Selective Electroreduction of CO2 to C2+ Biofuels using Graphitic Frustrated Lewis Pair Catalyst

Abstract Efficient electroreduction of CO2 to multicarbon products is a complicated reaction because of the high energy barriers for CO2 activation and C–C coupling. Here, we design a graphitic frustrated Lewis pair catalyst doped with boron and nitrogen (BN-GFLP) for reducing CO2 to multicarbon products. Multicarbon (C2+) biofuels (i.e., ethanol and n-propanol) are identified as the major products with a C2+ Faradaic efficiency of 87.9% at a partial current density of −6.0 mA/cm2 (C2+ Faradaic efficiency of 70.7% at a partial current density of −10.6 mA/cm2). Furthermore, density functional theory calculations reveal that the dual binding site of FLP reduces the reaction free energies required for CO2 activation and C–C coupling. Consequently, energetically favourable CO2-reduction pathways are proposed, and selectivity for the production of ethanol and n-propanol are determined. Based on our results, we suggest a molecular design strategy for the next-generation CO2 reduction catalysts for green oceans and the atmosphere.