Mechanically Interlocked Polymer Electrolyte with Built‐In Fast Molecular Shuttles for All‐Solid‐State Lithium Batteries
Jiae Seo, Jiae Seo, Gwang‐Hee Lee, Joon Hur, Myeong‐Chang Sung, Ji‐Hun Seo, Ji‐Hun Seo, Dong‐Wan Kim
Abstract
Abstract The mobility of molecular shuttles inside a mechanically interlocked polymer (MIP) can improve the ionic conductivity and electron transport capacity of a solid polymer electrolyte (SPE) and maintain a mechanically tough structure. The polyrotaxane‐based MIP electrolyte with a necklace‐like molecular structure exhibits high ionic conductivity (σ = 5.93 × 10 −3 S cm −1 at 25 °C and 1.44 × 10 −2 S cm −1 at 60 °C), a high Li + ion transference number ( t + = 0.71), and high electrochemical oxidation stability (≈4.7 V vs Li + /Li). When SPEs are used in Li‐based batteries, a high Coulombic efficiency (≥98.5%), an excellent rate capability, and fast charging (≥2C) can be achieved using a “built‐in molecular shuttle” design.