化学
试剂
水溶液
质谱法
化学反应
大气化学
化学电离
环境化学
光化学
有机化学
化学工程
离子
电离
色谱法
臭氧
工程类
作者
Liselotte Tinel,Stéphane Rossignol,Angelica Bianco,Monica Passananti,Sébastien Perrier,Xinming Wang,Marcello Brigante,D. J. Donaldson,Christian George
标识
DOI:10.1021/acs.est.6b03165
摘要
Interfaces are ubiquitous in the environment and many atmospheric key processes, such as gas deposition, aerosol, and cloud formation are, at one stage or another, strongly impacted by physical and chemical processes occurring at interfaces. Here, the photoinduced chemistry of an air/water interface coated with nonanoic acid-a fatty acid surfactant we use as a proxy for chemically complex natural aqueous surface microlayers-was investigated as a source of volatile and semivolatile reactive organic species. The carboxylic acid coating significantly increased the propensity of photosensitizers, chosen to mimic those observed in real environmental waters, to partition to the interface and enhance reactivity there. Photochemical formation of functionalized and unsaturated compounds was systematically observed upon irradiation of these coated surfaces. The role of a coated interface appears to be critical in providing a concentrated medium allowing radical-radical reactions to occur in parallel with molecular oxygen additions. Mechanistic insights are provided from extensive analysis of products observed in both gas and aqueous phases by online switchable reagent ion-time of flight-mass spectrometry and by off-line ultraperformance liquid chromatography coupled to a Q Exactive high resolution mass spectrometer through heated electrospray ionization, respectively.
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