Realizing long-cycling all-solid-state Li-In||TiS2 batteries using Li6+xMxAs1-xS5I (M=Si, Sn) sulfide solid electrolytes

Abstract

Inorganic sulfide solid-state electrolytes, especially Li₆PS₅X (X = Cl, Br, I), are considered viable materials for developing all-solid-state batteries because of their high ionic conductivity and low cost. However, this class of solid-state electrolytes suffers from structural and chemical instability in humid air environments and a lack of compatibility with layered oxide positive electrode active materials. To circumvent these issues, here, we propose Li_6+xM_xAs_1-xS₅I (M=Si, Sn) as sulfide solid electrolytes. When the Li_6+xSi_xAs_1-xS₅I (x = 0.8) is tested in combination with a Li-In negative electrode and Ti₂S-based positive electrode at 30 °C and 30 MPa, the Li-ion lab-scale Swagelok cells demonstrate long cycle life of almost 62500 cycles at 2.44 mA cm^-2, decent power performance (up to 24.45 mA cm^-2) and areal capacity of 9.26 mAh cm^-2 at 0.53 mA cm^-2.