Keywood M D, Kroll J H, Varutbangkul V, Bahreini R, Flagan R C, Seinfeld J H
Department of Environmental Science, California Institute of Technology, Pasadena, California 91125, USA.
Environ Sci Technol. 2004 Jun 15;38(12):3343-50. doi: 10.1021/es049725j.
To isolate secondary organic aerosol (SOA) formation in ozone-alkene systems from the additional influence of hydroxyl (OH) radicals formed in the gas-phase ozone-alkene reaction, OH scavengers are employed. The detailed chemistry associated with three different scavengers (cyclohexane, 2-butanol, and CO) is studied in relation to the effects of the scavengers on observed SOA yields in the ozone-cyclohexene system. Our results confirm those of Docherty and Ziemann that the OH scavenger plays a role in SOA formation in alkene ozonolysis. The extent and direction of this influence are shown to be dependent on the specific alkene. The main influence of the scavenger arises from its independent production of HO2 radicals, with CO producing the most HO2, 2-butanol an intermediate amount, and cyclohexane the least. This work provides evidence for the central role of acylperoxy radicals in SOA formation from the ozonolysis of alkenes and generally underscores the importance of gas-phase radical chemistry beyond the initial ozone-alkene reaction.
为了将臭氧 - 烯烃体系中二次有机气溶胶(SOA)的形成与气相臭氧 - 烯烃反应中形成的羟基(OH)自由基的额外影响隔离开来,人们采用了OH清除剂。研究了与三种不同清除剂(环己烷、2 - 丁醇和CO)相关的详细化学过程,以及这些清除剂对臭氧 - 环己烯体系中观测到的SOA产率的影响。我们的结果证实了多赫蒂(Docherty)和齐曼(Ziemann)的研究结果,即OH清除剂在烯烃臭氧化过程中对SOA的形成起作用。这种影响的程度和方向取决于特定的烯烃。清除剂的主要影响源于其独立产生HO₂自由基,其中CO产生的HO₂最多,2 - 丁醇产生的量居中,环己烷产生的最少。这项工作为酰基过氧自由基在烯烃臭氧化形成SOA过程中的核心作用提供了证据,并总体强调了气相自由基化学在初始臭氧 - 烯烃反应之外的重要性。