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Isotopic Composition of Atmospheric Mercury in China: New Evidence for Sources and Transformation Processes in Air and in Vegetation

机译:中国大气汞的同位素组成:空气和植被的来源和转化过程的新证据

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摘要

The isotopic composition of atmospheric total gaseous mercury (TGM) and particle-bound mercury (PBM) and mercury (Hg) in litterfall samples have been determined at urban/industrialized and rural sites distributed over mainland China for identifying Hg sources and transformation processes. TGM and PBM near anthropogenic emission sources display negative δ~(202)Hg and near-zero △~(199)Hg in contrast to relatively positive δ~(202)Hg and negative △~(199)Hg observed in remote regions, suggesting that different sources and atmospheric processes force the mass-dependent fractionation (MDF) and mass-independent fractionation (MIF) in the air samples. Both MDF and MIF occur during the uptake of atmospheric Hg by plants, resulting in negative δ~(202)Hg and △~(199)Hg observed in litter-bound Hg. The linear regression resulting from the scatter plot relating the δ~(202)Hg to △~(199)Hg data in the TGM samples indicates distinct anthropogenic or natural influences at the three study sites. A similar trend was also observed for Hg accumulated in broadleaved deciduous forest foliage grown in areas influenced by anthropogenic emissions. The relatively negative MIF in litter-bound Hg compared to TGM is likely a result of the photochemical reactions of Hg~(2+) in foliage. This study demonstrates the diagnostic stable Hg isotopic composition characteristics for separating atmospheric Hg of different source origins in China and provides the isotopic fractionation clues for the study of Hg bioaccumulation.
机译:已确定了分布在中国大陆各地的城市/工业化和农村地区的凋落物样本中的大气总气态汞(TGM)和颗粒结合汞(PBM)和汞(Hg)的同位素组成,以确定汞的来源和转化过程。人为排放源附近的TGM和PBM的δ〜(202)Hg负值△〜(199)Hg接近零,而偏远地区的δ〜(202)Hg和△〜(199)Hg值相对较正,表明不同的来源和大气过程迫使空气样品中的质量分数(MDF)和质量分数(MIF)。 MDF和MIF都在植物吸收大气中的Hg时发生,导致与凋落物结合的Hg中观测到负的δ〜(202)Hg和△〜(199)Hg。由TGM样品中δ〜(202)Hg与△〜(199)Hg数据相关的散点图得出的线性回归表明,在三个研究地点存在明显的人为或自然影响。在受人为排放影响的地区生长的阔叶落叶林中,汞的累积趋势也相似。与TGM相比,凋落物中Hg相对较弱的MIF可能是叶片中Hg〜(2+)发生光化学反应的结果。该研究证明了中国分离出不同来源的大气汞的诊断稳定的汞同位素组成特征,并为研究汞的生物富集提供了同位素分级线索。

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  • 来源
    《Environmental Science & Technology》 |2016年第17期|9262-9269|共8页
  • 作者单位

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China,Department of Civil and Environmental Engineering, Lamar University, Beaumont, Texas United States;

    University of Chinese Academy of Sciences, Beijing 100049, China,Key Laboratory of Tropical Forest Ecology, Xishuangbanna Tropical Botanical Garden, Chinese Academy of Sciences, Mengla, 666303, China;

    Key Laboratory of Tropical Forest Ecology, Xishuangbanna Tropical Botanical Garden, Chinese Academy of Sciences, Mengla, 666303, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

    Observatoire Midi-Pyrenees, Laboratoire Geosciences Environnement Toulouse, CNRS/IRD/Universite Paul Sabatier, 14 Avenue Edouard-Belin, 31400 Toulouse, France;

    Observatoire Midi-Pyrenees, Laboratoire Geosciences Environnement Toulouse, CNRS/IRD/Universite Paul Sabatier, 14 Avenue Edouard-Belin, 31400 Toulouse, France;

    Laboratoire d'Aerologie, Universite de Toulouse, CNRS, UPS, 14 Avenue Edouard-Belin, 31400 Toulouse, France;

    State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China;

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