DOI: 10.1016/j.atmosenv.2015.04.056
Scopus记录号: 2-s2.0-84928742695
论文题名: A study of global atmospheric budget and distribution of acetone using global atmospheric model STOCHEM-CRI
作者: Khan M ; A ; H ; , Cooke M ; C ; , Utembe S ; R ; , Archibald A ; T ; , Maxwell P ; , Morris W ; C ; , Xiao P ; , Derwent R ; G ; , Jenkin M ; E ; , Percival C ; J ; , Walsh R ; C ; , Young T ; D ; S ; , Simmonds P ; G ; , Nickless G ; , O'Doherty S ; , Shallcross D ; E
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2015
卷: 112 起始页码: 269
结束页码: 277
语种: 英语
英文关键词: Acetone
; Mace Head
; Monoterpenes
; Photochemical production
; STOCHEM-CRI model
Scopus关键词: Atmospheric chemistry
; Budget control
; Methanol
; Monoterpenes
; Oxidation
; Photolysis
; Troposphere
; Atmospheric budget
; Global atmospheric models
; Mace Head
; Modeling and measurement
; Oxidation mechanisms
; Photochemical activity
; Photochemical production
; Surface distributions
; Acetone
; acetone
; methanol
; terpene
; acetone
; atmospheric chemistry
; dry deposition
; global perspective
; oxidation
; photochemistry
; seasonal variation
; troposphere
; volatile organic compound
; aircraft
; altitude
; Article
; atmosphere
; autumn
; biosphere
; boundary layer
; controlled study
; decomposition
; degradation
; dry deposition
; measurement
; nonhuman
; Northern Hemisphere
; photochemistry
; photolysis
; photooxidation
; priority journal
; process model
; seasonal variation
; spring
; summer
; troposphere
; United States
; wet deposition
; winter
; California
; Connacht
; County Galway
; Ireland
; Mace Head
; 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 impact of including a more detailed VOC oxidation scheme (CRI v2-R5) with a multi-generational approach for simulating tropospheric acetone is investigated using a 3-D global model, STOCHEM-CRI. The CRI v2-R5 mechanism contains photochemical production of acetone from monoterpenes which account for 64% (46.8Tg/yr) of the global acetone sources in STOCHEM-CRI. Both photolysis and oxidation by OH in the troposphere contributes equally (42%, each) and dry deposition contributes 16% of the atmospheric sinks of acetone. The tropospheric life-time and the global burden of acetone are found to be 18 days and 3.5Tg, respectively, these values being close to those reported in the study of Jacob etal. (2002). A dataset of aircraft campaign measurements are used to evaluate the inclusion of acetone formation from monoterpenes in the CRI v2-R5 mechanism used in STOCHEM-CRI. The overall comparison between measurements and models show that the parameterised approach in STOCHEM-NAM (no acetone formation from monoterpenes) underpredicts the mixing ratios of acetone in the atmosphere. However, using a detailed monoterpene oxidation mechanism forming acetone has brought the STOCHEM-CRI into closer agreement with measurements with an improvement in the vertical simulation of acetone. The annual mean surface distribution of acetone simulated by the STOCHEM-CRI shows a peak over forested regions where there are large biogenic emissions and high levels of photochemical activity. Year-long observations of acetone and methanol at the Mace Head research station in Ireland are compared with the simulated acetone and methanol produced by the STOCHEM-CRI and found to produce good overall agreement between model and measurements. The seasonal variation of model and measured acetone levels at Mace Head, California, New Hampshire and Minnesota show peaks in summer and dips in winter, suggesting that photochemical production may have the strongest effect on its seasonal trend. © 2015 The Authors. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/81711
Appears in Collections: 气候变化事实与影响
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作者单位: Atmospheric Chemistry Research Group, 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. A study of global atmospheric budget and distribution of acetone using global atmospheric model STOCHEM-CRI[J]. Atmospheric Environment,2015-01-01,112