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<p>Aqueous aluminum-ion batteries (AAIBs) are promising candidates for large-scale energy storage systems due to their inherent safety, the sustainability of aluminum resources, and theoretical high capacity. However, the sluggish electron/ion transport in conventional cathodes, such as metal-oxide cathodes, still limits their rate capability. To address the limitations of conventional materials, we first propose high-entropy engineering of metal oxides (HEOs) as cathodes in AAIBs, leveraging their unique “cocktail effect” and abundant electron transport pathways to significantly enhance the rate-capacity. The atomic-level interaction between different metal atoms broadens the d-band with reduced electronic level degeneracy towards HEOs, facilitating rapid electron transport with one of the best rate capability (119.4 mAh g<sup>−1</sup> at 10.0 A g<sup>−1</sup>) in metal-oxide cathodes. Meanwhile, the disordered layered oxides formed with a high-entropy framework have alleviated the strong electrostatic repulsion between aluminum ions and the fixed lattice, mitigating structural degradation and imparting excellent cycling stability towards the HEOs (over 95.1 mAh g<sup>−1</sup> after 500 cycles at 2.0 A g<sup>−1</sup>). Overall, the newly proposed HEOs cathodes in AAIBs pave the way for high-performance AAIBs and other aqueous multivalent metal ion batteries by rationally designing high-entropy engineering.</p>

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Entropy-driven modulation enables atomic-level interactions for high-rate capacity cathode materials in rechargeable aqueous aluminum-ion batteries

  • 期刊论文

  • 发表日期：

    2026年3月30日

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  • Kai Du,
  • Shaokang Su,
  • Chunhao Sun,
  • Shengjie Wei,
  • Yujie Liu,
  • Yunfei Yang,
  • Pengcheng Liu,
  • Mingshan Han,
  • Yixin Li,
  • Yuxiang Hu

摘要

Aqueous aluminum-ion batteries (AAIBs) are promising candidates for large-scale energy storage systems due to their inherent safety, the sustainability of aluminum resources, and theoretical high capacity. However, the sluggish electron/ion transport in conventional cathodes, such as metal-oxide cathodes, still limits their rate capability. To address the limitations of conventional materials, we first propose high-entropy engineering of metal oxides (HEOs) as cathodes in AAIBs, leveraging their unique “cocktail effect” and abundant electron transport pathways to significantly enhance the rate-capacity. The atomic-level interaction between different metal atoms broadens the d-band with reduced electronic level degeneracy towards HEOs, facilitating rapid electron transport with one of the best rate capability (119.4 mAh g−1 at 10.0 A g−1) in metal-oxide cathodes. Meanwhile, the disordered layered oxides formed with a high-entropy framework have alleviated the strong electrostatic repulsion between aluminum ions and the fixed lattice, mitigating structural degradation and imparting excellent cycling stability towards the HEOs (over 95.1 mAh g−1 after 500 cycles at 2.0 A g−1). Overall, the newly proposed HEOs cathodes in AAIBs pave the way for high-performance AAIBs and other aqueous multivalent metal ion batteries by rationally designing high-entropy engineering.