Atmospheric budget of acetone

被引:222
作者
Jacob, DJ
Field, BD
Jin, EM
Bey, I
Li, QB
Logan, JA
Yantosca, RM
Singh, HB
机构
[1] Harvard Univ, Dept Earth & Planetary Sci, Div Engn & Appl Sci, Cambridge, MA 02138 USA
[2] NASA, Ames Res Ctr, Moffett Field, CA 94035 USA
关键词
acetone; tropospheric chemistry; propane; inverse modeling; sea-air exchange; biosphere-atmosphere interactions;
D O I
10.1029/2001JD000694
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] The atmospheric budget and distribution of acetone are investigated by using a priori estimates of sources and sinks to constrain a global three-dimensional atmospheric model simulation and then using atmospheric observations from 14 surface sites and 5 aircraft missions to improve these estimates through an inversion analysis. Observations over the South Pacific imply a large photochemical marine source of acetone, either from the ocean or from marine organic aerosol. Low concentrations of acetone measured at European sites in winter-spring and in the Arctic in summer suggest a large microbial ocean sink. The summer-to-fall decrease of concentrations observed in Europe argues against a large source from plant decay. Continental observations in the tropics and at northern midlatitudes in summer imply a large source from terrestrial vegetation. Observations in the Northern Hemisphere outside summer imply a large source from atmospheric oxidation of anthropogenic isoalkanes (propane, isobutane, isopentane). Model simulation of isoalkanes and comparison to observations yields best global emission estimates of 12 Tg C yr(-1) for propane (including only 0.6 Tg C yr(-1) from biomass burning), 3.6 Tg C yr(-1) for isobutane, and 5.0 Tg C yr(-1) for isopentane. Our best estimate of the global acetone source is 95 Tg yr(-1). The mean tropospheric lifetime of acetone is estimated to be 15 days. Terrestrial vegetation and oceans are the principal sources of acetone in the tropopause region (0.1-0.7 ppbv) except in the extratropical Northern Hemisphere, where oxidation of isoalkanes is more important.
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相关论文
共 91 条
[71]   ATMOSPHERIC CONCENTRATIONS AND TEMPORAL VARIATIONS OF C-1 C-3 CARBONYL-COMPOUNDS AT 2 RURAL SITES IN CENTRAL ONTARIO [J].
SHEPSON, PB ;
HASTIE, DR ;
SCHIFF, HI ;
POLIZZI, M ;
BOTTENHEIM, JW ;
ANLAUF, K ;
MACKAY, GI ;
KARECKI, DR .
ATMOSPHERIC ENVIRONMENT PART A-GENERAL TOPICS, 1991, 25 (09) :2001-2015
[72]   Evidence from the Pacific troposphere for large global sources of oxygenated organic compounds [J].
Singh, H ;
Chen, Y ;
Staudt, A ;
Jacob, D ;
Blake, D ;
Heikes, B ;
Snow, J .
NATURE, 2001, 410 (6832) :1078-1081
[73]   Distribution and fate of selected oxygenated organic species in the troposphere and lower stratosphere over the Atlantic [J].
Singh, H ;
Chen, Y ;
Tabazadeh, A ;
Fukui, Y ;
Bey, I ;
Yantosca, R ;
Jacob, D ;
Arnold, F ;
Wohlfrom, K ;
Atlas, E ;
Flocke, F ;
Blake, D ;
Blake, N ;
Heikes, B ;
Snow, J ;
Talbot, R ;
Gregory, G ;
Sachse, G ;
Vay, S ;
Kondo, Y .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D3) :3795-3805
[74]   ACETONE IN THE ATMOSPHERE - DISTRIBUTION, SOURCES, AND SINKS [J].
SINGH, HB ;
OHARA, D ;
HERLTH, D ;
SACHSE, W ;
BLAKE, DR ;
BRADSHAW, JD ;
KANAKIDOU, M ;
CRUTZEN, PJ .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D1) :1805-1819
[75]   PEROXYACETYL NITRATE (PAN) IN THE UNPOLLUTED ATMOSPHERE - AN IMPORTANT RESERVOIR FOR NITROGEN-OXIDES [J].
SINGH, HB ;
HANST, PL .
GEOPHYSICAL RESEARCH LETTERS, 1981, 8 (08) :941-944
[76]   HIGH-CONCENTRATIONS AND PHOTOCHEMICAL FATE OF OXYGENATED HYDROCARBONS IN THE GLOBAL TROPOSPHERE [J].
SINGH, HB ;
KANAKIDOU, M ;
CRUTZEN, PJ ;
JACOB, DJ .
NATURE, 1995, 378 (6552) :50-54
[77]  
SINGH HB, 1992, GASEOUS POLLUTANTS C, P177
[78]   Carbonyls and nonmethane hydrocarbons at rural European sites from the Mediterranean to the Arctic [J].
Solberg, S ;
Dye, C ;
Schmidbauer, N ;
Herzog, A ;
Gehrig, R .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 1996, 25 (01) :33-66
[79]   Three-dimensional climatological distribution of tropospheric OH: Update and evaluation [J].
Spivakovsky, CM ;
Logan, JA ;
Montzka, SA ;
Balkanski, YJ ;
Foreman-Fowler, M ;
Jones, DBA ;
Horowitz, LW ;
Fusco, AC ;
Brenninkmeijer, CAM ;
Prather, MJ ;
Wofsy, SC ;
McElroy, MB .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D7) :8931-8980
[80]   Global simulation of tropospheric O3-NOx-hydrocarbon chemistry 1.: Model formulation [J].
Wang, YH ;
Jacob, DJ ;
Logan, JA .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1998, 103 (D9) :10713-10725