Selective Electroreduction of CO2 to C2+ Alcohols 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 the CO₂ activation and C–C coupling. Here, we design a graphitic frustrated Lewis pair catalyst doped with boron and nitrogen (BN-GFLP) for reducing the amount of 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 favorable CO₂ reduction pathways are proposed, and selectivities for the production of ethanol and n-propanol are determined. Based on our results, we propose a molecular design strategy for the selective CO₂ reduction catalysts aimed at facilitating C₂₊ alcohols production.