气候变化领域集成服务门户(CCPortal): Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)

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DOI	10.5194/acp-21-8999-2021
	Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)
	Dovrou E.; Bates K.H.; Rivera-Rios J.C.; Cox J.L.; Shutter J.D.; Keutsch F.N.
发表日期	2021
ISSN	1680-7316
起始页码	8999
结束页码	9008
卷号	21 期号:11
英文摘要	In-cloud chemistry has important ramifications for atmospheric particulate matter formation and gas-phase chemistry. Recent work has shown that, like hydrogen peroxide (H2O2), the two main isomers of isoprene hydroxyl hydroperoxide (ISOPOOH) oxidize sulfur dioxide dissolved in cloud droplets (SO2,aq) to sulfate. The work revealed that the pathway of SO2,aq oxidation with ISOPOOH differs from that of H2O2. We investigate the chemical mechanisms of oxidation of SO2,aq with ISOPOOH in the cloud-relevant pH range of 3-6 and compare them with the previously reported mechanisms of oxidation of SO2,aq with H2O2, methyl hydroperoxide and peroxyacetic acid. The organic products of the reaction are identified, and two pathways are proposed. For 1,2-ISOPOOH, a higher yield pathway via proposed radical intermediates yields methyl vinyl ketone (MVK) and formaldehyde, which can react to hydroxymethanesulfonate (HMS) when SO2,aq is present. A lower yield non-fragmentation oxygen addition pathway is proposed that results in the formation of isoprene-derived diols (ISOPOH). Based on global simulations, this mechanism is not a significant pathway for formation of MVK and formaldehyde relative to their gas-phase formation but, as previously reported, it can be regionally important for sulfate production. The study adds to previous work that highlights similarities and differences between gas-phase and cloud-droplet processing of reactive organic carbon. © Copyright:
语种	英语
scopus关键词	atmospheric chemistry; chemical reaction; hydrogen peroxide; isoprene; oxidation; sulfur dioxide
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/246810
作者单位	John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Harvard University Center for the Environment, Cambridge, MA 02138, United States; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, United States; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, United States; Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany; School of ChemicalĝandĝBiomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States
推荐引用方式 GB/T 7714	Dovrou E.,Bates K.H.,Rivera-Rios J.C.,et al. Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)[J],2021,21(11).
APA	Dovrou E.,Bates K.H.,Rivera-Rios J.C.,Cox J.L.,Shutter J.D.,&Keutsch F.N..(2021).Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH).ATMOSPHERIC CHEMISTRY AND PHYSICS,21(11).
MLA	Dovrou E.,et al."Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.11(2021).