DOI: 10.1016/j.atmosenv.2017.05.038
Scopus记录号: 2-s2.0-85020194457
论文题名: The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies
作者: Wu H ; , Wang Y ; , Li H ; , Huang L ; , Huang D ; , Shen H ; , Xing Y ; , Chen Z
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2017
卷: 164 起始页码: 61
结束页码: 70
语种: 英语
英文关键词: OH-oxidation
; Peroxyacetic acid
; Rate constant
; Reaction channel
; Sink
Scopus关键词: Chemical compounds
; Free radicals
; Molecules
; Oxidation
; Rate constants
; Reaction kinetics
; Rural areas
; Experimental conditions
; Kinetics and mechanism
; Master chemical mechanism
; North China Plain
; Peroxyacetic acid
; Reaction channels
; Reference compounds
; Sink
; Atmospheric chemistry
; formaldehyde
; formic acid
; hydroxyl radical
; peracetic acid
; atmospheric chemistry
; chemical reaction
; concentration (composition)
; experimental study
; formaldehyde
; formic acid
; hydroxyl radical
; model test
; organic acid
; oxidant
; oxidation
; reaction kinetics
; Article
; atmosphere
; humidity
; oxidation
; photolysis
; priority journal
; rate constant
; reaction analysis
; rural area
; simulation
; water vapor
; China
; North China Plain
; Paa
Scopus学科分类: Environmental Science: Water Science and Technology
; Earth and Planetary Sciences: Earth-Surface Processes
; Environmental Science: Environmental Chemistry
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 (kPAA+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 (9.4–11.9) × 10−12 cm3 molecule−1 s−1 at 298 K and 1 atm, which is about (2.5–3.2) times larger than that parameter used in Master Chemical Mechanism v3.3.1 (MCM v3.3.1) (3.70 × 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 ∼30% of the total loss. Moreover, the major terminal products of PAA–OH 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 PAA–OH reaction, which may also provide routes to HCHO and HC(O)OH formation. © 2017 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/82518
Appears in Collections: 气候变化事实与影响
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作者单位: State Key Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China; School of Earth Sciences, Zhejiang University, Hangzhou, Zhejiang, China
Recommended Citation:
Wu H,, Wang Y,, Li H,et al. The OH-initiated oxidation of atmospheric peroxyacetic acid: Experimental and model studies[J]. Atmospheric Environment,2017-01-01,164