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Deposition of atmospheric mercury (Hg) is the most important Hg source on the high-altitude Himalayas and Tibetan Plateau. Herein, total gaseous Hg (TGM) at an urban and a forest site on the Tibetan Plateau was collected respectively from May 2017 to October 2018, and isotopic compositions were measured to clarify the influences of landforms and monsoons on the transboundary transport of atmospheric Hg to the Tibetan Plateau. The transboundary transported anthropogenic emissions mainly originated over Indo-Gangetic Plain and carried over the Himalayas by convective storms and mid-tropospheric circulation, contributing over 50% to the TGM at the Lhasa urban site, based on the binary mixing model of isotopes. In contrast, during the transport of TGM from South Asia with low altitude, the uptake by evergreen forest in Yarlung Zangbo Grand Canyon largely decreased the TGM level and shifted isotopic compositions in TGM at the Nyingchi forest site, which are located at the high-altitude end of the canyon. Our results provided direct evidence from Hg isotopes to reveal the distinct patterns of transboundary transport to the Tibetan Plateau shaped by landforms and climates, which is critical to fully understand the biogeochemical cycling of Hg in the high-altitude regions.

This study reports a sensitive online method for Hg isotope analysis at ultratrace levels by automated P&T-MC-ICPMS.

Clarifying the sources and fates of atmospheric mercury (Hg) in the Antarctic is crucial to understand the global Hg circulation and its impacts on the fragile ecosystem of the Antarctic. Herein, the annual variations in the isotopic compositions of total gaseous Hg (TGM), with 5-22 days of sampling duration for each sample, were presented for the first time to provide isotopic evidence of the sources and environmental processes of gaseous Hg around the Chinese Great Wall Station (GWS) in the western Antarctic. Different from the Arctic tundra and lower latitude areas in the northern hemisphere, positive δ202Hg (0.58 ± 0.21‰, mean ± 1SD) and negative Δ199Hg (-0.30 ± 0.10‰, mean ± 1SD) in TGM at the GWS indicated little impact from the vegetation-air exchange in the Antarctic. Correlations among TGM Δ199Hg, air temperature, and ozone concentrations suggested that enhanced katabatic wind that transported inland air masses to the continental margin elevated TGM Δ199Hg in the austral winter, while the surrounding marine surface emissions controlled by sea-ice dynamics lowered TGM Δ199Hg in the austral summer. The oxidation of Hg(0) might elevate Δ199Hg in TGM during atmospheric Hg depletion events but have little impact on the seasonal variations of atmospheric Hg isotopes. The presented atmospheric Hg isotopes were essential to identify the transport and transformation of atmospheric Hg and further understand Hg cycling in the Antarctic.

Although global mercury (Hg) emission from chlor-alkali industry is decreasing, the legacy Hg may still have potential risks due to its environmental persistence. The objective of this work is to study the biogeochemical cycling and potential risk of Hg in the Ya-Er Lake, which was heavily contaminated by historical chlor-alkali production. Higher concentrations of total Hg (THg) in Ya-Er Lake water (16.8 ± 8.4 ng L−1) and sediment (547 ± 489 ng g−1) than other lake systems were observed, reflecting serious Hg pollution in this system. Diffusion rates of Hg at sediment-water interface and budget of Hg showed that release of legacy Hg in sediment (accounting for ∼80%) dominated THg in water, and about 80% methylmercury (MeHg) of total was diffused from sediment. Significant correlations between total organic carbon (TOC) derived from aquaculture and THg diffusion and MeHg concentrations in sediment suggest that TOC plays important roles in controlling legacy Hg release and MeHg production. The actual weekly intakes of Hg via consumption of cultured catfish and wild topmouth culter were higher than the established provisional tolerable weekly intake (PTWI) of MeHg. These results indicated that although the nearby chlor-alkali plant has been shut down for three decades, the release of legacy Hg stored in the sediment still adversely affects this ecosystem. Moreover, aquaculture could enhance MeHg production and control MeHg distribution in the polluted aquatic ecosystem, potentially posing a health risk to surrounding inhabitants through consumption of fish.

Marine boundary layer (MBL) is the largest transport place and reaction vessel of atmospheric mercury (Hg). The transformations of atmospheric Hg in MBL are crucial for the global transport and deposition of Hg. Herein, Hg isotopic signatures in total gaseous mercury (TGM) and particulate bound Hg (PBM) collected during three cruises to Chinese seas in summer and winter were measured to reveal the transformation processes of atmospheric Hg in the MBL. Unlike the observation results at inland sites, isotopic compositions in TGM from MBL were shaped not only by mixing continental emissions, but also largely by the oxidation of Hg0 primarily derived by Br atoms. Lower air temperature could promote the positive MIF in TGM in summer, while the relative processes might be weak in winter. In contrast, the positive Δ199Hg and high ratios of Δ199Hg / Δ201Hg in PBM indicated that alternative oxidants other than Br or Cl atoms played a major role in the formation of Hg(II) in PBM, likely following the nuclear volume effect. Our results suggested the importance of local Hg environmental behaviours caused by an abundance of highly reactive species, and provided new evidence for understanding the complicated transformations of atmospheric Hg in the MBL.

The Bohai Sea (BS) and Yellow Sea (YS), which are adjacent to the most urbanized and industrialized areas in China, are facing a variety of environmental problems. Two cruises were conducted to investigate the pollution status of toxic metals in BS and YS sediments. They generally presented a decreasing trend from near shore to offshore. In addition, two high concentration areas were observed in the central south YS and north of the Shandong Peninsula. The results of multiple regression analyses suggest that Hg is mainly controlled by anthropogenic loading, whereas for Cr, Cu, Ni, Pb and Zn, sediment properties, especially the Fe oxides content, play a more important role. For As and Cd, the contribution of anthropogenic loading and sediment properties are comparable. The risk assessment indicates that Hg, As, Cd and Ni should be listed as the primary contaminant metals in the BS and YS.