DOI: 10.1016/j.atmosenv.2015.02.020
Scopus记录号: 2-s2.0-84922354003
论文题名: Global analysis of peroxy radicals and peroxy radical-water complexation using the STOCHEM-CRI global chemistry and transport model
作者: Khan M ; A ; H ; , Cooke M ; C ; , Utembe S ; R ; , Archibald A ; T ; , Derwent R ; G ; , Jenkin M ; E ; , Morris W ; C ; , South N ; , Hansen J ; C ; , Francisco J ; S ; , Percival C ; J ; , Shallcross D ; E
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2015
卷: 106 起始页码: 278
结束页码: 287
语种: 英语
英文关键词: Global sinks
; Global sources
; Peroxy radical
; Peroxy radical-water complexation
; STOCHEM-CRI
Scopus关键词: Atmospheric chemistry
; Chemical analysis
; Isoprene
; Tropics
; Troposphere
; Atmospheric process
; Chemical transport models
; Chemistry and transport models
; Global sinks
; Global sources
; Northern Hemispheres
; Peroxy radicals
; STOCHEM-CRI
; Complexation
; isoprene
; peroxy radical
; peroxy radical water complex
; terpene
; unclassified drug
; water
; atmospheric chemistry
; complexation
; global perspective
; Northern Hemisphere
; peroxy radical
; source-sink dynamics
; Southern Hemisphere
; tropopause
; troposphere
; Article
; chemistry
; complex formation
; environmental temperature
; oxidation
; priority journal
; seasonal variation
; summer
; troposphere
; winter
; Australia
; Cape Grim
; Connacht
; County Galway
; Hawaii [(ISL) Hawaiian Islands]
; Hawaii [United States]
; Hawaiian Islands
; Ireland
; Mace Head
; Mauna Loa
; Tasmania
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 importance of peroxy radical (RO2) chemistry in the troposphere is investigated using the STOCHEM-CRI global chemistry and transport model. The oxidation of VOCs leads to the formation of RO2 radicals which are dominated by CH3O2 (83%), RCO3 (5%), isoprene derived peroxy radicals (6%), and terpene derived peroxy radicals (1%). A good correlation between model and field measurements for total RO2 for most of the selected stations suggests that they are appropriate background sites as the atmospheric processes occurring at these stations are representative of the chemistry taking place within the entire model grid square in which they are located. The seasonality exhibited by RO2 has been studied, with well-defined cycles (highest in summer and lowest in winter) seen in both hemispheres. Peroxy radical-water complexes, whilst not represented using Chemical Transport Models (CTMs) previously, are postulated to perturb RO2 chemistry. The significance of water clusters (RO2.H2O) is investigated using the STOCHEM-CRI model and reveals that at 300K the proportion of RO2 participating in complexation with water is approximately 12% in the tropics. Isoprene derived radicals are the most strongly bound of RO2 species investigated and their degree of complexation at approx. 300K far surpasses that of the generic peroxy radicals by 3-5%. At higher altitudes (approx. 8km) characterized by sub-ambient temperatures, the fraction of RO2.H2O complex that can exist is approximately 17% in the upper troposphere above Mace Head (Northern Hemisphere), 14% above Cape Grim (Southern Hemisphere), and 8% above Mauna Loa (Tropics). © 2015 The Authors. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/81878
Appears in Collections: 气候变化事实与影响
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作者单位: Biogeochemistry Research Centre, School of Chemistry, University of Bristol, Cantock's Close, Bristol, United Kingdom; Rdscientific, Newbury, Berkshire, United Kingdom; Atmospheric Chemistry Services, Okehampton, Devon, United Kingdom; Department of Chemistry and Biochemistry, Brigham Young University, Provo, UT, United States; Department of Earth Atmospheric Planetary Sciences, Purdue University, West Lafayette, IN, United States; The Centre for Atmospheric Science, The School of Earth, Atmospheric and Environmental Science, The University of Manchester, Simon Building, Brunswick Street, Manchester, United Kingdom; Met Office, FitzRoy Road, Exeter, Devon, United Kingdom; The School of Earth Sciences, University of Melbourne, Parkville, VIC, Australia; The NCAS- Climate and the Centre for Atmospheric Science, University of Cambridge, Cambridge, United Kingdom
Recommended Citation:
Khan M,A,H,et al. Global analysis of peroxy radicals and peroxy radical-water complexation using the STOCHEM-CRI global chemistry and transport model[J]. Atmospheric Environment,2015-01-01,106