近日,广东工业大学安太成团队揭示了硫酸盐促进大气气溶胶中胺盐臭氧化。这一研究成果于2025年9月10日发表在《美国化学会志》上。
低分子量胺通过酸碱反应促进硫酸盐(SO42-和HSO4-)的形成,形成细颗粒物(PM)。臭氧化将无毒胺盐转化为剧毒产物,但臭氧化激活机制尚不清楚。
研究组通过结合先进的质谱法和从头计算方法揭示了细颗粒物中胺盐以硫酸盐为主的臭氧化机制。在•OH引发的氧化协同作用下,SO42-通过去质子化作用激活胺离子,生成亚胺分子作为臭氧氧化的中间产物。随后,HSO4-加速中间产物氨基甲醇和臭氧氧化产物的形成。此外,这种胺盐的新型臭氧氧化机制已被证实对硫酸盐细颗粒物(PM)有效,而对氯化物或硝酸盐细颗粒物则不可行。研究组强调了硫酸盐在惰性有机化合物臭氧氧化中的关键作用,这一作用在细颗粒物化学中需予以考虑。
附:英文原文
Title: Sulfate Promotes Amine Salt Ozonation in Atmospheric Aerosols
Author: Weina Zhang, Dayuan Zheng, Jiale Lao, Ruijing Li, Baihang Chen, Jiangyao Chen, Jie Zhong, Yuemeng Ji, Guiying Li, Joseph S. Francisco, Taicheng An
Issue&Volume: September 10, 2025
Abstract: Low molecular weight amines promote sulfate (SO42– and HSO4–) formation through acid–base reactions, contributing to fine particulate matter (PM). Heterogeneous ozonation converts nontoxic amine salts into highly toxic products, yet the ozonation activation mechanism is unclear. This work reveals a sulfate-dominant ozonation mechanism of amine salts in fine PM by combining advanced mass spectrometry and ab initio calculation methods. With the synergy of OH-initiated oxidation, SO42– activates amine ions through deprotonation, producing imine molecules as ozonation intermediates. Subsequently, HSO4– accelerates the formation of the intermediate aminomethanol and ozonation products. Moreover, this novel ozonation mechanism of amine salt is verified to be efficient for sulfate fine PM and is not feasible for chloride or nitrate fine PM. In this study, the key role of sulfate in the ozonation of inert organic compounds is highlighted, which needs to be considered in fine PM chemistry.
DOI: 10.1021/jacs.5c04343
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c04343
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
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