作者
Chengli Rong,Fangzhou Liu,Hamidreza Arandiyan,Yuan Wang,Yuehua Chen
摘要
The electrochemical reduction of carbon dioxide (CO 2 ) to methanol (CH 3 OH) offers a promising route for coupling carbon mitigation with renewable energy storage. Among molecular electrocatalysts, cobalt phthalocyanine (CoPc) and its derivatives have emerged as leading platforms owing to their well-defined Co N 4 coordination environment, tunable electronic structure, and adjustable intermediate-binding properties. Recent advances in ligand engineering, multinuclear architectures, catalyst–support interactions, and reaction microenvironment modulation have led to notable improvements in CH 3 OH selectivity and activity, with reported Faradaic efficiencies exceeding 30% and current densities above 100 mA cm −2 . However, achieving simultaneously high selectivity, activity, and durability remains challenging, and the mechanistic origins of CH 3 OH formation are not yet fully understood. In particular, the interplay among CO 2 activation, *CO stabilization, proton-coupled electron transfer kinetics, competitive CO desorption, and catalyst degradation continues to restrain rational catalyst design. This review summarizes recent advances in CoPc-based catalysts for electrochemical CO 2 -to-CH 3 OH conversion, with emphasis on reaction mechanisms, structure–reactivity relationships, degradation pathways, and molecular and interfacial engineering strategies. By integrating insights from operando spectroscopy, theoretical modeling, and membrane-electrode-assembly development, we highlight key design principles and identify remaining challenges toward the development of efficient, selective, and durable CoPc-based systems for practical CH 3 OH electrosynthesis.