Selective Electroreduction\nof CO₂ to C₂₊ Alcohols Using Graphitic Frustrated\nLewis Pair Catalyst

Abstract

Efficient electroreduction of CO₂ to multicarbon\nproducts\nis a complicated reaction because of the high energy barriers for\nthe CO₂ activation and C–C coupling. Here, we design\na graphitic frustrated Lewis pair catalyst doped with boron and nitrogen\n(BN-GFLP) for reducing the amount of CO₂ to multicarbon\nproducts. Multicarbon (C₂₊) biofuels (i.e., ethanol and <i>n</i>-propanol) are identified as the major products with a\nC₂₊ Faradaic efficiency of 87.9% at a partial current density\nof −6.0 mA/cm² (C₂₊ Faradaic efficiency\nof 70.7% at a partial current density of −10.6 mA/cm²). Furthermore, density functional theory calculations reveal that\nthe dual binding site of FLP reduces the reaction free energies required\nfor CO₂ activation and C–C coupling. Consequently,\nenergetically favorable CO₂ reduction pathways are proposed,\nand selectivities for the production of ethanol and <i>n</i>-propanol are determined. Based on our results, we propose a molecular\ndesign strategy for the selective CO₂ reduction catalysts\naimed at facilitating C₂₊ alcohols production.