Extreme Enhancement of Carbon Hydrogasification via Mechanochemistry

Angew Chem Int Ed Engl. 2022 Apr 25;61(18):e202117851. doi: 10.1002/anie.202117851. Epub 2022 Mar 4.

Abstract

Carbon hydrogasification is the slowest reaction among all carbon-involved small-molecule transformations. Here, we demonstrate a mechanochemical method that results in both a faster reaction rate and a new synthesis route. The reaction rate was dramatically enhanced by up to 4 orders of magnitude compared to the traditional thermal method. Simultaneously, the reaction exhibited very high selectivity (99.8 % CH4 , versus 80 % under thermal conditions) with a cobalt catalyst. Our study demonstrated that this extreme increase in reaction rate originates from the continuous activation of reactive carbon species via mechanochemistry. The high selectivity is intimately related to the activation at low temperature, at which higher hydrocarbons are difficult to form. This work is expected to advance studies of carbon hydrogasification, and other solid-gas reactions.

Keywords: Carbon-Neutral; Hydrogenation; Internal Field NMR; Mechanochemistry; Solid-Gas Reaction.