Key role of organic carbon in the sunlight-enhanced atmospheric aging of soot by O2

Abstract

Soot particles are ubiquitous in the atmosphere and have important climatic and health effects. The aging processes of soot during long-range transport result in variability in its morphology, microstructure, and hygroscopic and optical properties, subsequently leading to the modification of soot's climatic and health effects. In the present study the aging process of soot by molecular O2 under simulated sunlight irradiation is investigated. Organic carbon components on the surface of soot are found to play a key role in soot aging and are transformed into oxygen-containing organic species including quinones, ketones, aldehydes, lactones, and anhydrides. These oxygen-containing species may become adsorption centers of water and thus enhance the cloud condensation nuclei and ice nuclei activities of soot. Under irradiation of 25 mW·cm-2, the apparent rate constants (k1,obs) for loss or formation of species on soot aged by 20% O2 were larger by factors of 1.5-3.5 than those on soot aged by 100 ppb O3. Considering the abundance of O2 in the troposphere and its higher photoreactivity rate, the photochemical oxidation by O2 under sunlight irradiation should be a very important aging process for soot.