Enhancing interfacial stability in lithium orthosilicate/polymer blended novel hybrid solid-state electrolytes for all-solid-state lithium metal batteries

Hybrid solid-state electrolyte (HSSE) is a key component for the advancement of all-solid-state lithium metal batteries. The key challenges with the existing HSSEs are to ensure high ionic conductivity, activate dead inorganic/organic interface, and stimulate interfacial stability with electrodes. In this study, a novel HSSE is fabricated by integration of appropriately engineered end-of-life photovoltaic recycled high purity silicon derived nano size inorganic lithium orthosilicate and poly (vinylidene fluoride-co-hexafluoropropylene) polymer matrix through entrapping ionic liquid electrolytes. The obtained lithium orthosilicate-polymer blended HSSE is self-standing, soft, and flexible which delivers a low activation energy, leading a high ionic conductivity of 4.4 × 10 −4 Scm −1 . A critical lithium plating/stripping behaviour shows improved interfacial stability (both inorganic/organic interface and interfaces of HSSE/electrodes) under different current densities (0.05 mA cm −2 to 0.13 mA cm −2 ) when a drop of ionic liquid electrolyte is added, permitting cycling of an all-solid-state full cell (Li/HSSE/LiFePO 4 ) at room temperature with high capacity (132 mAh g −1 ), stable cycle life and high Coulombic efficiency (initial ∼98 %; subsequent >99.5 %). Shaping the interfaces between inorganic/organic phases in the HSSE as well as the interfaces between electrodes/HSSE appears to be a workable path towards constructing very effective HSSE for the advancement of all-solid-state lithium metal batteries. The obtained HSSE demonstrates remarkable structural integrity (including self-standing, soft, flexible, conductive and bendable) and incredible electrochemical properties, showing promising prospective for the development of all-solid-state lithium metal batteries. • A novel hybrid solid-state electrolyte (HSSE) is reported. • The obtained HSSE is ionically highly conductive, soft, and flexible. • The HSSE ensures higher Li + transport at the phase boundaries. • The HSSE delivers admirable battery performance.