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Effects of Aqueous-Phase and Photochemical Processing on Secondary Organic Aerosol Formation and Evolution in Beijing, China

机译：水相和光化学处理对北京地区次生有机气溶胶形成和演化的影响

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摘要

Secondary organic aerosol (SOA) constitutes a large fraction of OA, yet remains a source of significant uncertainties in climate models due to incomplete understanding of its formation mechanisms and evolutionary processes. Here we evaluated the effects of photochemical and aqueous-phase processing on SOA composition and oxidation degrees in three seasons in Beijing, China, using high-resolution aerosol mass spectrometer measurements along with positive matrix factorization. Our results show that aqueous-phase processing has a dominant impact on the formation of more oxidized SOA (MO-OOA), and the contribution of MO-OOA to OA increases substantially as a function of relative humidity or liquid water content. In contrast, photochemical processing plays a major role in the formation of less oxidized SOA (LO-OOA), as indicated by the strong correlations between LO-OOA and odd oxygen (O_x = O_3 + NO_2) during periods of photochemical production (R~2 = 0.59-0.80). Higher oxygen-to-carbon ratios of SOA during periods with higher RH were also found indicating a major role of aqueous-phase processing in changing die oxidation degree of SOA in Beijing. Episodes analyses further highlight that LO-OOA plays a more important role during the early stage of the formation of autumn/winter haze episodes while MO-OOA is more significant during the later evolution period.
机译：次生有机气溶胶（SOA）构成了OA的很大一部分，但由于对它的形成机理和进化过程的不完全了解，仍然是气候模型中重大不确定性的来源。在这里，我们使用高分辨率气溶胶质谱仪测量和正矩阵分解，评估了中国北京三个季节中光化学和水相处理对SOA组成和氧化度的影响。我们的结果表明，水相处理对更多氧化的SOA（MO-OOA）的形成具有主要影响，而MO-OOA对OA的贡献随着相对湿度或液态水含量的增加而大大增加。相比之下，光化学加工在形成较少氧化的SOA（LO-OOA）中起主要作用，这在光化学生产期间（R〜 2 = 0.59-0.80）。在较高的相对湿度下，SOA的氧碳比也更高，这表明水相处理在改变北京SOA的氧化程度方面起着重要作用。情节分析进一步突出表明，LO-OOA在秋/冬霾情节形成的早期起着更重要的作用，而MO-OOA在较晚的演变时期更重要。

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  • 来源
    《Environmental Science & Technology》 |2017年第2期|762-770|共9页
  • 作者

    Weiqi Xu; Tingting Han; Wei Du; Qingqing Wan; Chen Chen; Jian Zhao; Yingjie Zhang; Jie Li; Pingqing Fu; Zifa Wang; Douglas R. Worsnop; Yele Sun;

  • 作者单位

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,University of Chinese Academy of Sciences, Beijing 100049, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Nanjing University of Information Science & Technology, Nanjing 210044, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;

    Aerodyne Research, Inc., Billerica, Massachusetts 01821, United States;

    State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China,Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China,Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Nanjing University of Information Science & Technology, Nanjing 210044, China;

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