Construction of single lithium-ion conducting solid-state electrolyte by amorphous metal-organic framework

Single-ion conductors are one of the methods to achieve efficient ionic conduction, which can be realized by introducing metal-organic frameworks (MOFs) into solid-state electrolytes. However, there is an interfacial mismatch between crystalline MOFs and amorphous polymers. Herein, we propose an effective method to convert crystalline MOFs into amorphous status rich in open metal sites (OMSs) and dangling bonds to construct high-speed ion transfer routes and tight interface contact for composite polymer electrolytes (CPEs). It has been discovered that CPEs fabricated by amorphous MOFs and polymers are capable of effectively controlling ion migration, thereby enabling the uniform deposition of Li⁺. As a result, the Li⁺ transference number reaches 0.87, and the ionic conductivity reaches 0.71 mS cm^-1. The Li||Li cell can stably cycle for more than 2400 h at a current density of 0.1 mA cm^-2, while the Li||NCM811 cell can still retain 84% of its initial capacity after 500 cycles at a rate of 0.2 C.