<p>All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability<sup><CitationRef AdditionalCitationIDS="CR2" CitationID="CR1">1</CitationRef>–<CitationRef CitationID="CR3">3</CitationRef></sup>. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li<sup>+</sup>/<i>e</i><sup>−</sup> conductivity, mechanical robustness and structural stability<sup><CitationRef AdditionalCitationIDS="CR5 CR6 CR7 CR8 CR9 CR10 CR11 CR12 CR13" CitationID="CR4">4</CitationRef>–<CitationRef CitationID="CR14">14</CitationRef></sup>. Here we present Li<sub>1.3</sub>Fe<sub>1.2</sub>Cl<sub>4</sub>, a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe<sup>2+</sup>/Fe<sup>3+</sup> redox and rapid Li<sup>+</sup>/<i>e</i><sup>−</sup> transport within its framework, Li<sub>1.3</sub>Fe<sub>1.2</sub>Cl<sub>4</sub> achieves an electrode energy density of 529.3 Wh kg<sup>−1</sup> versus Li<sup>+</sup>/Li. Critically, Li<sub>1.3</sub>Fe<sub>1.2</sub>Cl<sub>4</sub> shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li<sub>1.3</sub>Fe<sub>1.2</sub>Cl<sub>4</sub> with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg<sup>−1</sup>. By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.</p>

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A cost-effective all-in-one halide material for all-solid-state batteries

  • Jiamin Fu,
  • Changhong Wang,
  • Shuo Wang,
  • Joel W. Reid,
  • Jianwen Liang,
  • Jing Luo,
  • Jung Tae Kim,
  • Yang Zhao,
  • Xiaofei Yang,
  • Feipeng Zhao,
  • Weihan Li,
  • Bolin Fu,
  • Xiaoting Lin,
  • Yang Hu,
  • Han Su,
  • Xiaoge Hao,
  • Yingjie Gao,
  • Shutao Zhang,
  • Ziqing Wang,
  • Jue Liu,
  • Hamid Abdolvand,
  • Tsun-Kong Sham,
  • Yifei Mo,
  • Xueliang Sun

摘要

All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability13. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li+/e conductivity, mechanical robustness and structural stability414. Here we present Li1.3Fe1.2Cl4, a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe2+/Fe3+ redox and rapid Li+/e transport within its framework, Li1.3Fe1.2Cl4 achieves an electrode energy density of 529.3 Wh kg−1 versus Li+/Li. Critically, Li1.3Fe1.2Cl4 shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li1.3Fe1.2Cl4 with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg−1. By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.