期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2022
卷号：119
期号：14
DOI：10.1073/pnas.2119857119
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Significance
Russian rivers are the predominant source of riverine mercury to the Arctic Ocean, where methylmercury biomagnifies to high levels in food webs. Pollution controls are thought to have decreased late–20th-century mercury loading to Arctic watersheds, but there are no published long-term observations on mercury in Russian rivers. Here, we present a unique hydrochemistry dataset to determine trends in Russian river particulate mercury concentrations and fluxes in recent decades. Using hydrologic and mercury deposition modeling together with multivariate time series analysis, we determine that 70 to 90% declines in particulate mercury fluxes were driven by pollution reductions and sedimentation in reservoirs. Results suggest that Russian rivers likely dominated over all other sources of mercury to the Arctic Ocean until recently.
High levels of methylmercury accumulation in marine biota are a concern throughout the Arctic, where coastal ocean ecosystems received large riverine inputs of mercury (Hg) (40 Mg⋅y
−1) and sediment (20 Tg⋅y
−1) during the last decade, primarily from major Russian rivers. Hg concentrations in fish harvested from these rivers have declined since the late 20th century, but no temporal data on riverine Hg, which is often strongly associated with suspended sediments, were previously available. Here, we investigate temporal trends in Russian river particulate Hg (PHg) and total suspended solids (TSS) to better understand recent changes in the Arctic Hg cycle and its potential future trajectories. We used 1,300 measurements of Hg in TSS together with discharge observations made by Russian hydrochemistry and hydrology monitoring programs to examine changes in PHg and TSS concentrations and fluxes in eight major Russian rivers between ca. 1975 and 2010. Due to decreases in both PHg concentrations (micrograms per gram) and TSS loads, annual PHg export declined from 47 to 7 Mg⋅y
−1 overall and up to 92% for individual rivers. Modeling of atmospheric Hg deposition together with published inventories on reservoir establishment and industrial Hg release point to decreased pollution and sedimentation within reservoirs as predominant drivers of declining PHg export. We estimate that Russian rivers were the primary source of Hg to the Arctic Ocean in the mid to late 20th century.
