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

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Read Full Article (file size: 1619453 bytes) Cited by JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 112, D06312, doi:10.1029/2006JD007853, 2007 Space-based formaldehyde measurements as constraints on volatile organic compound emissions in east and south Asia and implications for ozone Tzung-May Fu Department of Earth and Planetary Sciences and School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA Daniel J. Jacob Department of Earth and Planetary Sciences and School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA Paul I. Palmer School of Earth and Environment, University of Leeds, Leeds, UK Kelly Chance Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, USA Yuxuan X. Wang Department of Earth and Planetary Sciences and School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA Barbara Barletta Department of Chemistry, University of California, Irvine, California, USA Donald R. Blake Department of Chemistry, University of California, Irvine, California, USA Jenny C. Stanton Department of Chemistry, University of Leeds, Leeds, UK Michael J. Pilling Department of Chemistry, University of Leeds, Leeds, UK Abstract 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. Received 28 July 2006; accepted 3 November 2006; published 31 March 2007. Keywords: emission inventory; GOME; formaldehyde. Index Terms: 0365 Atmospheric Composition and Structure: Troposphere: composition and chemistry; 0345 Atmospheric Composition and Structure: Pollution: urban and regional (0305, 0478, 4251); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0315 Atmospheric Composition and Structure: Biosphere/atmosphere interactions (0426, 1610); 0394 Atmospheric Composition and Structure: Instruments and techniques. Read Full Article (file size: 1619453 bytes) Cited by Citation: Fu, T.-M., D. J. Jacob, P. I. Palmer, K. Chance, Y. X. Wang, B. Barletta, D. R. Blake, J. C. Stanton, and M. J. Pilling (2007), Space-based formaldehyde measurements as constraints on volatile organic compound emissions in east and south Asia and implications for ozone, J. Geophys. Res., 112, D06312, doi:10.1029/2006JD007853. Copyright 2007 by the American Geophysical Union.

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