期刊
ADVANCED ENERGY MATERIALS
卷 11, 期 32, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202100836
关键词
all-solid-state Li-ion batteries; anodic (oxidation) stability; cathode-electrolyte interface; F-rich passivating interface; ultrahigh voltage
类别
资金
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Canada Research Chair Program (CRC)
- Canada Foundation for Innovation (CFI)
- Ontario Research Foundation (ORF)
- China Automotive Battery Research Institute Co., Ltd.
- Glabat Solid-State Battery Inc.
- University of Western Ontario (UWO)
- CFI
- NSERC
- National Research Council (NRC)
- Canadian Institutes of Health Research (CIHR)
- Government of Saskatchewan
- University of Saskatchewan
- National Science Foundation [1550423]
- Ontario Trillium Scholarship (OTS)
- Direct For Computer & Info Scie & Enginr
- Office of Advanced Cyberinfrastructure (OAC) [1550423] Funding Source: National Science Foundation
This study addresses the stability issue of solid-state electrolytes in high-voltage operations by designing a dual-halogen Li-ion conductor, improving both ionic conductivity and stability. The dual-halogen solid electrolyte shows great potential for high-voltage all-solid-state Li-ion batteries and provides a new design strategy for fast Li-ion conductors with high oxidation stability.
Solid-state electrolytes (SEs) with high anodic (oxidation) stability are essential for achieving all-solid-state Li-ion batteries (ASSLIBs) operating at high voltages. Until now, halide-based SEs have been one of the most promising candidates due to their compatibility with cathodes and high ionic conductivity. However, the developed chloride and bromide SEs still show limited electrochemical stability that is inadequate for ultrahigh voltage operations. Herein, this challenge is addressed by designing a dual-halogen Li-ion conductor: Li3InCl4.8F1.2. F is demonstrated to selectively occupy a specific lattice site in a solid superionic conductor (Li3InCl6) to form a new dual-halogen solid electrolyte (DHSE). With the incorporation of F, the Li3InCl4.8F1.2 DHSE becomes dense and maintains a room-temperature ionic conductivity over 10(-4) S cm(-1). Moreover, the Li3InCl4.8F1.2 DHSE exhibits a practical anodic limit over 6 V (vs Li/Li+), which can enable high-voltage ASSLIBs with decent cycling. Spectroscopic, computational, and electrochemical characterizations are combined to identify a rich F-containing passivating cathode-electrolyte interface (CEI) generated in situ, thus expanding the electrochemical window of Li3InCl4.8F1.2 DHSE and preventing the detrimental interfacial reactions at the cathode. This work provides a new design strategy for the fast Li-ion conductors with high oxidation stability and shows great potential to high-voltage ASSLIBs.
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