Development of thin solid-state electrolyte with high ionic conductivity and mechanical strength is of great importance for high-performance all-solid-state lithium−sulfur battery. However, the state-of-the-art solid polymer electrolyte suffers from poor...

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Inorganic superionic conductor holds great promise for high-performance all-solid-state lithium batteries.H owever,t he ionic conductivity of traditional inorganic solid electrolytes (ISEs) is always unsatisfactory owingt ot he grain boundary resistance and large thickness.H ere,a13 mm-thick laminar framework with % 1.3 nm interlayer channels is fabricated by self-assembling rigid, hydrophilic vermiculite (Vr) nanosheets.T hen, Li 0.33 La 0.557 TiO 3 (LLTO)p recursors are impregnated in interlayer channels and afterwards in situ sintered to large-size,o riented, 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 mm-thick Vr-LLTO electrolyte an ionic conductivity of 8.22 10 À5 Scm À1 and conductance of 87.2 mS at 30 8 8C. These values are several times higher than that of traditional LLTO-based electrolytes. Moreover,Vr-LLTO electrolyte has acompressive modulus of 1.24 GPa. Excellent cycling performance is demonstrated with all-solid-state Li/LiFePO 4 battery.

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