Magnetic Regulation of Defect-Engineered Fe ₃ GeTe ₂ Monolayer for Enhancing Electrocatalytic CO ₂ Reduction

The electrochemical CO2 reduction reaction (CO2RR) offers a sustainable route to mitigating CO2 emissions while producing valuable fuels. In this study, we demonstrated that defective Fe3GeTe2 monolayers serve as high-performance CO2RR electrocatalysts for efficient CH4 production. Our first-principles calculations reveal that although a perfect Fe3GeTe2 substrate is inert to CO2 adsorption, defect engineering activates the surface, significantly enhancing its affinity for CO2. Notably, the increased magnetic moment of Fe shifts the d-band center, optimizing the binding of the oxygen-containing intermediate and thereby boosting catalytic activity. The defect-modified Fe3GeTe2 monolayer achieves a low overpotential of −0.46 V versus the reversible hydrogen electrode (RHE). Our findings highlight the potential of magnetic modulation in two-dimensional materials for efficient CO2 conversion, providing an effective and feasible approach for sustainable catalysis.