Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 15, Pages 7012-7022Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c00134
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Funding
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- GLABAT Solid-State Battery Inc.
- China Automotive Battery Research Institute Co. Ltd
- Canada Research Chair Program (CRC)
- Canada Foundation for Innovation (CFI)
- Ontario Research Fund
- Canada Light Source at University of Saskatchewan (CLS)
- Canada MITACS fellowships
- University of Western Ontario
- National Science Foundation [1550423]
- Direct For Computer & Info Scie & Enginr
- Office of Advanced Cyberinfrastructure (OAC) [1550423] Funding Source: National Science Foundation
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The enabling of high energy density of all-solid-state lithium batteries (ASSLBs) requires the development of highly Lit-conductive solid-state electrolytes (SSEs) with good chemical and electrochemical stability. Recently, halide SSEs based on different material design principles have opened new opportunities for ASSLBs. Here, we discovered a series of LixScCl3+x SSEs (x = 2.5, 3, 3.5, and 4) based on the cubic close-packed anion sublattice with room-temperature ionic conductivities up to 3 x 10(-3) S cm(-1). Owing to the low eutectic temperature between LiCl and ScCl3, LixScCl3+x SSEs can be synthesized by a simple co-melting strategy. Preferred orientation is observed for all the samples. The influence of the value of x in LixScCl3+x, on the structure and Li+ diffusivity were systematically explored. With increasing x value, higher Li+, lower vacancy concentration, and less blocking effects from Sc ions are achieved, enabling the ability to tune the Li+ migration. The electrochemical performance shows that Li3ScCl6 possesses a wide electrochemical window of 0.9-4.3 V vs Li+/Li, stable electrochemical plating/stripping of Li for over 2500 h, as well as good compatibility with LiCoO2. LiCoO2/Li3ScCl6/In ASSLB exhibits a reversible capacity of 104.5 mAh g(-1) with good cycle life retention for 160 cycles. The observed changes in the ionic conductivity and tuning of the site occupations provide an additional approach toward the design of better SSEs.
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