中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China

文献类型:期刊论文

作者Zeng, Yaling1,2; Shen, Zhenxing1,3; Takahama, Satoshi2; Zhang, Leiming4,5; Zhang, Tian1; Lei, Yali1; Zhang, Qian1; Xu, Hongmei1; Ning, Yanli6; Huang, Yu3
刊名GEOPHYSICAL RESEARCH LETTERS
出版日期2020-05-28
卷号47期号:10页码:11
ISSN号0094-8276
关键词brown carbon molecular absorption carbon conjugation N-addition oxidation and sulfur addition
DOI10.1029/2020GL087977
英文摘要

Knowledge of the molecular-level chemistry of brown carbon (BrC) is important in reducing the uncertainties in aerosol radiative forcing. Time-resolved ambient PM2.5 samples were collected during a severe pollution episode in January 2017 over Xi'an, China for a comprehensive nontarget and full scanning of BrC molecules and their absorption properties using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis, which apportioned the overall ultraviolet absorption to individual molecules. The estimated absorption of CHNO and CHNOS molecules exhibited nighttime prevalence, whereas CHOS, CHNS, CHN, CHO, CHS, and CH molecules presented a dynamic trend. Carbon conjugation was positively correlated with estimated absorption by CHO and CHNO molecules, while exhibiting a mixed relationship with CHNOS. Higher nitrogen content was associated with enhanced light-absorption properties of BrC molecules, while higher oxygen and sulfur content appeared to be associated with photobleaching during secondary transformation. Plain Language Summary Individual molecular absorption has significant implications for ambient brown carbon analysis, but existing studies mostly focused on bulk absorption properties for the sample as a whole. A novel method is presented here to evaluate individual brown carbon absorption at the molecular level through high resolution mass spectrometry, and partial least squares regression analysis was applied to PM2.5 samples collected during a heavy pollution episode in Xi'an, China. Nitrogen-containing compounds were found to be the strongest contributor to brown carbon absorption, especially during the nighttime, while processes involving oxidation and sulfur addition appeared to weaken the molecular absorption. This study bridges the gap between real atmospheric PM2.5 absorption and knowledge from controlled laboratory studies, which support these findings.

WOS关键词SECONDARY ORGANIC AEROSOLS ; COMPLEX REFRACTIVE-INDEX ; OPTICAL-PROPERTIES ; PARTICULATE MATTER ; LIGHT-ABSORPTION ; GUANZHONG PLAIN ; OXIDATION ; URBAN ; ORGANOSULFATES ; PARTICLES
资助项目Natural Science Foundation of China[41877383] ; Natural Science Foundation of China[91644219] ; Natural Science Foundation of China[21661132005] ; SKLLQG, Chinese Academy of Sciences[SKLLQG1919] ; China Scholarship Council[201806280091]
WOS研究方向Geology
语种英语
出版者AMER GEOPHYSICAL UNION
WOS记录号WOS:000560371700034
资助机构Natural Science Foundation of China ; SKLLQG, Chinese Academy of Sciences ; China Scholarship Council
源URL[http://ir.ieecas.cn/handle/361006/15225]  
专题地球环境研究所_粉尘与环境研究室
通讯作者Shen, Zhenxing
作者单位1.Xi An Jiao Tong Univ, Dept Environm Sci & Engn, Xian, Peoples R China
2.ENAC IIE Swiss Fed Inst Technol Lausanne EPFL, Lausanne, Switzerland
3.Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Xian, Peoples R China
4.Environm & Climate Change Canada, Sci Branch, Air Qual Res Div, Toronto, ON, Canada
5.Environm & Climate Change Canada, Technol Branch, Air Qual Res Div, Toronto, ON, Canada
6.Xian Modern Chem Res Inst, Sate Key Lab Fluorine & Nitrogen Chem, Xian, Peoples R China
推荐引用方式
GB/T 7714
Zeng, Yaling,Shen, Zhenxing,Takahama, Satoshi,et al. Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China[J]. GEOPHYSICAL RESEARCH LETTERS,2020,47(10):11.
APA Zeng, Yaling.,Shen, Zhenxing.,Takahama, Satoshi.,Zhang, Leiming.,Zhang, Tian.,...&Rudolf, Hohn.(2020).Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China.GEOPHYSICAL RESEARCH LETTERS,47(10),11.
MLA Zeng, Yaling,et al."Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China".GEOPHYSICAL RESEARCH LETTERS 47.10(2020):11.

入库方式: OAI收割

来源:地球环境研究所

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