Dimensional engineering of covalent organic frameworks derived carbons for electrocatalytic carbon dioxide reduction

Abstract

AbstractCovalent organic frameworks (COFs) have been developed as the precursors to construct porous carbons for electrocatalytic systems. However, the influences of carbon dimensions on the catalytic performance are still underexplored. In this work, we have first constructed COF‐derived carbons by template‐synthesis strategy in different dimensions to catalyze the carbon dioxide reduction (CO2RR). By using different templates, the one‐dimensional (1D), two‐dimensional (2D), and three‐dimensional (3D) COF‐derived carbons have been employed to anchor Co‐porphyrin to form the Co‐N5 sites to catalyze CO2RR. The 1D catalyst templated by carbon nano tubes presents high binding ability of CO2, more defective sites, and higher electronic conductivity, resulting in a higher catalytic activity for CO2 and selectivity of CO than 2D and 3D carbon‐based catalysts. The 1D catalyst delivers the turnover frequency values of 1150 h−1 and the FECO of 94.5% at 0.7 V versus RHE, which is significantly better than those of 2D and 3D carbon‐based catalysts.