A high-entropy mixed ionic and electronic conductor for accelerating the cathode dynamics in all solid-state lithium metal batteries.

Kong, Xiangkun; Jin, Zongzi; Chen, Linwang; Huang, Xianzhun; Feng, Bingzi; Huang, Huang; Xu, Yifan; Wu, Weihao et al. · Sci Adv · 2025

basic_science · Level V

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Abstract

Both electron and ion transports determine the dynamics of the cathode in all solid-state lithium metal batteries (ASSLMBs). Traditional composite strategies combining solid electrolytes and electronic conductors cause complex solid-state interfaces that hinder carrier migration. We present a high-entropy mixed ionic and electronic conductor (HE-O-MIEC), Li<sub>1/6-x</sub>(LaPrNdSrBa)<sub>1/6</sub>CoO<sub>3-δ</sub>, based on oxidation-resistant electronic conductors. HE-O-MIEC exhibits an electronic conductivity of 1150 siemens per centimeter and a Li<sup>+</sup> conductivity of 2.3 × 10<sup>-4</sup> siemens per centimeter at room temperature. The enhanced Li<sup>+</sup> conductivity is attributed to the large configurational entropy, promoting multicomponent solubility and increased Li<sup>+</sup> concentration. HE-O-MIEC exhibits electrochemical and thermodynamic compatibility with LiCoO<sub>2</sub> and stabilizes ion/electron transport in the ASSLMB using the Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> electrolyte. Without organic electrolyte or additional pressure, the ASSLMB achieves 115-milliampere·hours per gram initial discharge capacity at 30°C and retains 83% capacity after 500 cycles. Homogeneous electron and ion transport in the HE-O-MIEC demonstrates potential to improve active material utilization and address interfacial challenges in ceramic-based ASSLMBs.