Francisco Bay.

The accumulation of plastic debris that concentrates hydrophobic compounds and microbial communities creates the potential for altered aquatic biogeochemical cycles. This study investigated the role of plastic debris in the biogeochemical cycling of mercury in surface waters of the San Francisco Bay, Sacramento River, Lake Erie, and in coastal seawater. Total mercury and monomethylmercury were measured on plastic debris from all study sites. Plastic-bound microbial communities from Lake Erie and San Francisco Bay contained several lineages of known mercury methylating microbes, however the hgcAB gene cluster was not detected using polymerase chain reaction. These plastic-bound microbial communities also contained species that possess the mer operon, and merA genes were detected using polymerase chain reaction. In coastal seawater incubations, rapid mercury methylation percentages were greater in the presence of microplastics and demethylation percentages decreased as monomethylmercury additions adsorbed to microplastics. These findings suggest that plastic pollution has the potential to alter the biogeochemical cycling of mercury in aquatic ecosystems.

Mercury methylation by metabolically versatile and cosmopolitan marine bacteria.

Microbes transform aqueous mercury (Hg) into methylmercury (MeHg), a potent neurotoxin that accumulates in terrestrial and marine food webs, with potential impacts on human health. This process requires the gene pair hgcAB, which encodes for proteins that actuate Hg methylation, and has been well described for anoxic environments. However, recent studies report potential MeHg formation in suboxic seawater, although the microorganisms involved remain poorly understood. In this study, we conducted large-scale multi-omic analyses to search for putative microbial Hg methylators along defined redox gradients in Saanich Inlet, British Columbia, a model natural ecosystem with previously measured Hg and MeHg concentration profiles. Analysis of gene expression profiles along the redoxcline identified several putative Hg methylating microbial groups, including Calditrichaeota, SAR324 and Marinimicrobia, with the last the most active based on hgc transcription levels. Marinimicrobia hgc genes were identified from multiple publicly available marine metagenomes, consistent with a potential key role in marine Hg methylation. Computational homology modelling predicts that Marinimicrobia HgcAB proteins contain the highly conserved amino acid sites and folding structures required for functional Hg methylation. Furthermore, a number of terminal oxidases from aerobic respiratory chains were associated with several putative novel Hg methylators. Our findings thus reveal potential novel marine Hg-methylating microorganisms with a greater oxygen tolerance and broader habitat range than previously recognized.

Dinoflagellates alter their carbon and nutrient metabolic strategies across environmental gradients in the central Pacific Ocean.

Marine microeukaryotes play a fundamental role in biogeochemical cycling through the transfer of energy to higher trophic levels and vertical carbon transport. Despite their global importance, microeukaryote physiology, nutrient metabolism and contributions to carbon cycling across offshore ecosystems are poorly characterized. Here, we observed the prevalence of dinoflagellates along a 4,600-km meridional transect extending across the central Pacific Ocean, where oligotrophic gyres meet equatorial upwelling waters rich in macronutrients yet low in dissolved iron. A combined multi-omics and geochemical analysis provided a window into dinoflagellate metabolism across the transect, indicating a continuous taxonomic dinoflagellate community that shifted its functional transcriptome and proteome as it extended from the euphotic to the mesopelagic zone. In euphotic waters, multi-omics data suggested that a combination of trophic modes were utilized, while mesopelagic metabolism was marked by cytoskeletal investments and nutrient recycling. Rearrangement in nutrient metabolism was evident in response to variable nitrogen and iron regimes across the gradient, with no associated change in community assemblage. Total dinoflagellate proteins scaled with particulate carbon export, with both elevated in equatorial waters, suggesting a link between dinoflagellate abundance and total carbon flux. Dinoflagellates employ numerous metabolic strategies that enable broad occupation of central Pacific ecosystems and play a dual role in carbon transformation through both photosynthetic fixation in the euphotic zone and remineralization in the mesopelagic zone.

Spatial Heterogeneity in Particle-Associated, Light-Independent Superoxide Production Within Productive Coastal Waters.

