Seasonal variations in the highly time-resolved aerosol composition, sources and chemical processes of background submicron particles in the North China Plain

Abstract

Abstract. For the first time in the North China Plain (NCP), we investigated the seasonal variations of submicron particles (NR-PM1) and its chemical composition at a background mountain station using Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The averaged NR-PM1 were highest in autumn (15.1\u2009μg\u2009m−3) and lowest in summer (12.4\u2009μg\u2009m−3), with the abundance of more nitrate in spring (34\u2009%), winter (31\u2009%), and autumn (34\u2009%), and elevated organics (40\u2009%) and sulfate (38\u2009%) proportion in summer. The submicron particles were almost neutralized by excess ammonium in all four seasons except summer, when the aerosol particles appeared to be slightly acidic. The size distribution of all PM1 species showed a consistent accumulation mode peaked at approximately 600–800\u2009nm (dva), indicating the highly aged and internally mixed nature of the background aerosols, which further supported by the source appointment using multilinear engine (ME-2) and significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (>\u200977\u2009%), especially in summer (95\u2009%). The oxidation degree and evolution process of OAs in the four seasons were further investigated, and enhanced carbon oxidation state (−0.45–0.10), O\u2009/\u2009C (0.54–0.75) and OM\u2009/\u2009OC (1.86–2.13) ratios compared with urban studies were observed, with the highest oxidation degree of which appeared in summer, likely due to the relatively stronger photochemical processing which dominated the processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA) formations. Aqueous-phase processing also contributed to the SOA formation but prevailed in autumn and winter and the role of which to MO-OOA and LO-OOA also varied in different seasons. In addition, compared with the urban atmosphere, LO-OOA formation in the background atmosphere exhibited more regional characteristics, as photochemical and aqueous-phase processing enhanced during the transport in summer and autumn, respectively. Furthermore, the backward trajectories analysis showed that higher submicron particles were associated with air mass for short distance transported from the southern regions in four seasons, while the long-range transport from Inner Mongolia (west and north regions) also contributed to the summer particle pollutions in the background areas of NCP. Our results illustrate the background particles in NCP are influenced significantly by aging processing and transport, and the more neutralized state of submicron particles with the abundance of nitrate compared with those in the background atmosphere in southern and western China, highlighting the regional reductions in emissions of nitrogen oxide and ammonia are critical for remedying the increased occurrence of nitrate-dominated haze event in the NCP.