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Discussion papers | Copyright
https://doi.org/10.5194/acp-2017-1136
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 15 Jan 2018

Research article | 15 Jan 2018

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This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Chemistry and Physics (ACP).

Adjoint inversion of Chinese non-methane volatile organic compound emissions using space-based observations of formaldehyde and glyoxal

Hansen Cao1, Tzung-May Fu1, Lin Zhang1, Daven K. Henze2, Christopher Chan Miller3, Christophe Lerot4, Gonzalo González Abad3, Isabelle De Smedt4, Qiang Zhang5, Michel Van Roozendael4, Kelly Chance3, Jie Li6, Junyu Zheng7, and Yuanhong Zhao1 Hansen Cao et al.
  • 1Department of Atmospheric and Oceanic Sciences and Laboratory for Climate and Ocean-Atmosphere Studies, School of Physics, Peking University, Beijing, 100871, China
  • 2Department of Mechanical Engineering, University of Colorado, Boulder, USA
  • 3Atomic and Molecular Physics Division, Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, USA
  • 4Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, Belgium
  • 5Center for Earth System Science, Tsinghua University, Beijing, China
  • 6Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China
  • 7College of Environmental Science and Engineering, South China University of Technology, Guangzhou, China

Abstract. We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the vertical column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring Experiment-2A (GOME-2A) instrument and the Ozone Monitoring Instrument (OMI) as constraints. We conducted a series of inversion experiments using different combinations of satellite observations to explore the impacts on top-down emission estimates due to different satellite retrievals. Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 (average 30.8)TgCy−1, including 13.5 to 19.7 (average 17.0)TgCy−1 from anthropogenic sources, 8.9 to 14.8 (average 12.6)TgCy−1 from biogenic sources, and 1.1 to 1.5 (average 1.2)TgCy−1 from biomass burning. In comparison, the most widely-used bottom-up estimate for Chinese annual total NMVOC emission was 27.4TgCy−1, including 15.5TgCy−1 from anthropogenic sources, 10.8TgCy−1 from biogenic sources, and 1.1TgCy−1 from biomass burning. The simultaneous use of glyoxal and formaldehyde observations helped distinguish the NMVOC species from different sources and was essential in constraining anthropogenic emissions. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. Our top-down estimates for the Chinese annual emission of anthropogenic aromatics (benzene, toluene, and xylene) ranged from 5.0 to 7.3TgCy−1, 2% to 49% larger than the estimate of the bottom-up inventory (4.9TgCy−1). Model simulations using the average of our top-down NMVOC emission estimates showed that surface afternoon ozone concentrations over northern and central China increased 5–12ppb in June and decreased 5–13ppb in December relative to the simulations using the a priori emissions and were in better agreement with measurements. We concluded that the satellite observations of glyoxal and formaldehyde together provided quantitative constraints on the emissions and source types of NMVOCs over China and improved our understanding on regional chemistry.

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Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 Tg C y−1, including 13.5 to 19.7 Tg C y−1 from anthropogenic sources, 8.9 to 14.8 Tg C y−1 from biogenic sources, and 1.1 to 1.5 Tg C y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal-formaldehyde constraints helped distinguish the NMVOC species from different sources.
Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 Tg C y−1,...
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