From pollutant to chemical feedstock: Valorising anthropogenic carbon dioxide using carbon nitride-based architectures as powerful photocatalysts

该项目的目标是开发基于聚合物氮化碳(g-C3N4)的结构，通过结构调制、碳量子点敏化和分子氧化还原催化剂的异质结构建，具有定制的光学和光氧化还原性能。该项目旨在研究定制g-C3N4材料界面上导带和价带边缘位置的变化以及光生载流子的转移动力学。该项目还旨在探索基于g-C3N4的结构在有机合成中直接激活和利用二氧化碳的光催化潜力，并研究二氧化碳作为直接或间接氧化剂和羧化剂的作用。为了实现这些目标，各种分析、电化学、光电化学、时间分辨光谱和机理研究将被用来确定影响载流子动力学、分离、复合过程和催化剂周转的因素。该项目的成果有望推进有机合成中基于g-C3N4的结构的二氧化碳光还原和固定的知识，并为可见光响应型g-C3N4结构提供新的设计规则。

The objectives of this project are to develop polymeric carbon nitride (g-C3N4)-based architectures with tailored optical and photoredox properties through structural modulation, sensitization with carbon quantum dots, and heterojunction construction with molecular redox catalysts. The project aims to investigate the alteration of conduction and valence bands' edge positions and the transfer kinetics of photo-generated carriers at interfaces of tailored g-C3N4 materials. The project also aims to explore the photocatalytic potential of g-C3N4-based architectures towards direct CO2 activation and utilization in organic synthesis and investigate CO2 as a direct or indirect oxidant and carboxylative agent. To achieve these objectives, various analytical, electrochemical, photoelectrochemical, time-resolved spectroscopic, and mechanistic studies will be employed to determine the factors affecting charge carriers' dynamics, separation, recombination process, and catalytic turnover. The project's outcomes are expected to advance the knowledge of g-C3N4-based architectures for CO2 photoreduction and fixation in organic synthesis and provide novel design rules for visible light-responsive g-C3N4-based architectures.