Probing isoprene photochemistry at atmospherically relevant nitric oxide levels

Probing isoprene photochemistry at atmospherically relevant nitric oxide levels
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在大气相关一氧化氮水平下探测异戊二烯光化学

DOI：
10.1016/j.chempr.2022.08.003
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发表时间：
2022
期刊：
Chem
影响因子：
23.5
通讯作者：
Brune, William H.
Brune, William H.
中科院分区：
化学1区
文献类型：
--
作者：
Zhang, Xuan;Wang, Siyuan;Apel, Eric C.;Schwantes, Rebecca H.;Hornbrook, Rebecca S.;Hills, Alan J.;DeMarsh, Kate E.;Moo, Zeyi;Ortega, John;Brune, William H.

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异戊二烯是生物排放物中的主要碳氢化合物，其反应性化学对全球大气的组成和净化能力具有控制性影响。尽管经过数十年的研究，异戊二烯在其大气化学中继续提供惊喜，特别是在低至中等水平的氮氧化物（NOx）的环境中。在这里，我们通过检查两种主要氧化产物的产率分布来探测这种“中间体-NOx”制度中的异戊二烯光化学氧化，即，甲基丙烯醛和甲基乙烯基酮，使用室内实验和飞机测量。这样的数据集提供了强大的约束异戊二烯过氧自由基相互转化的动力学-一个新发现的机制，基本上支配异戊二烯氧化碳流。通过对测量和模型的比较得出的见解进一步揭示了这一机制在地球仪上所有植被覆盖的大陆上的有效运作，不断调节自由基循环，并促进大气中臭氧和有机气溶胶的形成。
The reactive chemistry of isoprene, which is the dominant hydrocarbon in biogenic emissions, has a controlling influence on the composition and cleansing capacity of the global atmosphere. Despite decades of research, isoprene continues to offer surprises in its atmospheric chemistry, particularly in environments with low-to-moderate levels of nitrogen oxides (NOx). Here, we probe the isoprene photochemical oxidation in this "intermediate-NOx" regime by examining the yield distributions of two major oxidation products, i.e., methacrolein and methyl vinyl ketone, using chamber experiments and aircraft measurements. Such a dataset provides strong constraints on the kinetics of the isoprene peroxy radical interconversion—a newly discovered mechanism that essentially governs the isoprene oxidation carbon flow. Insights from measurement-model comparisons further reveal an efficient operation of this mechanism across all the vegetated continents over the globe, constantly modulating the radical cycling and contributing to the formation of ozone and organic aerosols in the atmosphere.
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发表时间： 2021-10
期刊： Bulletin of the American Meteorological Society
影响因子： 8
作者：
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发表时间： 2014-12
期刊： Atmospheric Chemistry and Physics
影响因子： 6.3
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DOI： 10.5194/acp-19-9613-2019
发表时间： 2019-07-31
期刊： ATMOSPHERIC CHEMISTRY AND PHYSICS
影响因子： 6.3
作者：
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DOI： 10.1038/ngeo1271
发表时间： 2011-10
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影响因子： 18.3
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Theoretically derived mechanisms of HPALD photolysis in isoprene oxidation.
异戊二烯氧化中 HPALD 光解作用的理论推导机制。
DOI： --
发表时间： 2017
期刊： Physical Chemistry, Chemical Physics - PCCP
影响因子： --
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