Characterization and source apportionment of organic aerosol at 260m on a?meteorological tower in Beijing, China

摘要

Despite extensive efforts toward the characterization of submicron aerosols at ground level in the megacity of Beijing, our understanding of aerosol sources and processes at high altitudes remains low. Here we conducted a?3-month real-time measurement of non-refractory submicron aerosol (NR-PM1) species at a?height of 260m from 10?October 2014 to 18?January 2015 using an aerosol chemical speciation monitor. Our results showed a?significant change in aerosol composition from the non-heating period (NHP) to the heating period (HP). Organics and chloride showed clear increases during HP due to coal combustion emissions, while nitrate showed substantial decreases from 28 to 15–18%. We also found that NR-PM1 species in the heating season can have average mass differences of 30–44% under similar emission sources yet different meteorological conditions. Multi-linear engine?2 (ME-2) using three primary organic aerosol (OA) factors as constraints, i.e., fossil-fuel-related OA (FFOA) dominantly from coal combustion emissions, cooking OA (COA), and biomass burning OA (BBOA) resolved from ground high-resolution aerosol mass spectrometer measurements, was applied to OA mass spectra of ACSM. Two types of secondary OA (SOA) that were well correlated with nitrate and chloride–CO, respectively, were identified. SOA played a?dominant role in OA during all periods at 260m although the contributions were decreased from 72% during NHP to 58–64% during HP. The SOA composition also changed significantly from NHP to HP. While the contribution of oxygenated OA (OOA) was decreased from 56–63 to 32–40%, less oxidized OOA (LO-OOA) showed a?large increase from 9–16 to 24–26%. COA contributed a?considerable fraction of OA at high altitude, and the contribution was relatively similar across different periods (10–13%). In contrast, FFOA showed a?large increase during HP due to the influences of coal combustion emissions. We also observed very different OA composition between ground level and 260m. Particularly, the contributions of COA and BBOA at the ground site were nearly twice those at 260m, while SOA at 260m was ～15–34% higher than that at ground level. Bivariate polar plots and back-trajectory analysis further illustrated the different source regions of OA factors in different seasons.