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Stabilizing Lattice Oxygen Mechanism on Ru Single Atoms via a High-Entropy Support for Acidic Oxygen Evolution
Luqi Wang1,2, Yixin Hao3, Suwan Bi2
1Confucius Energy Storage Lab, School of Energy and Environment & Z Energy Storage Center, Southeast University, Nanjing 211189, China.
Abstract:
The lattice oxygen mechanism (LOM) has emerged as an effective route to enhance acidic oxygen evolution reaction (OER) activity. However, extensive lattice-oxygen participation often leads to defect accumulation and framework destabilization, severely limiting catalyst durability. Herein, we propose that anchoring Ru single atoms on a high-entropy oxide (Ru-(FeCoNiCrMn)3O4) establishes a stabilized LOM pathway at the Ru sites, combining high activity with long-term structural integrity. The high-entropy effect strengthens Ru 4d-O 2p hybridization, lowering the energetic barrier for lattice-oxygen oxidation and facilitating direct Olat-Oad coupling between lattice oxygen near the Ru sites and adsorbed oxygen species. In parallel, disruption of the interfacial hydrogen-bond network enriches weakly hydrogen-bonded free water with high reactivity, enabling rapid incorporation of water-derived oxygen into lattice-oxygen defects. This dynamic defect-refilling process preserves the local coordination environment of Ru sites and prevents irreversible structural degradation. Consequently, the Ru-(FeCoNiCrMn)3O4 catalyst only needs an overpotential of 204 mV to reach 10 mA cm-2 in 0.5 M H2SO4 and delivers a high mass activity of 5235.42 A gRu-1 at 1.50 V vs RHE. The proton exchange membrane electrolyzer with a Ru-(FeCoNiCrMn)3O4 anode can operate stably for over 320 h at 500 mA cm-2. This work presents a novel strategy for simultaneously enhancing catalyst activity and stability.
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