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

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.