In the marine environment, the reactive oxygen species (ROS) superoxide is produced through a diverse array of light-dependent and light-independent reactions, the latter of which is thought to be primarily controlled by microorganisms. Marine superoxide production influences organic matter remineralization, metal redox cycling, and dissolved oxygen concentrations, yet the relative contributions of different sources to total superoxide production remain poorly constrained. Here we investigate the production, steady-state concentration, and particle-associated nature of light-independent superoxide in productive waters off the northeast coast of North America. We find exceptionally high levels of light-independent superoxide in the marine water column, with concentrations ranging from 10 pM to in excess of 2,000 pM. The highest superoxide concentrations were particle associated in surface seawater and in aphotic seawater collected meters off the seafloor. Filtration of seawater overlying the continental shelf lowered the light-independent, steady-state superoxide concentration by an average of 84%. We identify eukaryotic phytoplankton as the dominant particle-associated source of superoxide to these coastal waters. We contrast these measurements with those collected at an off-shelf station, where superoxide concentrations did not exceed 100 pM, and particles account for an average of 40% of the steady-state superoxide concentration. This study demonstrates the primary role of particles in the production of superoxide in seawater overlying the continental shelf and highlights the importance of light-independent, dissolved-phase reactions in marine ROS production.

Mercury biogeochemical cycling: A synthesis of recent scientific advances.

The focus of this paper is to briefly discuss the major advances in scientific thinking regarding: a) processes governing the fate and transport of mercury in the environment; b) advances in measurement methods; and c) how these advances in knowledge fit in within the context of the Minamata Convention on Mercury. Details regarding the information summarized here can be found in the papers associated with this Virtual Special Issue of STOTEN.

A global perspective on mercury cycling in the ocean.

Mercury (Hg) is a ubiquitous metal in the ocean that undergoes in situ chemical transformations in seawater and marine sediment. Most relevant to public health is the production of monomethyl-Hg, a neurotoxin to humans that accumulates in marine fish and mammals. Here we synthesize 30 years of Hg measurements in the ocean to discuss sources, sinks, and internal cycling of this toxic metal. Global-scale oceanographic survey programs (i.e. CLIVAR and GEOTRACES), refined protocols for clean sampling, and analytical advancements have produced over 200 high-resolution, full-depth profiles of total Hg, methylated Hg, and gaseous elemental Hg throughout the Atlantic, Pacific, Arctic, and Southern Oceans. Vertical maxima of methylated Hg were found in surface waters, near the subsurface chlorophyll maximum, and in low-oxygen thermocline waters. The greatest concentration of Hg in deep water was measured in Antarctic Bottom Water, and in newly formed Labrador Sea Water, Hg showed a decreasing trend over the past 20 years. Distribution of Hg in polar oceans was unique relative to lower latitudes with higher concentrations of total Hg near the surface and vertical trends of Hg speciation driven by water column stratification and seasonal ice cover. Global models of Hg in the ocean require a better understanding of biogeochemical controls on Hg speciation and improved accuracy of methylated Hg measurements within the international community.

The Mercury-Tolerant Microbiota of the Zooplankton Daphnia Aids in Host Survival and Maintains Fecundity under Mercury Stress.

Many aquatic organisms can thrive in polluted environments by having the genetic capability to withstand suboptimal conditions. However, the contributions of microbiomes under these stressful environments are poorly understood. We investigated whether a mercury-tolerant microbiota can extend its phenotype to its host by ameliorating host survival and fecundity under mercury-stress. We isolated microbiota members from various clones of Daphnia magna, screened for the mercury-biotransforming merA gene, and determined their mercury tolerance levels. We then introduced the mercury-tolerant microbiota, Pseudomonas-10, to axenic D. magna and quantified its merA gene expression, mercury reduction capability, and measured its impact on host survival and fecundity. The expression of the merA gene was up-regulated in Pseudomonas-10, both in isolation and in host-association with mercury exposure. Pseudomonas-10 is also capable of significantly reducing mercury concentration in the medium. Notably, mercury-exposed daphnids containing only Pseudomonas-10 exhibited higher survival and fecundity than mercury-exposed daphnids supplemented with parental microbiome. Our study showed that zooplankton, such as Daphnia, naturally harbor microbiome members that are eco-responsive and tolerant to mercury exposure and can aid in host survival and maintain host fecundity in a mercury-contaminated environment. This study further demonstrates that under stressful environmental conditions, the fitness of the host can depend on the genotype and the phenotype of its microbiome.

