Modeling diurnal variation of surface PM2.5 concentrations over East China with WRF-Chem: Impacts from boundary-layer mixing and anthropogenic emission

Abstract

Diurnal variation of surface PM2.5 concentration (diurnal PM2.5) could dramatically affect aerosol radiative and health impacts and can also well reflect the physical and chemical mechanisms of air pollution formation and evolution. So far, diurnal PM2.5 and its modeling capability over East China have not been investigated and therefore are examined in this study. Based on the observations, the normalized diurnal amplitude of surface PM2.5 concentrations averaged over East China is weakest (1:2) in winter and reaches 1:5 in other seasons. The diurnal PM2.5 shows the peak concentration during the night in spring and fall and during the daytime in summer. The simulated diurnal PM2.5 with WRF-Chem and its contributions from multiple physical and chemical processes are examined in the four seasons. The simulated diurnal PM2.5 with WRF-Chem is primarily controlled by planetary boundary layer (PBL) mixing and emission variations and is significantly overestimated against the observation during the night. This modeling bias is likely primarily due to the inefficient PBL mixing of primary PM2.5 during the night. The simulated diurnal PM2.5 is sensitive to the PBL schemes and vertical-layer configurations with WRF-Chem. Besides the PBL height, the PBL mixing coefficient is also found to be the critical factor determining the PBL mixing of pollutants in WRF-Chem. With reasonable PBL height, the increase in the lower limit of the PBL mixing coefficient during the night can significantly reduce the modeling biases in diurnal PM2.5 and also the mean concentrations, particularly in the major cities of East China. It can also reduce the modeling sensitivity to the PBL vertical-layer configurations. The diurnal variation and injection height of anthropogenic emissions also play roles in simulating diurnal PM2.5, but the impact is relatively smaller than that from the PBL mixing. This study underscores that more efforts are needed to improve the boundary mixing process of pollutants in models with observations of PBL structure and mixing fluxes in addition to PBL height, in order to simulate reasonably the diurnal PM2.5 over East China. The diurnal variation and injection height of anthropogenic emissions must also be included to simulate the diurnal PM2.5 over East China.