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Discussion papers
https://doi.org/10.5194/acp-2018-1015
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1015
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 04 Oct 2018

Research article | 04 Oct 2018

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

Possible heterogeneous hydroxymethanesulfonate (HMS) chemistry in northern China winter haze and implications for rapid sulfate formation

Shaojie Song1, Meng Gao1, Weiqi Xu2,3, Yele Sun2,3,4, Douglas R. Worsnop5, John T. Jayne5, Yuzhong Zhang1, Lei Zhu1, Mei Li6,7, Zhen Zhou6,7, Chunlei Cheng6,7, Yibing Lv8, Ying Wang9, Wei Peng9, Xiaobin Xu9, Nan Lin10, Yuxuan Wang11, Shuxiao Wang12, J. William Munger1, Daniel Jacob1, and Michael B. McElroy1 Shaojie Song et al.
  • 1School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
  • 2State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
  • 3College of Earth Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
  • 4Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
  • 5Aerodyne Research, Inc., Billerica, MA 01821, USA
  • 6Institute of Mass Spectrometer and Atmospheric Environment, Jinan University, Guangzhou 510632, China
  • 7Guangdong Provincial Engineering Research Center for Online Source Apportionment System of Air Pollution, Guangzhou 510632, China
  • 8China National Environmental Monitoring Center, Beijing 100012, China
  • 9State Key Laboratory of Severe Weather & Key Laboratory for Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China
  • 10Department of Earth System Science, Tsinghua University, Beijing 100084, China
  • 11Department of Earth and Atmospheric Sciences, University of Houston, Houston, TX 77004, USA
  • 12School of Environment, Tsinghua University, Beijing 100084, China

Abstract. Chemical mechanisms responsible for rapid sulfate production, an important driver of winter haze formation in northern China, remain unclear. Here, we propose a potentially important heterogeneous hydroxymethanesulfonate (HMS) chemical mechanism. Through analyzing field measurements with aerosol mass spectrometry, we show evidence for a possible significant existence in haze aerosols of organosulfur primarily as HMS, misidentified as sulfate in previous observations. We estimate that HMS can account for up to about one-third of the sulfate concentrations unexplained by current air quality models. In addition, HMS in the presence of hydroxyl radicals can trigger rapid sulfate production in aerosol water. Heterogeneous production of HMS by SO2 and formaldehyde is favored under northern China winter haze conditions due to high aerosol water content, moderately acidic pH values, high gaseous precursor levels, and low temperature. These analyses identify an unappreciated importance of formaldehyde in secondary aerosol formation and calls for more research on sources and on the chemistry of formaldehyde in northern China winter.

Shaojie Song et al.
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate. Formaldehyde may play a far more important role in Chinese haze formation than previously recognized.
Chemistry responsible for sulfate production in northern China winter haze remains mysterious....
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