Abstract

Designing composite structures to enhance the performance of manganese-based sodium-ion battery (SIB) cathodes now represents a significant research focus. However, the development of composite-phase cathodes is hindered by an incomplete understanding of their structural transformation mechanisms. Herein, we elucidate the relationship between the transition metal bond energy and material structure, proposing a coordination bond reorganization strategy to drive structural transformations. This concept is demonstrated using the cathode material Na<sub>0.63</sub>Mn<sub>1-<i>x</i></sub>Ti<sub><i>x</i></sub>O<sub>2</sub>, showing that the bond energy of transition metals plays a critical role in the structural transformation process. By introducing stronger Ti-O covalent bonds, we achieved the transition from a layered to tunnel structure. Furthermore, the layered-tunnel intergrowth structure Na<sub>0.63</sub>Mn<sub>0.95</sub>Ti<sub>0.05</sub>O<sub>2</sub> demonstrates a remarkable specific capacity of 194.68 mAh g<sup>-1</sup> alongside excellent stability while exhibiting good compatibility with hard carbon anodes. This work validates the feasibility of coordination bond reorganization as a mechanism for autonomous structural transformations, offering new insights for the precise design of high-energy-density materials for next-generation SIBs.

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2025
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Kang Chen, Qilin Zheng, Min Wen et al. (2025). Layered-to-Tunnel Transformation Enabled by Coordination Bond Reorganization in Oxide Cathodes for Sodium–Ion Batteries. ACS Applied Materials & Interfaces . https://doi.org/10.1021/acsami.5c18702

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DOI
10.1021/acsami.5c18702