铜基固相芬顿催化剂的研制及其去除污染物机制

Based on the current progress of Fenton treatment technology, this project focuses on the preparation of Cu+/Cu2+-containing Fenton catalysts to remove toxic organic pollutants in water under natural conditions. Cu+ and Cu2+ will be combined in the framework of mesoporous materials, and their forms in the structure will be controlled to accelerate the electron circulation of Cu+/Cu2+, the stability of the catalysts and the generation efficiency of •OH. And the studies will investigate the degradation kinetics and reaction mechanism to remove refractory organic pollutants (i.e., pesticides and pharmaceuticals). We will try to demonstrate the relationship between the existence forms of copper and the electron circulation of Cu+/Cu2+, the existence forms of copper and the degradation efficiency of organic pollutants. The above research helps to explore the heterogeneous Fenton catalysts with high activity and stability. Further, the effect of various factors on Fenton reaction efficiency will be investigated to optimize the reaction process and finally build an efficient Fenton fixed-bed treatment system, to provide theoretical basis and technical support for the practical application of heterogeneous Fenton oxidation technology.

针对水中难降解有机污染物的去除问题，基于当前多相芬顿催化发展的状况，本项目提出研制Cu+和Cu2+复合固相芬顿催化剂，将Cu+和Cu2+共同螯合于中孔材料的骨架结构中，调控其存在形态，加速Cu+/Cu2+电子循环，提高催化剂的稳定性和H2O2分解产生•OH的效率。重点处理水中典型难降解有机污染物（农药和医药品），研究其降解动力学和反应机制，揭示催化剂结构中铜的化学形态对Cu+/Cu2+电子循环作用规律，及其与有机污染物降解效率的关系，为新型高效多相芬顿催化剂的制备提供依据。考察不同因素对芬顿反应效率的影响，优化反应工艺，建立高效芬顿固定床水处理系统，为多相芬顿催化氧化技术实际应用提供理论依据与技术支持。

针对水中难降解有机污染物的去除问题，基于多相芬顿催化剂的发展现状，本项目以介孔氧化铝、蒲公英状二氧化硅纳米球、磷酸铝分子筛、铝酸镧等孔材料为基体，通过原位掺杂的方式获得了Cu+和Cu2+在骨架结构中共存的铜基固相芬顿催化剂，在中性室温条件下对不同有机污染物显示出很高的催化去除效果，H2O2利用率大幅提高。研究了催化剂、H2O2及有机污染物之间的相互作用机制，揭示了催化剂结构中铜的化学形态对Cu+/Cu2+电子循环过程的影响，阐明了骨架铜与不同有机污染物的作用规律，证实了骨架铜有机络合和原位掺杂产生的氧空位作用促使H2O2有效分解产生羟基自由基，为多相芬顿催化剂的发展提供了理论依据和技术支持。进一步建立了铜基固定床反应器，实现了对水中农药、医药品等不同有机污染物的高效降解和稳定连续去除，具有很好的应用前景。相关研究结果目前已经发表SCI论文11篇（平均影响因子7.122），中文核心期刊论文1篇，申请发明专利1项。