金属-有机聚合体络合物构建与多相类芬顿催化水净化机理

In view of the degradation of the refractory organic pollutants in water and the application bottlenecks of the classical Fenton technology, this project breaks through the classical Fenton mechanism and proposes to develop transition-metal compounds-organic polymer complexes to accelerate the interfacial electron transfer, resulting in the direct contact of metal ions and H2O2 being no longer a necessary condition for the Fenton reaction. A new Fenton-like system based on the developed transition-metal compounds-organic polymer complexes will be established to degrade the typical refractory organic pollutants such as pesticides, pharmaceuticals and endocrine disrupting chemicals in water. The interaction of catalyst, pollutants and H2O2 will be studied thoroughly to reveal the interfacial electron transfer rules and the micro-interfacial reaction processes, which can provide the theoretical foundation for developing new heterogeneous Fenton-like catalyst. Finally, we will investigate the degradation kinetics of the Fenton-like system, optimize the reaction conditions and establish an efficient fixed Fenton-like water treatment system in pilot scale to provide technical support for the removal of refractory organic pollutants.

本项目针对水中难降解有机污染物的去除和经典芬顿技术的应用瓶颈问题，提出通过构建过渡金属化合物-有机聚合体络合物加速界面电子传输，突破经典芬顿反应原理，使过氧化氢与金属离子直接接触不再是催化反应进行的必要条件。进而基于过渡金属化合物-有机聚合体络合物建立新型类芬顿催化体系处理水中典型的难降解有机污染物如农药、医药和内分泌干扰素。深入研究催化剂、污染物以及过氧化氢三者的相互作用机制，揭示其界面电子迁移转化规律和污染物的界面微观反应过程，为新型多相芬顿催化剂的研制提供依据。最后考察体系降解动力学过程，优化此多相芬顿催化反应工艺，建立高效类芬顿固定床水处理系统，为难降解有机污染物去除提供技术支撑。

本项目针对水中难降解有机污染物的去除和经典芬顿技术的应用瓶颈问题，基于Cu、Fe、Co、Mo和V等不同物种构建过渡金属化合物-有机聚合体络合物加速界面电子传输，突破经典芬顿反应原理，通过构建和强化“金属阳离子-π”相互作用，实现了不同类型污染物供电子和溶解氧得电子联动效应，显著降低了类芬顿水处理中的H2O2消耗。并深入研究了催化剂、污染物、H2O2和溶解氧之间的相互作用过程，揭示了界面电子迁移转化规律和污染物降解机制。最后基于优化的催化剂建立了高效类芬顿固定床水处理中试系统，为新型多相芬顿催化剂的研制和应用提供了技术支撑。在Environ. Sci. Technol.、Appl. Catal. B-Environ.、J. Hazard. Mater.等权威学术期刊总共发表高水平SCI论文18篇，其中1篇已成为ESI高被引论文，获得授权发明专利3项。