光驱动原位产H2O2的共价键合的多酸/g-C3N4催化剂的构建

The iron containing-polyoxometalates (Fe-POMs) clusters have been covalent combined with graphitic carbon nitride (g-C3N4) to construct the covalent combined Fe-POMs/g-C3N4 catalysts for the degradation of typical antibiotics with light-driven in-situ H2O2 production. We will optimize the structure and composition of Fe-POMs/g-C3N4 catalysts, investigate the process of H2O2 production and the conversion of the formed hydroxyl radical (•OH), and reveal the mechanism for the degradation of typical antibiotics by Fe-POMs/g-C3N4 catalysts. Based on the above results, we will construct the POMs/g-C3N4 catalytic system with light-driven in-situ H2O2 production, the in-situ produced H2O2 can react with iron cations of POMs to produce the •OH, enhance the separation of photo-generated carriers and the oxidation ability of the photo-generated hole for photo catalytic oxidation process due to the energy level differences between POMs and g-C3N4; the photo-generated electron can increase the two electron reduction of O2 to H2O2 and the recycle of Fe3+/Fe2+ for Fenton oxidation process. The above processes jointly remove the typical antibiotics.

本项目以典型抗生素污染物为去除对象，采用有机连接基元共价修饰的方式，引入含铁多酸(Fe-POMs)构建共价键合的Fe-POMs/g-C3N4催化剂，在光驱动原位产H2O2的基础上，优化设计Fe-POMs/g-C3N4催化剂，详细研究H2O2的光驱动产生与•OH自由基生成及转化的过程，阐明Fe-POMs/g-C3N4催化剂去除典型抗生素污染物的途径与机理，构建基于光驱动原位产H2O2的共价键合的多酸/g-C3N4催化体系，利用原位产生的H2O2与多酸中的铁离子反应产生•OH自由基，同时多酸半导体由于能级差别，提高了g-C3N4基催化剂光催化氧化过程光生载流子的分离性能和光生空穴的氧化能力；光生电子也促进了O2双电子还原为H2O2的反应和Fe3+/Fe2+的循环过程，强化了Fenton反应过程。上述多过程使典型抗生素污染物得到了协同催化氧化去除。

本项目引入多酸(POMs)构建POMs/g-C3N4催化剂，在光驱动原位产H2O2的基础上，优化设计POMs/g-C3N4催化剂，详细研究H2O2的光驱动产生与活性物种生成及转化的过程，阐明POMs/g-C3N4催化剂去污染物的途径与机理，构建基于光驱动原位产H2O2的共价键合的POMs/g-C3N4催化体系，利用原位产生的H2O2与多酸反应产生活性物种，同时多酸半导体由于能级差别，提高了g-C3N4基催化剂光催化氧化过程光生载流子的分离性能和光生空穴的氧化能力；光生电子也促进了O2双电子还原为H2O2的反应，上述多过程使污染物得到了协同催化氧化去除。项目执行期间，共发表相关SCI收录论文7篇，申请专利2项。项目研究成果为污染物的高效去除提供基础性支持，也丰富了光催化氧化的净水理论。