Journal
CHEMICAL ENGINEERING JOURNAL
Volume 442, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136154
Keywords
Composite solid-state electrolyte; Interfacial phase construction; Lithium polymeric salt; In-situ polymerization; Solvent-free process
Categories
Funding
- National Natural Science Foundation of China [51872159, 51572145]
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Solid-state lithium metal batteries are a promising direction for developing lithium-based energy storage devices due to their superior energy density and safety performance compared to lithium-ion batteries with liquid electrolytes. However, the design, preparation, and optimization of solid-state electrolytes, particularly composite solid-state electrolytes, still face challenges in construction and composite processes. This study proposes and designs a method to construct a highly compatible and lithium-ion conductive interfacial phase, which improves the cycle performance and stability of composite solid electrolytes in lithium metal batteries. Two different modification methods are investigated to demonstrate the practical value of this design, showing enhanced ionic conductivity and electrochemical stability.
The solid-state lithium metal batteries are considered a promising direction for developing lithium-based energy storage devices because of their superiority over lithium-ion batteries containing liquid electrolytes in energy density and safety performance. However, the design, preparation, and optimization of solid-state electrolytes (SSEs), especially composite solid-state electrolytes (CSEs), still face critical construction design and composite process challenges. This work proposes and designs a method to construct a highly compatible and lithium-ion conductive interfacial phase by coating the inorganic phase with polymeric lithium salt in the composite solid electrolytes. The introduction of the lithium salt interfacial phase efficiently improves the cycle performance and stability of CSEs in lithium metal batteries by synergistic optimization of the composite interfacial phase. We investigate two different modification methods (solvent-free and in-situ methods) in two different inorganic systems (Li6.4La3Zr1.4Ta0.6O12 (LLZTO) and LiTa2PO8 (LTPO)) to demonstrate the practical value of this design. The highest ionic conductivity of the modified PEO/LTPO CSEs (50 wt%) can be improved to 9.3 x 10(-4) S.cm(-1) at 80 degrees C and 4.0 x 10(-5 )at RT (~25 degrees C, hereinafter inclusive), while those of the modified PEO/LLZTO CSEs can reach 1.4 x 10(-3) S.cm(-1) at 80 degrees C and 5.5 x 10(-5) at RT. The results demonstrate that the interfacial phase also enhances the electrochemical and cycle stability of CSEs.
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