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DOI | 10.1073/pnas.1912235117 |
Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation | |
Ji Y.; Shi Q.; Li Y.; An T.; Zheng J.; Peng J.; Gao Y.; Chen J.; Li G.; Wang Y.; Zhang F.; Zhang A.L.; Zhao J.; Molina M.J.; Zhang R. | |
发表日期 | 2020 |
ISSN | 0027-8424 |
起始页码 | 13294 |
结束页码 | 13299 |
卷号 | 117期号:24 |
英文摘要 | Secondary organic aerosol (SOA) represents a major constituent of tropospheric fine particulate matter, with profound implications for human health and climate. However, the chemical mechanisms leading to SOA formation remain uncertain, and atmospheric models consistently underpredict the global SOA budget. Small α-dicarbonyls, such as methylglyoxal, are ubiquitous in the atmosphere because of their significant production from photooxidation of aromatic hydrocarbons from traffic and industrial sources as well as from biogenic isoprene. Current experimental and theoretical results on the roles of methylglyoxal in SOA formation are conflicting. Using quantum chemical calculations, we show cationic oligomerization of methylglyoxal in aqueous media. Initial protonation and hydration of methylglyoxal lead to formation of diols/tetrol, and subsequent protonation and dehydration of diols/tetrol yield carbenium ions, which represent the key intermediates for formation and propagation of oligomerization. On the other hand, our results reveal that the previously proposed oligomerization via hydration for methylglyoxal is kinetically and thermodynamically implausible. The carbenium ion-mediated mechanism occurs barrierlessly on weakly acidic aerosols and cloud/fog droplets and likely provides a key pathway for SOA formation from biogenic and anthropogenic emissions. © 2020 National Academy of Sciences. All rights reserved. |
英文关键词 | Aqueous; Brown carbon; Cationic; Oligomerization; Secondary organic aerosol |
语种 | 英语 |
scopus关键词 | carbenium ion; diol; ion; methylglyoxal; organic compound; tetrol; unclassified drug; aqueous solution; Article; controlled study; hydration; kinetics; oligomerization; priority journal; protonation; quantum chemistry; secondary organic aerosol; thermodynamics |
来源期刊 | Proceedings of the National Academy of Sciences of the United States of America |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/160912 |
作者单位 | Ji, Y., Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, 510006, China, Guangzhou Key Laboratory Environmental Catalysis and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China, Department of Atmospheric Sciences, Texas A & M University, College Station, TX 77843, United States, Department of Chemistry, Texas A & M University, College Station, TX 77843, United States; Shi, Q., Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, 510006, China, Guangzhou Key Laboratory Environmental Catalysis and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China; Li, Y., Department of Atmospheric Sciences, Texas ... |
推荐引用方式 GB/T 7714 | Ji Y.,Shi Q.,Li Y.,et al. Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation[J],2020,117(24). |
APA | Ji Y..,Shi Q..,Li Y..,An T..,Zheng J..,...&Zhang R..(2020).Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation.Proceedings of the National Academy of Sciences of the United States of America,117(24). |
MLA | Ji Y.,et al."Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation".Proceedings of the National Academy of Sciences of the United States of America 117.24(2020). |
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