title: Room-Temperature All-solid-state Rechargeable Sodium-ion Batteries with a Cl-doped Na3PS4 Superionic Conductor.
abstract: 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 Na3PS4 (t-Na3-xPS4-xClx) solid electrolyte with a room-temperature Na(+) conductivity exceeding 1 mS cm(-1). We demonstrate that an all-solid-state TiS2/t-Na3-xPS4-xClx/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" Na3PS4 has on the formation of an electronically insulating, ionically conducting solid electrolyte interphase.
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Iek-Heng
authors.initials: IH
authors.lastname: Chu
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Christopher S
authors.initials: CS
authors.lastname: Kompella
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Han
authors.initials: H
authors.lastname: Nguyen
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Zhuoying
authors.initials: Z
authors.lastname: Zhu
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Sunny
authors.initials: S
authors.lastname: Hy
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Zhi
authors.initials: Z
authors.lastname: Deng
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Ying Shirley
authors.initials: YS
authors.lastname: Meng
authors.affiliation: Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, Mail Code 0448, La Jolla, CA 92093, USA.
authors.forename: Shyue Ping
authors.initials: SP
authors.lastname: Ong