可见-近红外光响应铜硫化物/氮化碳复合光催化剂的构筑及其性能研究

The development of photocatalysts with high quantum efficiency and high solar energy utilization ability is the important and difficult point of photocatalytic technology. To solve the problems of serious recombination of photogenerated charge carriers and insufficient absorption of near-infrared light of carbon nitride polymer, this project will be focused on controlling the composition, morphology and band structure of carbon nitride and copper sulfide, as well as constructing the copper sulfide/carbon nitride composite photocatalysts with near-infrared plasmon resonance effect. These strategies will enhance the absorption ability of visible and near-infrared light, and promote the separation of photogenerated charge carriers in order to construct photocatalytic systems with high efficiency and wide spectral response. The controllable preparation method of copper sulfide and carbon nitride composite photocatalysts will be explored, and their photocatalytic activities in water splitting and organic synthesis reaction (Suzuki coupling and selective oxidation of benzyl alcohol) with visible and near-infrared light irradiation will be investigated. The effect of chemical composition, degree of copper defect, band structure, surface plasmon resonance effect, morphology and size on the separation efficiency of photogenerated charge carriers of the catalysts will be investigated. The interaction between copper sulfide and carbon nitride will be explored, the structure-activity relationship of catalysts will be revealed, and the mechanism of photocatalytic water splitting and organic synthesis will be elucidated. This project will provide theoretical guidance and experimental basis for the design and preparation of highly efficient and broad-spectrum photocatalysts.

开发具有高量子效率和高太阳能利用率的光催化剂是当前光催化研究的重点和难点。针对氮化碳聚合物光生载流子复合严重和近红外光吸收不足的问题，本项目拟通过对氮化碳和铜硫化物进行组成、形貌、能带调控，并构筑具有近红外等离子体共振效应的铜硫化物/氮化碳复合光催化剂，增强可见-近红外光吸收能力，促进光生载流子的分离，旨在构建高效宽光谱响应的光催化体系。探索铜硫化物与氮化碳复合光催化剂的可控制备方法，考察其在可见-近红外光下光催化分解水和有机合成反应（Suzuki偶联、苯甲醇的选择性氧化）的性能。研究催化剂的化学组成、铜缺陷程度、能带结构、表面等离子体共振效应、形貌尺寸对光生载流子分离效率的影响。探究铜硫化物和氮化碳之间的相互作用，揭示催化剂的构效关系，阐明光催化分解水和有机合成的机理，为高效宽光谱响应光催化剂的设计和制备提供理论指导与实验依据。

设计和开发具有高量子效率和高太阳能利用率的氮化碳聚合物光催化剂是当前光催化研究领域的核心任务。本项目采用多种方法对氮化碳聚合物进行光吸收与光生载流子动力学调控，设计和构筑可见-近红外光响应的异质结构光催化剂，并揭示其构效关系及反应机理。首先，通过采用共聚合法构筑电子给体-受体结构、超分子静电自组装法组建介孔薄壁纳米管、溶剂热法进行端氰基修饰等方式来实现氮化碳聚合物的光吸收性能与光生载流子动力学调控，阐述氮化碳聚合物的分子结构和纳米结构对光吸收性能及光生载流子分离效率的影响规律。其次，通过将氮化碳聚合物与具有近红外光吸收性能的窄带隙半导体复合来构建异质结构光催化剂，并利用等离子体共振效应和热电子注入方式，增强近红外光吸收性能并提高光生载流子分离效率。最后，阐明了可见-近红外光响应复合光催化剂的异质结构设计与光催化性能之间的内在联系，揭示了氮化碳聚合物及其复合材料的光催化分解水、二氧化碳还原和污染物降解反应机理，为开发高效宽光谱响应的光催化剂提供理论和实验依据。