Advanced High-Entropy Halide Solid Electrolytes Enabling High-Voltage, Long-Cycling All-Solid-State Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 40015691.
- Also identified by DOI 10.1021/acs.nanolett.4c05460.
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Abstract
Stable solid electrolytes are essential for advancing the safety and energy density of lithium batteries, especially in high-voltage applications. In this study, we designed an innovative high-entropy chloride solid electrolyte (HE-5, Li<sub>2.2</sub>In<sub>0.2</sub>Sc<sub>0.2</sub>Zr<sub>0.2</sub>Hf<sub>0.2</sub>Ta<sub>0.2</sub>Cl<sub>6</sub>), using multielement doping to optimize both ionic conductivity and high-voltage stability. The high-entropy disordered lattice structure facilitates lithium-ion mobility, achieving an ionic conductivity of 4.69 mS cm<sup>-1</sup> at 30 °C and an activation energy of 0.300 eV. Integration of HE-5 into all-solid-state batteries (ASSBs) with NCM83 cathodes and a Li-In anode enables outstanding electrochemical performance, sustaining 70% capacity retention over 1600 cycles at a 4 C rate. Moreover, the high configurational entropy stabilizes the electrolyte's structure at elevated voltages, enabling stable operation at 5.0 V without significant degradation. Our work presents the dual advantages of high-entropy engineering in boosting high ionic conductivity and voltage stability, providing a broad roadmap for next-generation energy-dense ASSBs.