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Volume 16, issue 16
Atmos. Chem. Phys., 16, 10707–10724, 2016
https://doi.org/10.5194/acp-16-10707-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 16, 10707–10724, 2016
https://doi.org/10.5194/acp-16-10707-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 30 Aug 2016

Research article | 30 Aug 2016

Simulations of sulfate–nitrate–ammonium (SNA) aerosols during the extreme haze events over northern China in October 2014

Dan Chen1, Zhiquan Liu1, Jerome Fast2, and Junmei Ban1 Dan Chen et al.
  • 1National Center for Atmospheric Research, Boulder, CO, USA
  • 2Pacific Northwest National Laboratory, Richland, WA, USA

Abstract. Extreme haze events have occurred frequently over China in recent years. Although many studies have investigated the formation mechanisms associated with PM2.5 for heavily polluted regions in China based on observational data, adequately predicting peak PM2.5 concentrations is still challenging for regional air quality models. In this study, we evaluate the performance of one configuration of the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) and use the model to investigate the sensitivity of heterogeneous reactions on simulated peak sulfate, nitrate, and ammonium concentrations in the vicinity of Beijing during four extreme haze episodes in October 2014 over the North China Plain. The highest observed PM2.5 concentration of 469 µg m−3 occurred in Beijing. Comparisons with observations show that the model reproduced the temporal variability in PM2.5 with the highest PM2.5 values on polluted days (defined as days in which observed PM2.5 is greater than 75 µg m−3), but predictions of sulfate, nitrate, and ammonium were too low on days with the highest observed concentrations. Observational data indicate that the sulfur/nitric oxidation rates are strongly correlated with relative humidity during periods of peak PM2.5; however, the model failed to reproduce the highest PM2.5 concentrations due to missing heterogeneous/aqueous reactions. As the parameterizations of those heterogeneous reactions are not well established yet, estimates of SO2-to-H2SO4 and NO2/NO3-to-HNO3 reaction rates that depend on relative humidity were applied, which improved the simulation of sulfate, nitrate, and ammonium enhancement on polluted days in terms of both concentrations and partitioning among those species. Sensitivity simulations showed that the extremely high heterogeneous reaction rates and also higher emission rates than those reported in the emission inventory were likely important factors contributing to those peak PM2.5 concentrations.

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Extreme haze events occurred frequently over China recently, and adequately predicting peak PM2.5 concentrations is still challenging. In this study, the sulfate–nitrate–ammonium relevant heterogeneous reactions were parameterized for the first time in the WRF-Chem model. We evaluated the performance of WRF-Chem and used the model to investigate the sensitivity of heterogeneous reactions on simulated peak sulfate, nitrate, and ammonium concentrations in the vicinity of Beijing during October 2014.
Extreme haze events occurred frequently over China recently, and adequately predicting peak...
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