Organic Peroxides in Aerosol: Key Reactive Intermediates for Multiphase Processes in the Atmosphere

化学 激进的 大气(单位) 光解 气溶胶 环境化学 反应中间体 大气化学 分解 光化学 臭氧 化学物理 有机化学 气象学 催化作用 物理
作者
Shunyao Wang,Yue Zhao,Arthur W. H. Chan,Min Yao,Zhongming Chen,Jonathan P. D. Abbatt
出处
期刊:Chemical Reviews [American Chemical Society]
卷期号:123 (4): 1635-1679 被引量:89
标识
DOI:10.1021/acs.chemrev.2c00430
摘要

Organic peroxides (POs) are organic molecules with one or more peroxide (−O–O−) functional groups. POs are commonly regarded as chemically labile termination products from gas-phase radical chemistry and therefore serve as temporary reservoirs for oxidative radicals (HOx and ROx) in the atmosphere. Owing to their ubiquity, active gas-particle partitioning behavior, and reactivity, POs are key reactive intermediates in atmospheric multiphase processes determining the life cycle (formation, growth, and aging), climate, and health impacts of aerosol. However, there remain substantial gaps in the origin, molecular diversity, and fate of POs due to their complex nature and dynamic behavior. Here, we summarize the current understanding on atmospheric POs, with a focus on their identification and quantification, state-of-the-art analytical developments, molecular-level formation mechanisms, multiphase chemical transformation pathways, as well as environmental and health impacts. We find that interactions with SO2 and transition metal ions are generally the fast PO transformation pathways in atmospheric liquid water, with lifetimes estimated to be minutes to hours, while hydrolysis is particularly important for α-substituted hydroperoxides. Meanwhile, photolysis and thermolysis are likely minor sinks for POs. These multiphase PO transformation pathways are distinctly different from their gas-phase fates, such as photolysis and reaction with OH radicals, which highlights the need to understand the multiphase partitioning of POs. By summarizing the current advances and remaining challenges for the investigation of POs, we propose future research priorities regarding their origin, fate, and impacts in the atmosphere.
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