References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-11-28219-2011

Carbonaceous aerosols in China: top-down constraints on primary sources and estimation of secondary contribution

T.-M.

¹ Cao

J. J.

² Zhang

X. Y.

³ Lee

S. C.

⁴ Zhang

⁵ Han

Y. M.

² Qu

W. J.

⁶ Han

⁷ Zhang

⁷ Wang

Y. X.

⁵ Chen

⁸ Henze

D. K.

⁹

Department of Atmospheric and Oceanic Sciences and Laboratory for Climate and Ocean-Atmosphere Studies, School of Physics, Peking University, Beijing, China

State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an, China

Key Laboratory for Atmospheric Chemistry, Centre for Atmosphere Watch & Services of CMA, Chinese Academy of Meteorological Sciences, Beijing, China

Research Center of Urban Environmental Technology and Management, Department of Civil and Structural Engineering, Hong Kong Polytechnic University, Kowloon, Hong Kong

Ministry of Education Key Laboratory for Earth System Modeling, Center for Earth System Science, Institute for Global Change Studies, Tsinghua University, Beijing, China

Physical Oceanography Laboratory, Ocean-Atmosphere Interaction and Climate Laboratory, Ocean University of China, Qingdao, China

Key Laboratory of Regional Climate-Environment Research for Temperate East Asia, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China

Department of Atmospheric & Oceanic Sciences, University of California, Los Angeles, Los Angeles, USA

Department of Mechanical Engineering, University of Colorado at Boulder, Boulder, USA

20 10 2011

11 10 28219 28272

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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We simulate elemental carbon (EC) and organic carbon (OC) aerosols in China and compare model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We include in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 Tg C yr−1) and OC (3.95 Tg C yr−1), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background site is 1.1 μg C m−3, 56% lower than the observed 2.5 μg C m−3. The average simulated annual mean OC concentration at rural and background sites is 3.4 μg C m−3, 76% lower than the observed 14 μg C m−3. Multiple regression to fit surface monthly mean EC observations at rural and background sites yields best estimate of Chinese EC source of 3.05 ± 0.78 Tg C yr−1. Based on the top-down EC emission estimate and observed seasonal primary OC/EC ratios, we estimate Chinese OC total emissions to be 6.67 ± 1.30 Tg C yr−1. Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites significantly improved to 1.9 μg C m−3. However, the model still significantly underestimates observed OC in all seasons (simulated average annual mean OC at rural and background sites is 5.4 μg C m−3), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21% of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62% of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to three shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is severely underestimated, particularly for OC; (2) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (3) sources in fall are not well represented, either because the seasonal shifting of emissions and/or secondary formation are poorly captured or because specific fall emission events are missing. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

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