Covalent 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 undere...Covalent 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(CO_(2)RR).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 CO_(2)RR.The 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)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.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:52303288,21878322,22075309,22378413Youth Innovation Promotion Association of Chinese Academy of Sciences and Biomaterials and Regenerative Medicine Institute Cooperative Research Project Shanghai Jiao Tong University School of Medicine,Grant/Award Number:2022LHA09。
文摘Covalent 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(CO_(2)RR).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 CO_(2)RR.The 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)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.