Covalently Grafted Cobalt Porphyrin on Carbon Nanotube for Efficient CO2 Electroreduction

Molecular complexes with inexpensive transition metal center have drawn extensive attention as they exhibit high selectivity for electrochemical CO2‐to‐CO conversion. In this work, we propose a new strategy to covalently graft cobalt porphyrin onto the surface of carbon nanotube through a substitution reaction at metal centers. Material characterization and electrochemical studies revealed that porphyrin molecules were well dispersed at a high loading of 10 wt. %. As a result, the turnover frequency for CO formation was improved by a factor of three than a traditional physically mixed catalyst at the same cobalt content, leading to an outstanding overall current density of 25.1 mA/cm2 and Faradaic efficiency of 98.3% at 490 mV overpotential with excellent long‐term stability. This work provides an effective pathway for the improvement of electrocatalysts performance that could inspire future rational design of molecular catalysts.

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