Dual CO2${\rm CO}_2$ Activation Assisted C–C Coupling on Mn3${\rm Mn}_3$@C2N${\rm C}_2{\rm N}$ Electrocatalyst for Selective CO2${\rm CO}_2$ Conversion

Abstract The renewable energy‐driven electrocatalytic reduction reaction () offers a sustainable pathway to convert into valuable products, addressing both emissions and energy demands. However, achieving efficient conversion to multi‐carbon products remains a challenge due to the complexity of C–C coupling. In this study, we systematically screen monomer, dimer, and trimer configurations of transition metal‐doped two‐dimensional (@) to identify optimal catalysts for enhanced performance. Our findings reveal @ as a highly effective catalyst, capable of dual activation, promoting C–C coupling, and selectively producing products, while simultaneously suppressing hydrogen evolution (HER) and CO evolution. Notably, this research highlights alternative C–C coupling pathways beyond the conventional CO dimerization mechanism. These insights represent a significant advance in the design of efficient and selective catalysts, paving the way for sustainable conversion into valuable multi‐carbon products.