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首页> 外文期刊>Environmental Science & Technology >A Theoretical Study of the Oxidation of Hg{sup}0 to HgBr{sub}2 in the Troposphere
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A Theoretical Study of the Oxidation of Hg{sup}0 to HgBr{sub}2 in the Troposphere

机译：对流层中Hg {sup} 0氧化为HgBr {sub} 2的理论研究

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摘要

The oxidation of elemental mercury (Hg{sup}0) to the divalent gaseous mercury dibromide (HgBr2) has been proposed to account for the removal of Hg° during depletion events in the springtime Arctic. The mechanism of this process is explored in this paper by theoretical calculations of the relevant rate coefficients. Rice-Ramsberger-Kassel- Marcus (RRKM) theory, together with ab initio quantum calculations where required, are used to estimate the following: recombination rate coefficients of Hg with Br, I, and 0; the thermal dissociation rate coefficient of HgBr; and the recombination rate coefficients of HgBr with Br, I, OH, and 62. A mechanism based on the initial recombination of Hg with Br, followed by the addition of a second radical (Br, I, or OH) in competition with thermal dissociation of HgBr, is able to account for the observed rate of Hg{sup}0removal, both in Arctic depletion events and at lower latitudes.
机译：已提出将元素汞（Hg {sup} 0）氧化为二价气态二溴化汞（HgBr2），以解决春季北极地区消耗事件中Hg°的去除问题。本文通过相关速率系数的理论计算来探索这一过程的机理。 Rice-Ramsberger-Kassel-Marcus（RRKM）理论，以及必要时从头算量子计算，均被用来估算以下各项：Hg与Br，I和0的复合率系数； HgBr的热解离速率系数；以及HgBr与Br，I，OH和62的复合速率系数。一种基于Hg与Br的初始复合，然后在热解离竞争中添加第二个自由基（Br，I或OH）的机理不论是在北极的耗竭事件还是在低纬度地区，HgBr的迁移率都能解释Hg {sup} 0的去除率。

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