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

在这个由化学学部化学催化项目资助的项目中，新罕布什尔大学的李功虎教授正在研究将二氧化碳回收为化学品、材料和燃料。然而，二氧化碳在热力学上是稳定的，它的转化通常需要很高的能量。本研究项目构建了创新的催化系统，使二氧化碳通过低能途径活化，其中两个金属中心一起工作，在光照射下将二氧化碳减少为燃料。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，以增加国家在清洁能源、材料和催化科学方面的人才储备。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，这将随后减少对化石燃料的依赖，并有助于减缓气候变化。李正在研究表面金属中心在光催化二氧化碳还原中的合作相互作用。特别是，通过共价连接剂将铼、锰、镍和钴的配位配合物接枝到介孔二氧化硅上，可以合成多相分子催化剂。将对连接剂和多孔表面进行优化，以达到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于研究低能量，双核途径的二氧化碳还原使用多相分子催化剂。研究方向为表面化学和受限环境下二氧化碳还原光催化的基本问题。该奖项还支持教育活动，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。这项工作的更广泛的影响包括潜在的社会效益，从创新的催化系统的发展，有效的太阳能转换和可持续的二氧化碳利用。

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.