可变活性中间价态锰在电化学阴极活化KMnO4的原位调控与水污染控制

自由态/固态活性中间价态锰可通过吸附、氧化还原和催化作用高效去除水中难降解有机物、重金属离子和耐药菌及其抗性基因等多种污染物。针对现有原位产生活性中间价态锰方法存在二次污染风险且无法对中间价态锰的价态、相态和形态结构进行灵活精准调控的局限性，提出通过电化学阴极活化KMnO4原位调控产生可变活性中间价态锰高效去除水中多种难去除特征污染物的新思路。探究固液界面自由态中间价态锰产生过程及价态调控机理；探索电场诱导Mn(VII)演变固态锰氧化物的组成变化规律及其结构、形貌精准构筑机制；基于对转化规律和调控原理的系统研究，揭示阴极材料通过表面作用和电化学机制协同活化KMnO4过程中存在的微观反应机理；并通过理论计算和对水中多种特征污染物去除试验，明确不同形态中间价态锰与其吸附、氧化及催化活性等物化特性之间的构效关系；最终为开发基于电化学调控可变活性中间价态锰的新型水污染控制方法提供理论和技术支持。

Free state/solid state active manganese intermediates can effectively remove a variety of pollutants such as refractory organics, heavy metal ions, antibiotic-resistant bacteria, and their resistance genes in water by adsorption, redox, and catalysis. However, the current methods to generate manganese intermediates have the drawback of secondary pollutants risk as well as inflexible and inaccurate control for the valence, phase, and morphological structure of the manganese intermediates. In view of the limitations of current methods to generate manganese intermediates in situ, we propose a novel idea of electrochemical reductive activation of KMnO4 to generate corresponding manganese intermediates with variable physicochemical property in situ to remove target pollutants with different character in water. The evolution process and control mechanism of free manganese intermediates at solid-liquid interface are suggested to be explored while the composition change rule and the accurate building mechanism of solid manganese oxide involved in the evolution of Mn(VII) induced by electric field are also suggested to be investigated. Then, based on the systematic study on the production, transformation, and adjust law of different manganese intermediates, the fundamental microcosmic reactions in the process of co-activation of KMnO4 by electrode materials surface and electrochemical mechanism are anticipated to be revealed. Moreover, the adsorption, redox, and catalytic properties of active manganese intermediates with different structure and interface characteristics were verified by theoretical calculation and removal test of various pollutants with different character in water. Finally, theoretical and technical supports for the development of a novel method for water pollution control based on electrochemical generation of variable active manganese intermediates are proposed.