Co-ZIFs/g-CN复合光催化体系的构建及其还原CO2性能研究

Reducing CO2 to chemical materials with the photocatalytic technology is an ideal way to solve both energy and environmental problems. In view of the lack of design and regulation of photocatalysts for the adsorption and activation of CO2 molecules, this project proposes a new design idea to realize the effective conversion of CO2 by creating a new system that can simultaneously satisfy the high-efficiency supply and catalytic conversion of photo-generated charge. While modifying and modifying the photocatalyst, a heterogeneous cocatalyst with adsorption and activation function for CO2 will be designed and synthesized to improve the efficient conversion of CO2 in the system. It is proposed to select carbon nitride (g-CN) as a model photocatalyst, and to design a main integrated Co-ZIFs/g-CN with cobalt-based zeolitic imidazole ester three-dimensional porous framework (Co-ZIFs) as a promoter. The effects of Co-ZIFs/g-CN surface functional groups and pore structure on CO2 adsorption activation and kinetics will be investigated from the molecular and catalytic levels. The light absorption, charge separation and CO2 of Co-ZIFs/g-CN composite catalysts will be characterized. The interaction between Co-ZIFs cocatalyst and g-CN photocatalyst and the intrinsic relationship between catalyst structure and activity will be revealed, and the mechanism of Co-ZIFs/g-CN photocatalytic reduction of CO2 reaction will be elucidated.

利用光催化技术将CO2转化为化工原料是同时解决能源与环境问题的理想途径。本项目针对目前光催化剂对CO2分子吸附活化缺乏可设计性和调控性等问题，提出通过创建能同时满足CO2高效供给和催化转化光生电荷能力的新体系，来实现CO2有效转化的设计新思路，在对光催化剂进行修饰改性的同时，设计合成对CO2具有吸附活化性能的多相助催化剂，以实现体系CO2的高效转化。拟选择氮化碳(g-CN)作为模型光催化剂，以钴基沸石咪唑骨架(Co-ZIFs)为助催化剂，创建Co-ZIFs/g-CN复合光催化还原CO2新体系。从分子水平和催化层面上探究Co-ZIFs/g-CN表面官能团和孔结构对CO2吸附活化的影响及动力学规律，系统表征其光吸收、电荷分离及CO2吸附活化对CO2还原的影响，揭示Co-ZIFs与g-CN之间的相互作用及催化剂结构与活性间的内在联系，阐明Co-ZIFs/g-CN光催化还原CO2反应的作用机制。

利用光催化技术将CO2转化为化工原料是同时解决能源与环境问题的理想途径。针对目前光催化剂对CO2分子吸附活化缺乏可设计性和调控性等问题，本项目通过创建能同时满足CO2高效供给和催化转化光生电荷能力的新体系，即在对光催化剂g-C3N4、ZnIn2S4、LaPO4等进行修饰改性的同时，设计合成了对CO2具有吸附活化性能的助催化剂CoFeOX超薄纳米片和Pt纳米粒子，从而实现了体系CO2的高效转化。系统表征了催化剂结构、形态和比表面积等对CO2吸附活化的影响及动力学规律，从分子水平和催化层面上探索了催化剂光吸收、电荷分离及CO2吸附活化对CO2还原的影响，揭示了催化剂结构与活性间的内在联系，阐明了光催化还原CO2反应的作用机制。同时，我们还将目标反应扩展到了光（电）催化分解水以及光催化降解环境污染物等方面，均取得了良好的效果。.通过本项目资助，在国内外刊物 Nature Communications、Applied Catalysis B: Environmental、Chemical Engineering Journal、Journal of Energy Chemistry、Applied Surface Science等上发表论文10篇（其中SCI一区论文5篇），申请中国发明专利8项，培养硕士研究生5名。