Super Long‐Cycling All‐Solid‐State Battery with Thin Li6PS5Cl‐Based Electrolyte

• Published in: Advanced energy materials 2022-07, Vol.12 (25), p.n/a
• Main Authors: Liu, Sijie, Zhou, Le, Han, Jian, Wen, Kaihua, Guan, Shundong, Xue, Chuanjiao, Zhang, Zheng, Xu, Ben, Lin, Yuanhua, Shen, Yang, Li, Liangliang, Nan, Ce‐Wen
• Format: Article
• Language: English
• Subjects: ASSLBs; composite solid electrolytes; Cycles; Electrolytes; Electrolytic cells; Ion currents; Ions; Li 6PS 5Cl; Lithium; Lithium niobates; Membranes; P(VDF‐TrFE); Room temperature; Solid electrolytes; sulfide electrolytes; Vinylidene; Vinylidene fluoride
• ISSN: 1614-6832; 1614-6840
• DOI: 10.1002/aenm.202200660

All‐solid‐state batteries (ASSBs) using sulfide electrolytes have attracted ever‐increasing interest due to high ionic conductivity of the sulfides. Nevertheless, a thin, strong solid‐state sulfide electrolyte membrane maintaining high ionic conductivity is highly desired for ASSBs. Here, a thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li6PS5Cl and a polar poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) framework is prepared via an electrospinning‐infiltration‐hot‐pressing method. The interaction between Li6PS5Cl and polar P(VDF‐TrFE) ensures a high lithium‐ion conductivity (≈1.2 mS cm–1) at room temperature and good mechanical ductility of the composite electrolyte membrane. The coin‐type ASSB cells with the thin composite electrolyte membrane, a composite cathode of LiNbO3‐coated LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl, and a lithium‐indium anode, show super cycling performance, and the capacity retention is 92% after 1000 cycles and 71% even after 20 000 cycles at 1.0 mA cm–2 (i.e., 1.61 C) at room temperature. Moreover, pouch‐type ASSB cells with a high mass loading of active materials are made to demonstrate the potential and feasibility in future commercial applications. A thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li6PS5Cl and a polar poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) framework, prepared via a facile electrospinning‐infiltration‐hot‐pressing method, enables super long‐cycling performance of all‐solid‐state batteries with a composite cathode of LiNbO3‐coated LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl.