DOI: 10.1002/jgrd.50160
论文题名: Implications of low volatility SOA and gas-phase fragmentation reactions on SOA loadings and their spatial and temporal evolution in the atmosphere
作者: Shrivastava M. ; Zelenyuk A. ; Imre D. ; Easter R. ; Beranek J. ; Zaveri R.A. ; Fast J.
刊名: Journal of Geophysical Research Atmospheres
ISSN: 21698996
出版年: 2013
卷: 118, 期: 8 起始页码: 3328
结束页码: 3342
语种: 英语
英文关键词: fragmentation
; low volatility
; secondary organic aerosol
Scopus关键词: Aerosols
; Chemical reactions
; Evaporation
; Loading
; Phase transitions
; Three dimensional computer graphics
; Chemical transport models
; Formation and evolutions
; fragmentation
; Fragmentation reactions
; Gas-phase fragmentation
; low volatility
; Mass accommodation coefficient
; Secondary organic aerosols
; Three dimensional
; aerosol composition
; atmospheric pollution
; evaporation
; gas phase reaction
; parameterization
; spatiotemporal analysis
; volatilization
英文摘要: We investigate issues related to volatility and multi-generational gas-phase aging parameterizations affecting the formation and evolution of secondary organic aerosol (SOA) in models. We show that when assuming realistic values for the mass accommodation coefficient, experimentally observed SOA evaporation rates imply significantly lower "effective volatility" than those derived from SOA growth in smog chambers, pointing to the role of condensed phase processes and suggesting that models need to use different parameters to describe the formation and evolution of SOA. We develop a new, experimentally driven paradigm to represent SOA as a non-absorbing semi-solid with very low "effective volatility." We modify both a box model and a 3D chemical transport model, to include simplified parameterizations capturing the first-order effects of gas-phase fragmentation reactions and investigate the implications of treating SOA as a non-volatile, non-absorbing semi-solid (NVSOA). Box model simulations predict SOA loadings decrease with increasing fragmentation, and similar SOA loadings are calculated in the traditional, semi-volatile (SVSOA) approach and with the new paradigm (NVSOA) before evaporation reduces loadings of SVSOA. Box-model-calculated O:C ratios increase with aging in both the SVSOA and the NVSOA paradigms. Consistent with box model results, 3D model simulations demonstrate that predicted SOA loadings decrease with the addition of fragmentation reactions. The NVSOA paradigm predicts higher SOA loadings compared to the SVSOA paradigm over nearly the entire 3D modeling domain, with larger differences close to the surface and in regions where higher dilution favors SVSOA evaporation. Low effective volatility of SOA Gas phase fragmentation reaction Box and regional modeling ©2013. American Geophysical Union. All Rights Reserved. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/63803
Appears in Collections: 影响、适应和脆弱性 气候减缓与适应
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作者单位: Pacific Northwest National Laboratory, Richland, WA 99352, United States; Imre Consulting, Richland WA, United States
Recommended Citation:
Shrivastava M.,Zelenyuk A.,Imre D.,et al. Implications of low volatility SOA and gas-phase fragmentation reactions on SOA loadings and their spatial and temporal evolution in the atmosphere[J]. Journal of Geophysical Research Atmospheres,2013-01-01,118(8)