Spatially Confined Engineering Toward Deep Eutectic Electrolyte in Metal-Organic Framework Enabling Solid-State Zinc-Ion Batteries.

Uncontrollable interfacial side reactions generated from common aqueous electrolytes, just like the hydrogen evolution reaction (HER) and dendrite growth, have severely prevented the practical application of zinc-ion batteries (ZIBs). Solid-state ZIBs are considered to be an efficient strategy by adopting high-quality solid-state electrolytes (SSEs). Here, by confining deep eutectic electrolyte (DEE) into the nanochannels of metal-organic framework (MOF)-PCN-222, a stable DEE@PCN-222 SSE with internal Zn 2+ transport channels was obtained. A distinctive ion-transport network composed of DEE and PCN-222 in the interior of DEE@PCN-222 realizes the efficient Zn 2+ conduction, contributing to high ionic conductivity of 3.13×10 -4  S cm -1 at room temperature, low activation energy of 0.12 eV, and a high Zn 2+ transference number of 0.74. Furthermore, experimental and theoretical investigations demonstrate that DEE@PCN-222 with its unique channel structure could homogeneously regulate the Zn 2+ distribution and effectively alleviate the side reactions. Highly reversible Zn plating/stripping performance of 2476 h can be realized by the SSE. The solid-state ZIBs show a specific capacity of 306 mAh g -1 and display cycling stability of 517 cycles. This unique design concept provides a new perspective in realizing the high-safety and high-performance ZIBs.