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electric vehicles because of their high energy density and long cycle life, etc. However, traditional LIBs are composed of organic liquid electrolytes in which there exists latent danger of fire and even explosion. [1] Thanks to the remarkable mechanical strength and inflammable nature of solid-state electrolytes, solid-state batteries (SSBs) are expected to address the critical safety issues of the traditional LIBs. [2] Simultaneously, the solid-state electrolytes are capable to resist the growth of lithium dendrites enabling possible use of lithium-metal anodes to replace graphite thus markedly improving the energy density.With the discovery of sodium super ion conductor (NASICON) in 1976 by Goodenough et al., [3] numerous research has been focused on oxide ceramic electrolytes (OCEs), including several crystal structures like NASICON-type, perovskite-type, LISICON-type (lithium superionic conductor), and garnet-type, etc. [4] The OCEs have been shown to be very promising for the development of SSBs given their advantages of high ionic conductivity (10 −4 -10 −3 S cm −1 at 25 °C), wide electrochemical High room-temperature ionic conductivities, large Li + -ion transference numbers, and good compatibility with both Li-metal anodes and high-voltage cathodes of the solid electrolytes are the essential requirements for practical solid-state lithium-metal batteries. Herein, a unique "superconcentrated ionogel-in-ceramic" (SIC) electrolyte prepared by an in situ thermally initiated radical polymerization is reported. Solid-state static 7 Li NMR and molecular dynamics simulation reveal the roles of ceramic in Li + local environments and transport in the SIC electrolyte. The SIC electrolyte not only exhibits an ultrahigh ionic conductivity of 1.33 × 10 −3 S cm −1 at 25 °C, but also a Li + -ion transference number as high as 0.89, together with a low electronic conductivity of 3.14 × 10 −10 S cm −1 and a wide electrochemical stability window of 5.5 V versus Li/Li + . Applications of the SIC electrolyte in Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 and Li||LiFePO 4 batteries further demonstrate the high rate and long cycle life. This study, therefore, provides a promising hybrid electrolyte for safe and high-energy lithium-metal batteries.

We report rare-earth triflate catalyst Sc(OTf)3 for ring-opening polymerization of 1,3-dioxolane in-situ producing quasi-solid-state poly(1,3-dioxolane) electrolyte, which not only demonstrates superior ionic conductivity of 1.07 mS cm-1 at room temperature,...

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Exploring quasi-solid electrolytes with superior ionic conductivities, wide electrochemical stability window, desirable compatibility toward lithium metal, and facile processability for high-energy lithium metal batteries remains a challenge. In this work, all of these issues are fully addressed via a composite hybrid design, of which poly­(ethylene oxide) (PEO) is used as a polymeric host and guarantees the interfacial compatibility toward lithium metal, highly conductive and thermally stable ionogel aims at suppressing PEO crystallization and enhancing conductivity, and garnet conductor enhances mechanical and electrochemical stabilities. Such a composite hybrid design yields the required quasi-solid electrolyte, which not only shows a high ionic conductivity of 7.4 × 10–4 S cm–1 at 25 °C but also extends the electrochemical stability window to 5.5 V vs Li/Li+, demonstrated with the interacted and monolithic structure of the composite hybrid quasi-solid electrolyte by XPS. Moreover, the composite hybrid quasi-solid electrolyte suppresses dendrite growth with a current density up to 0.7 mA cm–2. The quasi-solid Li∥LiNi0.5Co0.2Mn0.3O2 and Li∥LiFePO4 cells using this composite hybrid quasi-solid electrolyte are demonstrated. This study suggests that engineering integration of ionogel, polymer, and inorganic conductor offers an alternative to explore new electrolytes for lithium metal batteries.

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