Carbonyl sulfide and carbon disulfide: Large-scale distributions over the western Pacific and emissions from Asia during TRACE-P

被引:44
作者
Blake, NJ
Streets, DG
Woo, JH
Simpson, IJ
Green, J
Meinardi, S
Kita, K
Atlas, E
Fuelberg, HE
Sachse, G
Avery, MA
Vay, SA
Talbot, RW
Dibb, JE
Bandy, AR
Thornton, DC
Rowland, FS
Blake, DR
机构
[1] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA
[2] Argonne Natl Lab, Argonne, IL 60439 USA
[3] Univ Iowa, Iowa Adv Technol Labs, Ctr Global & Reg Environm Res, Iowa City, IA 52242 USA
[4] Ibaraki Univ, Fac Sci, Dept Environm Sci, Mito, Ibaraki 3108512, Japan
[5] Natl Ctr Atmospher Res, Boulder, CO 80307 USA
[6] Florida State Univ, Dept Meteorol, Tallahassee, FL 32306 USA
[7] NASA, Langley Res Ctr, Hampton, VA 23681 USA
[8] Univ New Hampshire, Climate Change Res Ctr, Inst Study Earth Oceans & Space, Durham, NH 03824 USA
[9] Drexel Univ, Dept Chem, Philadelphia, PA 19104 USA
关键词
carbonyl sulfide (OCS); carbon disulfide (CS2); Asian emissions; emission inventories;
D O I
10.1029/2003JD004259
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
An extensive set of carbonyl sulfide (OCS) and carbon disulfide (CS2) observations were made as part of the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) project, which took place in the early spring 2001. TRACE-P sampling focused on the western Pacific region but in total included the geographic region 110degreesE to 290degreesE longitude, 5degreesN to 50degreesN latitude, and 0-12 km altitude. Substantial OCS and CS2 enhancements were observed for a great many air masses of Chinese and Japanese origin during TRACE-P. Over the western Pacific, mean mixing ratios of long-lived OCS and shorter-lived CS2 showed a gradual decrease by about 10% and a factor of 5-10, respectively, from the surface to 8-10 km altitude, presumably because land-based sources dominated their distribution during February through April 2001. The highest mean OCS and CS2 levels (580 and 20 pptv, respectively, based on 2.5degrees x 2.5degrees latitude bins) were observed below 2 km near the coast of Asia, at latitudes between 25degreesN and 35degreesN, where urban Asian outflow was strongest. Ratios of OCS versus CO for continental SE Asia were much lower compared to Chinese and Japanese signatures and were strongly associated with biomass burning/biofuel emissions. We present a new inventory of anthropogenic Asian emissions ( including biomass burning) for OCS and CS2 and compare it to emission estimates based on regional relationships of OCS and CS2 to CO and CO2. The OCS and CS2 results for the two methods compare well for continental SE Asia and Japan plus Korea and also for Chinese CS2 emissions. However, it appears that the inventory underestimates Chinese emissions of OCS by about 30-100%. This difference may be related to the fact that we did not include natural sources such as wetland emissions in our inventory, although the contributions from such sources are believed to be at a seasonal low during the study period. Uncertainties in OCS emissions from Chinese coal burning, which are poorly characterized, likely contribute to the discrepancy.
引用
收藏
页码:D15S051 / 15
页数:15
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