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 C(2+ )Faradaic efficiency of 87.9% at a partial current density of -6.0 mA/cm(2) (C2+ Faradaic efficiency of 70.7% at a partial current density of -10.6 mA/cm(2)). 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 C(2+ )alcohols production.