Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing-Tianjin-Hebei (BTH), China

doi:10.5194/acp-19-13341-2019

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	Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing-Tianjin-Hebei (BTH), China
	Liu, Lang 2,3,4; Bei, Naifang 1; Wu, Jiarui 2,3; Liu, Suixin 2,3; Zhou, Jiamao 2,3; Li, Xia 2,3; Yang, Qingchuan 2; Feng, Tian 2; Cao, Junji 2,3; Tie, Xuexi 2
刊名	ATMOSPHERIC CHEMISTRY AND PHYSICS
	2019-10-30
卷号	19 期号:20 页码:13341-13354
ISSN号	1680-7316
DOI	10.5194/acp-19-13341-2019
通讯作者	Li, Guohui(ligh@ieecas.cn)
英文摘要	Sulfate aerosols have profound impacts on the climate, ecosystem, visibility, and public health, but the sulfate formation pathway remains elusive. In the present study, a source-oriented WRF-Chem model is applied to simulate a persistent air pollution episode from 4 to 15 July 2015 in Beijing-Tianjin-Hebei (BTH), China, to study the contributions of four pathways to sulfate formation. When comparing simulations to measurements in BTH, the index of agreement (IOA) of meteorological parameters, air pollutants, and aerosol species generally exceeds 0.6. On average in BTH, the heterogeneous reaction of SO2 involving aerosol water and the SO2 oxidation by OH constitutes the two most important sulfate sources, with a contribution of about 35 %-38 % and 33 %-36 %, respectively. Primary sulfate emissions account for around 22 %-24 % of the total sulfate concentration. SO2 oxidation by stabilized Criegee intermediates (sCIs) also plays an appreciable role in sulfate formation, with a contribution of around 9 % when an upper limit of the reaction rate constant of sCIs with SO2 (kappa SCI+SO2 = 3.9 x 10(-11) cm(3) s(-1)) and a lower limit of the reaction rate constant of sCIs with H2O (kappa SCI+H2O = 1.97 x 10(-18) cm(3) s(-1)) are used. Sensitivity studies reveal that there are still large uncertainties in the sulfate contribution of SO2 oxidation by sCIs. The sulfate contribution of the reaction is decreased to less than 3 % when kappa SCI+SO2 is decreased to 6.0 x 10(-13) Cm-3 s(-1). Furthermore, when kappa SCI+H2O is increased to 2.38 x 10(-15) cm(3) s(-1) based on the reported ratio of kappa SCI+H2O to kappa SCI+SO2 (6.1 x 10(-5)), the sulfate contribution becomes insignificant at less than 2 %. Further studies need to be conducted to better determine kappa SCI+SO2 and kappa SCI+H2O to evaluate the effects of sCI chemistry on sulfate formation.
资助项目	National Key RD Plan[2017YFC0210000] ; National Research Program for Key Issues in Air Pollution Control[DQGG0105]
WOS关键词	ORGANIC AEROSOL CONCENTRATIONS ; MEXICO-CITY ; AIR-QUALITY ; METEOROLOGICAL UNCERTAINTIES ; GUANZHONG BASIN ; SULFUR-DIOXIDE ; HAZE FORMATION ; HONO SOURCES ; IMPACTS ; OXIDATION
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
语种	英语
出版者	COPERNICUS GESELLSCHAFT MBH
WOS记录号	WOS:000494285700001
资助机构	National Key RD Plan ; National Research Program for Key Issues in Air Pollution Control
内容类型	期刊论文
源URL	[http://ir.ieecas.cn/handle/361006/12939]
专题	地球环境研究所_粉尘与环境研究室第四纪科学与全球变化卓越创新中心
通讯作者	Li, Guohui
作者单位	1.Xi An Jiao Tong Univ, Sch Human Settlements & Civil Engn, Xian 710049, Shaanxi, Peoples R China 2.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, SKLLQG, Xian 710051, Shaanxi, Peoples R China 3.CAS Ctr Excellence Quaternary Sci & Global Change, Xian 710061, Shaanxi, Peoples R China 4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Liu, Lang,Bei, Naifang,Wu, Jiarui,et al. Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing-Tianjin-Hebei (BTH), China[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(20):13341-13354.
APA	Liu, Lang.,Bei, Naifang.,Wu, Jiarui.,Liu, Suixin.,Zhou, Jiamao.,...&Li, Guohui.(2019).Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing-Tianjin-Hebei (BTH), China.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(20),13341-13354.
MLA	Liu, Lang,et al."Effects of stabilized Criegee intermediates (sCIs) on sulfate formation: a sensitivity analysis during summertime in Beijing-Tianjin-Hebei (BTH), China".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.20(2019):13341-13354.