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Permanganate activation with Mn oxides at different oxidation states: Insight into the surface-promoted electron transfer mechanism
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2023-05-30 , DOI: 10.1016/j.jhazmat.2023.131746
Lu Ma 1 , Wenqiang Gong 2 , Qinghong Wu 2 , Xiong Zhou 2 , Shuaiqi Zhao 2 , Aimal Khan 2 , Xiaoxia Li 2 , Aihua Xu 1
Affiliation  

The development of new strategies to improve the removal of organic pollutants with permanganate (KMnO4) is a hot topic in water treatment. While Mn oxides have been extensively used in Advanced Oxidation Processes through an electron transfer mechanism, the field of KMnO4 activation remains relatively unexplored. Interestingly, this study has discovered that Mn oxides with high oxidation states including γ-MnOOH, α-Mn2O3 and α-MnO2, exhibited excellent performance to degrade phenols and antibiotics in the presence of KMnO4. The MnO4- species initially formed stable complexes with the surface Mn(III/IV) species and showed an increased oxidation potential and electron transfer reactivity, caused by the electron-withdrawing capacity of the Mn species acting as Lewis acids. Conversely, for MnO and γ-Mn3O4 with Mn(II) species, they reacted with KMnO4 to produce cMnO2 with very low activity for phenol degradation. The direct electron transfer mechanism in α-MnO2/KMnO4 system was further confirmed through the inhibiting effect of acetonitrile and the galvanic oxidation process. Moreover, the adaptability and reusability of α-MnO2 in complicated waters indicated its potential for application in water treatment. Overall, the findings shed light on the development of Mn-based catalysts for organic pollutants degradation via KMnO4 activation and understanding of the surface-promoted mechanism.



中文翻译:

不同氧化态的锰氧化物的高锰酸盐活化:深入了解表面促进的电子转移机制

开发新策略以提高高锰酸盐(KMnO 4)去除有机污染物的效果是水处理领域的热门话题。虽然Mn氧化物已通过电子转移机制广泛用于高级氧化过程,但KMnO 4活化领域仍然相对未经探索。有趣的是,这项研究发现,高氧化态的锰氧化物,包括γ-MnOOH、α-Mn 2 O 3和α-MnO 2 ,​​在KMnO 4存在下表现出优异的降解酚类和抗生素的性能。MnO 4 -Mn(III/IV)物质最初与表面Mn(III/IV)物质形成稳定的络合物,并且由于Mn物质作为路易斯酸的吸电子能力而表现出增加的氧化电位和电子转移反应性。相反,对于MnO和γ-Mn 3 O 4与Mn(II)物质,它们与KMnO 4反应生成cMnO 2,​​其苯酚降解活性非常低。通过乙腈的抑制作用和电偶氧化过程进一步证实了α-MnO 2 /KMnO 4体系中的直接电子转移机制。此外,α-MnO 2的适应性和可重复使用性复杂水域的研究表明其在水处理中的应用潜力。总体而言,这些发现揭示了通过 KMnO 4活化降解有机污染物的锰基催化剂的开发以及对表面促进机制的理解。

更新日期:2023-06-03
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