The need for safe storage systems with a high energy density has increased the interest in high-voltage solid-state Li-metal batteries (LMBs). Solid-state electrolytes, as a key material for LMBs, must be stable against both high-voltage cathodes and Li anodes. However, the weak interfacial contact between the electrolytes and electrodes poses challenges in the practical applications of LMBs. In this study, a double-layered solid composite electrolyte (DLSCE) was synthesized by introducing an antioxidative poly­(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP)-10 wt % Li1.3Al0.3Ti1.7(PO4)3 (LATP) to the cathode interface, whereas a lithium-friendly poly­(oxyethylene) (PEO)-5 wt % LATP was made to come into contact with Li metal. Owing to the heterogeneous double-layered structure of the DLSCE, a high ionic transfer number (0.43), high ionic conductivity (1.49 × 10–4 S/cm), and a wide redox window (4.82 V) were obtained at ambient temperature. Moreover, the DLSCE showed excellent Li-metal stability, thereby enabling the Li–Li symmetric cells to stably run for over 600 h at 0.2 mA/cm2 with effective lithium dendrite inhibition. When paired with a high-voltage LiNi1/3Co1/3Mn1/3O2 cathode, the Li/DLSCE/NCM111 cell exhibited excellent electrochemical performance: long-term cyclability with 85% capacity retention could be conducted at 0.2C after 100 cycles corresponding to 100% Coulombic efficiencies.

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In this study, V2O3@carbon nanofibers as flexible anode materials were synthesized via electrospinning. The electrode showed a specific discharge capacity with 495 mA h g–1 at 1000 mA g–1 after 1000 cycles. Surprisingly, the electrode fabricated from the V2O3@carbon nanofibers exhibited a specific capacity of 336 mA h g–1 at 5000 mA g–1. Even after 10,000 cycles, it still displayed a specific discharge capacity of 290 mA h g–1, indicating that it has outstanding capacity advantages and long-cycle lifespan. The large specific surface area and abundant active sites of urchinlike V2O3 were considered as the reasons for its outstanding electrochemical performance. The combination of V2O3 and the carbon nanofibers formed a complete conductive network that enhanced the conductivity of the sample, reduced the diffusion path of Li+, and eased the volume change during intercalation/deintercalation of Li+. These results not only demonstrated that the flexible V2O3@carbon nanofibers prepared herein have broad application prospects as an anode for LIBs but also offer a processing strategy for fabricating other state-of-the-art flexible electrode materials for energy storage systems.