Tuna Consumption, Mercury Exposure, and Knowledge about Mercury Exposure Risk from Tuna Consumption in University Students.

We examined the relationships among tuna consumption, hair mercury levels, and knowledge of mercury exposure risk from tuna consumption in university students that were offered tuna daily at university-run dining halls. Hair total mercury levels in tuna consumers were higher than those in non-tuna consumers (average = 0.466 µg/g ± 0.328 standard deviation [SD], n = 20 vs 0.110 µg/g ± 0.105 SD, n = 33, respectively; p < 0.0001, Mann-Whitney U test), with tuna eaters exhibiting a positive relationship between self-reported tuna consumption at dining halls and hair mercury levels (R2 = 0.868, p < 0.0001, n = 17, linear regression). For all tuna eaters surveyed, more than half (54%) self-reported eating ≥3 tuna meals/wk, potentially exceeding the US Environmental Protection Agency's reference dose for methylmercury of 0.1 µg/kg body weight/d. Seven percent of study participants reported they consumed >20 tuna meals/wk, which was related to hair mercury levels >1 µg/g, a level of concern. Study participants had an overall lack of knowledge and confidence in their knowledge about mercury exposure risk from tuna consumption, with >99% of participants reporting low knowledge and low confidence in survey answers. Our study highlights the importance of education about the risks of tuna consumption, particularly in institutional settings where individuals have unlimited access to tuna products. Environ Toxicol Chem 2019;38:1988-1994. © 2019 SETAC.

Global and Local Sources of Mercury Deposition in Coastal New England Reconstructed from a Multiproxy, High-Resolution, Estuarine Sediment Record.

Historical reconstruction of mercury (Hg) accumulation in natural archives, especially lake sediments, has been essential to understanding human perturbation of the global Hg cycle. Here we present a high-resolution chronology of Hg accumulation between 1727 and 1996 in a varved sediment core from the Pettaquamscutt River Estuary (PRE), Rhode Island. Mercury accumulation is examined relative to (1) historic deposition of polycyclic aromatic hydrocarbons (PAHs) and lead (Pb) and its isotopes (206Pb/207Pb) in the same core, and (2) other reconstructions of Hg deposition in urban and remote settings. Mercury deposition in PRE parallels the temporal patterns of PAHs, and both track industrialization and regional coal use between 1850 and 1950 as well as rising petroleum use after 1950. There is little indication of increased Hg deposition from late 19th-century silver and gold mining in the western U.S. A broad maximum of Hg deposition during 1930-1980, and not found in remote sites, is consistent with the predicted influence of additional industrial sources and commercial products. Our results imply that a significant portion of global anthropogenic Hg emissions during the 20th century was deposited locally, near urban and industrial centers of Hg use and release.

Presence of artisanal gold mining predicts mercury bioaccumulation in five genera of bats (Chiroptera).

Mercury, a toxic trace metal, has been used extensively as an inexpensive and readily available method of extracting gold from fine-grained sediment. Worldwide, artisanal mining is responsible for one third of all mercury released into the environment. By testing bat hair from museum specimens and field collected samples from areas both impacted and unimpacted by artisanal gold mining in Perú, we show monomethylmercury (MMHg) has increased in the last 100 years. MMHg concentrations were also greatest in the highest bat trophic level (insectivores), and in areas experiencing extractive artisanal mining. Reproductive female bats had higher MMHg concentrations, and both juvenile and adult bats from mercury contaminated sites had more MMHg than those from uncontaminated sites. Bats have important ecological functions, providing vital ecosystem services such as pollination, seed dispersal, and insect control. Natural populations can act as environmental sentinels and offer the chance to expand our understanding of, and responses to, environmental and human health concerns.

Continuous proxy measurements reveal large mercury fluxes from glacial and forested watersheds in Alaska.

