Microscopic Segregation Dominated Nano-Interlayer Boosts 4.5 V Cyclability and Rate Performance for Sulfide-Based All-Solid-State Lithium Batteries

Wei He; Niaz Ahmad; Shaorui SunXiao ZhangLeguan RanRuiwen ShaoXuefeng WangWen Yang

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Microscopic Segregation Dominated Nano-Interlayer Boosts 4.5 V Cyclability and Rate Performance for Sulfide-Based All-Solid-State Lithium Batteries

机译：Microscopic Segregation Dominated Nano-Interlayer Boosts 4.5 V Cyclability and Rate Performance for Sulfide-Based All-Solid-State Lithium Batteries

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To implement the growing requirement for higher energy density all-solid-state lithium batteries (ASSLBs), further increasing the working voltage of LiCoO_2 (LCO) is a key to breaking through the bottleneck. However, LiCoO_2 severe structural degradation and side reactions at the cathode interface obstruct the development of high-voltage sulfide-based ASSLBs (≥4.5 V). Herein, a nanometric Li_(1.175)Nb_(0.645)Ti_(0.4)O_3 (LNTO) coated LCO cathode where microscopic Ti and Nb segregation at the interface during cycling potentially stabilizes the cathode lattice, and minimizes side reactions, simultaneously, is designed. Advanced transmission electron microscopy reveals that the stable spinel phase minimizes the micro stress at the cathode interface, avoids structure fragmentation, and hence significantly enhances the long-term cyclic stability of LNTO@LCO @ 4.5 V. Moreover, the differential phase contrast scanning transmission electron microscopy (DPC-STEM) visualizes the nano-interlayer LNTO to boost Li+ migration at the cathode interface. Electrochemical impedance spectroscopy (EIS) reveals that sulfide-based cells with the LNTO nanolayer effectively reduce the interfacial resistance to 140 Ω compared to LiNbO_3 (235 Ω) over 100 cycles. Therefore, 4.5 V sulfide-based ASSLBs offer gratifying long-cycle stability (0.5 C for 1000 cycles, 88.6%), better specific capacity, and rate performance (179.8 mAh g~(-1) at 0.1 C, 97 mAh g~(-1) at 2 C).

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来源
《Advanced energy materials》 |2023年第3期|2203703.1-2203703.13|共13页
作者
Wei He; Niaz Ahmad; Shaorui SunXiao ZhangLeguan RanRuiwen ShaoXuefeng WangWen Yang;
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作者单位

Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology 5# Zhongguancun Road, Haidian District,;

Beijing Key Laboratory for Green Catalysis and Separation College of Environmental and Energy Engineering Beijing University of Technology Beijing 100124, China;

Beijing Advanced Innovation Center for Intelligent Robots and Systems Institute of Engineering Medicine Beijing Institute of Technology Beijing 100081, ChinaBeijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100081, China,College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Science Beijing 100049, China;

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ASSLBs; coating layers; high voltage; microscopic segregation; sulfide electrolytes;

Microscopic Segregation Dominated Nano-Interlayer Boosts 4.5 V Cyclability and Rate Performance for Sulfide-Based All-Solid-State Lithium Batteries

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