Flexible self-supporting inorganic nanofiber membrane-reinforced solid-state electrolyte for dendrite-free lithium...

Compounding of suitable fillers with PEO-based polymers is the key to forming high-performance electrolytes with robust network structures and homogeneous Li⁺-transport channels. In this work, we innovatively and efficiently prepared Al₂O₃ nanofibers and deposited an aqueous dispersion of Al₂O₃ into a membrane via vacuum filtration to construct a nanofiber membrane with a three-dimensional (3D) network structure as the backbone of a PEO-based solid-state electrolyte. The supporting effect of the nanofiber network structure improved the mechanical properties of the reinforced composite solid-state electrolyte and its ability to inhibit the growth of Li dendrites. Meanwhile, interconnected nanofibers in the PEO-based electrolyte and the strong Lewis acid-base interactions between the chemical groups on the surface of the inorganic filler and the ionic species in the PEO matrix provided facilitated pathways for Li⁺ transport and regulated the uniform deposition of Li⁺. Moreover, the interaction between Al₂O₃ and lithium salts as well as the PEO polymer increased free Li⁺ concentration and maintained its stable electrochemical properties. Hence, assembled Li/Li symmetric cells achieved a cycle life of more than 2000 h. LFP/Li and NMC811/Li cells provided high discharge specific capacities of up to 146.9 mA h g^-1 (0.5C and 50 °C) and 166.9 mA h g^-1 (0.25C and 50 °C), respectively. The prepared flexible self-supporting 3D nanofiber network structure construction can provide a simple and efficient new strategy for the exploitation of high-performance solid-state electrolytes.