Unlocking the Potential for Methanol Synthesis via Electrochemical CO₂ Reduction Using CoPc-Based Molecular Catalysts

The electrochemical CO₂ reduction reaction (CO₂RR) to produce methanol (CH₃OH) is an attractive yet challenging approach due to a lack of selective electrocatalysts. An immobilized cobalt phthalocyanine (CoPc) molecular catalyst has emerged as a promising electrocatalyst for CH₃OH synthesis, demonstrating decent activity and selectivity through a CO₂-CO-CH₃OH cascade reaction. However, CoPc’s performance is limited by its weak binding strength toward the CO intermediate. Recent advancements in molecular modification aimed at enhancing CO intermediate binding have shown great promise in improving CO₂-to-CH₃OH performance. In this Perspective, we discuss the competitive binding mechanism between CO₂ and CO that hinders CH₃OH formation and summarize effective molecular modification strategies that can enhance both the binding of the CO intermediate and the conversion of the CO₂-to-CH₃OH activity. Finally, we offer future perspectives on optimization strategies to inspire further research efforts to fully unlock the potential for methanol synthesis via the CO₂RR using molecular catalysts. © 2024 American Chemical Society.