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

• Published in: ACS applied materials & interfaces Vol. 13; no. 19; pp. 22708 - 22716
• Main Authors: Spencer Jolly, Dominic, Ning, Ziyang, Hartley, Gareth O, Liu, Boyang, Melvin, Dominic L. R, Adamson, Paul, Marrow, James, Bruce, Peter G
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 19.05.2021
• Subjects: Energy, Environmental, and Catalysis Applications; X-ray tomography; lithium anode; temperature dependence; interfaces; solid-state battery
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.1c06706

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.