Search for: All records

Methylmercury (MeHg) is a neurotoxin that bioaccumulates to potentially harmful concentrations in Arctic and Subarctic marine predators and those that consume them. Monitoring and modeling MeHg bioaccumulation and biogeochemical cycling in the ocean requires an understanding of the mechanisms behind net mercury (Hg) methylation. The key functional gene pair for Hg methylation,hgcAB, is widely distributed throughout ocean basins and spans multiple microbial phyla. While multiple microbially mediated anaerobic pathways for Hg methylation in the ocean are known, the majority ofhgcAhomologs have been found in oxic subsurface waters, in contrast to other ecosystems. In particular, microaerophilicNitrospina, a genera of nitrite-oxidizing bacteria containing ahgcA-like sequence, have been proposed as a potentially important Hg methylator in the upper ocean. The objective of this work was therefore to examine the potential of nitrifiers as Hg methylators and quantify total Hg and MeHg across three Arctic and Subarctic seas (the Gulf of Alaska, the Bering Sea and the Chukchi Sea) in regions whereNitrospinaare likely present. In Spring 2021, samples for Hg analysis were obtained with a trace metal clean rosette across these seas. Mercury methylation rates were quantified in concert with nitrification rates using onboard incubation experiments with additions of stable isotope-labeled Hg and NH₄⁺. A significant correlation between Hg methylation and nitrification was observed across all sites (R²= 0.34,p< 0.05), with the strongest correlation in the Chukchi Sea (R²= 0.99,p< 0.001).Nitrospina-specifichgcA-like genes were detected at all sites. This study, linking Hg methylation and nitrification in oxic seawater, furthers understanding of MeHg cycling in these high latitude waters, and the ocean in general. Furthermore, these studies inform predictions of how climate and human interactions could influence MeHg concentrations across the Arctic in the future.

 

The downward flux of sinking particles is a prominent Hg removal and redistribution process in the ocean; however, it is not well-constrained. Using data from three U.S. GEOTRACES cruises including the Pacific, Atlantic, and Arctic Oceans, we examined the mercury partitioning coefficient, K d , in the water column. The data suggest that the K d varies widely over three ocean basins. We also investigated the effect of particle concentration and composition on K d by comparing the concentration of small-sized (1–51 μm) suspended particulate mass (SPM) as well as its compositional fractions in six different phases to the partitioning coefficient. We observed an inverse relationship between K d and suspended particulate mass, as has been observed for other metals and known as the “particle concentration effect,” that explains much of the variation in K d . Particulate organic matter (POM) and calcium carbonate (CaCO 3 ) dominated the Hg partitioning in all three ocean basins while Fe and Mn could make a difference in some places where their concentrations are elevated, such as in hydrothermal plumes. Finally, our estimated Hg residence time has a strong negative correlation with average log bulk K d , indicating that K d has significant effect on Hg residence time. 

Humans are exposed to potentially harmful amounts of the neurotoxin monomethylmercury (MMHg) through consumption of marine fish and mammals. However, the pathways of MMHg production and bioaccumulation in the ocean remain elusive. In anaerobic environments, inorganic mercury (Hg) can be methylated to MMHg through an enzymatic pathway involving thehgcABgene cluster. Recently,hgcA‐like genes have been discovered in oxygenated marine water, suggesting thehgcABmethylation pathway, or a close analog, may also be relevant in the ocean. Using polymerase chain reaction amplification and shotgun metagenomics, we searched for but did not find thehgcABgene cluster in Arctic Ocean seawater. However, we detected Hg‐cycling genes from themeroperon (including organomercury lyase,merB), andhgcA‐like paralogs (i.e.,cdhD) in Arctic Ocean metagenomes. Our analysis of Hg biogeochemistry and marine microbial genomics suggests that various microorganisms and metabolisms, and not just thehgcABpathway, are important for Hg methylation in the ocean.

 

A major surface circulation feature of the Arctic Ocean is the Transpolar Drift (TPD), a current that transports river‐influenced shelf water from the Laptev and East Siberian Seas toward the center of the basin and Fram Strait. In 2015, the international GEOTRACES program included a high‐resolution pan‐Arctic survey of carbon, nutrients, and a suite of trace elements and isotopes (TEIs). The cruises bisected the TPD at two locations in the central basin, which were defined by maxima in meteoric water and dissolved organic carbon concentrations that spanned 600 km horizontally and ~25–50 m vertically. Dissolved TEIs such as Fe, Co, Ni, Cu, Hg, Nd, and Th, which are generally particle‐reactive but can be complexed by organic matter, were observed at concentrations much higher than expected for the open ocean setting. Other trace element concentrations such as Al, V, Ga, and Pb were lower than expected due to scavenging over the productive East Siberian and Laptev shelf seas. Using a combination of radionuclide tracers and ice drift modeling, the transport rate for the core of the TPD was estimated at 0.9 ± 0.4 Sv (10⁶ m³ s⁻¹). This rate was used to derive the mass flux for TEIs that were enriched in the TPD, revealing the importance of lateral transport in supplying materials beneath the ice to the central Arctic Ocean and potentially to the North Atlantic Ocean via Fram Strait. Continued intensification of the Arctic hydrologic cycle and permafrost degradation will likely lead to an increase in the flux of TEIs into the Arctic Ocean.