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The origin of methylmercury in pelagic fish remains unclear, with many unanswered questions regarding the production and degradation of this neurotoxin in the water column. We used mercury (Hg) stable isotope ratios of marine particles and biota to elucidate the cycling of methylmercury prior to incorporation into the marine food web. The Hg isotopic composition of particles, zooplankton, and fish reveals preferential methylation of Hg within small (< 53 µm) marine particles in the upper 400 m of the North Pacific Ocean. Mass-dependent Hg isotope ratios (δ 202 Hg) recorded in small particles overlap with previously estimated δ 202 Hg values for methylmercury sources to Pacific and Atlantic Ocean food webs. Particulate compound specific isotope analysis of amino acids (CSIA-AA) yield δ 15 N values that indicate more-significant microbial decomposition in small particles compared to larger particles. CSIA-AA and Hg isotope data also suggest that large particles (> 53 µm) collected in the equatorial ocean are distinct from small particles and resemble fecal pellets. Additional evidence for Hg methylation within small particles is provided by a statistical mixing model of even mass-independent (Δ 200 Hg and Δ 204 Hg) isotope values, which demonstrates that Hg within near-surface marine organisms (0-150 m) originates from a combination of rainfall and marine particles. In contrast, in meso- and upper bathypelagic organisms (200-1,400 m), the majority of Hg originates from marine particles with little input from wet deposition. The occurrence of methylation within marine particles is supported further by a correlation between Δ 200 Hg and Δ 199 Hg values, demonstrating greater overlap in the Hg isotopic composition of marine organisms with marine particles than with total gaseous Hg or wet deposition.

In Hawaii, some of the most important commercial and recreational fishes comprise an assemblage of lutjanids and carangids called bottomfish. Despite their importance, we know little about their trophic ecology or where the mercury (Hg) that ultimately resides in their tissue originates. Here we investigated these topics, by analyzing muscle samples for mercury content, nitrogen, carbon, and amino acid specific nitrogen isotope ratios in six species distributed across different depths from the Northwestern Hawaiian Islands (NWHI) and the Main Hawaiian Islands (MHI). Fishes had different sources of nitrogen and carbon, with isotopic values suggesting benthic food sources for shallow nearshore species. High trophic position lutjanids that foraged in deeper water, benthic environments generally had higher Hg levels. Model results also suggested that benthic Hg methylation was an important source of Hg for shallow benthic feeders, while deepwater sources of mercury may be important for those with a diet that derives, at least in part, from the pelagic environment. Further, despite the lack of freshwater sources of Hg in the NWHI, statistical models explaining the variation in tissue Hg in the MHI and NWHI were nearly identical, suggesting freshwater Hg inputs were not a major source of Hg in fish tissue.

Mercury distribution in the oceans is controlled by complex biogeochemical cycles, resulting in retention of trace amounts of this metal in plants and animals. Inter- and intra-specific variations in mercury levels of predatory pelagic fish have been previously linked to size, age, trophic position, physical and chemical environmental parameters, and location of capture; however, considerable variation remains unexplained. In this paper, we focus on differences in ecology, depth of occurrence, and total mercury levels in 9 species of commercially important pelagic fish (Thunnus obesus, T. albacares, Katsuwonus pelamis, Xiphias gladius, Lampris guttatus, Coryphaena hippurus, Taractichthys steindachneri, Tetrapturus audax, and Lepidocybium flavobrunneum) and in numerous representatives (fishes, squids, and crustaceans) of their lower trophic level prey sampled from the central North Pacific Ocean. Results indicate that total mercury levels of predatory pelagic fishes and their prey increase with median depth of occurrence in the water column and mimic concentrations of dissolved organic mercury in seawater. Stomach content analysis results from this study and others indicate a greater occurrence of higher-mercury containing deeper-water prey organisms in the diets of the deeper-ranging predators, X. gladius, T. obesus, and L. guttatus. While present in trace amounts, dissolved organic mercury increases with depth in the water column suggesting that the mesopelagic habitat is a major entry point for mercury into marine food webs. These data suggest that a major determinant of mercury levels in oceanic predators is their depth of forage.