Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China

doi:10.5194/acp-22-6919-2022

	Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China
	Jiang, Hongxing 1,2,3,4,6,7; Li, Jun 1,2,4; Tang, Jiao 1,2,4; Cui, Min 5; Zhao, Shizhen 1,2,4; Mo, Yangzhi 1,2,4; Tian, Chongguo6 ; Zhang, Xiangyun 1,2,4; Jiang, Bin 1,2,4; Liao, Yuhong 1,2,4; Chen, Yingjun 3; Zhang, Gan 1,2,4
发表期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN	1680-7316
	2022-05-30
卷号	22 期号:10 页码:6919-6935
DOI	10.5194/acp-22-6919-2022
英文摘要	Organosulfur compounds (OrgSs), especially organosulfates, have been widely reported to be present in large quantities in particulate organic matter found in various atmospheric environments. Despite hundreds of organosulfates and their formation mechanisms being previously identified, a large fraction of OrgSs remain unexplained at the molecular level, and a better understanding of their formation pathways and critical environmental parameters is required to explain the variations in their concentrations. In this study, the abundance and molecular composition of OrgSs in fine particulate samples collected in Guangzhou were reported. The results revealed that the ratio of the annual average mass of organic sulfur to total particulate sulfur was 33 +/- 12 %, and organic sulfur had positive correlations with SO2 (r = 0.37, p < 0.05) and oxidant (NOx + O-3, r = 0.40, p < 0.01). A Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis revealed that more than 80 % of the sulfur-containing formulas detected in the samples had the elemental composition of o/(4s + 3n) >= 1, indicating that they were largely in the form of oxidized organosulfates or nitrooxy organosulfates. Many OrgSs that were previously tentatively identified as having biogenic or anthropogenic origins were also present in freshly emitted aerosols derived from combustion sources. The results indicated that the formation of OrgSs through an epoxide intermediate pathway could account for up to 46 % of OrgSs from an upper bound estimation, and the oxidant levels could explain 20 % of the variation in the mass of organic sulfur. The analysis of our large dataset of FT-ICR MS results suggested that relative humidity, oxidation of biogenic volatile organic compounds via ozonolysis, and NOx-related nitrooxy organosulfate formation were the major reasons for the molecular variation of OrgSs, possibly highlighting the importance of the acid-catalyzed ring-opening of epoxides, oxidation processes, and heterogeneous reactions involving either the uptake of SO2 or the heterogeneous oxidation of particulate organosulfates into additional unrecognized OrgSs.
收录类别	SCI
语种	英语
关键词[WOS]	SECONDARY ORGANIC AEROSOL ; PEARL RIVER DELTA ; UNSATURATED FATTY-ACIDS ; MASS-SPECTROMETRY ; PARTICULATE ORGANOSULFATES ; ATMOSPHERIC ORGANOSULFATES ; CHEMICAL-CHARACTERIZATION ; NITROOXY ORGANOSULFATES ; HETEROGENEOUS REACTION ; QUANTITATIVE-ANALYSIS
研究领域[WOS]	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000802267500001
引用统计	被引频次：23[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.yic.ac.cn/handle/133337/31123
专题	中国科学院海岸带环境过程与生态修复重点实验室中国科学院海岸带环境过程与生态修复重点实验室_海岸带环境过程实验室
通讯作者	Li, Jun
作者单位	1.Chinese Acad Sci, Guangzhou Inst Geochem, State Key Lab Organ Geochem, Guangdong Prov Key Lab Environm Protect & Resourc, Guangzhou 510640, Peoples R China 2.Chinese Acad Sci, Guangzhou Inst Geochem, Guangdong Hong Kong Macao Joint Lab Environm Poll, Guangzhou 510640, Peoples R China 3.Fudan Univ, Shanghai Key Lab Atmospher Particle Pollut & Prev, Dept Environm Sci & Engn, Shanghai 200433, Peoples R China 4.CAS Ctr Excellence Deep Earth Sci, Guangzhou 510640, Peoples R China 5.Yangzhou Univ, Coll Environm Sci & Engn, Yangzhou 225009, Jiangsu, Peoples R China 6.Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Environm Proc & Ecol Remediat, Yantai 264003, Peoples R China 7.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Jiang, Hongxing,Li, Jun,Tang, Jiao,et al. Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2022,22(10):6919-6935.
APA	Jiang, Hongxing.,Li, Jun.,Tang, Jiao.,Cui, Min.,Zhao, Shizhen.,...&Zhang, Gan.(2022).Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(10),6919-6935.
MLA	Jiang, Hongxing,et al."Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.10(2022):6919-6935.