High Energy Sulfide-Based All-Solid-State Lithium Batteries Enabled by Single-Crystal Li-Rich Cathodes
Yuqi Wu, Cheng Li, Xuefan Zheng, Wengao Zhao, Huanran Wang, Jiabao Gu, Yong Cheng, Yipeng Lin, Yu Su, Fucheng Ren, Dan Feng, Jun Liu, Jinxue Peng, Zhongwei Lv, Zhenyu Wang, Torsten Brezesinski, Zhengliang Gong, Yong Yang
Abstract
High-capacity Li-rich Mn-based oxides (LRMOs) show great potential for enhancing the energy density of all-solid-state lithium batteries (ASSLBs). However, the intrinsically low electronic/ionic conductivity of LRMOs and bulk structural degradation lead to an inferior electrochemical performance. Herein, a single-crystal Li 1.2 Ni 0.13 Mn 0.54 Co 0.13 O 2 (SC- LRMO) cathode is developed to address the challenges associated with charge-transport limitations and mechanical degradation of conventional polycrystalline (PC)-LRMO in ASSLBs. The results indicate that composite cathodes using small SC-LRMO achieve excellent electrochemical performance. Specifically, SC-LRMO not only delivers a high specific capacity of 316 mAh g –1 at 0.05C but also exhibits a capacity retention of 86% after 300 cycles at 1C, outperforming the PC-LRMO (243 mAh g –1, 84%). Comprehensive characterization reveals that the small single-crystal microstructure of SC-LRMO facilitates electrochemical reaction and mitigates detrimental mechanical degradation. Overall, this work expedites the practical application of LRMO cathodes in high-energy-density ASSLBs through dedicated morphology design.