SusChEM: Solar CO2 Reduction (SCO2RE) with Non-Innocent Ligand Transition Metal Photocatalysts

在这个项目中，由化学系的化学催化计划资助，麻省大学波士顿分校的乔纳森罗奇福德教授寻求对太阳能驱动的二氧化碳化学原料生产的机械见解。 其中一种产品一氧化碳是进一步减少碳基燃料以及合成气的有价值的前体，合成气是石化工业中使用的起始材料。在分子系统中从单光子引发的过程中有效地利用这种多电子跃迁之前，仍然存在要克服的主要障碍。在这种情况下，罗奇福德教授和他的研究小组设计了具有非无辜配体的双（I）羰基系统，这些配体能够在可见光谱中有效地捕光，同时还显示出作为二氧化碳还原光催化剂的强大潜力。 虽然稀土是一种贵金属，其供应量有限，但该研究项目反复重复使用少量的金属来生产大量所需的产品，使整体努力比目前生产燃料和工业原料的技术更加环保。 这项研究被认为是在“SusChEM”倡议下，因为它将非石油基原料（二氧化碳）转化为有用的含碳材料。 通过结合合理的程序的合成，电化学，和电物理分析，对太阳能二氧化碳转换的设计策略有了更好的理解。通过收集太阳能来模仿自然光合作用，以可持续的方式生产燃料，这是当今科学面临的重大挑战之一。该项目有助于进一步了解人工光合作用，并为马萨诸塞大学波士顿分校的学生提供多学科培训。此外，该项目的关键概念和研究结果被整合到马萨诸塞大学波士顿分校的本科课程中，以教育未来几代科学家利用太阳能的重要性，因为我们的社会正在努力实现可持续和绿色的未来。

In this project, funded by the Chemical Catalysis Program of the Chemistry Division, Professor Jonathan Rochford of UMass Boston seeks mechanistic insight into the solar driven production of chemical feedstocks from carbon dioxide. One such product, carbon monoxide, is a valuable precursor towards further reduced carbon-based fuels as well as syngas, a staring material used in the petrochemical industry. There remain major obstacles to overcome before such multi-electron photocatalysis can be efficiently utilized from single photon initiated processes in molecular systems. In this context, Professor Rochford and his research group designs rhenium(I)carbonyl systems with non-innocent ligands that are capable of efficient light harvesting in the visible spectrum while also displaying strong potential as carbon dioxide reduction photocatalysts. While rhenium is a precious metal and its supply is limited, this research project repeatedly reuses tiny amounts of the metal to create significant amounts of desired product, making the overall effort more environmentally friendly than current techniques for the production of fuels and industrial feedstocks. This research is considered under the "SusChEM" initiative as it converts a non-petroleum based feedstock (carbon dioxide) into useful carbon-containing materials. By combining a rational program of synthesis, electrochemistry, and photophysical analyses, a greater understanding of design strategies towards solar carbon dioxide conversion is developed. Mimicking natural photosynthesis by harvesting the sun's energy towards a sustainable process for fuel production represents one of the grand challenges of science today. This project aids in further understanding artificial photosynthesis and provides multi-disciplinary training for students at UMass Boston. Furthermore, key concepts and findings of this project are integrated into the undergraduate curriculum at UMass Boston to educate future generations of scientists on the importance of utilizing solar energy as our society works towards a sustainable and greener future.