Unrivaled single atom catalytic efficiency of Fe@Mg₁₂O₁₂ toward N₂ reduction reaction (NRR) for NH₃ generation

The quest for efficient and sustainable catalytic processes for ammonia synthesis has led to the exploration of transition metal (TM) doped single-atom catalysts (SACs) due to their exceptional catalytic properties and potential for overcoming the limitations of conventional catalysts. This study investigates the application of iron-doped Mg₁₂O₁₂ nanocage (Fe@Mg₁₂O₁₂) as a novel SAC for the nitrogen reduction reaction (NRR), employing density functional theory (DFT) calculations. The optimum reaction mechanism pathway of the NRR has been investigated and obtained by considering the stability of the different possible intermediates. Our analysis reveals that the high spin nature of Fe in Fe@Mg₁₂O₁₂ can stabilize the NRR intermediates by facilitating different total spin-states of the intermediates. Moreover, the importance of the role of support is highlighted as it stabilizes the adsorbed moiety by binding to it is crucial. This study promotes the use SACs for the realization of a sustainable and active electrocatalyst for the NRR, offering new avenues for addressing global energy and environmental challenges through the advancement of sustainable catalytic technologies.