C3N4 表面金属有机光催化剂的合成及其光催化产氢性能的研究

At present, partly due to the structure and active reaction-site is not clear, the development of C3N4 based heterogeneous photo-catalyst always employ semi-empirical method by the synthesis of composite heterojunction. This project is aim to design the C3N4 based photo-catalyst “from bottom to top” with the surface organometallic chemistry strategy, focus on the research of the C3N4 surface structure and chemical property, take the advantage of plenty of amino group which can be grafted existing on the C3N4 surface, establish the way to introduce single-molecule level organometallic catalysis active site onto the C3N4 surface, turn the photon-generated carrier shift between the C3N4 and the hydrogen evolution active site into intramolecular by directly connecting these two parts by covalent bond. A series of new C3N4 photo-catalysts can be prepared with different ligands, active metal catalysis species and C3N4 material. By screening the hydrogen evolution properties of these catalysts, the relationship between the function and the structure can be mapped and help to produce high efficiency photo catalyst. The research will develop cheap,high efficiency and environmental friendly C3N4 photo-catalysts, and provide valuable solutions for the reaction mechanism, catalysis efficiency improvement, cost cutting of C3N4 photo-catalysts.

针对目前C3N4光催化剂开发普遍使用复合异质结的半经验方法，结构及活性反应位点不是很明确的现状，本项目将利用表面金属有机化学的理念，实现准分子的C3N4光催化剂的设计开发。重点研究C3N4材料表面的结构、化学性质，基于这一有机聚合物材料表面具有大量可接枝氨基的性质，建立在C3N4材料表面引入单分子级别的金属有机催化中心的方法，将C3N4与电产氢单元通过共价键进行直接连接，实现光生电子从C3N4到电产氢催化中心的分子内迁移。通过使用不同的配体、金属产氢中心及C3N4材料设计并合成一系列光产氢催化剂，考察并优化其光催化产氢性能。开发出廉价、高效、环保的C3N4光催化剂，并为解决C3N4光催化剂催化效率、反应机制、应用成本等方面问题提供有效途径。

针对目前光催化剂及电催化剂开发普遍使用半经验方法，结构及活性反应位点不明确的现状，本项目将利用表面金属有机化学的理念，实现准分子的C3N4光催化剂及电催化剂的设计开发。重点研究C3N4材料及其它基底材料表面的结构、化学性质，基于基底材料表面具有大量可修饰基团的性质，建立在基底材料表面引入单分子级别的金属有机催化中心的方法，将C3N4与电产氢单元通过共价键进行直接连接，实现光生电子从C3N4到电产氢催化中心的分子内迁移。通过在基底上引入不同电催化活性中心，还可以优化其电催化性能。通过使用不同的配体、金属产氢中心及C3N4材料设计并合成一系列光产氢催化剂，考察并优化其光催化产氢性能。开发出廉价、高效、环保的C3N4光催化剂，并为解决C3N4光催化剂催化效率、反应机制、应用成本等方面问题提供有效途径。