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DOI | 10.5194/acp-22-9843-2022 |
Functionality-based formation of secondary organic aerosol from m-xylene photooxidation | |
Li, Yixin; Zhao, Jiayun; Gomez-Hernandez, Mario; Lavallee, Michael; Johnson, Natalie M.; Zhang, Renyi | |
发表日期 | 2022 |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
起始页码 | 9843 |
结束页码 | 9857 |
卷号 | 22期号:15页码:15 |
英文摘要 | Photooxidation of volatile organic compounds (VOCs) produces condensable oxidized organics (COOs) to yield secondary organic aerosol (SOA), but the fundamental chemical mechanism for gas-to-particle conversion remains uncertain. Here we elucidate the production of COOs and their roles in SOA and brown carbon (BrC) formation from m-xylene oxidation by simultaneously monitoring the evolution of gas-phase products and aerosol properties in an environmental chamber. Four COO types with the distinct functionalities of dicarbonyls, carboxylic acids, polyhydroxy aromatics/quinones, and nitrophenols are identified from early-generation oxidation, with the yields of 25 %, 37 %, 5 %, and 3 %, respectively. SOA formation occurs via several heterogeneous processes, including interfacial interaction, ionic dissociation/acid-base reaction, and oligomerization, with the yields of (20 +/- 4) % and (32 +/- 7) % at 10 % and 70 % relative humidity (RH), respectively. Chemical speciation shows the dominant presence of oligomers, nitrogen-containing organics, and carboxylates at high RH and carboxylates at low RH. The identified BrC includes N-heterocycles/N-heterochains and nitrophenols, as evident from reduced single scattering albedo. The measured uptake coefficient (gamma) for COOs is dependent on the functionality, ranging from 3.7 x 10(-4) to 1.3 x 10(-2). A functionality-based kinetic framework is developed to predict SOA production from the observed concentrations and uptake coefficients for COOs, which reproduces the measurement from m-xylene oxidation. Our results reveal that photochemical oxidation of m-xylene represents a major source for SOA and BrC formation under urban environments, because of its large abundance, high reactivity with OH, and high yields for COOs. |
学科领域 | Environmental Sciences; Meteorology & Atmospheric Sciences |
语种 | 英语 |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
WOS记录号 | WOS:000835272400001 |
来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/273522 |
作者单位 | Texas A&M University System; Texas A&M University College Station; University of California System; University of California Irvine; Texas A&M University System; Texas A&M University College Station; Texas A&M University System; Texas A&M University College Station; Texas A&M Health Science Center |
推荐引用方式 GB/T 7714 | Li, Yixin,Zhao, Jiayun,Gomez-Hernandez, Mario,et al. Functionality-based formation of secondary organic aerosol from m-xylene photooxidation[J],2022,22(15):15. |
APA | Li, Yixin,Zhao, Jiayun,Gomez-Hernandez, Mario,Lavallee, Michael,Johnson, Natalie M.,&Zhang, Renyi.(2022).Functionality-based formation of secondary organic aerosol from m-xylene photooxidation.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(15),15. |
MLA | Li, Yixin,et al."Functionality-based formation of secondary organic aerosol from m-xylene photooxidation".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.15(2022):15. |
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