Discerning the Relevance of Singlet Oxygen in Pollutant Degradation in Peroxymonosulfate Activation Processes,Environmental Science & Technology

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Discerning the Relevance of Singlet Oxygen in Pollutant Degradation in Peroxymonosulfate Activation Processes
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2024-07-22 , DOI: 10.1021/acs.est.4c02809
Hongchao Li ₁ , Xinyue Zhang ₁ , Shuai Yang ₁ , Yibing Sun ₁ , Jieshu Qian ₂

Affiliation

Significant efforts have recently been exerted toward construction of singlet oxygen (¹O₂)-dominated catalytic oxidation systems for selective removal of organic contaminants from wastewater, with peroxides serving as the chemical source. However, the relevance of ¹O₂ in the removal of pollutants remains ambiguous and requires elucidation. In this study, we scrupulously exclude the significant role of ¹O₂ in contaminant degradation in various peroxymonosulfate (PMS) activation systems. Multiple experimental results indicate that the activation of PMS catalyzed by CuO, MnO₂, Fe-doped g-C₃N₄ (Fe–CN), or N-doped graphite does not predominantly follow the ¹O₂ pathway. More importantly, the reactivity of ¹O₂ is remarkably overestimated in the literature, given its inferior capacity in degradation of a range of heterocyclic contaminants and aromatic compounds possessing electron-withdrawing groups. In addition, the strong physical quenching effect of water, coupled with the low oxidizing ability of ¹O₂, would notably reduce the utilization efficiency of peroxide, which is particularly apparent in the degradation of micropollutants. We reckon that this study is expected to end the long-running dispute associated with the relevance of ¹O₂ in pollutant removal.

中文翻译：

辨别单线态氧在过一硫酸盐活化过程中污染物降解中的相关性

最近，人们在构建以单线态氧（ ¹ O ₂ ）为主的催化氧化系统方面付出了巨大的努力，以过氧化物作为化学源，选择性地去除废水中的有机污染物。然而， ¹ O ₂在去除污染物方面的相关性仍然不明确，需要阐明。在本研究中，我们严格排除了¹ O ₂在各种过一硫酸盐 (PMS) 活化系统中污染物降解中的重要作用。多项实验结果表明，CuO、MnO ₂ 、Fe掺杂gC ₃ N ₄ (Fe-CN)或N掺杂石墨催化的PMS活化并不主要遵循¹ O ₂途径。更重要的是，文献中明显高估了¹ O ₂的反应性，因为它在降解一系列杂环污染物和具有吸电子基团的芳香族化合物方面能力较差。此外，水的强物理猝灭作用，加上¹ O ₂的低氧化能力，会显着降低过氧化物的利用效率，这在微污染物的降解中尤为明显。我们认为这项研究有望结束与¹ O ₂污染物去除相关性相关的长期争议。

更新日期：2024-07-22

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