Weilhard Andreas, Argent Stephen P, Sans Victor
Faculty of Engineering, University of Nottingham, Nottingham, NG7 2RD, UK.
School of Chemistry, University of Nottingham, Nottingham, NG7 2RD, UK.
Nat Commun. 2021 Jan 11;12(1):231. doi: 10.1038/s41467-020-20291-0.
The efficient transformation of CO into chemicals and fuels is a key challenge for the decarbonisation of the synthetic production chain. Formic acid (FA) represents the first product of CO hydrogenation and can be a precursor of higher added value products or employed as a hydrogen storage vector. Bases are typically required to overcome thermodynamic barriers in the synthesis of FA, generating waste and requiring post-processing of the formate salts. The employment of buffers can overcome these limitations, but their catalytic performance has so far been modest. Here, we present a methodology utilising IL as buffers to catalytically transform CO into FA with very high efficiency and comparable performance to the base-assisted systems. The combination of multifunctional basic ionic liquids and catalyst design enables the synthesis of FA with very high catalytic efficiency in TONs of >810 and TOFs > 2.110 h.
将一氧化碳高效转化为化学品和燃料是合成生产链脱碳面临的关键挑战。甲酸（FA）是一氧化碳加氢的首个产物，它可以作为高附加值产品的前体，或用作储氢载体。在甲酸合成过程中，通常需要碱来克服热力学障碍，这会产生废物并需要对甲酸盐进行后处理。使用缓冲剂可以克服这些限制，但到目前为止它们的催化性能一般。在此，我们提出一种利用离子液体作为缓冲剂的方法，可将一氧化碳高效催化转化为甲酸，其性能与碱辅助体系相当。多功能碱性离子液体与催化剂设计相结合，能够以大于8×10的TONs和大于2.1×10 h的TOFs实现非常高的催化效率来合成甲酸。
