Acylperoxy Radicals as Key Intermediates in the Formation of Dimeric Compounds in a-Pinene Secondary Organic Aerosol

Yue Zhao; Min Yao; Yingqi Wang

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Acylperoxy Radicals as Key Intermediates in the Formation of Dimeric Compounds in a-Pinene Secondary Organic Aerosol

机译：Acylperoxy Radicals as Key Intermediates in the Formation of Dimeric Compounds in a-Pinene Secondary Organic Aerosol

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High molecular weight dimeric compounds constitute a significant.fraction of secondary organic aerosol(SOA)and have profound impacts on the properties and lifecycle of particles in the atmosphere.Although different formation mechanisms involving reactive intermediates and/or closed-shell monomeric species have been proposed for the particle-phase dimers,their relative importance remains in debate.Here,we report unambiguous experimental evidence of the important role of acyl organic peroxy radicals(RO2)and a small but non-negligible contribution from stabilized Criegee intermediates(SCIs)in the formation of particle-phase dimers during ozonolysis of a-pinene,one of the most important precursors for biogenic SOA.Specifically,we find that acyl RO2-involved reactions explain 50-80% of total oxygenated dimer signals(C_(15)-C_(20),O/C ≥ 0.4)and 20-30% of the total less oxygenated(O/C< 0.4)dimer signals.In particular,they contribute to 70% of C_(15)-C_(19)dimer ester formation,likely mainly via the decarboxylation of diacyl peroxides arising from acyl RO2 cross-reactions.In comparison,SCIs play a minor role in the formation of C_(15)-C_(19)dimer esters but react noticeably with the most abundant C_9 and C_(10)carboxylic acids and/or carbonyl products to form C_(19)-C_(20)dimeric peroxides,which are prone to particle-phase transformation to form more stable dimers without the peroxide functionality.This work provides a clearer view of the formation pathways of particle-phase dimers from a-pinene oxidation and would help reduce the uncertainties in future atmospheric modeling of the budget,properties,and health and climate impacts of SOA.

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《Environmental Science & Technology: ES&T》 |2022年第20期|14249-14261|共13页
作者
Yue Zhao; Min Yao; Yingqi Wang;
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作者单位

School of Environmental Science and Engineering,Shanghai Jiao Tong University,Shanghai 200240,China;

School of Environmental Science and Engineering Shanghai Jiao Tong University,Shanghai 200240,China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
secondary organic aerosol a-pinene oxidation; acylperoxy radicals; stabilized Criegee intermediates; dimers; formation mechanisms;

Acylperoxy Radicals as Key Intermediates in the Formation of Dimeric Compounds in a-Pinene Secondary Organic Aerosol

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