In this study, a stream from a glacially dominated watershed and one from a wetland, temperate forest dominated watershed in southeast Alaska were continuously monitored for turbidity and fluorescence from dissolved organic matter (FDOM) while grab samples for unfiltered (UTHg), particulate (PTHg), and filtered mercury (FTHg) where taken over three 4-day periods (May snowmelt, July glacial melt, and September rainy season) during 2010. Strong correlations were found between FDOM and UTHg concentrations in the wetland, temperate forest watershed (r2=0.81), while turbidity and UTHg were highly correlated in the glacially dominated watershed (r2=0.82). Both of these parameters (FDOM and turbidity) showed stronger correlations than concentration-discharge relationships for UTHg (r2=0.55 for glacial stream, r2=0.38 for wetland/forest stream), thus allowing for a more precise determination of temporal variability in UTHg concentrations and fluxes. The association of mercury with particles and dissolved organic matter (DOM) appears to depend on the watershed characteristics, such as physical weathering and biogeochemical processes regulating mercury transport. Thus employing watershed-specific proxies for UTHg (such as FDOM and turbidity) can be effective for quantifying mercury export from watersheds with variable landcover. The UTHg concentration in the forest/wetland stream was consistently higher than in the glacial stream, in which most of the mercury was associated with particles; however, due to the high specific discharge from the glacial stream during the melt season, the watershed area normalized flux of mercury from the glacial stream was 3-6 times greater than the wetland/forest stream for the three sampling campaigns. The annual specific flux for the glacial watershed was 19.9gUTHgkm-2y-1, which is higher than any non-mining impacted stream measured to date. This finding indicates that glacial watersheds of southeast Alaska may be important conduits of total mercury to the Gulf of Alaska.

Extensive Dark Biological Production of Reactive Oxygen Species in Brackish and Freshwater Ponds.

Within natural waters, photodependent processes are generally considered the predominant source of reactive oxygen species (ROS), a suite of biogeochemically important molecules. However, recent discoveries of dark particle-associated ROS production in aquatic environments and extracellular ROS production by various microorganisms point to biological activity as a significant source of ROS in the absence of light. Thus, the objective of this study was to explore the occurrence of dark biological production of the ROS superoxide (O2(-)) and hydrogen peroxide (H2O2) in brackish and freshwater ponds. Here we show that the ROS superoxide and hydrogen peroxide were present in dark waters at comparable concentrations as in sunlit waters. This suggests that, at least for the short-lived superoxide species, light-independent processes were an important control on ROS levels in these natural waters. Indeed, we demonstrated that dark biological production of ROS extensively occurred in brackish and freshwater environments, with greater dark ROS production rates generally observed in the aphotic relative to the photic zone. Filtering and formaldehyde inhibition confirmed the biological nature of a majority of this dark ROS production, which likely involved phytoplankton, particle-associated heterotrophic bacteria, and NADH-oxidizing enzymes. We conclude that biological ROS production is widespread, including regions devoid of light, thereby expanding the relevance of these reactive molecules to all regions of our oxygenated global habit.

An examination of the role of particles in oceanic mercury cycling.

Recent models of global mercury (Hg) cycling have identified the downward flux of sinking particles in the ocean as a prominent Hg removal process from the ocean. At least one of these models estimates the amount of anthropogenic Hg in the ocean to be about 400 Mmol, with deep water formation and sinking fluxes representing the largest vectors by which pollutant Hg is able to penetrate the ocean interior. Using data from recent cruises to the Atlantic, we examined the dissolved and particulate partitioning of Hg in the oceanic water column as a cross-check on the hypothesis that sinking particle fluxes are important. Interestingly, these new data suggest particle-dissolved partitioning (Kd) that is approximately 20× greater than previous estimates, which thereby challenges certain assumptions about the scavenging and active partitioning of Hg in the ocean used in earlier models. For example, the new particle data suggest that regenerative scavenging is the most likely mechanism by which the association of Hg and particles occurs.This article is part of the themed issue 'Biological and climatic impacts of ocean trace element chemistry'.

