CuLa dual-site catalyst for high-efficiency CO2-to-CO electrocatalytic conversion with ultralow overpotential

Abstract

To achieve high-performance electrocatalytic CO 2 reduction (CO 2 RR) at low potentials, we synthesized an atomically dispersed CuLa/NC catalyst derived from a metalloporphyrin-based metalorganic framework. This catalyst exhibits an exceptional Faradaic efficiency of 97%, with half-cell energy efficiency reaching 91% at an ultra-low potential of -0.20 V for the conversion of CO 2 to CO. Impressively, the reaction can even be powered by a 1.5 V battery. This study offers a refined strategy for the rational design of dualatom catalysts geared toward highly efficient CO 2 RR.Electrocatalytic CO 2 reduction reaction (CO 2 RR) is regarded as a valuable supplement to carbon resource recycling, enabling both the storage of intermittent renewable electricity and the effective use of carbon feedstocks. 1, 2 However, the realization of high-efficiency CO 2 RR remains a formidable challenge. The inherent chemical inertness of CO 2 molecules imposes substantial thermodynamic and kinetic barriers, necessitating the application of high external voltages to overcome activation energy thresholds and drive the electrochemical reduction. 3 This results in considerable energy input requirements for CO 2 conversion, posing a major bottleneck in energy efficiency for practical applications. Converting CO 2 to CO involves only a two-electron transfer process, corresponding to faster reaction kinetics, reduced overpotentials, and lower energy consumption. 4 In catalyst design, dual-atom catalysts (DACs) have emerged as a research frontier due to their atomically dispersed metal centers, which maximize metal utilization and often outperform traditional nanocatalysts in reactions including CO 2 RR. 5- 9