Interparticle Delivery and Detection of Volatile Singlet Oxygen at Air/Solid Interfaces

Interparticle Delivery and Detection of Volatile Singlet Oxygen at Air/Solid Interfaces
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DOI:
10.1021/acs.est.0c07922
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发表时间:
2021-03-04
影响因子:
11.4
通讯作者:
Greer, Alexander
Greer, Alexander
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Durantini, Andres M.;Greer, Alexander

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已经设计了一种粒子间系统,允许空气中的单线态氧在粒子表面之间转移。单线态氧在敏化剂颗粒上光生,然后通过空气传播到带有可氧化化合物的第二个颗粒--这是一种基于颗粒的方法,与大气中的活性氧猝灭有一些相似之处。在大气光化学中,单线态氧是由天然颗粒物产生的,但它在颗粒之间的形成和猝灭至今尚未确定。确定单线态氧如何在第二表面上反应是有用的,并且是通过具有可调猝灭特性的三相系统(粒子-粒子)颗粒间光反应开发的。我们确定单线态氧猝灭直接通过近红外磷光在空气中的状态和在空气/颗粒界面的总猝灭速率常数(k(T))的吸附蒽捕集剂。单重态氧通过蒽包覆颗粒的气/固界面k(T)为9,10-二甲基蒽为(2.8 +/- 0.8)x 10(7)g mol(-1)s(-1),(2.1 +/- 0.9)× 10(7)g mol(-1)s(-1),空气中单线态氧的寿命测得为550 μ s。这些实时相互作用和粒子诱导的猝灭步骤为研究大气和颗粒物过程的单线态氧开辟了新的机会。
An interparticle system has been devised, allowing airborne singlet oxygen to transfer between particle surfaces. Singlet oxygen is photogenerated on a sensitizer particle, where it then travels through air to a second particle bearing an oxidizable compound-a particulate-based approach with some similarities to reactive oxygen quenching in the atmosphere. In atmospheric photochemistry, singlet oxygen is generated by natural particulate matter, but its formation and quenching between particles has until now not been determined. Determining how singlet oxygen reacts on a second surface is useful and was developed by a three-phase system (particleair-particle) interparticulate photoreaction with tunable quenching properties. We identify singlet oxygen quenching directly by near-IR phosphorescence in the airborne state and at the air/particle interface for total quenching rate constants (k(T)) of adsorbed anthracene trapping agents. The air/solid interface k(T) of singlet oxygen by anthracene-coated particles was (2.8 +/- 0.8) x 10(7) g mol(-1) s(-1) for 9,10-dimethylanthracene and (2.1 +/- 0.9) x 10(7) g mol(-1) s(-1) for 9,10-anthracene dipropionate dianion, and the lifetime of airborne singlet oxygen was measured to be 550 mu s. These real-time interactions and particle-induced quenching steps open up new opportunities for singlet oxygen research of atmospheric and particulate processes.