Mercury stable isotopes constrain atmospheric sources to the ocean

Human exposure to toxic mercury (Hg) is dominated by the consumption of seafood(1,2). Earth system models suggest that Hg in marine ecosystems is supplied by atmospheric wet and dry Hg(ii) deposition, with a three times smaller contribution from gaseous Hg(0) uptake(3,4). Observations of marine Hg(ii) deposition and Hg(0) gas exchange are sparse, however(5), leaving the suggested importance of Hg(ii) deposition(6) ill-constrained. Here we present the first Hg stable isotope measurements of total Hg (tHg) in surface and deep Atlantic and Mediterranean seawater and use them to quantify atmospheric Hg deposition pathways. We observe overall similar tHg isotope compositions, with median Delta Hg-200 signatures of 0.02 parts per thousand, lying in between atmospheric Hg(0) and Hg(ii) deposition end-members. We use a Delta Hg-200 isotope mass balance to estimate that seawater tHg can be explained by the mixing of 42% (median; interquartile range, 24-50%) atmospheric Hg(ii) gross deposition and 58% (50-76%) Hg(0) gross uptake. We measure and compile additional, global marine Hg isotope data including particulate Hg, sediments and biota and observe a latitudinal Delta Hg-200 gradient that indicates larger ocean Hg(0) uptake at high latitudes. Our findings suggest that global atmospheric Hg(0) uptake by the oceans is equal to Hg(ii) deposition, which has implications for our understanding of atmospheric Hg dispersal and marine ecosystem recovery. Mercury deposition pathways from the atmosphere to the ocean remain uncertain, but mercury stable isotope measurements from the Atlantic and Mediterranean show that ocean uptake of gaseous elemental mercury is more important than previously thought.

Automated summary

Mercury exposure through consumption of seafood is a significant pathway for human exposure. Earth system models suggest that mercury in marine ecosystems mainly comes from atmospheric wet and dry deposition of Hg(II), with a smaller contribution from gaseous Hg(0) uptake. Studies on marine Hg deposition and gas exchange are limited, but stable isotope measurements in Atlantic and Mediterranean seawater indicate a significant contribution of atmospheric Hg and gaseous elemental mercury uptake to ocean mercury levels.