Temperature Dependence of Lithium Anode Voiding in Argyrodite Solid-State Batteries

Dominic Spencer Jolly, Ziyang Ning, Gareth O. Hartley, Boyang Liu, Dominic L. R. Melvin, Paul Adamson, James Marrow, Peter G. Bruce*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Void formation at the Li/ceramic electrolyte interface of an all-solid-state battery on discharge results in high local current densities, dendrites on charge, and cell failure. Here, we show that such voiding is reduced at the Li/Li6PS5Cl interface at elevated temperatures, sufficient to increase the critical current before voiding and cell failure from <0.25 mA cm-2 at 25 °C to 0.25 mA cm-2 at 60 °C and 0.5 mA cm-2 at 80 °C under a relatively low stack-pressure of 1 MPa. Increasing the stack-pressure to 5 MPa and temperature to 80 °C permits stable cycling at 2.5 mA cm-2. It is also shown that the charge-transfer resistance at the Li/Li6PS5Cl interface depends on pressure and temperature, with relatively high pressures required to maintain low charge-transfer resistance at -20 °C. These results are consistent with the plastic deformation of Li metal dominating the performance of the Li anode, posing challenges for the implementation of solid-state cells with Li anodes.

Original languageEnglish
Pages (from-to)22708-22716
Number of pages9
JournalACS Applied Materials and Interfaces
Volume13
Issue number19
Early online date7 May 2021
DOIs
Publication statusPublished - 19 May 2021

Bibliographical note

Funding Information:
P.G.B. is indebted to the Engineering and Physical Sciences Research Council (EPSRC) [EP/M009521/1], the Henry Royce Institute for Advanced Materials [EP/R00661X/1, EP/S019367/1, EP/R010145/1], and the Faraday Institution [FIRG007, FIRG008] for financial support. The X-ray tomography facilities were funded by EPSRC Grant [EP/M02833X/1] “University of Oxford: experimental equipment upgrade”.

Publisher Copyright:
© 2021 American Chemical Society.

Keywords

  • interfaces
  • lithium anode
  • solid-state battery
  • temperature dependence
  • X-ray tomography

ASJC Scopus subject areas

  • General Materials Science

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