Design of High-Entropy Tape Electrolytes for Compression-Free Solid-State Batteries.

Advanced solid electrolytes with strong adhesion to other components are the key for the successes of solid-state batteries. Unfortunately, traditional solid electrolytes have to work under high compression to maintain the contact inside owing to their poor adhesion. Here, a concept of high entropy tape electrolyte (HETE) is proposed to simultaneously achieve tape-like adhesion, liquid-like ion-conduction and separator-like mechanical properties. This HETE is designed with adhesive skin-layer on both sides and robust skeleton-layer in the middle. The significant properties of the three layers are enabled by high-entropy microstructures which are realized by harnessing polymer-ion interactions. As a result, the HETE shows high ionic conductivity (3.50 ± 0.53×10-4 S cm-1 at R.T), good mechanical properties (toughness 11.28 ± 1.12 MJ m-3, strength 8.18 ± 0.28 MPa), and importantly, tape-like adhesion (interfacial toughness 231.6 ± 9.6 J m-2). Moreover, a compression-free solid-state tape battery is finally demonstrated by adhesion-based assembling, which shows good interfacial and electrochemical stability even under harsh mechanical conditions, such as twisting and bending. The concept of HETE and compression-free solid-state tape batteries may bring promising solutions and inspiration to conquer the interface challenges in solid-state batteries and their manufacturing. This article is protected by copyright. All rights reserved.