A cost-effective all-in-one halide material for all-solid-state batteries
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- doe_osti · checked 2025-06-25
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All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability. 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>/e<sup>−</sup> conductivity, mechanical robustness and structural stability. Here, in this work, 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>/e<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.. Authors: Fu, Jiamin [Univ. of Western Ontario, London, ON (Canada)] (ORCID:000000021874111X); Wang, Changhong [Univ. of Western Ontario, London, ON (Canada); Eastern Institute of Technology (China); Ningbo Key Laboratory of All-Solid-State Battery (China)]; Wang, Shuo [Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000279079676); Reid, Joel W. [Univ. of Saskatchewan, Saskatoon, SK (Canada)] (ORCID:0000000174158642); Liang, Jianwen [Foshan Key Laboratory of Advanced Electrochemical Functional Materials and Technology (China)]. DOE Contract: AC05-00OR22725. Subjects: 25 ENERGY STORAGE; batteries; chemical physics