气候变化领域集成服务门户(CCPortal): Chemical transformation of alpha-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates

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DOI	10.5194/acp-22-5685-2022
	Chemical transformation of alpha-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates
	Xu, Rongshuang; Ng, Sze In Madeleine; Chow, Wing Sze; Wong, Yee Ka; Wang, Yuchen; Lai, Donger; Yao, Zhongping; So, Pui-Kin; Yu, Jian Zhen; Chan, Man Nin
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	5685
结束页码	5700
卷号	22 期号:8 页码:16
英文摘要	Organosulfur compounds are found to be ubiquitous in atmospheric aerosols - a majority of which are expected to be organosulfates (OSs). Given the atmospheric abundance of OSs, and their potential to form a variety of reaction products upon aging, it is imperative to study the transformation kinetics and chemistry of OS s to better elucidate their atmospheric fates and impacts. In this work, we investigated the chemical transformation of an alpha-pinene-derived organosulfate (C10H17O5SNa, alpha pOS-249) through heterogeneous OH oxidation at a relative humidity of 50 % in an oxidation flow reactor (OFR). The aerosol-phase reaction products were characterized using high-performance liquid chromatography-electrospray ionization-high-resolution mass spectrometry and ion chromatography. By monitoring the decay rates of alpha pOS-249, the effective heterogeneous OH reaction rate was measured to be (6.72 +/- 0.55) x 10(-13) cm(3) molecule(-1) s(-1). This infers an atmospheric lifetime of about 2 weeks at an average OH concentration of 1.5 x 10(6) molecules cm(-3). Product analysis shows that OH oxidation of alpha pOS-249 can yield more oxygenated OSs with a nominal mass-to-charge ratio (m/z) at 247 (C10H15O5S-), 263 (C10H5O6S-), 265 (C10H7O6S-), 277 (C10H3O7S-), 279 (C10H5O7S-), and 281 (C10H7O7S-). The formation of fragmentation products, including both small OSs (C < 10) and inorganic sulfates, is found to be insignificant. These observations suggest that functionalization reactions are likely the dominant processes and that multigenerational oxidation possibly leads to formation of products with one or two hydroxyl and carbonyl functional groups adding to alpha pOS-249. Furthermore, all product ions except m/z = 277 have been detected in laboratory-generated alpha-pinene-derived secondary organic aerosols as well as in atmospheric aerosols. Our results reveal that OSs freshly formed from the photochemical oxidation of alpha-pinene could react further to form OSs commonly detected in atmospheric aerosols through heterogeneous OH oxidation. Overall, this study provides more insights into the sources, transformation, and fate of atmospheric OSs.
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:000788649500001
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/273020
作者单位	Chinese University of Hong Kong; Hong Kong University of Science & Technology; Hong Kong University of Science & Technology; Hong Kong Polytechnic University; Hong Kong Polytechnic University; Hong Kong Polytechnic University; Chinese University of Hong Kong
推荐引用方式 GB/T 7714	Xu, Rongshuang,Ng, Sze In Madeleine,Chow, Wing Sze,et al. Chemical transformation of alpha-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates[J],2022,22(8):16.
APA	Xu, Rongshuang.,Ng, Sze In Madeleine.,Chow, Wing Sze.,Wong, Yee Ka.,Wang, Yuchen.,...&Chan, Man Nin.(2022).Chemical transformation of alpha-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(8),16.
MLA	Xu, Rongshuang,et al."Chemical transformation of alpha-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.8(2022):16.