ACETONE IN THE ATMOSPHERE - DISTRIBUTION, SOURCES, AND SINKS

被引:328
作者
SINGH, HB
OHARA, D
HERLTH, D
SACHSE, W
BLAKE, DR
BRADSHAW, JD
KANAKIDOU, M
CRUTZEN, PJ
机构
[1] UNIV CALIF IRVINE, IRVINE, CA 92717 USA
[2] GEORGIA INST TECHNOL, ATLANTA, GA 30332 USA
[3] MAX PLANCK INST CHEM, W-6500 MAINZ, GERMANY
[4] CTR FAIBLES RADIOACT, LAB MIXTE CNRS CEA, F-91198 GIF SUR YVETTE, FRANCE
[5] SAN JOSE STATE UNIV FDN, MOFFETT FIELD, CA 94035 USA
[6] NASA, LANGLEY RES CTR, HAMPTON, VA 23665 USA
关键词
D O I
10.1029/93JD00764
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
Acetone (CH3COCH3) was found to be the dominant nonmethane organic species present in the atmosphere sampled primarily over eastern Canada 0-6 km, 35 degrees-65 degrees N) during ABLE3B (July to August 1990). A concentration range of 357 to 2310 ppt (=10(-12) v/v) with a mean value of 1140 +/- 413 ppt was measured. Under extremely clean conditions, generally involving Arctic flows, lowest (background) mixing ratios of 550 +/- 100 ppt were present in much of the troposphere studied. Correlations between atmospheric mixing ratios of acetone and select species such as C2H2, CO, C3H8, C2Cl4 and isoprene provided important clues to its possible Sources and to the causes of its atmospheric variability. Biomass burning as a source of acetone has been identified for the first time. By using atmospheric data and three-dimensional photochemical models, a global acetone source of 40-60 Tg (=10(12) g)/yr is g)/yr is estimated to be present. Secondary formation from the atmospheric oxidation of precursor hydrocarbons (principally propane, isobutane, and isobutene) provides the single largest source (51%). The remainder is attributable to biomass burning (26%), direct biogenic emissions (21%), and primary anthropogenic emissions (3%). Atmospheric removal of acetone is estimated to be due to photolysis (64%), reaction with OH radicals (24%), and deposition (12%). Model calculations also suggest that acetone photolysis contributed significantly to PAN formation (100-200 ppt) in the middle and upper troposphere of the sampled region and may be important globally. While the source-sink equation appears to be roughly balanced, much more atmospheric and source data, especially from the southern hemisphere, are needed to reliably quantify the atmospheric budget of acetone.
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页码:1805 / 1819
页数:15
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