Selective Electroreduction of CO<sub>2</sub> to C<sub>2+</sub> Alcohols Using Graphitic Frustrated Lewis Pair Catalyst
Hyun‐Tak Kim, Jaehyun Park, Jinhong Mun, HyeonOh Shin, Deok‐Ho Roh, Junhyeok Kwon, Sung‐Tae Kim, Sang‐Joon Kim, Geunsik Lee, Seok Ju Kang, Tae‐Hyuk Kwon
Abstract
Efficient electroreduction of CO 2 to multicarbon products is a complicated reaction because of the high energy barriers for the CO 2 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 CO 2 to multicarbon products. Multicarbon (C 2+ ) 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 (C 2+ 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 CO 2 activation and C–C coupling. Consequently, energetically favorable CO 2 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 CO 2 reduction catalysts aimed at facilitating C 2+ alcohols production.