Jakobsen Joakim B, Rønne Magnus H, Daasbjerg Kim, Skrydstrup Troels
Carbon Dioxide Activation Center (CADIAC), Interdisciplinary Nanoscience Center, Department of Chemistry, Aarhus University, Gustav Wieds Vej 14, 8000, Aarhus C, Denmark.
Interdisciplinary Nanoscience Center, Department of Chemistry, Aarhus University, Gustav Wieds Vej 14, 8000, Aarhus C, Denmark.
Angew Chem Int Ed Engl. 2021 Apr 19;60(17):9174-9179. doi: 10.1002/anie.202014255. Epub 2021 Mar 5.
The selective and efficient reduction of carbon dioxide represents a key solution to producing non-fossil-fuel-based feedstocks for the chemical industry, while alleviating the increasing atmospheric concentration of this greenhouse gas. A variety of catalytic methods for the CO reduction reaction (CO RR) have been developed, including hydrogenations and electrochemical or photochemical reductions. For many of the most significant breakthroughs reported in the last decade, we realized that amines or closely related functional groups play a critical role for such transformations, and in several cases, are directly associated with the catalyst as a pendant group. Amines play multiple roles, such as CO trapping agents, proton shuttles, electron donors, or facilitators of CO reductions through formamide derivatives. In this Viewpoint, we compile some of these recent findings, and discuss their significance in a broader context in an attempt to provide guidelines for the design of new catalysts with enhanced activity and selectivity.
选择性高效还原二氧化碳是为化学工业生产非化石燃料基原料的关键解决方案,同时可缓解这种温室气体在大气中浓度不断增加的问题。人们已开发出多种用于二氧化碳还原反应(CO RR)的催化方法,包括氢化反应以及电化学或光化学还原反应。对于过去十年报道的许多重大突破,我们意识到胺类或密切相关的官能团在这类转化中起着关键作用,并且在某些情况下,作为侧基直接与催化剂相关联。胺类发挥多种作用,例如作为CO捕获剂、质子穿梭体、电子供体,或通过甲酰胺衍生物促进CO还原。在本观点文章中,我们汇总了一些近期的研究发现,并在更广泛的背景下讨论它们的意义,试图为设计具有更高活性和选择性的新型催化剂提供指导。