Impact of reactive bromine chemistry in the troposphere

被引:176
作者
von Glasow, R [1 ]
von Kuhlmann, R
Lawrence, MG
Platt, U
Crutzen, PJ
机构
[1] Heidelberg Univ, Inst Environm Phys, D-6900 Heidelberg, Germany
[2] Univ Calif San Diego, Scripps Inst Oceanog, Ctr Atmospher Sci, San Diego, CA 92103 USA
[3] Max Planck Inst Chem, Div Atmospher Chem, D-55128 Mainz, Germany
关键词
D O I
10.5194/acp-4-2481-2004
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Recently several field campaigns and satellite observations have found strong indications for the presence of bromine oxide (BrO) in the free troposphere. Using a global atmospheric chemistry transport model we show that BrO mixing ratios of a few tenths to 2 pmol mol(-1) lead to a reduction in the zonal mean O-3 mixing ratio of up to 18% in widespread areas and regionally up to 40% compared to a model run without bromine chemistry. A lower limit approach for the marine boundary layer, that does not explicitly include the release of halogens from sea salt aerosol, shows that for dimethyl sulfide (DMS) the effect is even larger, with up to 60% reduction of its tropospheric column. This is accompanied by dramatic changes in DMS oxidation pathways, reducing its cooling effect on climate. In addition there are changes in the HO2 : OH ratio that also affect NOx and PAN. These results imply that potentially significant strong sinks for O-3 and DMS have so far been ignored in many studies of the chemistry of the troposphere.
引用
收藏
页码:2481 / 2497
页数:17
相关论文
共 53 条
[1]   HETEROGENEOUS REACTION OF HOBR WITH HBR AND HCL ON ICE SURFACES AT 228-K [J].
ABBATT, JPD .
GEOPHYSICAL RESEARCH LETTERS, 1994, 21 (08) :665-668
[2]   Uptake and reaction of HOBr on frozen and dry NaCl/NaBr surfaces between 253 and 233 K [J].
Adams, JW ;
Holmes, NS ;
Crowley, JN .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2002, 2 :79-91
[3]   The BrO+Ch3O2 reaction: Kinetics and role in the atmospheric ozone budget [J].
Aranda, A ;
LeBras, G ;
LaVerdet, G ;
Poulet, G .
GEOPHYSICAL RESEARCH LETTERS, 1997, 24 (22) :2745-2748
[4]   Evaluated kinetic and photochemical data for atmospheric chemistry: Supplement VI - IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry [J].
Atkinson, R ;
Baulch, DL ;
Cox, RA ;
Hampson, RF ;
Kerr, JA ;
Rossi, MJ ;
Troe, J .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1997, 26 (06) :1329-1499
[5]  
ATKINSON R, 2003, SUMMARY EVALUATED KI
[6]  
ATKINSON R, 1999, SUMMARY EVALUATED KI
[7]   Detection of bromine monoxide in a volcanic plume [J].
Bobrowski, N ;
Hönninger, G ;
Galle, B ;
Platt, U .
NATURE, 2003, 423 (6937) :273-276
[8]   DMS atmospheric concentrations and sulphate aerosol indirect radiative forcing: a sensitivity study to the DMS source representation and oxidation [J].
Boucher, O ;
Moulin, C ;
Belviso, S ;
Aumont, O ;
Bopp, L ;
Cosme, E ;
von Kuhlmann, R ;
Lawrence, MG ;
Pham, M ;
Reddy, MS ;
Sciare, J ;
Venkataraman, C .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2003, 3 :49-65
[9]  
Brasseur G.P., 1999, Atmospheric Chemistry and Global Change
[10]   High-latitude, summertime NOx activation and seasonal ozone decline in the lower stratosphere:: Model calculations based on observations by HALOE on UARS [J].
Bruhl, C ;
Crutzen, PJ ;
Grooss, JU .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1998, 103 (D3) :3587-3597