CuFe dual-atom catalysts embedded in N-doped graphene for enhanced CO2 electroreduction to methane

Developing new electrocatalytic materials becomes a critical issue in advancing the CO 2 reduction reaction (CO 2 RR) process. In this work, based on density functional theory, we designed a series of dual-atom catalysts (DACs) with CuFe metal dimer embedded onto a 6 N-doped graphene monolayer (CuFe@6NG). These DAC catalysts exhibit high thermodynamic, kinetic, and electrochemical stabilities. Their catalytic activities and mechanisms for the CH 4 production were comprehensively investigated. The coordination environment of the CuFe dimer yields distinct surface-induced catalytic activities. Notably, the CuFe@6NG-V3 structure, with the CuFe dimer occupying three vacancies, exhibits higher activity with a lower limiting potential. This can be attributed to its unique surface electron nature and the cooperative CuFe interaction. Additionally, we discuss the scaling relationships associated with the adsorption strength of intermediates. Our simulation studies demonstrate the high catalytic performances of CuFe-based DACs and offer new catalytic mechanisms, which are expected to further advance the CO 2 RR technologies.