Space-based formaldehyde measurements as constraints on volatile organic compound emissions in east and south Asia and implications for ozone

被引:217
作者
Fu, Tzung-May
Jacob, Daniel J.
Palmer, Paul I.
Chance, Kelly
Wang, Yuxuan X.
Barletta, Barbara
Blake, Donald R.
Stanton, Jenny C.
Pilling, Michael J.
机构
[1] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
[2] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA
[3] Univ Leeds, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England
[4] Harvard Smithsonian Ctr Astrophys, Cambridge, MA USA
[5] Univ Calif Irvine, Dept Chem, Irvine, CA 92717 USA
[6] Univ Leeds, Dept Chem, Leeds LS2 9JT, W Yorkshire, England
关键词
D O I
10.1029/2006JD007853
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
We use a continuous 6-year record (1996 - 2001) of GOME satellite measurements of formaldehyde (HCHO) columns over east and south Asia to improve regional emission estimates of reactive nonmethane volatile organic compounds (NMVOCs), including isoprene, alkenes, HCHO, and xylenes. Mean monthly HCHO observations are compared to simulated HCHO columns from the GEOS-Chem chemical transport model using state-of-science, "bottom-up" emission inventories from Streets et al. (2003a) for anthropogenic and biomass burning emissions and Guenther et al. (2006) for biogenic emissions (MEGAN). We find that wintertime GOME observations can diagnose anthropogenic reactive NMVOC emissions from China, leading to an estimate 25% higher than Streets et al. (2003a). We attribute the difference to vehicular emissions. The biomass burning source for east and south Asia is almost 5 times the estimate of Streets et al. (2003a). GOME reveals a large source from agricultural burning in the North China Plain in June missing from current inventories. This source may reflect a recent trend toward in-field burning of crop residues as the need for biofuels diminishes. Biogenic isoprene emission in east and south Asia derived from GOME is 56 +/- 30 Tg yr(-1), similar to 52 Tg yr(-1) from MEGAN. We find, however, that MEGAN underestimates emissions in China and overestimates emissions in the tropics. The higher Chinese biogenic and biomass burning emissions revealed by GOME have important implications for ozone pollution. We find 5 to 20 ppb seasonal increases in surface ozone in GEOS-Chem for central and northern China when using GOME-derived versus bottom-up emissions. Our methodology can be adapted for other regions of the world to provide top-down constraints on NMVOC emissions where multiple emission source types overlap in space and time.
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页数:15
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