构筑"限域型"多孔碳/非均相芬顿催化剂及其可见光"增效"降解水中新兴有机污染物的机制研究

This project aims at the application of visible light-assisted heterogeneous Fenton process to study the degradation performance and mechanism of emerging organic contaminants (EOCs) in waterborne. We plan to construct a series of porous carbon/heterogeneous Fenton catalysts in which the metal (hydro)xides were confined within the porous networks and the obtained catalysts can adsorb and be activated by visible light. We plan to systematically study the preparing methods, visible light photo-assisted heterogeneous Fenton process. We plan to study the physical and chemical properties of the interface, the photo-generated charge transfer, and then solve the bottleneck problems that restricts the catalytic process of the traditional heterogeneous Fenton. The porous carbon carriers will be prepared by the hard/soft template strategy. The transition metal based (hydro)xides (such as iron compounds) are designed and confined in the porous carrier, and the interface is controlled to form a stable composite structure with effective coupling at the nanometer scale. The project mainly includes three parts: 1) design and controllable preparation of porous carbon/heterogeneous Fenton catalyst with "confinement effect "; 2) several selected porous carbon/heterogeneous Fenton catalysts for structural analysis, interfacial charge transfer mechanism and catalytic reaction process characterizations; 3) systematically studying the degradation efficiency of EOCs by visible light assisted heterogeneous Fenton process and the catalytic kinetics of hydrogen peroxide. The above basic research provides important research basis and theoretical guidance for the research and development of new heterogeneous Fenton catalyst and the utilization of solar energy in advanced oxidation technology.

本项目针对水中新兴有机污染物（EOCs），拟采用可见光"增效"非均相芬顿过程，研究污染物的降解机制和催化剂失活机理。通过构筑具有可见光响应的"限域型"多孔碳/非均相芬顿催化剂，系统研究催化剂制备、光辅助"增效"非均相芬顿反应过程机理，旨在解决制约传统非均相芬顿催化过程的瓶颈问题。采用软硬模板法制备多孔碳基载体，设计合成以铁基过渡金属（水合）氧化物"限域"在多孔载体内，调控界面生长，形成在纳米尺度有效耦合的稳定复合结构。项目研究内容主要涵盖三部分：1）"限域型"多孔碳/非均相芬顿催化剂的设计、结构可控制备；2）优选出若干催化剂进行结构分析、界面电荷传递机理及催化反应过程表征；3）系统研究催化剂光辅助非均相芬顿降解EOCs的反应活性，双氧水催化分解动力学以及光辅助"增效"催化降解机制与催化剂失活机理。以上研究将为新型非均相芬顿催化剂的开发及其在高级氧化技术中的应用提供理论支持。

本项目针对水中新兴有机污染物（EOCs）的去除，围绕传统芬顿反应过程铁泥二次污染问题，开发了多种非均相芬顿材料，并针对材料性质分别研究了暗反应过程铁离子循环机理以及可见光"增效"非均相芬顿过程。分别围绕4种非均相材料开展研究，包括非金属基和铁、锰基材料，非均相芬顿材料具有与均相芬顿试剂相当或更佳降解性能，操作pH 值条件范围较宽；其中研发的一种纳米碳点胶体材料已经进行模型装置测试，具有高于芬顿试剂的性能；用于实际多环芳烃污染土壤的化学氧化以及传质测试，发现纳米碳胶粒在土壤中具有良好的扩散能力，较芬顿试剂能显著提高化学氧化去除多环芳烃的性能。光照条件下，研究了非金属基多孔碳三氮四和介孔碳-铁离子的类芬顿反应，分别揭示了光生载流子活化过硫酸盐产生优势活性氧化剂物种以及铁离子与介孔碳含氧基团形成的配合物结构光生电子促进铁离子循环的机制。