Preprints
https://doi.org/10.5194/acp-2021-628
https://doi.org/10.5194/acp-2021-628

  28 Jul 2021

28 Jul 2021

Review status: a revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Process-based and Observation-constrained SOA Simulations in China: The Role of Semivolatile and Intermediate-Volatility Organic Compounds and OH Levels

Ruqian Miao1, Qi Chen1, Manish Shrivastava2, Youfan Chen3, Lin Zhang4, Jianlin Hu5, Yan Zheng1, and Keren Liao1 Ruqian Miao et al.
  • 1State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China
  • 2Pacific Northwest National Laboratory, Richland, Washington, 99352, USA
  • 3Sichuan Academy of Environmental policy and planning, Chengdu, Sichuan, 610041, China
  • 4Laboratory for Climate and Ocean–Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, 100871, China
  • 5Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing, Jiangsu, 210044, China

Abstract. Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties to reproduce the variability of OA concentrations in polluted areas, hindering understanding of the OA budget. Herein, we applied both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model-observation comparisons. In the revised schemes, updates of the emissions, volatility distributions, and SOA yields of semivolatile and intermediate volatility organic compounds (S/IVOCs) were made. These updates are however insufficient to reproduce the SOA concentrations in observations. The addition of nitrous acid sources is an important model modification, which improves the simulation of surface concentrations of hydroxyl radical (OH) in winter in northern China. The increased surface OH concentrations enhance the SOA formation and lead to greater SOA mass concentrations by over 30 %, highlighting the importance of having good OH simulations in air quality models. There is a greater sensitivity of the SOA formation to the oxidant levels in winter than in summer in China. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic S/IVOCs are the dominant source of SOA in China with a contribution of over 50 %. The residential sector may be the predominant source of S/IVOCs in winter, despite large uncertainty remains in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More S/IVOC measurements are needed to constrain their emissions.

Ruqian Miao et al.

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-628', Anonymous Referee #1, 08 Sep 2021
  • RC2: 'Comment on acp-2021-628', Anonymous Referee #2, 15 Sep 2021

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-628', Anonymous Referee #1, 08 Sep 2021
  • RC2: 'Comment on acp-2021-628', Anonymous Referee #2, 15 Sep 2021

Ruqian Miao et al.

Ruqian Miao et al.

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Short summary
This study conducted comprehensive model-observation comparisons in China for organic aerosol. The results show the importance of having good simulations of hydroxyl radicals (OH) for secondary organic aerosol (SOA) modeling, especially in northern China in winter. Anthropogenic semivolatile and intermediate volatility organic compounds (S/IVOCs) are the main source of SOA in polluted regions in China, for which the residential sector is perhaps the predominant contributor.
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