CO2还原二维层状复合光催化剂的构建与机理研究

Design and fabrication of highly efficient CO2-reduction photocatalysts are one of photocatalytic research leading edge and hotspot. On the basis of the progress of international photocatalytic research, the previous investigation work and results of our group, and the principle of chemical thermodynamics and kinetics, a new research program is proposed, which mainly focuses on the design and fabrication of photocatalytic CO2 reduction two-dimensional layered composite photocatalysts and systems by solvothermal and hydrothermal methods. These photocatalytic CO2 reduction materials are two-dimensional layered composites of g-C3N4, graphene, metal sulfide and bismuth-based oxides. The composition-thickness-morphology-performance intrinsic relationship and synergistic effect among g-C3N4, graphene, metal sulfide and bismuth-based oxide photocatalysts will be carefully investigated and discussed. The transfer and separation mechanism of photogenerated electrons and holes within two-dimensional layered composite photocatalysts under light irradiation will also be investigated and discussed. The design principal of composition and structure of two-dimensional layered composite photocatalysts will be developed and proposed by this project. The relationship among composition, thickness, microstructure, and CO2-reduction performance, and control methods of the two-dimensional layered composite photocatalyst will be revealed by this project. To improve the CO2 reduction to solar fuel efficiency, the intrinsic cause, synergistic mechanism and control principle of the photocatalytic CO2 reduction will be carefully investigated and explained. This is of great significance in promoting the development of photocatalytic theory and increasing new knowledge of photocatalytic CO2 reduction to solar fuel production. This investigation will also provide new insight into the design and fabrication of two-dimensional layered composite photocatalysts for CO2 reduction to solar fuels.

高效光催化CO2还原材料体系的设计与构建是光催化领域的研究前沿和热点。项目根据国际最新研究动态,并结合我们的研究积累和前期工作基础，基于化学热力学和动力学原理，提出通过溶剂热和水热化学方法制备g-C3N4和石墨烯与硫化物、铋基氧化物二维层状复合光催化CO2还原材料；研究g-C3N4、石墨烯、硫化物、铋基氧化物二维层状复合光催化材料的组成、厚度及形貌与光催化CO2还原活性之间的内在关系、协同效应和光生载流子转移分离机理，以发展新型二维层状复合光催化CO2还原材料的组成和结构设计原理、揭示二维层状复合光催化剂组成-厚度-结构-CO2还原性能的构效关系和调控方法，阐明二维层状光催化过程的微观机理、协同作用和调控规律，以提高光催化CO2还原制备太阳燃料效率为研究目标，为新型高效光催化CO2还原材料体系的构建提供理论基础和科学依据，通过本项目研究可以丰富光催化CO2还原材料的制备方法和材料体系。

项目执行期间通过溶剂热和水热化学等方法制备了g-C3N4和石墨烯与硫化物、铋基氧化物二维层状复合光催化CO2还原材料；研究了g-C3N4、石墨烯、硫化物、铋基氧化物二维层状复合光催化材料的组成、厚度及形貌与光催化CO2还原活性之间的内在关系、协同效应和光生载流子转移分离机理，发展了新型二维层状复合光催化CO2还原材料的组成和结构设计原理、揭示了二维层状复合光催化剂组成-厚度-结构-CO2还原性能的构效关系和调控方法，阐明了二维层状光催化过程的微观机理、协同作用和调控规律，提高了光催化CO2还原制备太阳燃料效率，为新型高效光催化CO2还原材料体系的构建提供了理论基础和科学依据，项目研究丰富了光催化CO2还原材料的制备方法和材料体系。多篇研究论文发表在多种国际刊物上，如：Adv. Mater.、Mater. Today、Adv. Funct. Mater.、Small、Appl. Catal. B等，发表SCI 收录论文79篇，发表论文中有ESI高被引论文29篇，发表论文被SCI他人引文4300余次。项目执行期间所在课题组共毕业了11位博士研究生和9位硕士研究生, 出站博士后4人。研究成果获得湖北省自然科学一等奖1项(排名第三)，项目负责人入选2019年全球化学学科高被引研究人员名单。