Affiliation:
1. Mechanical Engineering Department University of Louisville Louisville KY 40292 USA
2. Conn Center for Renewable Energy Research University of Louisville Louisville KY 40292 USA
3. NASA Glenn Research Center Cleveland OH 44135 USA
Abstract
AbstractSolid composite electrolytes (SCEs) have attracted serious attention for solid‐state Li metal batteries. In particular, SCEs that incorporate inorganic sulfide into polymer electrolytes provide a feasible approach to address the air sensitivity and (electro)chemical instability of sulfides. Nevertheless, there is still little research on pairing sulfide‐SCEs with high‐voltage cathodes. In this work, reports on efforts to synthesize and compare SCEs that embedding sulfides (Li7PS6 and Li3PS4) into PVDF/HFP polymer using a strong polar solvent (DMF). Two sulfides show distinct behaviors when dispersed in the DMF solvent. The Li7PS6‐SCE exhibits an ionic conductivity of 2.5 × 10−4 S cm−1 at room temperature, higher than the Li3PS4‐SCE (1.75 × 10−4 S cm−1). Moreover, Li7PS6‐SCE displays better electrochemical cycling performance in solid‐state Li metal batteries with LiNi1/3Mn1/3Co1/3O2 (NMC 111) cathode.. When increasing upper cut‐off voltages from 4.0 to 4.4 V, Li| Li7PS6‐SCE |NMC111 cells deliver higher discharge capacities but exhibit worse cycling stability. Interface analysis using X‐ray photoelectron spectroscopy (XPS) reveals the formation of LiF under a high voltage of 4.4 V, while t not present with 4.0 V. This work explores the synthesis of SCEs with different sulfides in a strong polar solvent and highlights the interface reactions between sulfide/PVDF‐HFP SCEs with oxide cathodes.