A scalable and flexible hybrid solid electrolyte based on NASICON-structure Li3Zr2Si2PO12 for high-voltage hybrid batteries

Abstract

To enhance the safety and performance of high-voltage lithium-ion batteries (LIBs) with LiNi0.5Mn1.5O4 (LNMO) cathodes, we have developed an advanced hybrid solid electrolyte (HSE). This HSE comprises a porous- structured polymer-in-ceramic (PIC) Li3Zr2Si2PO12- Poly(vinylidene fluoride) (LZSP-PVDF) composite solid electrolyte (CSE) fabricated via a phase inversion method, with the addition of a minimal amount of liquid electrolyte. This unique design offers exceptional scalability, flexibility, and strong compatibility with lithium metal, effectively mitigating lithium dendrite formation. The HSE exhibits an ionic conductivity of 3.49 x 10-3 S cm- 1 at 30 degrees C, enabling stable operation of solid-state LIBs at ambient temperatures. Furthermore, when integrated with a high-voltage LNMO cathode, the HSE effectively suppresses side reactions due to Mn dissolution from the cathode, significantly improving cycling stability, lifespan, and rate performance. The Li/HSE/LNMO cell maintains 77.0% of its initial capacity after 130 cycles at 0.2 C, far surpassing the conventional Li/PE/LNMO cell, which retained only 49.5 %. These compelling results underscore the potential of the Li/HSE/LNMO configuration in advancing the development of high-voltage, solid-state LIBs for practical applications.