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All-solid-state sodium-ion batteries are promising candidates for large-scale energy storage applications. The key enabler for an all-solid-state architecture is a sodium solid electrolyte that exhibits high Na +  conductivity at ambient temperatures, as well as excellent phase and electrochemical stability. In this work, we present a first-principles-guided discovery and synthesis of a novel Cl-doped tetragonal Na 3 PS 4  (t-Na 3− x  PS 4− x  Cl  x  ) solid electrolyte with a room-temperature Na +  conductivity exceeding 1 mS cm −1 . We demonstrate that an all-solid-state TiS 2 /t-Na 3− x  PS 4− x  Cl  x  /Na cell utilizing this solid electrolyte can be cycled at room-temperature at a rate of C/10 with a capacity of about 80 mAh g −1  over 10 cycles. We provide evidence from density functional theory calculations that this excellent electrochemical performance is not only due to the high Na +  conductivity of the solid electrolyte, but also due to the effect that “salting” Na 3 PS 4  has on the formation of an electronically insulating, ionically conducting solid electrolyte interphase.

Room-Temperature All-solid-state Rechargeable Sodium-ion Batteries with a Cl-doped Na3PS4 Superionic Conductor