Bulk/Interfacial Structure Design of Li-Rich Mn-Based Cathodes for All-Solid-State Lithium Batteries

作者：Wei-Jin Kong, Chen‐Zi Zhao, Liang Shen, Shuo Sun, Xueyan Huang, Pan Xu, Yangcheng Lü, Wenze Huang, Jinliang Li, Jia‐Qi Huang, Qiang Zhang · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c08115 · 被引用次数：108 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Extraction and Separation Processes

High Resolution Image Download MS PowerPoint Slide Li-rich Mn-based cathode materials (LRMO) are promising for enhancing energy density of all-solid-state batteries (ASSBs). Nonetheless, the development of efficient Li + /e – pathways is hindered by the poor electrical conductivity of LRMO cathodes and their incompatible interfaces with solid electrolytes (SEs). Herein, we propose a strategy of in - situ bulk/interfacial structure design to construct fast and stable Li + /e – pathways by introducing Li 2 WO 4, which reduces the energy barrier for Li + migration and enhances the stability of the surface oxygen structure. The reversibility of oxygen redox was improved, and the voltage decay of the LRMO cathode was addressed significantly. As a result, the bulk structure of the LRMO cathodes and the high-voltage solid–solid interfacial stability are improved. Therefore, the ASSBs achieve a high areal capacity (∼3.15 mAh/cm 2 ) and outstanding cycle stability of ≥1200 cycles with 84.1% capacity retention at 1 C at 25 °C. This study offers new insights into LRMO cathode design strategies for ASSBs, focusing on ultrastable high-voltage interfaces and high-loading composite electrodes.