Atomically proximate FeN4 sites and molybdenum-sulfur clusters for efficient bifunctional oxygen electrocatalysis in rechargeable zinc-air batteries.

作者：Zi-Han Wang, Zongge Li, Xiaodong Chen, Huiqin Zhao, Zhi-Qiang Wang, Wenjun Kang, You-Xun Li, Jie Ding, Xiangting Min, Haibo Li · 发表于：Journal of Colloid and Interface Science · 年份：2026 · DOI：10.1016/j.jcis.2026.141094 · 研究领域：Medicine

Rechargeable aqueous zinc-air batteries (ZABs) are severely hindered by the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Simultaneous promotion of both processes on a minimum and well-defined catalytic motif is highly challenging. Herein, we report an electrocatalyst (Fe1-N/Mo-SAC) with proximate FeN4 and undercoordinated MoS clusters in a carbon framework, exhibiting outstanding bifunctional ORR-OER performance in alkaline media via interfacial synergy, with a narrow ΔE of 0.789 V and favorable kinetics and durability. No direct covalent FeMo or FeS bonds exist between FeN4 and adjacent MoS species, and evident interfacial charge redistribution elevates the Fe valence state while reducing the oxidation level of Mo sites. The assembled aqueous ZAB with Fe1-N/Mo-SAC as the air-cathode material exhibits an open-circuit potential of 1.571 V, a peak power density up to 206.4 mW cm-2, and remarkable cycling durability of >800 h (2400 cycles). Density functional theory calculations demonstrate that neighboring MoS clusters electronically modulate the Fe center, shifting the Fe d-band center downward, and lowering the rate-determining energy barrier toward bifunctional oxygen electrocatalysis. This study identifies nonbonded, atomically proximate interfacial coupling as an effective strategy to develop high-efficiency bifunctional electrocatalysts toward rechargeable metal-air batteries.