DOI: 10.1016/j.atmosenv.2014.08.074
Scopus记录号: 2-s2.0-84906830135
论文题名: Sensitivity of atmospheric models to rate terms within complex chemical mechanisms
作者: Dunker A ; M ; , Koo B ; , Yarwood G
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2014
卷: 98 起始页码: 224
结束页码: 230
语种: 英语
英文关键词: Carbon Bond 2005
; Chemical rate terms
; Decoupled direct method
; Isoprene
; Sensitivity analysis
Scopus关键词: Air quality
; Atmospheric chemistry
; Forecasting
; Isoprene
; Ketones
; Nitrates
; Nitrogen oxides
; Oxidation
; Ozone
; Rural areas
; Sensitivity analysis
; Sensitivity analysis
; Atmospheric model
; Carbon bond
; Chemical mechanism
; Comprehensive air quality model with extensions
; Decoupled direct methods
; Full three-dimensional
; Methyl vinyl ketones
; Oxidation products
; Complex chemicals
; Computer simulation
; Isoprene
; formaldehyde
; isoprene
; ketone
; organic nitrate
; ozone
; hydroxide
; nitric acid
; nitrogen dioxide
; organic compound
; propionaldehyde
; air quality
; atmospheric modeling
; chemical reaction
; isoprene
; oxidation
; simulation
; organic compound
; ozone
; rural atmosphere
; sensitivity analysis
; air quality
; article
; atmosphere
; chemical reaction
; controlled study
; oxidation
; photolysis
; priority journal
; rural area
; sensitivity analysis
; simulation
; urban area
; Article
; computer simulation
; 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: The decoupled direct method for sensitivity analysis was extended to the rate terms for the loss of reactants and formation of products to provide a detailed understanding of the predictions of chemical mechanisms used in atmospheric models. A box-model version and the full three-dimensional (3-D) version of the Comprehensive Air Quality Model with Extensions were used to calculate sensitivities to rate terms in the Carbon Bond 2005 chemical mechanism. The processes studied were formation of products from oxidation of the more reactive organic compounds, removal of NOx by organic nitrate formation, re-formation of NOx from organic nitrates, and loss of OH and NO2 and formation of HNO3 in the reaction OH+NO2→HNO3. Simulations of the box model for four scenarios representing urban and rural atmospheres indicated that the largest sensitivities of ozone, formaldehyde and HOx were to rate terms for certain products of the oxidation of isoprene and to the reactants in OH+NO2→HNO3. The 3-D model was then applied to calculate sensitivities to these rate terms for an eastern U.S. ozone episode in July, 2008. The 3-D simulation results were better correlated with the more NOx-limited rural scenario of the box model and showed that the isoprene oxidation products with the greatest impact on O3 formation are methacrolein, methyl vinyl ketone, HO2 radical, and species converting NO to NO2 and organic nitrates. The 3-D results also showed that loss of NO2 was more important than loss of OH for O3 formation in most areas of the eastern U.S. This work emphasizes the need for continued experimental work to understand the oxidation of isoprene because the isoprene chemistry influenced modeled ozone predictions for both urban as well as rural areas. © 2014 The Authors. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/81178
Appears in Collections: 气候变化事实与影响
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作者单位: A.M. Dunker, LLC, 727 Robinhood Circle, Bloomfield Hills, MI 48304, United States; ENVIRON International Corporation, 773 San Marin Drive, Suite 2115, Novato, CA 94998, United States
Recommended Citation:
Dunker A,M,, Koo B,et al. Sensitivity of atmospheric models to rate terms within complex chemical mechanisms[J]. Atmospheric Environment,2014-01-01,98