DOI: 10.1016/j.atmosenv.2015.04.048
Scopus记录号: 2-s2.0-84955702675
论文题名: Impacts of heterogeneous HONO formation on radical sources and ozone chemistry in Houston, Texas
作者: Couzo E ; , Lefer B ; , Stutz J ; , Yarwood G ; , Karamchandani P ; , Henderson B ; , Vizuete W
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2014
卷: 112 起始页码: 344
结束页码: 355
语种: 英语
英文关键词: Houston
; Nitrous acid
; Ozone
; Process analysis
; Radicals
; Surface chemistry
Scopus关键词: Air quality
; Carbon monoxide
; Chemical analysis
; Functional groups
; Nitric oxide
; Nitrogen oxides
; Ozone
; Photolysis
; Surface chemistry
; Air quality models
; Carbon monoxide oxidation
; Comprehensive air quality model with extensions
; Heterogeneous formation
; Houston
; Nitrous acid
; Process analysis
; Radicals
; Inorganic acids
; carbon monoxide
; hydrocarbon
; hydroxyl radical
; nitric oxide
; nitrogen dioxide
; nitrous acid
; oxidizing agent
; ozone
; air quality
; atmospheric chemistry
; carbon monoxide
; chemical cycle
; concentration (composition)
; hydrocarbon
; hydroxyl radical
; nitrous oxide
; oxidation
; ozone
; adsorption
; air quality
; Article
; controlled study
; dry deposition
; oxidation
; photolysis
; priority journal
; United States
; Houston
; Texas
; 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 chemical mechanisms used in regulatory air quality models typically allow for only homogeneous formation of nitrous acid (HONO), an important radical precursor. This study adds heterogeneous formation on surfaces as a HONO source to the Comprehensive Air quality Model with extensions (CAMx). Modeling was performed for the Houston, Texas, region on April 21, 2009. Comparisons to measurements made at Moody Tower during the Study of Houston Atmospheric Radical Precursors (SHARP) show that adding heterogeneous formation increases HONO concentrations, particularly in the early morning and at night. Heterogeneous HONO formation reduces normalized mean error for morning, daytime, and nighttime HONO concentrations from 77% to 67%, 66%-28%, and 99%-67%. Maximum daily 8-hr O3 concentrations were up to 3.5 ppb greater as a result of heterogeneous HONO formation. Direct HONO emissions equal to 0.8% of NOx emissions were also added to the model, but they were considered separately from heterogeneous HONO formation. Increases over the base case of HONO and O3 were seen, though the magnitudes are not as great as with heterogeneous HONO formation. Maximum daily 8-hr O3 concentrations were up to 0.4 ppb greater than with homogeneous HONO formation alone. Significant early morning and nighttime HONO under predictions were seen compared to SHARP measurements in the direct emissions scenario. Direct HONO emissions led to local increases of HONO and O3 in areas with high NOx emissions, but heterogeneous HONO formation led to regional increases of both. Process analysis was used to determine the effect on O3 chemistry in downtown Houston. Daily total hydroxyl radical (OH) production from HONO photolysis was 3.94 ppb/day with heterogeneous HONO formation, 2.40 ppb/day with direct emissions, and 1.40 ppb/day in the base case. A 10% increase of hydrocarbon and carbon monoxide oxidation by OH was seen with heterogeneous HONO formation, while the increase in the direct emissions scenario was 3%. Nitric oxide (NO) to NO2 conversion increased by 8% with heterogeneous formation, while the increase was only 3% with direct HONO emissions. Radical sources, radical propagation, and oxidant production were enhanced at each step in the chemical cycle - particularly just after sunrise - by the addition of heterogeneous HONO formation and direct HONO emissions, but the effects were greater with heterogeneous formation. © 2015 Elsevier Ltd. All rights reserved. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/80633
Appears in Collections: 气候变化事实与影响
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作者单位: Department of Environmental Sciences and Engineering, University of North Carolina, Chapel Hill, NC, United States; Earth and Atmospheric Sciences Department, University of Houston, Houston, TX, United States; Department of Atmospheric and Oceanic Sciences, University of California-Los Angeles, Los Angeles, CA, United States; Ramboll Environ International Corporation, Novato, CA, United States; Department of Environmental Engineering Sciences, University of Florida, Gainesville, FL, United States; Engineering Systems Division, Massachusetts Institute of Technology, Cambridge, MA, United States
Recommended Citation:
Couzo E,, Lefer B,, Stutz J,et al. Impacts of heterogeneous HONO formation on radical sources and ozone chemistry in Houston, Texas[J]. Atmospheric Environment,2014-01-01,112