Methanol production from CO2via an integrated, formamide-assisted approach

Abstract

The synthesis of fuels from CO₂ has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO₂via formamide intermediates, which are initially reduced using NaBH₄ to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO₂/NaBH₄. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations.