DOI: 10.1016/j.atmosenv.2015.03.045
Scopus记录号: 2-s2.0-84925400324
论文题名: The global budgets of organic hydroperoxides for present and pre-industrial scenarios
作者: Khan M ; A ; H ; , Cooke M ; C ; , Utembe S ; R ; , Xiao P ; , Morris W ; C ; , Derwent R ; G ; , Archibald A ; T ; , Jenkin M ; E ; , Percival C ; J ; , Shallcross D ; E
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2015
卷: 110 起始页码: 65
结束页码: 74
语种: 英语
英文关键词: HOx recycling mechanism
; Organic hydroperoxides
; Pre-industrial scenario
; Present day simulation
; STOCHEM-CRI model
Scopus关键词: Antigen-antibody reactions
; Boundary layers
; Isoprene
; Photolysis
; Recycling
; Chemistry transport model
; Global distribution
; Organic hydroperoxides
; Peroxy radicals
; Photochemical activity
; Pre-industrial
; Present day simulation
; Surface distributions
; Budget control
; beta pinene
; hydroperoxide
; isoprene
; peroxy radical
; pinene
; atmospheric chemistry
; boundary layer
; concentration (composition)
; global perspective
; hydrogen peroxide
; industrial emission
; peroxy radical
; photochemistry
; photolysis
; seasonal variation
; tropical forest
; volatile organic compound
; Article
; boundary layer
; budget
; cross reaction
; isomerization
; light intensity
; oxidation
; photochemistry
; photolysis
; priority journal
; recycling
; simulation
; stratosphere
; summer
; temperature
; troposphere
; water vapor
; wet deposition
; winter
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 global 3-D chemistry-transport model, STOCHEM-CRI (Utembe etal., 2010), has been used to simulate the global distribution of organic hydroperoxides (ROOH) for both present day and pre-industrial scenarios. Globally, the formation of ROOH is solely from the reaction between RO2 and HO2 , being more significant under NOx -limited conditions; here the self and cross reactions of RO2 and HO2 radicals dominate over their reaction with NO. The predominant global loss processes for ROOH are reaction with OH (95%) and by photolysis (4.4%) with a minor loss (<1%) by deposition, in the present day scenario. The associated global burden of ROOH in our model study is found to be 3.8Tg. The surface distribution of ROOH shows a peak near the equator corresponding with higher photochemical activity and large (biogenic) VOC emissions. The simulated abundances of ROOH are comparable with those recorded in field campaigns, but generally show a tendency towards underestimation, particularly in the boundary layer. ROOH displayed seasonal cycles with higher concentrations during the summer months and lower concentrations during the winter months. The effects of including proposed HOx recycling schemes, including isomerisation of isoprene-derived peroxy radicals on the global budget of ROOH have also been investigated for the present and the pre-industrial environment. The present day simulations showed significant increases in CH3 OOH and ROOH (up to 80% and 30%, respectively) over tropical forested regions, due to a general increase in HO2 and RO2 levels in isoprene-rich regions at low NOx levels. In the pre-industrial scenario, the increases in CH3 OOH and total ROOH abundances are even larger, reflecting the more efficient operation of HOx recycling mechanisms at lower NOx levels. RCO3 H species contribute 40-50% of the global burden of ROOH; inclusion of HOx recycling mechanisms leads to an increase in these RCO3 H species but there is no discernible change in the remaining ROOH (ROOH-RCO3 H) burden. © 2015 The Authors. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/81776
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; 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; School of Earth Sciences, University of Melbourne, Parkville, VIC, Australia; NCAS-Climate and the Centre for Atmospheric Science, University of Cambridge, Cambridge, United Kingdom
Recommended Citation:
Khan M,A,H,et al. The global budgets of organic hydroperoxides for present and pre-industrial scenarios[J]. Atmospheric Environment,2015-01-01,110