CCPortal
DOI10.1073/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
ISSN0027-8424
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).
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Ji Y.]的文章
[Shi Q.]的文章
[Li Y.]的文章
百度学术
百度学术中相似的文章
[Ji Y.]的文章
[Shi Q.]的文章
[Li Y.]的文章
必应学术
必应学术中相似的文章
[Ji Y.]的文章
[Shi Q.]的文章
[Li Y.]的文章
相关权益政策
暂无数据
收藏/分享

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。