Wintertime secondary organic aerosol formation in Beijing–Tianjin–Hebei (BTH): contributions of HONO sources and heterogeneous reactions

Abstract

Organic aerosol (OA) concentrations are simulated over the Beijing–Tianjin–Hebei (BTH) region from 9 to 26 January 2014 using the Weather Research and Forecasting model coupled with chemistry (WRF-CHEM), with the goal of examining the impact of heterogeneous HONO sources on SOA formation and SOA formation from different pathways during wintertime haze days. The model generally shows good performance with respect to simulating air pollutants and organic aerosols against measurements in BTH. Model results show that heterogeneous HONO sources substantially enhance near-surface SOA formation, increasing the regional average near-surface SOA concentration by about 46.3 % during the episode. Oxidation and partitioning of primary organic aerosols treated as semi-volatile dominate SOA formation, contributing 58.9 % of the near-surface SOA mass in BTH. Irreversible uptake of glyoxal and methylglyoxal on aerosol surfaces constitutes the second most important SOA formation pathway during the episode, with the SOA contribution increasing from 8.5 % under non-haze conditions to 30.2 % under haze conditions. Additionally, direct emissions of glyoxal and methylglyoxal from residential sources contribute about 25.5 % of the total SOA mass on average in BTH. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation over the BTH region in winter.