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DOI | 10.1073/pnas.1812147115 |
Quantitative constraints on autoxidation and dimer formation from direct probing of monoterpene-derived peroxy radical chemistry | |
Zhao, Yue1,2; Thornton, Joel A.2; Pye, Havala O. T.2,3 | |
2018-11-27 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2018 |
卷号 | 115期号:48页码:12142-12147 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China; USA |
英文摘要 | Organic peroxy radicals (RO2) are key intermediates in the atmospheric degradation of organic matter and fuel combustion, but to date, few direct studies of specific RO2 in complex reaction systems exist, leading to large gaps in our understanding of their fate. We show, using direct, speciated measurements of a suite of RO2 and gas-phase dimers from O-3-initiated oxidation of alpha-pinene, that similar to 150 gaseous dimers (C16-20H24-34O4-13) are primarily formed through RO2 cross-reactions, with a typical rate constant of 0.75-2 x 10(-12) cm(3) molecule(-1) s(-1) and a lower-limit dimer formation branching ratio of 4%. These findings imply a gaseous dimer yield that varies strongly with nitric oxide (NO) concentrations, of at least 0.2-2.5% by mole (0.5-6.6% by mass) for conditions typical of forested regions with low to moderate anthropogenic influence (i.e., <= 50-parts per trillion NO). Given their very low volatility, the gaseous C16-20 dimers provide a potentially important organic medium for initial particle formation, and alone can explain 5-60% of alpha-pinene secondary organic aerosol mass yields measured at atmospherically relevant particle mass loadings. The responses of RO2, dimers, and highly oxygenated multifunctional compounds (HOM) to reacted alpha-pinene concentration and NO imply that an average similar to 20% of primary alpha-pinene RO2 from OH reaction and 10% from ozonolysis autoxidize at 3-10 s(-1) and >= 1 s(-1), respectively, confirming both oxidation pathways produce HOM efficiently, even at higher NO concentrations typical of urban areas. Thus, gas-phase dimer formation and RO2 autoxidation are ubiquitous sources of low-volatility organic compounds capable of driving atmospheric particle formation and growth. |
英文关键词 | monoterpenes peroxy radicals autoxidation dimers particle formation |
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:000451351000046 |
WOS关键词 | SECONDARY ORGANIC AEROSOL ; ALPHA-PINENE OZONOLYSIS ; GAS-PHASE OZONOLYSIS ; OLIGOMER FORMATION ; PARTICLE FORMATION ; CRIEGEE INTERMEDIATE ; VOLATILITY ; PRODUCTS ; GROWTH ; EMISSIONS |
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/205018 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China; 2.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA; 3.US EPA, Natl Exposure Res Lab, Res Triangle Pk, NC 27711 USA |
推荐引用方式 GB/T 7714 | Zhao, Yue,Thornton, Joel A.,Pye, Havala O. T.. Quantitative constraints on autoxidation and dimer formation from direct probing of monoterpene-derived peroxy radical chemistry[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2018,115(48):12142-12147. |
APA | Zhao, Yue,Thornton, Joel A.,&Pye, Havala O. T..(2018).Quantitative constraints on autoxidation and dimer formation from direct probing of monoterpene-derived peroxy radical chemistry.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,115(48),12142-12147. |
MLA | Zhao, Yue,et al."Quantitative constraints on autoxidation and dimer formation from direct probing of monoterpene-derived peroxy radical chemistry".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 115.48(2018):12142-12147. |
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