The OH-initiated oxidation of atmospheric peroxyacetic acid:   Experimental and model studies

doi:10.1016/j.atmosenv.2017.05.038

CORC > 北京大学 > 环境科学与工程学院

	The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies
	Wu, Huihui ; Wang, Yin ; Li, Huan ; Huang, Liubin ; Huang, Dao ; Shen, Hengqing ; Xing, Yanan ; Chen, Zhongming
刊名	ATMOSPHERIC ENVIRONMENT
	2017
关键词	Peroxyacetic acid OH-oxidation Rate constant Reaction channel Sink IONIZATION MASS-SPECTROMETRY VOLATILE ORGANIC-COMPOUNDS MASTER CHEMICAL MECHANISM MCM V3 PART HYDROGEN-PEROXIDE GAS-PHASE TROPOSPHERIC DEGRADATION DRY DEPOSITION BOREAL FOREST NITRATE PAN
DOI	10.1016/j.atmosenv.2017.05.038
英文摘要	Peroxyacetic acid (PAA, CH3C(O)OOH) plays an important role in atmospheric chemistry, serving as reactive oxidant and affecting radical recycling. However, previous studies revealed an obvious gap between modelled and observed concentrations of atmospheric PAA, which may be partly ascribed to the uncertainty in the kinetics and mechanism of OH-oxidation. In this study, we measured the rate constant of OH radical reaction with PAA (k(PAA+OH)) and investigated the products in order to develop a more robust atmospheric PAA chemistry. Using the relative rates technique and employing toluene and meta-xylene as reference compounds, the kPAA+OH was determined to be (9.411.9) x 10(-12) cm(3) molecule(-1) s(-1) at 298 K and 1 atm, which is about (2.53.2) times larger than that parameter used in Master Chemical Mechanism v3.3.1 (MCM v3.3.1) (3.70 x 10(-12) cm3 molecule(-1) s(-1)). Incorporation of a box model and MCM v3.3.1 with revised PAA chemistry represented a better simulation of atmospheric PAA observed during Wangdu Campaign 2014, a rural site in North China Plain. It is found that OH-oxidation is an important sink of atmospheric PAA in this rural area, accounting for similar to 30% of the total loss. Moreover, the major terminal products of PAAOH reaction were identified as formaldehyde (HCHO) and formic acid (HC(O)OH). The modelled results show that both primary and secondary chemistry play an important role in the large HCHO and HC(O)OH formation under experimental conditions. There should exist the channel of methyl H-abstraction for PAAOH reaction, which may also provide routes to HCHO and HC(O)OH formation. (C) 2017 Elsevier Ltd. All rights; National Natural Science Foundation of China [21477002]; National Key Research and Development Program of China [2016YFCO202704]; SCI(E); ARTICLE; 61-70; 164
语种	英语
内容类型	期刊论文
源URL	[http://ir.pku.edu.cn/handle/20.500.11897/471296]
专题	环境科学与工程学院
推荐引用方式 GB/T 7714	Wu, Huihui,Wang, Yin,Li, Huan,et al. The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies[J]. ATMOSPHERIC ENVIRONMENT,2017.
APA	Wu, Huihui.,Wang, Yin.,Li, Huan.,Huang, Liubin.,Huang, Dao.,...&Chen, Zhongming.(2017).The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies.ATMOSPHERIC ENVIRONMENT.
MLA	Wu, Huihui,et al."The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies".ATMOSPHERIC ENVIRONMENT (2017).