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The low lithium-ion conductivity of polyethylene oxide (PEO)-based polymer electrolytes limits their application in solid-state lithium batteries and related fields. Here, ionic liquids (ILs) are injected into hollow silicon nanorods (HSNRs) to prepare a composite solid polymer electrolyte (CSPE) with aligned HSNRs containing ILs (F-ILs@HSNRs). Applying a magnetic field promoted uniform dispersion and orientation of F-ILs@HSNRs in CSPE. The addition of F-ILs@HSNRs reduced PEO crystallinity and formed Li + transport pathways at the F-ILs@HSNRs/PEO interface. Calculations and multi-physics simulations reveal that ILs within F-ILs@HSNRs contribute most to lithium-ion conduction, followed by the F-ILs@HSNRs/PEO interface. When F-ILs@HSNRs are arranged perpendicular to the electrodes, the CSPE exhibits the shortest Li + migration pathways, resulting in stable and efficient lithium-ion conduction. The conductivity (2.14 × 10 -4 S cm -1 ) and lithium-ion migration number t Li+ (0.307) are the highest, being 125 times and 184% higher, respectively, than those of PEO-LiTFSI, when compared to CSPEs with randomly arranged or parallel-aligned F-ILs@HSNRs. Furthermore, Li|CSPE|Li batteries and LiFePO 4 |CSPE|Li batteries display stable cycling for over 2000 h, with coulombic efficiency approaching 100%. Excellent electrochemical reversibility is also confirmed in the rate performance test., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

In the current challenging energy storage and conversion landscape, solid-state lithium metal batteries with high energy conversion efficiency, high energy density, and high safety stand out. Due to the limitations of material properties, it is difficult to achieve the ideal requirements of solid electrolytes with a single-phase electrolyte. A composite solid electrolyte is composed of two or more different materials. Composite electrolytes can simultaneously offer the advantages of multiple materials. Through different composite methods, the merits of various materials can be incorporated into the most essential part of the battery in a specific form. Currently, more and more researchers are focusing on composite methods for combining components in composite electrolytes. The ion transport capacity, interface stability, machinability, and safety of electrolytes can be significantly improved by selecting appropriate composite methods. This review summarizes the composite methods used for the components of composite electrolytes, such as filler blending, embedded framework, and multilayer bonding. It also discusses the future development trends of all-solid-state lithium batteries (ASSLBs)., (© 2024 Wiley-VCH GmbH.)

Solid-state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid-state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self-supported three-dimensional porous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 framework, the as-assembled solid-state battery employing 4.5 V LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid-state nuclear magnetic resonance results reveal that Li + migrates fast along the continuous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 phase and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 /polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10 -4  S cm -1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 from being reduced by lithium metal. As a consequence of the compatible solid-solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid-state lithium metal battery., Competing Interests: The authors declare no conflict of interest., (© 2021 The Authors. Advanced Science published by Wiley‐VCH GmbH.)