CH3O2与BrO自由基之间的反应：对流层上部-平流层下部羟基自由基的新来源。
Reaction between CH3O2 and BrO radicals: a new source of upper troposphere lower stratosphere hydroxyl radicals.
作者信息
Shallcross Dudley E, Leather Kimberley E, Bacak Asan, Xiao Ping, Lee Edmond P F, Ng Maggie, Mok Daniel K W, Dyke John M, Hossaini Ryan, Chipperfield Martyn P, Khan M Anwar H, Percival Carl J
机构信息
†School of Chemistry, University of Bristol, Bristol BS8 1TS, U.K.
‡School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Williamson Building, Oxford Road, Manchester M13 9PL, U.K.
出版信息
J Phys Chem A. 2015 May 14;119(19):4618-32. doi: 10.1021/jp5108203. Epub 2015 Mar 27.
Over the last two decades it has emerged that measured hydroxyl radical levels in the upper troposphere are often underestimated by models, leading to the assertion that there are missing sources. Here we report laboratory studies of the kinetics and products of the reaction between CH3O2 and BrO radicals that shows that this could be an important new source of hydroxyl radicals:BrO + CH3O2 → products (1). The temperature dependent value in Arrhenius form of k(T) is k1 = (2.42–0.72+1.02) × 10–14 exp[(1617 ± 94)/T] cm3 molecule–1 s–1. In addition, CH2OO and HOBr are believed to be the major products. Global model results suggest that the decomposition of H2COO to form OH could lead to an enhancement in OH of up to 20% in mid-latitudes in the upper troposphere and in the lower stratosphere enhancements in OH of 2–9% are inferred from model integrations. In addition, reaction 1 aids conversion of BrO to HOBr and slows polar ozone loss in the lower stratosphere.
在过去二十年中，人们发现对流层上层实测的羟基自由基水平常常被模型低估，这导致有人断言存在未被考虑的来源。在此我们报告了关于CH3O2与BrO自由基反应动力学及产物的实验室研究，结果表明这可能是羟基自由基的一个重要新来源：BrO + CH3O2 → 产物 (1)。k(T)的Arrhenius形式的温度依赖值为k1 = (2.42–0.72 + 1.02) × 10–14 exp[(1617 ± 94)/T] cm3 molecule–1 s–1。此外，CH2OO和HOBr被认为是主要产物。全球模型结果表明，H2COO分解形成OH可能导致对流层上层中纬度地区的OH增加高达20%，并且从模型积分推断，平流层下层的OH增加了2 - 9%。此外，反应(1)有助于将BrO转化为HOBr，并减缓平流层下层极地臭氧的损耗。
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