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  • Title: Incorporation and improvement of a heterogeneous chemistry mechanism in the atmospheric chemistry model GRAPES_Meso5.1/CUACE and its impacts on secondary inorganic aerosol and PM2.5 simulations in Middle-Eastern China.
    Author: Liu Z, Wang H, Zhang L, Zhou Y, Zhang W, Peng Y, Zhang Y, Che H, Zhao M, Hu J, Liu H, Wang Y, Li S, Han C, Zhang X.
    Journal: Sci Total Environ; 2022 Nov 15; 847():157530. PubMed ID: 35878848.
    Abstract:
    Heterogeneous chemistry is considered one of the critical pathways of secondary inorganic aerosol (SIA) productions. In this study, a heterogeneous chemistry mechanism is incorporated into the atmospheric chemistry model GRAPES_Meso5.1/CUACE. Varying uptake coefficient schemes of SO2 and NO2 are compared and the equivalent ratio of inorganic aerosol (ER)-dependent scheme for SO2 and relative humidity (RH)/ER-dependent scheme for NO2 are used to form the improved heterogeneous chemistry. Focusing on a severe haze episode in Middle-Eastern China, the impacts of heterogeneous mechanism on SIA and PM2.5 composition are investigated based on the updated model. Study results show that the differences in RH or ER uptake coefficients result in obvious differences in sulfate and nitrate concentrations, especially during the severe pollution period, because the ER schemes restrict the excessive production of sulfate and nitrate under high RH effectively by including the self-limitation of heterogeneous reactions, which shows better performance in capturing the magnitude and temporal variations of surface SIA and PM2.5. Normalized mean bias of sulfate, nitrate, ammonium, and PM2.5 in megacity Beijing decreases from -27.0, -28.3, -58.2, and -26.3 to 1.0, -2.2, -47.2, and -16.5 %, respectively. And the fractions of sulfate, nitrate, ammonium, and organics during the polluted period change from 13.7, 19.3, 6.9, and 60.1 to 16.5, 23.0, 7.6, and 52.9 %, respectively, which is more consistent with the observation (16.0, 23.2, 14.1, and 46.7 %). SIA and PM2.5 simulations in another megacity Shanghai have the similar improvements. The modeled SIA by heterogeneous processes contributes 11.7 % of total PM2.5 in Beijing and 22.5 % in Shanghai. That is 13.5 % in the Chinese megalopolis Beijing-Tianjin-Hebei and 19.8 % in Yangtze-River-Delta, indicating a considerable contribution of heterogeneous pathways to haze pollution. This work indicates the importance of detailed and reasonable heterogeneous schemes for better SIA and haze/fog prediction in the atmospheric chemistry model.
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