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Discussion papers | Copyright
© Author(s) 2018. This work is distributed under
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Research article 04 Apr 2018

Research article | 04 Apr 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).

Production of N2O5 and ClNO2 in summer in urban Beijing, China

Wei Zhou1,2,*, Jian Zhao1,2,*, Bin Ouyang3, Archit Mehra4, Weiqi Xu1,2, Yuying Wang5, Thomas J. Bannan4, Stephen D. Worrall4,a, Michael Priestley4, Asan Bacak4, Qi Chen6, Conghui Xie1,2, Qingqing Wang1, Junfeng Wang7, Wei Du1,2, Yingjie Zhang1, Xinlei Ge7, Penglin Ye8,11, James D. Lee9, Pingqing Fu1,2, Zifa Wang1,2, Douglas Worsnop8, Roderic Jones3, Carl J. Percival4,b, Hugh Coe4, and Yele Sun1,2,10 Wei Zhou et al.
  • 1State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
  • 2University of Chinese Academy of Sciences, Beijing 100049, China
  • 3Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
  • 4Centre for Atmospheric Science, School of Earth, Atmospheric and Environmental Science, University of Manchester, Manchester M13 9PL, UK
  • 5College of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, China
  • 6College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 7School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing, 210044, China
  • 8Aerodyne Research, Inc., Billerica, Massachusetts 01821, USA
  • 9National Centre for Atmospheric Science, University of York, Heslington, York YO10 5DD, UK
  • 10Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
  • 11Nanjing DiLu Scientific Instrument Inc, Nanjing, 210036, China
  • anow at: School of Materials, University of Manchester, M13 9PL, UK
  • bnow at: Jet Propulsion Laboratory, 4800 Oak Grove Drive, Pasadena, CA 91109
  • *These authors contributed equally to this work.

Abstract. The heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) has a significant impact on both nocturnal particulate nitrate formation and photochemistry the following day through photolysis of nitryl chloride (ClNO2), yet these processes in highly polluted urban areas remain poorly understood. Here we present measurements of gas-phase N2O5 and ClNO2 by high-resolution time-of-flight chemical ionization mass spectrometers (ToF-CIMS) during summer in urban Beijing, China as part of the Air Pollution and Human Health (APHH) campaign. N2O5 and ClNO2 show large day-to-day variations with average (±1σ) mixing ratios of 79.2±157.1 and 174.3±262.0pptv, respectively. High reactivity of N2O5, with τ (N2O5)−1 ranging from 0.20×10−2 to 1.46×10−2s−1, suggests active nocturnal chemistry and a large nocturnal nitrate formation potential via N2O5 heterogeneous uptake. The life time of N2O5, τ(N2O5), decreases rapidly as the increase of aerosol surface area, yet it varies differently as a function of relative humidity with the highest value peaking at ~40%. The N2O5 uptake coefficients estimated from the product formation rates of ClNO2 and particulate nitrate are in the range of 0.017–0.19, corresponding to direct N2O5 loss rates of 0.00044–0.0034s−1. Further analysis indicates that the fast N2O5 loss in the nocturnal boundary layer in urban Beijing is mainly attributed to its indirect loss via NO3, for example through the reactions with volatile organic compounds and NO, while the contribution of heterogeneous uptake of N2O5 is comparably small (7–33%). High ClNO2 yields ranging from 0.10 to 0.35 were also observed which might have important implications for air quality by affecting nitrate and ozone formation.

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We present the measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The life time of N2O5 as a function of aerosol surface area and relative humidity was characterized, and the N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via the reactions of NO3 with VOCs and NO.
We present the measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban...