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Oxygen Edge-Sharing Strategy in P2-Type Na0.67MnO2 Cathodes: Synergistic Enhancement of Intercalation Kinetics and Air Stability

Yuanming Liu, Shiyu Wang, Weijie Fu,Shuyun Yao, Yingjie Ji, Jingxian Li, Lanlan Shi,Xiaojun Wang, Feike Zhang, Jinghua Yang, Ruilong Liu,Jiangzhou Xie,Zhiyu Yang,Yi-Ming Yan

ADVANCED FUNCTIONAL MATERIALS(2025)

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Abstract
Mn-based layered oxides have garnered significant attention as cathode materials for energy storage due to their environmental benignity and high theoretical specific capacity. However, practical applications remain constrained by sluggish Na+ intercalation kinetics and poor structural stability. In this study, it is engineered that the Mn-O-B unit through an oxygen edge-sharing strategy to modulate Mn & horbar;O covalency in P2-type Na0.67MnO2, thereby achieving high specific capacity and structural stability. Both experimental results and density functional theory (DFT) calculations reveal that increased TM-O covalency facilitates Na+ diffusion in P2-type Na0.67MnO2 while simultaneously enhancing air stability. The as-prepared P2-type Na0.67MnB0.05O2 exhibits a specific capacitance of 452 F g-1 at 1 A g-1, maintaining 96.75% capacity retention after 8800 cycles. This work elucidates the critical role of oxygen edge-sharing in optimizing interactions between transition metal and oxygen atoms, establishing a relationship between Mn & horbar;O structure and functional properties. These findings advance the development of high-performance energy storage technologies.
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electron transfer,orbital overlap,oxygen-sharing edges,TM-O covalency
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