配体介导强化多相芬顿氧化去除EDCs及其微界面机制

The catalytic oxidation and removal of organic micro-pollutants in heterogeneous Fenton system could be significantly enhanced by certain concomitant organic ligands. However, due to the lack of understanding of micro-interface mechanism in ligand-mediated heterogeneous Fenton system, it is still difficult to utilize and regulate the function of ligands, and restrict the development and application of heterogeneous Fenton process in practice. Based on the knowledge that organic ligand could enhance oxidation rate of pollutants in homogeneous Fenton as electron transfer mediator, the present project proposed using natural ligand to enhance the oxidation for EDCs removal in the heterogeneous Fenton system. This project will focus on the effects of natural organic ligands (NOL) on the kinetics of EDCs removal in heterogeneous Fenton catalytic system, investigate the removal and transformation of EDCs and NOL and the reaction mechanism, evaluate the removal efficency of high risk precusors in the NOL-EDCs complex matrix, reveal the mechasnim of ligand-mediated strengthening effect, clarify the structure-activity relationship between the structure characteristics and complexation properties of NOL and the role of NOL in catalytic oxidation. Therefore, expand the fundamental understanding of heterogeneous Fenton oxidation technology, and provide critical theorietical basis and technical support for establishment and development of health risks control-based innovative water purification process and technology.

有机配体的介导作用可以显著强化多相芬顿体系对水中微污染有机物的氧化去除，但限于对多相体系中微界面反应机制认识的不足，还不能很好利用和调控配体介导对有机物去除的强化作用，制约了多相芬顿技术的发展应用。基于有机配体作为电子转移介质可加速均相芬顿反应氧化速率的认识，本项目提出利用天然有机配体介导的方法强化多相芬顿氧化微污染有机物EDCs的氧化效能，针对天然有机配体对EDCs多相芬顿催化氧化动力学的影响，深入研究EDCs和天然有机配体在多相芬顿催化氧化过程中的转化去除和作用机制，评价氧化过程对天然有机配体-EDCs复合污染体系中高风险前体物的净化效能，揭示多相芬顿体系中配体介导的强化作用机制，阐明天然有机配体结构特征和络合特性与其多相芬顿氧化强化作用功能间的构效关系，拓展多相芬顿氧化技术的应用基础理论，为构建基于健康风险控制的水处理新工艺和技术发展提供关键的理论依据和技术支持。

本项目围绕配体对多相芬顿氧化系统的影响作用开展研究，研究多相芬顿催化氧化过程中高活性自由基生成的微界面反应机制。以铁基材料为基础，研究了还原铁粉、铁氧化物和铁铜、铁锰、铁钌等双金属氧化物对过氧化氢和过硫酸盐的活化分解产自由基的能力，以红霉素和四环素等具有内分泌干扰效应的抗生素为目标有机物，系统地研究了催化剂表面性质、有机物特性、以及共存配体对于多相芬顿反应的影响和机制。针对有机物在多相芬顿体系中催化氧化的动力学，分析识别发挥主要作用的活性氧物种形态，提出了有机物可能的降解历程和主要的降解产物，并对降解前后生成消毒副产物的情况进行了探究。研究结果为拓展多相芬顿氧化技术的应用基础理论提供了支持。