DOI: 10.1016/j.atmosenv.2014.11.008
Scopus记录号: 2-s2.0-84913553330
论文题名: Simulated impact of NOx on SOA formation from oxidation of toluene and m-xylene
作者: Xu J ; , Griffin R ; J ; , Liu Y ; , Nakao S ; , Cocker D ; R
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2015
卷: 101 起始页码: 217
结束页码: 225
语种: 英语
英文关键词: M-Xylene
; Nitrogen oxides
; Secondary organic aerosol
; Toluene
Scopus关键词: Aerosols
; Air quality
; Aromatic compounds
; Aromatization
; Atmospheric chemistry
; Cyclization
; Nitrogen
; Nitrogen oxides
; Toluene
; Chamber experiments
; Correction factors
; Formation mechanism
; m-Xylene
; Oxidation of toluenes
; Ring-opening products
; Secondary organic aerosols
; University of California
; Xylene
; hydroperoxide
; meta xylene
; nitrogen oxide
; peroxy radical
; toluene
; aerosol formation
; atmospheric chemistry
; nitrous oxide
; oxidation
; partitioning
; peroxy radical
; prediction
; simulation
; speciation (chemistry)
; toluene
; vapor pressure
; xylene
; aerosol
; air quality
; Article
; gas
; light intensity
; oxidation
; photooxidation
; secondary organic aerosol
; species composition
; vapor pressure
; California
; United States
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: Despite the crucial role of aromatic-derived secondary organic aerosol (SOA) in deteriorating air quality, its formation mechanism is not well understood, and the dependence of aromatic SOA formation on nitrogen oxides (NOx) is not captured fully by most SOA formation models. In this study, NOx-dependent mechanisms of toluene and m-xylene SOA formation are updated using the gas-phase Caltech Atmospheric Chemistry Mechanism (CACM) coupled to a gas/aerosol partitioning model. The updated models were optimized by comparison to eighteen chamber experiments performed under both high- and low-NOx conditions at the University of California - Riverside. Correction factors for vapor pressures imply uncharacterized association chemistry, likely in the aerosol phase. Difficulty of the presented model lies in predicting O3 production well, with overprediction (typically 20-40%), particularly under low NOxconditions (up to one fold). Mean normalized biases for other species (NO2 and SOA) and conditions are smaller (up to ±50%). The newly developed model can predict strong decreases of m-xylene SOA yield with increasing NOx. Simulated SOA speciation implies the importance of ring-opening products in governing SOA formation (up to ~40-60% for both aromatics). Speciation distributions under varied NOx levels imply that competition between hydroperoxide radical and NO for reaction with a bicyclic peroxide radical as the most commonly accepted mechanism may not be the only factor influencing SOA formation. The reaction of aromatic peroxy radicals with NO competing with self-cyclization (a new mechanism updated in this study) might also affect NOx-dependence of SOA formation. Different simulated importance of a phenolic route in governing SOA formation between toluene and m-xylene suggests that the number of methyl groups on the aromatic ring is important in SOA formation chemistry. © 2014 . Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/82138
Appears in Collections: 气候变化事实与影响
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作者单位: Department of Civil and Environmental Engineering, Rice University, Houston, TX, United States; Department of Chemical and Environmental Engineering, UC RiversideCA, United States; College of Engineering, Center for Environmental Research and Technology, UC Riverside, CA, United States; Halliburton Inc., 3000 North Sam Houston Pkwy E, Houston, TX, United States; Department of Chemical and Biomolecular Engineering, Clarkson University, Potsdam, NY, United States
Recommended Citation:
Xu J,, Griffin R,J,et al. Simulated impact of NOx on SOA formation from oxidation of toluene and m-xylene[J]. Atmospheric Environment,2015-01-01,101