Solid-state lithium batteries (SSLBs) are promising owing to enhanced safety and high energy density but plagued by the relatively low ionic conductivity of solid-state electrolytes and large electrolyte-electrode interfacial resistance. Herein, we design a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based polymer-in-salt solid electrolyte (PISSE) with high room-temperature ionic conductivity (1.24 10 À4 S cm À1 ) and construct a model integrated TiO 2 /Li SSLB with 3D fully infiltration of solid electrolyte. With forming aggregated ion clusters, unique ionic channels are generated in the PISSE, providing much faster Li + transport than common polymer electrolytes. The integrated device achieves maximized interfacial contact and electrochemical and mechanical stability, with performance close to liquid electrolyte. A pouch cell made of 2 SSLB units in series shows high voltage plateau (3.7 V) and volumetric energy density comparable to many commercial thin-film batteries.

Solid-state lithium batteries (SSLBs) are promising owing to enhanced safety and high energy density but plagued by the relatively low ionic conductivity of solid-state electrolytes and large electrolyte-electrode interfacial resistance. Herein, we design a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based polymer-in-salt solid electrolyte (PISSE) with high room-temperature ionic conductivity (1.24 10 À4 S cm À1 ) and construct a model integrated TiO 2 /Li SSLB with 3D fully infiltration of solid electrolyte. With forming aggregated ion clusters, unique ionic channels are generated in the PISSE, providing much faster Li + transport than common polymer electrolytes. The integrated device achieves maximized interfacial contact and electrochemical and mechanical stability, with performance close to liquid electrolyte. A pouch cell made of 2 SSLB units in series shows high voltage plateau (3.7 V) and volumetric energy density comparable to many commercial thin-film batteries.

Solid-state polymer lithium-ion batteries with better safety and higher energy density are one of the most promising batteries, which are expected to power future electric vehicles and smart grids. However, the low ionic conductivity at room temperature of solid polymer electrolytes (SPEs) decelerates the entry of such batteries into the market. Creating polymer-in-salt solid electrolytes (PISSEs) where the lithium salt contents exceed 50[Formula: see text]wt.% is a viable technology to enhance ionic conductivity at room temperature of SPEs, which is also suitable for scalable production. In this review, we first clarify the structure and ionic conductivity mechanism of PISSEs by analyzing the interactions between lithium salt and polymer matrix. Then, the recent advances on polyacrylonitrile (PAN)-based PISSEs and polycarbonate derivative-based PISSEs will be reviewed. Finally, we propose possible directions and opportunities to accelerate the commercializing of PISSEs for solid polymer Li-ion batteries.

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