Highly Efficient Electrochemical CO₂ Reduction Reaction to CO with One‐Pot Synthesized Co‐Pyridine‐Derived Catalyst Incorporated in a Nafion‐Based Membrane Electrode Assembly

Abstract There is great need for the development of an electrochemical CO₂ reduction reaction (CO₂RR) process with high Faraday efficiency (FE), energy efficiency (EE), and current density for practical utilization of CO₂. Here, a facile one‐pot synthesis of a catalyst is reported that is based on cobalt and poly‐4‐vinylpyridine that can perform CO₂RR to CO predominantly with respect to the hydrogen evolution reaction in a nafion‐based membrane electrode assembly and can work in pH ranging from 2 to 7. Cell optimization results in CO₂RR to CO with 92% FE and 58% EE at 85 mA cm⁻², while showing no noticeable degradation in FE at 20 h. These characteristics are attributed to synthesis and processing conditions which promote nearly uniform coordination of pyridine moieties with Co at the nanoscale in order to produce the appropriate complex necessary for catalysis. Outstanding performance combined with the ease of production, scalability of the method, and accessibility of components pave the way toward the commercialization of an electrochemical CO₂RR.