Changes in Physicochemical Properties of Organic Aerosol During Photochemical Aging of Cooking and Burning Emissions

Abstract

AbstractPhotochemical aging is a key atmospheric processing, yet the changes in physicochemical properties of organic aerosol (OA) during photochemical aging of primary emissions from cooking and burning are less understood. Here we conducted 12 burning (straw, wood, and coal) and cooking experiments to characterize the evolution of size distributions, volatility, and glass transition temperature (Tg) from fresh smoke to aged OA with an equivalent photochemical age of ∼1.5 days using an oxidation flow reactor‐thermodenuder‐aerosol mass spectrometer system. The mass spectra of OA showed significant changes during photochemical aging, for example, the rapid degradation of m/z 60 for straw and wood burning OA, and the large increase in f44 (fraction of m/z 44 in OA) for all OA. The contributions of non‐volatile compounds to the total OA in aged burning OA (1.6%–5.3%) decreased considerably compared with those in fresh burning smoke (2.3%–17.1%), suggesting that photochemical aging of primary emissions for ∼1.5 days produced more volatile secondary OA (SOA). Consistently, the pronounced formation of SOA below 150 nm was observed, and it showed more volatile properties than aged large particles. The Tg of OA under dry conditions (Tg,org) was estimated based on volatility distributions, and the results showed increased Tg,org during photochemical aging of biomass burning and coal combustion emissions, while decreased Tg,org for aged cooking OA. Overall, our results illustrate the different changes in size distributions, volatility, and Tg,org through photochemical aging of different primary emissions, which in turn affect their impacts on radiative forcing and human health.