钯/石墨烯-导电聚合物/泡沫钛电极的研制及其对卤代PPCPs电催化脱卤机制研究

The control and elimination of the adverse effects of halogenated pharmaceuticals and personal care products (PPCPs) on environment and human health is a matter of great urgency. Electrocatalysis has received much attention in water treatment due to the high efficiency and less by-product. Bad dispersion of catalyst, low electrocatalytic activity and poor stability are the critical problems that restrict the further development of electrocatalysis. The present study aims to eliminate the halogenated organic pollutants from water environment and focuses on the improvement of catalyst dispersion and on the enhancement of stability and activity of electrode. The preparation of palladium/graphene-conducting polymer/titanium foam electrode and electrocatalytic dehalogenation mechanism of typical halogenated PPCPs are studied. The internal relations between microstructure of electrodes and electrocatalytic activity are established. The optimization strategies for electrode structures are proposed. Based on the kinetics study, internal relations among electrocatalytic conditions, electrode microstructure and electrocatalytic performance are analyzed. The interface reaction mechanism and the control strategies for electrocatalytic system are proposed. In addition, electrocatalytic mechanism of halogenated PPCPs is put forward, according to the study of the pathways and kinetics of halogenated PPCPs with different structures and organics structures calculations based on Density Functional Theory. The fulfilling of this proposal has great significance in the reduction of harm of toxic halogenated organics to environment and human.

控制和消除卤代药物与个人护理品（PPCPs）对环境和人类的影响刻不容缓。电催化还原法处理卤代有机物，反应易于控制且副产物少，在水处理领域有良好应用前景。电极上催化金属分散性差、电极活性不高、稳定性差是制约其发展的关键问题。本项目以解决水体中卤代有机物污染问题为目标，以提高电极表面催化剂分散性和电极活性与稳定性为出发点，研究具有高催化活性的新型钯/石墨烯-导电聚合物/泡沫钛电极的制备和对卤代PPCPs电催化去除机制。建立电极微观结构与电催化活性和稳定性之间的构效关系，形成电极结构优化策略；在动力学研究基础上，解析电催化条件、电极结构与电催化脱卤的内在联系，阐明污染物在钯修饰电极上界面反应机制，提出电催化体系控制策略；研究不同结构卤代PPCPs反应路径及动力学，并基于密度泛函理论计算物质结构，阐明卤代PPCPs电催化去除机制。本项目的实施，对控制高毒性卤代有机物对环境和人类的危害具有重要意义。

本项目基于解决水体中卤代有机物污染问题，以提高电极表面催化剂分散性和电极活性与稳定性为出发点，可控构筑了高催化活性的新型钯/石墨烯-导电聚合物/泡沫钛和钯/石墨烯-导电聚合物/泡沫镍复合电极，并重点研究了聚合电位和吡咯浓度对复合电极结构和效能的影响规律；建立了电极微观结构与电催化活性和稳定性之间的内在联系，形成电极结构优化策略；在动力学研究基础上，研究了电催化条件如反应温度、电流强度和污染物初始浓度与电催化体系脱卤效能的关系；提出了水中典型卤代PPCPs电催化去除机制。本项目的研究结果为电催化还原法处理水中卤代有机物的研究提供基础数据和理论依据，对控制高毒性卤代有机物对环境和人类的危害具有重要意义。在完成上述研究内容的过程中，项目组已发表SCI收录论文8篇，培养硕士研究生6名，完成了项目的预期目标，并在此基础上开展了一些项目后期的探索性工作。