We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO2RR to ethanal, CH3CHO. In all reduction potentials tested from −0.2 to −1.0 V (vs RHE) in 0.5 M KHCO3 solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At −0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm–2 and mass activity of 3.4 A g–1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO2RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC–CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH3CHO.

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Observing and understanding the phenomena associated with the reaction mechanisms and catalyst deactivation in molecular catalysis is a very challenging task in green chemisty. This knowledge is crucial for applying...

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