Dramatic changes in Harbin aerosol during 2018–2020: the roles of open burning policy and secondary aerosol formation

Abstract. Despite the growing interest in understanding haze formation in Chinese megacities, air pollution has been largely overlooked for the Harbin-Changchun (HC) metropolitan area located in the severe cold climate region in Northeast China. In this study, we unfolded significant variations of fine particulate matter (PM2.5) in HC’s central city (Harbin) during two sequential heating seasons of 2018–2019 and 2019–2020, and explored major drivers for the observed variations. The two campaigns showed comparable organic carbon (OC) levels but quite different OC sources. The biomass burning (BB) to OC contribution decreased substantially for 2019–2020, which was attributed primarily to the transition of local policies on agricultural fires, i.e., from the “legitimate burning” policy released in 2018 to the “strict prohibition” policy in 2019. Meanwhile, the contribution of secondary OC (OCsec) increased significantly, associated with the much more frequent occurrences of high relative humidity (RH) conditions during the 2019–2020 measurement period. Similar to OCsec, the major secondary inorganic ions, i.e., sulfate, nitrate and ammonium (SNA), also exhibited RH-dependent increases. Given the considerable aerosol water contents predicted for the high-RH conditions, heterogeneous reactions were likely at play in secondary aerosol formation even in the frigid atmosphere in Harbin (e.g., with daily average temperatures down to below −20 °C). In brief, compared to 2018–2019, the 2019–2020 measurement period was characterized by a policy-driven decrease of biomass burning OC, a RH-related increase of OCsec and a RH-related increase of SNA, with the former two factors generally offsetting each other. In addition, we found that open burning activities were actually not eliminated by the “strict prohibition” policy released in 2019, based on a synthesis of air quality data and fire count results. Although not evident throughout the 2019–2020 measurement period, agricultural fires broke out within a short period before crop planting in spring of 2020, and resulted in off-the-chart air pollution for Harbin, with 1- and 24-hour PM2.5 concentrations peaking at ~2350 and 900 μg/m3, respectively. This study indicates that sustainable use of crop residues remains a difficult challenge for the massive agricultural sector in Northeast China.