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Aqueous-phase chloramine production as a missing chain in atmospheric chlorine chemistry
  • +22
  • Yijing Chen,
  • Men Xia,
  • Jinghui Zhang,
  • Chao Yan,
  • Runlong Cai,
  • Guangjie Zheng,
  • Yuyang Li,
  • Junchen Guo,
  • Zhaojin An,
  • Yiran Li,
  • Epameinondas Tsiligiannis,
  • Cheng Wu,
  • Qipeng Qu,
  • Boyang Feng,
  • Chenjie Hua,
  • Zongcheng Wang,
  • Shuxiao Wang,
  • Yongchun Liu,
  • Lina Cao,
  • Douglas R Worsnop,
  • Kebin He,
  • Mattias Hallquist,
  • Markku Kulmala,
  • Tao Wang,
  • Jingkun Jiang
Yijing Chen
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Men Xia
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology, Institute for Atmospheric and Earth System Research / Physics, Faculty of Science, University of Helsinki
Jinghui Zhang
Department of Intelligent Edge Cloud, Chinatelecom Cloud Technology Co
Chao Yan
School of Atmospheric Sciences, Joint International Research Laboratory of Atmospheric and Earth System Research (JirLATEST), Nanjing University, Institute for Atmospheric and Earth System Research / Physics, Faculty of Science, University of Helsinki
Runlong Cai
Department of Environmental Science & Engineering, Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Fudan University, Institute for Atmospheric and Earth System Research / Physics, Faculty of Science, University of Helsinki
Guangjie Zheng
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Yuyang Li
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Junchen Guo
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Zhaojin An
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Yiran Li
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Epameinondas Tsiligiannis
Department of Chemistry and Molecular Biology, University of Gothenburg, School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Cheng Wu
Department of Chemistry and Molecular Biology, University of Gothenburg
Qipeng Qu
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Boyang Feng
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Chenjie Hua
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology
Zongcheng Wang
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology
Shuxiao Wang
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Yongchun Liu
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology
Lina Cao
Department of Intelligent Edge Cloud, Chinatelecom Cloud Technology Co
Douglas R Worsnop
Aerodyne Research Inc, Institute for Atmospheric and Earth System Research / Physics, Faculty of Science, University of Helsinki
Kebin He
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University
Mattias Hallquist
Department of Chemistry and Molecular Biology, University of Gothenburg
Markku Kulmala
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology, Institute for Atmospheric and Earth System Research / Physics, Faculty of Science, University of Helsinki
Tao Wang
Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University
Jingkun Jiang
School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University

Corresponding Author:

Abstract

Chlorine radical (Cl•) profoundly impacts atmospheric oxidation capacity, and therefore climate change and air pollution. Chloramines, especially trichloramine (NCl 3), is a potentially important Cl• source, while their formation mechanism remains elusive. Here, we present evidence of aerosol aqueous-phase production of chloramines with observations in Beijing and develop a comprehensive box model which incorporates ~40 aerosol aqueous reactions initiated by Cl 2 and NH 3 and multiple phase transfer processes. The model can well reproduce the diurnal variation of NCl 3. We show that this atmospheric production of chloramines could be ubiquitous globally with the coexistence of aerosol water, Cl 2 , and NH 3 , while NCl 3 formation is mainly influenced by Cl 2 and relative humidity as NH 3 is typically in great excess. The contribution of chloramines (mostly NCl 3) to Cl• production is much higher in clean periods (up to 85%) than polluted periods (~5%) in Beijing, and in clean environments (e.g., ~64% in Canada) than polluted areas (e.g., ~1% in India). Therefore, chloramines can play an increasingly important role in a cleaner future and may partially offset the ongoing efforts on air pollution mitigation. The missing representation of chloramines in current models could significantly underestimate the climate, health and ecological impacts of Cl•.