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DOI | 10.1073/pnas.1912235117 |
Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation | |
Ji, Yuemen1,2,3,4; Shi, Qiuju1,2; Li, Yixin3,4; An, Taicheng1,2; Zheng, Jun5; Peng, Jianfei3,4; Gao, Yanpeng1,2; Chen, Jiangyao1,2; Li, Guiying1,2; Wang, Yuan6; Zhang, Fang3,4,7; Zhang, Annie L.8; Zhao, Jiayun3,4; Molina, Mario J.9; Zhang, Renyi3,4 | |
2020-06-03 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2020 |
卷号 | 117期号:24页码:13294-13299 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China; USA |
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 a-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. |
英文关键词 | secondary organic aerosol aqueous oligomerization brown carbon cationic |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000546040300025 |
WOS关键词 | SOLVATION ; CHEMISTRY ; MECHANISM ; KINETICS ; PATHWAY ; GLYOXAL ; PHASE ; HAZE |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/273368 |
专题 | 地球科学 |
作者单位 | 1.Guangdong Univ Technol, Inst Environm Hlth & Pollut Control, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou 510006, Peoples R China; 2.Guangdong Univ Technol, Guangzhou Key Lab Environm Catalysis & Pollut Con, Sch Environm Sci & Engn, Guangzhou 510006, Peoples R China; 3.Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA; 4.Texas A&M Univ, Dept Chem, College Stn, TX 77843 USA; 5.Nanjing Univ Informat Sci & Technol, Collaborat Innovat Ctr Atmospher Environm & Equip, Nanjing 210044, Peoples R China; 6.CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA; 7.Beijing Normal Univ, Coll Global Change & Earth Syst Sci, State Key Lab Earth Surface Proc & Resource Ecol, Beijing 100875, Peoples R China; 8.Univ Texas Austin, Coll Nat Sci, Dept Chem, Austin, TX 78712 USA; 9.Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA |
推荐引用方式 GB/T 7714 | Ji, Yuemen,Shi, Qiuju,Li, Yixin,et al. Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2020,117(24):13294-13299. |
APA | Ji, Yuemen.,Shi, Qiuju.,Li, Yixin.,An, Taicheng.,Zheng, Jun.,...&Zhang, Renyi.(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),13294-13299. |
MLA | Ji, Yuemen,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):13294-13299. |
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