Photosensitized Transformation of Peroxymonosulfate in Dissolved Organic Matter Solutions under Simulated Solar Irradiation.
Photosensitized Transformation of Peroxymonosulfate in Dissolved Organic Matter Solutions under Simulated Solar Irradiation.
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DOI：
10.1021/acs.est.1c07411
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发表时间：
2022-01
影响因子：
11.4
通讯作者：
Jianxin Nie;Jian-Yu Zou;Shuwen Yan;Weihua Song
中科院分区：
文献类型：
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作者：
Jianxin Nie;Jian-Yu Zou;Shuwen Yan;Weihua Song
通过过一硫酸盐 (PMS) 活化的硫酸根 (SO4•-) 介导的高级氧化过程已得到广泛研究。然而，之前尚未研究过阳光照射下的溶解有机物 (DOM) 溶液中 PMS 的光转化。首次观察到模拟太阳照射下富含 DOM 的溶液中 PMS 的光敏转化。通过电子顺磁共振证实了活性物质（包括 1O2、SO4•- 和•OH）的生成，并通过化学探针进行了定量。 SO4•- 是激发三重态 DOM (3DOM*) 与 PMS 反应生成的主要反应物种。 3DOM* 作为反应性还原剂，被 PMS 快速氧化，估计反应速率常数为 (4.09 ± 0.21) × 108 M-1 s-1。与3DOM*相比，单电子还原DOM (DOM•-)对PMS光敏转化的贡献较小，并且DOM•-的贡献依赖于酚类成分。此外，一系列不同类型的 DOM，包括陆地 DOM、本土 DOM 和污水有机物及其组分，被用来研究 PMS 的光敏转化动力学。总体而言，通过辐照 DOM 进行的 PMS 光敏转化可能是在环境相关条件下产生 SO4•- 的一种有用且经济的方法。
Sulfate radical (SO4•-)-mediated advanced oxidation processes via peroxymonosulfate (PMS) activation have been extensively investigated. However, the phototransformation of PMS in sunlit dissolved organic matter (DOM) solution has not been previously examined. For the first time, the photosensitized transformation of PMS in DOM-enriched solutions under simulated solar irradiation was observed. The generation of reactive species, including 1O2, SO4•-, and •OH, was confirmed by electron paramagnetic resonance and quantified by chemical probes. SO4•- was the primary reactive species generated via the reaction of excited triplet DOM (3DOM*) with PMS. 3DOM* acted as a reactive reductant and was quickly oxidized by PMS, with an estimated reaction rate constant of (4.09 ± 0.21) × 108 M-1 s-1. Compared to 3DOM*, one-electron-reducing DOM (DOM•-) was a minor contributor to the photosensitized transformation of PMS, and the contribution of DOM•- relied on the phenolic constituents. In addition, a series of different types of DOM, including terrestrial DOM, autochthonous DOM, and effluent organic matter and its fractions, were employed to examine the photosensitized transformation kinetics of PMS. Overall, the photosensitized transformation of PMS by irradiated DOM could be a useful and economical approach to generate SO4•- under environmentally relevant conditions.