非贵金属助催化剂/g-C3N4复合光催化材料的可控液相合成与产氢性能

Research into the development of high-performance and cost-effective visible light active photocatalyst is a hot topic, attracting the attention from scientific community. In the viewpoint of solving the problems including fast photogenerated electron–hole recombination of g-C3N4 and high cost of noble metal-based co-catalysts, this project aims to utilize metalliferous phosphide and other earth-abundant materials as co-catalyst for surface modification of g-C3N4. Moreover, this project will focus on the deposition mechanism of co-catalyst on the surface of g-C3N4, as well as the charge carrier separation and transportation between them. The corresponding hydrogen evolution performance and the concluded performance-strengthening approach will also be comprehensively studied. Furthermore, the effect of preparation procedure of g-C3N4, and class, size and loading content of co-catalyst on the photocatalytic hydrogen revolution performance of the g-C3N4 will be also systematically investigated. The interaction and synergistic effect between g-C3N4 and economic co-catalyst with different sizes, morphologies and nanostructures will also be revealed. The method for in-situ deposition of co-catalyst on the surface of g-C3N4 will be also proposed. In addition, the detailed photocatalytic enhancement mechanism of co-catalyst modified g-C3N4 for hydrogen production will also be elucidated. Finally, low-cost g-C3N4 based composite with high photocatalytic hydrogen revolution performance can be developed, accelerating the practical application of this technology.

合成高效廉价可见光催化分解水制氢材料体系是光催化领域备受关注的研究热点。针对g-C3N4自身光生电子与空穴容易复合以及贵金属助催化剂价格昂贵的关键科学问题，项目拟利用金属磷化物等地球丰富的材料作为助催化剂对g-C3N4进行表面改性，重点研究助催化剂在g-C3N4表面的沉积原理与合成方法，g-C3N4与助催化剂之间光生载流子分离、传输与催化产氢行为，助催化剂/g-C3N4复合光催化材料产氢速率增强方法。探索g-C3N4制备方法与厚度，助催化剂种类、颗粒大小与比例对g-C3N4光催化产氢活性的影响规律，揭示光催化剂g-C3N4与廉价助催化剂的颗粒大小、形貌、微纳结构与产氢性能的关系和协同效应，建立助催化剂在g-C3N4表面原位沉积的制备方法，阐明助催化剂修饰的g-C3N4光催化产氢活性增强机理。开发出具有自主知识产权廉价的高性能g-C3N4基复合产氢光催化材料，推动光催化制氢材料的实际应用。

项目按照申请时的计划执行，针对g-C3N4自身光生电子与空穴容易复合以及贵金属助催化剂价格昂贵的关键科学问题，利用助催化剂和其他半导体材料分别与g-C3N4复合制备了一系列新型g-C3N4基复合光催化材料。深入考察助催化剂和其他半导体材料与比例g-C3N4以及g-C3N4厚度等构建单元要素对催化剂微观结构、界面性质和能带结构的影响规律；系统研究催化剂构建单元与反应参数（如催化剂浓度、牺牲剂种类、反应pH值及温度）在可见光下光解水制氢性能的协同影响规律；揭示光解水制氢过程中界面光生载流子的迁移规律、催化反应机制以及动力学与热力学过程，阐明g-C3N4基复合光催化材料产氢活性增强机理。开发出具有自主知识产权廉价的高性能g-C3N4基复合产氢光催化材料，推动光催化制氢材料的实际应用。