Xiangkun Kong, Zongzi Jin, Linwang Chen, Xianzhun Huang, Bingzi Feng, Huang Huang, Yifan Xu, Weihao Wu, Wenkan Yang, Shiji Shen, Zhiwen Zhuo, Weiwei Ping, Ranran Peng, Chusheng Chen, Chengwei Wang
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 1/6-x (LaPrNdSrBa) 1/6 CoO 3-δ , based on oxidation-resistant electronic conductors. HE-O-MIEC exhibits an electronic conductivity of 1150 siemens per centimeter and a Li + conductivity of 2.3 × 10 −4 siemens per centimeter at room temperature. The enhanced Li + conductivity is attributed to the large configurational entropy, promoting multicomponent solubility and increased Li + concentration. HE-O-MIEC exhibits electrochemical and thermodynamic compatibility with LiCoO 2 and stabilizes ion/electron transport in the ASSLMB using the Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 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.