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题名: Mass-Dependent and -Independent Fractionation of Mercury Isotope during Gas-Phase Oxidation of Elemental Mercury Vapor by Atomic Cl and Br
作者: Sun, Guangyi1, 3; Sommar, Jonas1; Feng, Xinbin1; Lin, Che-Jen1, 4; Ge, Maofa5; Wang, Weigang5; Yin, Runsheng2, 6; Fu, Xuewu1; Shang, Lihai1
刊名: ENVIRONMENTAL SCIENCE & TECHNOLOGY
发表日期: 2016-09-06
卷: 50, 期:17, 页:9232-9241
收录类别: SCI
英文摘要: This study presents the first measurement of Hg stable isotope fractionation during gas-phase oxidation of Hg vapor by halogen atoms (Cl-center dot, Br-center dot) in the laboratory at 750 +/- 1 Torr and 298 +/- 3 K. Using a relative rate technique, the rate coefficients for Hg-0+Cl-center dot and Hg-0+Br-center dot reactions are determined to be (1.8 +/- 0.5) X 10(-11) and (1.6 +/- 0.8) X 10(-12) cm(3) molecule(-1) s(-1), respectively. Results show that heavier isotopes are preferentially enriched in the remaining Hg-0 during Cl-center dot initiated oxidation, whereas being enriched in the product during oxidation by Br-center dot. The fractionation factors for Hg-202/Hg-198 during the Cl-center dot and Br-center dot initiated oxidations are alpha(202/198) = 0.99941 +/- 0.00006 (2 sigma) and 1.00074 +/- 0.00014 (2 sigma), respectively. A Delta Hg-199/Delta Hg-201 ratio of 1.64 +/- 0.30 (2 sigma) during oxidation of Hg-0 by Br atoms suggests that Hg-MIF is introduced by the nuclear volume effect (NVE). In contrast, the Hg-0 + Cl-center dot reaction produces a Delta Hg-199/Delta Hg-201-slope of 1.89 +/- 0.18 (2 sigma), which in addition to a high degree of odd-mass-number isotope MIF suggests impacts from MIF effects other than NVE. This reaction also exhibits significant MIF of Hg-200 (Delta Hg-200, up to -0.17 parts per thousand in the reactant) and is the first physicochemical process identified to trigger Hg-200 anomalies that are frequently detected in atmospheric samples.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35137
Appears in Collections:分子动态与稳态结构实验室_期刊论文

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作者单位: 1.Chinese Acad Sci, Inst Geochem, SKLEG, Guiyang 550002, Peoples R China
2.Chinese Acad Sci, Inst Geochem, State Key Lab Ore Deposit Geochem, Guiyang 550002, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100190, Peoples R China
4.Lamar Univ, Ctr Adv Water & Air Qual, Beaumont, TX 77710 USA
5.Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China
6.Univ Wisconsin, Environm Chem & Technol Program, Madison, WI 53706 USA
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