Strain and Kinetics Synergy in Octahedral High‐Entropy Cathodes Enables Ultra‐Durable Sodium‐Ion Batteries
High-entropy oxides represent a paradigm shift in sodium-ion battery cathodes by utilizing entropy-driven structural stabilization to address the intrinsic challenges of lattice strain and sluggish ion kinetics. However, conventional high-entropy oxides face challenges in synthesis complexity and insufficient mechanistic insights into strain-kinetics coupling. Here, a high-entropy O3-type layered oxide, Na<sub>0.9</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Fe<sub>0.2</sub>Mn<sub>0.2</sub>Zn<sub>0.05</sub>Cu<sub>0.05</sub>Ti<sub>0.1</sub>O<sub>2</sub> (NNCFMZCT), is proposed featuring seven transition metals in a single crystallographic site, to synergistically optimize Na⁺ diffusion and structural resilience. Density functional theory calculations reveal that configurational disorder mitigates anisotropic lattice contraction during O/P phase transitions, while X-ray photoelectron spectroscopy and in situ X-ray diffraction confirm stable TMO₆ octahedra and suppressed irreversible phase transitions. The NNCFMZCT cathode delivers a high reversible capacity (>130 mAh g<sup>-1</sup> at 10 mA g<sup>-1</sup>), exceptional cycling stability (82.9% retention over 300 cycles at 500 mA g<sup>-1</sup>), and superior rate capability (>110 mAh g<sup>-1</sup> at 1000 mA g<sup>-1</sup>) within 2.0-4.0 V. When paired with commercial hard carbon in ampere-hour-level cylindrical cells, the full cell achieves 84% capacity retention after 200 cycles. This work demonstrates scalable viability for grid storage by establishing a universal strain-kinetics coupling strategy, which advances the rational design of entropy-stabilized cathodes for sustainable energy systems.
Authors
- Yiman Xie
- Jian Li (ORCID: https://orcid.org/0009-0007-3264-9161)
- Haiying Nie (ORCID: https://orcid.org/0009-0008-7308-1469)
- Lihua Wang (ORCID: https://orcid.org/0000-0002-6143-6348)
- Tiandu Sheng (ORCID: https://orcid.org/0000-0001-7751-7700)
Institutions
- Hunan Institute of Science and Technology (CN)
- Central South University (CN)
Publication Details
- Journal
- Small
- Published
- 2025-08-22
- DOI
- https://doi.org/10.1002/smll.202507895
- Citations
- 4
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 2.92
Funders
- National Natural Science Foundation of China