CAREER: Binuclear Chemistry of Heterogenized Molecular Catalysts in Solar CO2 Reduction

新罕布什尔州大学的李贡虎教授在化学系化学催化项目的资助下，正在研究将二氧化碳回收到化学品、材料和燃料中。然而，二氧化碳是化学稳定的，并且其转化通常需要高能量。该研究项目构建了创新的催化系统，使二氧化碳通过低能量途径活化，其中两个金属中心在光照射下共同工作，将二氧化碳还原为燃料。低能途径将使用实验和理论方法进行研究。该项目还将为教育能源相关领域的现有和新兴劳动力提供极好的机会，以增加清洁能源，材料和催化科学方面的国家人才管道。该项目的更广泛影响包括开发高效和强大的二氧化碳利用催化系统，从而减少对化石燃料的依赖，并有助于减缓气候变化。李博士正在研究表面金属中心在光催化二氧化碳还原中的协同作用。特别地，将通过将铼、锰、镍和钴的配位络合物经由共价连接体接枝到介孔二氧化硅上来合成多相化分子催化剂。将优化连接体和多孔表面以实现适当的分子间距离和几何形状。先进的光谱技术和密度泛函理论计算将被用来研究低能量，双核途径在二氧化碳还原使用的非均相分子催化剂。拟议的研究集中在表面化学和二氧化碳减排的基本问题在密闭环境中.该职业奖还支持教育活动，包括年度太阳能研讨会，以有效地向K-12学生和公众传播可持续发展概念。这项工作的更广泛影响包括开发创新的催化系统以实现高效的太阳能转换和可持续的二氧化碳利用所带来的潜在社会效益。

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Gonghu Li of the University of New Hampshire is investigating recycling carbon dioxide into chemicals, materials and fuels. However, carbon dioxide is thermodynamically stable, and its conversion often requires high energy. This research project constructs innovative catalytic systems to enable carbon dioxide activation via low-energy pathways, in which two metal centers work together to reduce carbon dioxide into fuels under light irradiation. The low-energy pathways will be investigated using both experimental and theoretical methods. This project will also provide excellent opportunities for educating the current and emerging workforce in energy-related fields to increase the national talent pipeline in clean energy, materials and catalysis science. The broader impacts of this project include the development of efficient and robust catalytic systems for carbon dioxide utilization, which will subsequently reduce dependency on fossil fuels and help to mitigate climate change.Dr. Li is investigating cooperative interactions of surface metal centers in photocatalytic carbon dioxide reduction. In particular, heterogenized molecular catalysts will be synthesized by grafting coordination complexes of Rhenium, Manganese, Nickel and Cobalt onto mesoporous silicas via covalent linkers. The linkers and porous surfaces will be optimized to achieve proper intermolecular distances and geometry. Advanced spectroscopic techniques and density functional theory calculations will be employed to investigate low-energy, binuclear pathways in carbon dioxide reduction using the heterogenized molecular catalysts. The proposed research focuses on fundamental issues in surface chemistry and carbon dioxide -reduction photocatalysis in confined environments. This CAREER award also supports educational activities, including annual solar energy workshops, to effectively disseminated sustainability concepts to K-12 students and the public. The broader impacts of this work include potential societal benefits from the development of innovative catalytic systems for efficient solar energy conversion and sustainable carbon dioxide utilization.