逐级功能化金属有机框架用于可见光催化二氧化碳的高效转化

太阳能驱动CO2高效催化转化制备化学燃料，将化石能源燃烧释放的终极产品CO2再次推入到自然界的碳循环，不仅有利于解决化石燃料短缺的问题，更有利于解决环境污染问题。对于CO2高效催化转化，材料的光吸收性能，活性位点与反应的微环境等因素的协同作用至关重要。本项目拟利用结构与组成明确的光活性金属有机框架(MOF)为载体，逐级整合多种功能性基元，探索可控、绿色环保的新策略实现光催化CO2还原。通过组装高活性的原子精度纳米团簇或单点催化剂于光活性MOF中构筑高效光催化材料，发挥多组分在微环境中的协同作用，促进不同组分间光生电子的快速转移，探索激发能与光生电子的转移过程，揭示催化机理。通过廉价量子点的引入构筑宽光谱与强可见光吸收的复合材料，实现多重电子共注于限域空间中的催化中心。该项目的顺利实施可显著增强复合材料的光催化性能，开发高效光催化体系实现CO2还原制备烃或醇等高附加值的化学燃料。

Solar-driven efficiently catalytic conversion of CO2 to chemical fuels can further utilize the CO2, one ultimate product of fossil energy combustion in the natural carbon cycle. It is not only conducive to solving the problem of fossil fuel shortage, but also conducive to solving the problem of environmental pollution. For high efficient conversion of CO2, the synergistic effects of light absorption ability, catalytic active sites and reaction microenvironment are very important. In this project, we attempt to explore a controllable, green and environmentally friendly strategy for photocatalytic reduction of CO2 by step by step integrating various functional units into photoactive metal organic framework (MOF) with well-defined structure and composition. The composite photocatalytic materials were constructed by assembling highly active nanoclusters or single-site catalysts to in photocatalytic MOFs, the synergistic effect of multi-components in micro-environment can promote rapid transfer of photogenerated electrons between different components. The transfer process of excitation energy and photogenerated electrons in the these composite with well-defined structure can be explored in detail to further reveal the catalytic mechanism. By introducing low-cost quantum dots, a composite material with broad spectrum and strong visible light absorption ability can be constructed to realize co-injection of multiple electrons into catalysts in the confined space of MOFs. The successful implementation of this project can significantly enhance the photocatalytic performance of the composite materials, and develop a highly efficient photocatalytic system to reduce CO2 to produce high value-added chemical fuels, such as hydrocarbons or alcohols.