Molecularly Dispersed Cobalt Phthalocyanine Mediates Selective and Durable CO2 Reduction in a Membrane Flow Cell

Abstract High‐rate electrochemical CO 2 ‐to‐CO conversion provides a favorable strategy for carbon neutrality. Molecular catalysts, especially those with isolated metal active centers, are known to be the efficient CO 2 ‐to‐CO electrocatalysts due to their high selectivity and outstanding instinct activity; however, the controllable scale‐up synthesis and durable utilization at industrial current densities still remain a challenge. Here, it is developed a molecularly dispersed cobalt phthalocyanine loaded on carbon nanotube for high‐current long‐term CO 2 ‐to‐CO electrolysis. The resultant catalyst exhibits a high CO selectivity with a maximum Faradaic efficiency of 97% and performs a current density of −200 mA cm −2 in a flow cell with a TOF of 83.9 s −1 , which is among the best of CO‐selective electrocatalysts. With a series of impregnation loading experiments, the process of molecular‐dispersion or aggregation is investigated. In addition, the application of selective and durable electrolysis at a current of 0.25 A is realized up to 38.5 h in a scale‐up MEA configuration. Subsequent characterization shows robust durability closely related to the dispersion of CoPc. This study provides a triumph to catalyze commercial‐scale CO production using molecularly dispersed phthalocyanine electrocatalysts.