Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 7, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202114220
Keywords
all-solid-state lithium battery; laminar composite solid-state electrolyte; Li+ transfer; ordered LLTO crystal; vermiculite nanosheet
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Funding
- National Natural Science Foundation of China [U2004199]
- Excellent Youth Foundation of Henan Province [202300410373]
- China Postdoctoral Science Foundation [2021T140615, 2020M672281]
- Natural Science Foundation of Henan Province [212300410285]
- Young Talent Support Project of Henan Province [2021HYTP028]
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A 13 µm-thick laminar framework with 1.3 nm interlayer channels was fabricated by self-assembling vermiculite nanosheets, enabling high ionic conductivity of the LLTO electrolyte for all-solid-state lithium batteries. The ordered arrangement of LLTO crystal along the c-axis significantly enhances Li+ transfer and leads to excellent cycling performance.
Inorganic superionic conductor holds great promise for high-performance all-solid-state lithium batteries. However, the ionic conductivity of traditional inorganic solid electrolytes (ISEs) is always unsatisfactory owing to the grain boundary resistance and large thickness. Here, a 13 mu m-thick laminar framework with approximate to 1.3 nm interlayer channels is fabricated by self-assembling rigid, hydrophilic vermiculite (Vr) nanosheets. Then, Li0.33La0.557TiO3 (LLTO) precursors are impregnated in interlayer channels and afterwards in situ sintered to large-size, oriented, and defect-free LLTO crystal. We demonstrate that the confinement effect permits ordered arrangement of LLTO crystal along the c-axis (the fastest Li+ transfer direction), permitting the resultant 15 mu m-thick Vr-LLTO electrolyte an ionic conductivity of 8.22x10(-5) S cm(-1) and conductance of 87.2 mS at 30 degrees C. These values are several times' higher than that of traditional LLTO-based electrolytes. Moreover, Vr-LLTO electrolyte has a compressive modulus of 1.24 GPa. Excellent cycling performance is demonstrated with all-solid-state Li/LiFePO4 battery.
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