Mechanistic insights into the adjustable electronic buffering effect of C60 under electric fields for single-atom Cu catalysis in CO electroreduction

Abstract

C₆₀ fullerene has been recognized as an electronic buffer, capable of regulating the charge state of anchored metals and thus enhancing the catalytic performance of metal centers. However, adjusting the built-in electric field at the fullerene-metal interface is challenging. This study presents a strategy for controllably regulating the properties of a C₆₀-supported single Cu catalyst (Cu₁/C₆₀) for CO electroreduction using external electric fields. Density functional theory calculations demonstrate that an external electric field can enhance reaction activity and product selectivity by leveraging the energy changes induced by the dipole differences between intermediates. At a moderate strength of 0.19 V/Å, the limiting potential of CO reduction reaches as small as −0.37 V, a 65 % reduction compared to that in the field-free state, and the competing hydrogen evolution reaction can be passivated.