金属基离子液体原位构筑表面浅电子陷阱卤化氧铋光子晶体及其增强光催化降解抗生素性能研究

In order to efficiently remove the novel antibiotics contaminants (such as tetracyclines and quinolones) in the water environment, three dimensionally ordered macroporous bismuth oxyhalides (BiOX, X = Cl, Br, I) photonic crystal photocatalysts with wide spectral response will be constructed. The influence rules of the interactions between functional colloidal template and ionic liquid on the morphology, optical adsorption properties and band-gap position of BiOX photonic crystal will be investigated. A high efficient photocatalytic system with dual enhancement of light absorption capacity and photo-induced carriers’ separation rate will be constructed by in-suit doping transition metal ions in the shallow lattice of BiOX photonic crystal. The photocatalytic performance and mineralization path of the degradation of antibiotic contaminants by transition metal ions doped BiOX photonic crystal will be investigated. Further studies on the effect of surface electron traps on the photogenerated electron-hole pairs’ separation rate of BiOX photonic crystal materials and the revelation of the relationship between the generation and separation of electron-hole pairs and the structure and composition of the photocatalyst will be conducted. At the same time, the rules of building three dimensionally ordered macroporous structure and doping transition metal ions on the stability of BiOX photonic crystal will also be discussed. This project will provide a distinct insight for the preparation of noval efficient three-dimensional ordered porous BiOX photonic crystal materials, and a far-reaching significance for highly efficient mineralization and degradation of the antibiotics contaminants in the water environment.

本项目以难降解的四环素类、喹诺酮类新型抗生素环境污染物的高效光催化去除为目标，利用光子晶体光吸收能力强和能带可调的特性，构建宽光谱响应型三维有序多孔卤化氧铋光子晶体光催化材料体系。探究功能化胶晶模板与离子液体间的相互作用对卤化氧铋光子晶体形貌、光吸收特性和能带结构的影响规律。原位浅晶格掺杂过渡金属离子，构筑光吸收能力、光生载流子分离率双提升的高效光催化体系，探究过渡金属离子原位掺杂卤化氧铋光子晶体材料降解抗生素污染物的性能及矿化路径。深入研究表面电子捕获陷阱对提高卤化氧铋光子晶体材料光生电子空穴对分离率的作用规律，揭示光生电子空穴对的产生和分离与催化剂结构、组成之间的关系，分析三维有序多孔结构及过渡金属离子的掺杂对卤化氧铋光子晶体材料稳定性的影响规律。本研究将为新型高效的三维有序多孔卤化氧铋光子晶体材料的设计与制备提供新的思路，对高效矿化降解水体中抗生素污染物具有积极意义。

本课题主要围绕金属基离子液体原位构筑表面浅电子陷阱卤化氧铋光子晶体及其增强光催化降解抗生素性能研究。主要运用异质结构筑、缺陷调控、形貌调控及贵金属负载等改性策略来构筑高性能光催化材料。通过X射线衍射（XRD）、扫描电镜（SEM）、透射电镜（TEM）和电子自旋共振（ESR）等测试手段对所制备材料的结构与形貌进行了表征，并对其进行光催化性能探究。实验结果表明，所制备的材料均展现出较好的光催化活性，其中，超薄MoS2纳米片复合Bi5O7I纳米棒、超薄BiOBr纳米片和局部表面等离子体共振效应增强的W18O49/BiOBr异质结光催化剂表现出优异的光催化降解抗生素解性能；相比于BiVO4，二维g-C3N4/BiVO4材料表现出增强的光催化降解有机物性能；有序大孔BiOCl材料、Bi19S27Br3/BiOBr复合材料及金纳米颗粒修饰的Bi12O17Br2纳米管材料表现出较高的光催化CO2还原性能。此外，多孔超薄氮化碳材料表现出良好的光催化产氢性能。本课题通过多种调控策略，成功实现了高光催化性能光催化剂的设计与可控制备。研究了不同策略制备的光催化剂的活性增强机理，并结合材料的结构与光催化活性结果，阐述材料结构与性能间的构效关系。