Creating Dual Active Sites in Ru‐doped FeMn‐MOF‐74 for Efficient Overall Water Splitting

Abstract The design of well‐engineered bifunctional electrocatalysts is crucial for achieving durable and efficient performance in overall water splitting. In this study, Ru‐doped FeMn‐MOF‐74 itself has Ru sites and generates FeMnOOH under catalytic conditions, forming dual active sites for overall water splitting. Density functional theory (DFT) calculations demonstrate that the Ru dopants exhibit optimized binding strength for H* and enhanced hydrogen evolution reaction (HER) performance. Moreover, the Mn sites within FeMnOOH lower the energy barrier for the rate‐determining step (from O* to OOH*), serving as the active centre for oxygen evolution reaction (OER). The incorporation of Ru significantly improves the electron transfer properties of FeMn‐MOF‐74 and enhances its water adsorption capacity, synergistically boosting its bifunctional activity. This strategy of designing dual active sites provides new insights into the development of bifunctional metal‐organic frameworks (MOFs) for efficient overall water splitting.