Measurement Report: Investigation on the sources and formation processes of dicarboxylic acids and related species in urban aerosols before and during the COVID-19 lockdown in Jinan, East China

Abstract

Dicarboxylic acid (diacid) homologs are essential indicators of secondary organic aerosols (SOA) that exert a considerable influence on climate changes and atmospheric chemistry. However, their sources and formation processes are poorly understood, leading to uncertainty in predicting the climate effect of SOA. A substantial drop in anthropogenic emissions during the COVID-19 lockdown (LCD) provides a “controlled experiment” to explore the effects of LCD measures and meteorological conditions on SOA. Here we investigated the difference in molecular distributions and stable carbon isotopic compositions (δ13C) of diacid homologs in PM2.5 before and during the LCD. We found that the concentration and contribution of diacid homologs during the LCD were higher than before the LCD, indicating that the enhanced secondary oxidation could offset the reduction in anthropogenic emissions during the LCD. A higher oxalic acid (C2) / diacid ratio and more positive δ13C values of major diacids during the LCD suggested more aged organic aerosols. The enhanced C2 and related species during the LCD were mainly derived from the promoted gaseous photochemical oxidation by the higher oxidants and stronger solar radiation. However, C2 and related species before the LCD were dominantly derived from the aqueous oxidation of α-dicarbonyls depending on relative humidity and liquid water content. The increased δ13C values of C2 and other major diacids along with the high ratios of C2 / glyoxal, C2 / methylglyoxal, and C2 / diacid confirmed an isotopic fractionation effect during the oxidation process of precursors. Our results indicate that atmospheric pollution treatment depends on a balanced strategy and a coordinated effort to control multiple pollutants.