Conductive Two‐Dimensional Phthalocyanine‐based Metal–Organic Framework Nanosheets for Efficient Electroreduction of CO2

Abstract The electrocatalytic conversion of CO 2 into value‐added chemicals is a promising approach to realize a carbon‐energy balance. However, low current density still limits the application of the CO 2 electroreduction reaction (CO 2 RR). Metal–organic frameworks (MOFs) are one class of promising alternatives for the CO 2 RR due to their periodically arranged isolated metal active sites. However, the poor conductivity of traditional MOFs usually results in a low current density in CO 2 RR. We have prepared conductive two‐dimensional (2D) phthalocyanine‐based MOF (NiPc‐NiO 4 ) nanosheets linked by nickel‐catecholate, which can be employed as highly efficient electrocatalysts for the CO 2 RR to CO. The obtained NiPc‐NiO 4 has a good conductivity and exhibited a very high selectivity of 98.4 % toward CO production and a large CO partial current density of 34.5 mA cm −2 , outperforming the reported MOF catalysts. This work highlights the potential of conductive crystalline frameworks in electrocatalysis.