Early View e202510773
Research Article

Self-Adapting Lattice Respiration Enabled by Crystal Design and d-p Orbital Hybridization Toward Highly Stable Rechargeable Aluminum Batteries

Huaizhi Wang

Huaizhi Wang

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

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Dr. Yu Li

Corresponding Author

Dr. Yu Li

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

Yangtze Delta Region Academy of Beijing Institute of Technology, Jiaxing, 314019 P.R. China

E-mail: [email protected], [email protected], [email protected]

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Bo Long

Bo Long

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

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Shuqiang Li

Shuqiang Li

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

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Xueying Lu

Xueying Lu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

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Shijie Zhou

Shijie Zhou

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

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Prof. Feng Wu

Prof. Feng Wu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

Yangtze Delta Region Academy of Beijing Institute of Technology, Jiaxing, 314019 P.R. China

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Prof. Ying Bai

Corresponding Author

Prof. Ying Bai

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

Yangtze Delta Region Academy of Beijing Institute of Technology, Jiaxing, 314019 P.R. China

E-mail: [email protected], [email protected], [email protected]

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Prof. Chuan Wu

Corresponding Author

Prof. Chuan Wu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 P.R. China

Yangtze Delta Region Academy of Beijing Institute of Technology, Jiaxing, 314019 P.R. China

E-mail: [email protected], [email protected], [email protected]

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First published: 25 June 2025

Graphical Abstract

Based on the dual considerations of crystal structure and electronic structure, we construct cathodes with “self-adapting lattice respiration (SALR)” effect. The effect effectively addresses the poor cycle stability of transition metal-based RABs cathodes caused by the strong electrostatic interaction between high charge density Al3+ and host lattice.

Abstract

Rechargeable aluminum batteries (RABs) are promising for large-scale energy storage due to the appealing three-electron transfer feature, low cost, and high safety. However, the strong electrostatic interaction between Al3+ and host lattice induces severe lattice distortion and structural collapse, leading to poor cycle stability in RABs. Herein, we develop a new-type FeWO4 cathode with a comprehensive consideration of the crystal structure and electronic structure. The 3D open framework and strong W─O covalent network of the FeWO4 greatly improve the storage of high charge density Al3+. Moreover, the d-p orbital hybridization between the transition metal and oxygen facilitates electron delocalization, which effectively weakens the interaction with the trivalent cation (Al3+). Importantly, combining in situ characterizations and theoretical calculations, it is demonstrated that as-prepared cathode exhibits a “self-adapting lattice respiration” (SALR) effect. Specifically, the reversible W–O bond elongation/compression (Δd ≈ 0.05 Å) during cycling reduces lattice strain and confines volume expansion to less than 3%. As results, the FeWO4 cathode delivers a high capacity of 192 mAh g−1 at 500 mA g−1 and long cycle life of over 2300 cycles with quiet low capacity decay of 0.01% per cycle in RABs.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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