期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 31, 页码 34806-34814出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c07003
关键词
energy storage; all-solid-state batteries; solid electrolytes; chloride solid electrolytes; materials design
资金
- Technology Development Program to Solve Climate Changes of the National Research Foundation (NRF) - Ministry of Science ICT of Korea [2017M1A2A2044482]
- Development Program of Core Industrial Technology - Ministry of Trade, Industry AMP
- Energy of Korea [20007045]
- Korea Institute of Science and Technology [2E30202]
- Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences
- National Research Foundation of Korea [2E30211] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li3MCl6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li3MCl6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, TI, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li3MCl6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M3+ with Zr4+. Zr-substituted phase (Li2.5M0.5Zr0.5Cl6, M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li3MCl6 SEs could lead to superionic Li3MCl6 SEs.
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