HgBr与O之间的反应：动力学研究及大气意义
The reaction between HgBr and O: kinetic study and atmospheric implications.
作者信息
Gómez Martín Juan Carlos, Lewis Thomas R, Douglas Kevin M, Blitz Mark A, Saiz-Lopez Alfonso, Plane John M C
机构信息
Instituto de Astrofísica de Andalucía, CSIC, 18008, Granada, Spain.
Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Serrano 119, 28006 Madrid, Spain.
出版信息
Phys Chem Chem Phys. 2022 May 25;24(20):12419-12432. doi: 10.1039/d2cp00754a.
The rate constants of many reactions currently considered to be important in the atmospheric chemistry of mercury remain to be measured in the laboratory. Here we report the first experimental determination of the rate constant of the gas-phase reaction between the HgBr radical and ozone, for which a value at room temperature of (HgBr + O) = (7.5 ± 0.6) × 10 cm molecule s (1) has been obtained. The rate constants of two reduction side reactions were concurrently determined: (HgBr + O) = (5.3 ± 0.4) × 10 cm molecule s and (HgBrO + O) = (9.1 ± 0.6) × 10 cm molecule s. The value of (HgBr + O) is slightly lower than the collision number, confirming the absence of a significant energy barrier. Considering the abundance of ozone in the troposphere, our experimental rate constant supports recent modelling results suggesting that the main atmospheric fate of HgBr is reaction with ozone to form BrHgO.
目前认为在汞的大气化学中许多重要反应的速率常数仍有待在实验室中测量。在此，我们报告了HgBr自由基与臭氧之间气相反应速率常数的首次实验测定结果，室温下得到的（HgBr + O）的值为(7.5 ± 0.6) × 10⁻¹² cm³ molecule⁻¹ s⁻¹ (1)。同时测定了两个还原副反应的速率常数：（HgBr + O） = (5.3 ± 0.4) × 10⁻¹² cm³ molecule⁻¹ s⁻¹ 和（HgBrO + O） = (9.1 ± 0.6) × 10⁻¹² cm³ molecule⁻¹ s⁻¹。（HgBr + O）的值略低于碰撞数，这证实不存在显著的能垒。考虑到对流层中臭氧的丰度，我们的实验速率常数支持了最近的模型结果，表明HgBr在大气中的主要归宿是与臭氧反应形成BrHgO。
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