Isotopic Composition of Gaseous Elemental Mercury in the Free Troposphere of the Pic du Midi Observatory, France

被引：88
作者：
Fu, Xuewu [1 ,2 ]
Marusczak, Nicolas [1 ]
Wang, Xun [2 ]
Gheusi, Francois [3 ]
Sonke, Jeroen E. [1 ]
机构：
[1] Univ Toulouse, Observ Midi Pyrenees, Lab Geosci Environm Toulouse, CNRS,IRD, 14 Ave Edouard Belin, F-31400 Toulouse, France
[2] Chinese Acad Sci, Inst Geochem, State Key Lab Environm Geochem, 46 Guanshui Rd, Guiyang 550002, Peoples R China
[3] Univ Toulouse, Observ Midi Pyrenees, Lab Aerol, CNRS,IRD, 14 Ave Edouard Belin, F-31400 Toulouse, France
来源：
ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2016年 / 50卷 / 11期
基金：
欧洲研究理事会; 美国国家科学基金会;
关键词：
MASS-INDEPENDENT FRACTIONATION; SPECIATED ATMOSPHERIC MERCURY; KCL-COATED DENUDERS; OXIDIZED MERCURY; COAL DEPOSITS; HG; EMISSIONS; OZONE; UNCERTAINTIES; PRECIPITATION;
D O I：
10.1021/acs.est.6b00033
中图分类号：
X [环境科学、安全科学];
学科分类号：
08 ; 0830 ;
摘要：
Understanding the sources and transformations of mercury (Hg) in the free troposphere is a critical aspect of global Hg research. Here we present one year of observations of atmospheric Hg speciation and gaseous elemental Hg (GEM) isotopic composition at the high-altitude Pic du Midi Observatory (2860 m above sea level) in France. Biweekly integrated GEM from February 2012 to January 2013 revealed significant variations in delta Hg-202(GEM) (-0.04 parts per thousand to 0.52 parts per thousand) but not in Delta Hg-199(GEM) (-0.17 parts per thousand to -0.27 parts per thousand) or Delta Hg-200(GEM) (-0.10 parts per thousand to 0.05 parts per thousand). delta Hg-202(GEM) was negatively correlated with CO and reflected air mass origins from Europe (high CO, low delta Hg-202(GEM)) and from the Atlantic Ocean (low CO, high delta Hg-202(GEM)). We suggest that the delta Hg-202(GEM) variations represent mixing of recent low delta Hg-202(GEM) European anthropogenic emissions with high delta Hg-202(GEM) northern hemispheric background GEM. In addition, Atlantic Ocean free troposphere air masses showed a positive correlation between delta Hg-202(GEM) and gaseous oxidized Hg (GOM) concentrations, indicative of mass-dependent Hg isotope fractionation during GEM oxidation. On the basis of atmospheric delta Hg-202(GEM) and speciated Hg observations, we suggest that the oceanic free troposphere is a reservoir within which GEM is readily oxidized to GOM.
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收藏
页码：5641 / 5650
页数：10
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