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The overestimated role of singlet oxygen for pollutants degradation in some non-photochemical systems
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-07-01 , DOI: 10.1016/j.cej.2020.126128
Xiaohui Lu , Wei Qiu , Jun Ma , Haodan Xu , Da Wang , Haijun Cheng , Wei Zhang , Xu He

Singlet oxygen (1O2) is considered as the dominant reactive oxygen species (ROS) responsible for micropollutants degradation in many non-photochemical systems. However, the role of 1O2 in non-photochemical systems is overrated due to overlooking the fast quenching of 1O2 in water and the false positive results of electron paramagnetic resonance (EPR) experiments for 1O2 identification. Herein, we systematically compared the classical 1O2-generation H2O2/OCl system and some non-photochemical systems in pollutants oxidation, electron paramagnetic resonance (EPR) experiments and dimol emission of singlet oxygen in different solvents for the first time. The results showed that almost all 1O2 were deactivated by water and hardly consumed by micropollutants in non-photochemical systems considering the high deactivation rate constant of 1O2 in water. Moreover, the EPR signals of TEMPO free radical detected in non-photochemical systems may not precisely represent the existence of 1O2. These results indicated that some others ROS rather than 1O2, for example, dioxiranes in the ketone-catalysed decomposition of peroxomonosulfate (PMS), were responsible for the degradation of micropollutants in some non-photochemical systems, and further investigation about the real ROS are needed.



中文翻译:

单线态氧在某些非光化学系统中对污染物降解的高估作用

单重态氧(1 O 2)被认为是导致许多非光化学系统中微污染物降解的主要活性氧(ROS)。但是,由于忽略了水中1 O 2的快速淬灭和1 O 2鉴定的电子顺磁共振(EPR)实验的假阳性结果,因此1 O 2在非光化学系统中的作用被高估了。在此,我们系统地比较了经典1 Ò 2 -generationħ 2 ö 2 / OCL -系统和一些非光化学系统首次用于污染物的氧化,电子顺磁共振(EPR)实验和单线态氧在不同溶剂中的二摩尔排放。结果表明,考虑到1 O 2在水中的高失活速率常数,在非光化学体系中几乎所有1 O 2都被水失活,而微污染物几乎不消耗。此外,在非光化学系统中检测到的TEMPO自由基的EPR信号可能无法精确表示1 O 2的存在。这些结果表明还有一些ROS而不是1 O 2例如,在一些非光化学体系中,酮催化的过氧单硫酸盐(PMS)分解中的二恶英类化合物是导致微污染物降解的原因,因此需要进一步研究真正的ROS。

更新日期:2020-07-07
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