Microbial- and thiosulfate-mediated dissolution of mercury sulfide minerals and transformation to gaseous mercury.

Mercury (Hg) is a toxic heavy metal that poses significant environmental and human health risks. Soils and sediments, where Hg can exist as the Hg sulfide mineral metacinnabar (ß-HgS), represent major Hg reservoirs in aquatic environments. Metacinnabar has historically been considered a sink for Hg in all but severely acidic environments, and thus disregarded as a potential source of Hg back to aqueous or gaseous pools. Here, we conducted a combination of field and laboratory incubations to identify the potential for metacinnabar as a source of dissolved Hg within near neutral pH environments and the underpinning (a)biotic mechanisms at play. We show that the abundant and widespread sulfur-oxidizing bacteria of the genus Thiobacillus extensively colonized metacinnabar chips incubated within aerobic, near neutral pH creek sediments. Laboratory incubations of axenic Thiobacillus thioparus cultures led to the release of metacinnabar-hosted Hg(II) and subsequent volatilization to Hg(0). This dissolution and volatilization was greatly enhanced in the presence of thiosulfate, which served a dual role by enhancing HgS dissolution through Hg complexation and providing an additional metabolic substrate for Thiobacillus. These findings reveal a new coupled abiotic-biotic pathway for the transformation of metacinnabar-bound Hg(II) to Hg(0), while expanding the sulfide substrates available for neutrophilic chemosynthetic bacteria to Hg-laden sulfides. They also point to mineral-hosted Hg as an underappreciated source of gaseous elemental Hg to the environment.

Deforestation and cultivation mobilize mercury from topsoil.

Terrestrial biomass and soils are a primary global reservoir of mercury (Hg) derived from natural and anthropogenic sources; however, relatively little is known about the fate and stability of Hg in the surface soil reservoir and its susceptibility to change as a result of deforestation and cultivation. In southwest Ohio, we measured Hg concentrations in soils of deciduous old- and new-growth forests, as well as fallow grassland and agricultural soils that had once been forested to examine how, over decadal to century time scales, man-made deforestation and cultivation influence Hg mobility from temperate surface soils. Mercury concentrations in surficial soils were significantly greater in the old-growth than new-growth forest, and both forest soils had greater Hg concentrations than cultivated and fallow fields. Differences in Hg:lead ratios between old-growth forest and agricultural topsoils suggest that about half of the Hg lost from deforested and cultivated Ohio soils may have been volatilized and the other half eroded. The estimated mobilization potential of Hg as a result of deforestation was 4.1 mg m(-2), which was proportional to mobilization potentials measured at multiple locations in the Amazon relative to concentrations in forested surface soils. Based on this relationship and an estimate of the global average of Hg concentrations in forested soils, we approximate that about 550 M mol of Hg has been mobilized globally from soil as a result of deforestation during the past two centuries. This estimate is comparable to, if not greater than, the amount of anthropogenic Hg hypothesized by others to have been sequestered by the soil reservoir since Industrialization. Our results suggest that deforestation and soil cultivation are significant anthropogenic processes that exacerbate Hg mobilization from soil and its cycling in the environment.

Increase in mercury in Pacific yellowfin tuna.

Mercury is a toxic trace metal that can accumulate to levels that threaten human and environmental health. Models and empirical data suggest that humans are responsible for a great deal of the mercury actively cycling in the environment at present. Thus, one might predict that the concentration of mercury in fish should have increased dramatically since the Industrial Revolution. Evidence in support of this hypothesis has been hard to find, however, and some studies have suggested that analyses of fish show no change in mercury concentration. By compiling and re-analyzing published reports on yellowfin tuna (Thunnus albacares) caught near Hawaii (USA) over the past half century, the authors found that the concentration of mercury in these fish currently is increasing at a rate of at least 3.8% per year. This rate of increase is consistent with a model of anthropogenic forcing on the mercury cycle in the North Pacific Ocean and suggests that fish mercury concentrations are keeping pace with current loading increases to the ocean. Future increases in mercury in yellowfin tuna and other fishes can be avoided by reductions in atmospheric mercury emissions from point sources.