Efficient Carbon Dioxide Electroreduction over Ultrathin Covalent Organic Framework Nanolayers with Isolated Cobalt...

Electrochemical CO₂ reduction represents a sustainable approach for the conversion of CO₂ into valuable fuels and chemicals. Here, we fabricated a series of composite nanomaterials through template-oriented polymerization of covalent organic frameworks (COFs) with isolated cobalt porphyrin units on amino-functionalized carbon nanotubes for efficient electrocatalytic CO₂ reduction reaction (CO₂RR). Compared with pure COFs, the hybrid form of ultrathin COF nanolayers wrapped on the conductive scaffold leads to distended current density and stable Faradaic efficiency for CO₂-to-CO conversion over a wide potential range. Specifically, the catalytic performances of the system can be finely optimized by the modification of the reticular structure with different functional groups. Our work gives a new strategy for the preparation of highly active and selective electrocatalysts for CO₂RR.