Magnetic fields promote electrocatalytic CO2 reduction via subtle modulations of magnetic moments and molecular bonding.

ABSTRACT

Introducing a magnetic-field gradient into an electrically driven chemical reaction is expected to give rise to intriguing research possibilities. In this work, we elaborate on the modes and mechanisms of electrocatalytic activity (from the perspective of alignment of magnetic moments) and selectivity (at the molecular level) for the CO2 reduction reaction in response to external magnetic fields. We establish a positive correlation between magnetic field strengths and apparent current densities. This correlation can be rationalized by the formation of longer-range ordering of magnetic moments and the resulting decrease in the scattering of conduction electrons and charge-transfer resistances as the field strength increases. Furthermore, aided by the magnetic-field-equipped operando infrared spectroscopy, we find that applied magnetic fields are capable of weakening the C-O bond strength of the key intermediate ∗COOH and elongating the C-O bond length, thereby increasing the faradaic efficiency for the electroreduction of CO2 to CO.