Characteristics and seasonal variations of high-molecular-weight oligomers in urban haze aerosols

摘要

Organic aerosols (OA) undergo sophisticated physiochemical processes in the atmosphere, playing a crucial role in extreme haze formations over the Northern China Plain. However, current understandings of the detailed composition and formation pathways are limited. In this study, high-molecular weight (HMW) species were observed in samples collected year-round in urban Beijing, especially in autumn and winter, during 2016-2017. The positive-ion-mode mass spectra of matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF-MS) showed that higher signal intensities were obtained in the mass-to-charge (m/z) ranges of 200-500 and 800-900, with repetitive mass difference patterns of m/z 12, 14, 16, and 18. This provided sound evidence that high-molecular-weight oligomers were generated as haze episodes became exacerbated. These oligomer signal intensities were enhanced in the presence of high relative humidity, aerosol water content, and PM_(2.5) (particles with an aerodynamic diameter ≤ 2.5 μm) mass, proving that the multiphase reaction processes play a fundamental role in haze formation in Beijing. Our study can form a basis for improved air pollution mitigation measures aimed at OA to improve health outcomes.