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Changes to simulated global atmospheric composition resulting from recent revisions to isoprene oxidation chemistry
Atmospheric Environment ( IF 5 ) Pub Date : 2021-01-01 , DOI: 10.1016/j.atmosenv.2020.117914
M. Anwar H. Khan , Billie-Louise Schlich , Michael E. Jenkin , Michael C. Cooke , Richard G. Derwent , Jessica L. Neu , Carl J. Percival , Dudley E. Shallcross

Abstract Recent revisions to our understanding of the oxidation chemistry of isoprene have been incorporated into a well-established global atmospheric chemistry and transport model, STOCHEM-CRI. These revisions have previously been shown to increase the production and recycling of HOx radicals at lower NOx levels characteristic of the remote troposphere. The main aim of this study is to assess the resultant broader changes to atmospheric composition due to the recent revisions to isoprene oxidation chemistry. The impact of the increased isoprene-related HOx recycling is found to be significant on the reduction of volatile organic compounds (VOCs) lifetime, e.g. a decrease in isoprene's tropospheric burden by ~17%. The analysis of lifetime reduction of the potent greenhouse gas, methane, associated with the increased HOx recycling, suggests its significant lifetime reduction by ~5% in terms of the current literature. The revisions to the isoprene chemistry also reduce the amount of ozone (by up to 10%), but provide a significant increase in NO3 (by up to 30%) over equatorial forested regions, which can alter the oxidizing capacity of the troposphere. The calculated mixing ratios of formic acid are decreased which in turn leads to an increase in the inferred concentrations of Criegee intermediates due to reduced loss through reaction with formic acid (up to 80%) over the dominant isoprene emitting regions.

中文翻译:

由于最近对异戊二烯氧化化学进行修订而导致模拟的全球大气成分发生变化

摘要 我们对异戊二烯氧化化学理解的最新修订已纳入完善的全球大气化学和传输模型 STOCHEM-CRI。这些修订先前已被证明可以在偏远对流层特征的较低 NOx 水平下增加 HOx 自由基的产生和再循环。本研究的主要目的是评估由于最近对异戊二烯氧化化学的修订而导致的大气成分更广泛的变化。发现增加的与异戊二烯相关的 HOx 循环的影响对减少挥发性有机化合物 (VOC) 的寿命具有显着影响,例如,异戊二烯的对流层负荷减少约 17%。分析与增加的 HOx 循环相关的强效温室气体甲烷的寿命减少,表明就当前文献而言,其使用寿命显着减少了约 5%。异戊二烯化学的修订也减少了臭氧量(最多 10%),但在赤道森林地区显着增加了 NO3(最多 30%),这会改变对流层的氧化能力。计算出的甲酸混合比例降低,这反过来又导致 Criegee 中间体的推断浓度增加,因为在主要异戊二烯发射区域与甲酸反应的损失减少(高达 80%)。这可以改变对流层的氧化能力。计算出的甲酸混合比例降低,这反过来又导致 Criegee 中间体的推断浓度增加,因为在主要异戊二烯发射区域与甲酸反应的损失减少(高达 80%)。这可以改变对流层的氧化能力。计算出的甲酸混合比例降低,这反过来又导致 Criegee 中间体的推断浓度增加,因为在主要异戊二烯发射区域与甲酸反应的损失减少(高达 80%)。
更新日期:2021-01-01
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