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Eliminating interfacial O-involving degradation in Li-rich Mn-based cathodes for all-solid-state lithium batteries

Shuo SunBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaChen‐Zi ZhaoBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaHong YuanAdvanced Research Institute for Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaZhongheng FuBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaXiang ChenBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaYang LuBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaYun-Fan LiBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaJiang‐Kui HuAdvanced Research Institute for Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaJuncai DongBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, ChinaJia‐Qi HuangAdvanced Research Institute for Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaMinggao OuyangState Key Laboratory of Automotive Safety and Energy, School of Vehicle and Mobility, Tsinghua University, Beijing 100084, ChinaQiang ZhangBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
2022en
ABI

Аннотация

In the pursuit of energy-dense all-solid-state lithium batteries (ASSBs), Li-rich Mn-based oxide (LRMO) cathodes provide an exciting path forward with unexpectedly high capacity, low cost, and excellent processibility. However, the cause for LRMO|solid electrolyte interfacial degradation remains a mystery, hindering the application of LRMO-based ASSBs. Here, we first reveal that the surface oxygen instability of LRMO is the driving force for interfacial degradation, which severely blocks the interfacial Li-ion transport and triggers fast battery failure. By replacing the charge compensation of surface oxygen with sulfite, the overoxidation and interfacial degradation can be effectively prevented, therefore achieving a high specific capacity (~248 mAh g −1 , 1.1 mAh cm −2 ; ~225 mAh g −1 , 2.9 mAh cm −2 ) and excellent long-term cycling stability of >300 cycles with 81.2% capacity retention at room temperature. These findings emphasize the importance of irreversible anion reactions in interfacial failure and provide fresh insights into constructing stable interfaces in LRMO-based ASSBs.

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