碳质材料活化过氧化物的直接电子转移机制研究进展

Research Progress on the Direct Electron Transfer Mechanism of Carbon-Based Material Activated Peroxides

摘要:

基于过硫酸盐、过氧乙酸等过氧化物的高级氧化技术（AOPs）成为近年来水环境处理中的研究热点，其对于土壤及地下水水环境中多环芳烃（PAHs）等新型污染物的降解有着较高的效率。同时，碳质材料作为新兴的过氧化物活化体系中的电子穿梭体，也由于其高比表面积、有丰富的官能团、有多种改性方法以及在水环境修复中低成本、几乎无二次污染的优势而得到广泛的关注。碳质材料易在催化活化过氧化物时诱导产生非自由基途径，其中的直接电子转移非自由基机制相较于单线态氧、高价金属诱导氧化等是学者们研究较少的方向，该电子转移过程与碳质材料和过氧化物形成的亚稳态中间体密切相关。因此，结合相关研究，描述了不同维度碳质材料活化过氧化物的直接电子转移机制，并总结了该机制可能的吸附活性位点以及影响因素，为相关领域的研究提供理论基础。最后介绍了电子转移过程的表征方法（电化学方法、化学猝灭法等）并提出该体系目前存在的问题以及未来的发展前景，期望能为该体系更深层次的研究及更广范围的应用提供可行的思路与方法。

Abstract:

Advanced oxidation processes （AOPs） based on peroxides such as persulfate and peracetic acid have become a research hotspot in water environment treatment in recent years， and they have high efficiency for the degradation of new pollutants such as polycyclic aromatic hydrocarbons （PAHs） in soil and groundwater environments. Meanwhile， carbon-based materials， as electron shuttles in emerging peroxide activation systems， have also attracted extensive attention due to their high specific surface area， abundant functional groups， diverse modification methods， and advantages of low cost and minimal secondary pollution in water environment remediation. Carbon-based materials readily induce non-radical pathways during the catalytic activation of peroxides， and the direct electron-transfer non-radical mechanism has received far less scholarly attention than pathways involving singlet oxygen or high-valent metal-induced oxidation. This electron-transfer process is closely related to metastable intermediates formed between carbon-based materials and peroxides. Therefore， this paper describes the direct electron transfer mechanism of activated peroxides of carbon-based materials in different dimensions based on related studies， and summarizes the possible adsorption active sites and influencing factors of this mechanism， so as to provide a theoretical foundation for research in related fields. Finally， the characterization methods of the electron transfer process （electrochemical method， chemical quenching method） are introduced， and the current problems and future development prospects of the system are proposed， hoping to provide feasible ideas and methods for the deeper research and wider application of the system.