4.8 Article

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

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 19, Pages 22708-22716

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c06706

Keywords

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

Funding

  1. Engineering and Physical Sciences Research Council (EPSRC) [EP/M009521/1]
  2. Henry Royce Institute for Advanced Materials [EP/R00661X/1, EP/S019367/1, EP/R010145/1]
  3. Faraday Institution [FIRG007, FIRG008]
  4. EPSRC Grant University of Oxford: experimental equipment upgrade [EP/M02833X/1]
  5. EPSRC [EP/M009521/1, EP/M02833X/1] Funding Source: UKRI

Ask authors/readers for more resources

It has been found that void formation at the Li/Li6PS5Cl interface can be reduced at elevated temperatures, leading to an increase in critical current and stable cycling. However, the charge-transfer resistance at the Li/Li6PS5Cl interface is pressure and temperature dependent, posing challenges for the implementation of solid-state cells with Li anodes.
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 degrees C to 0.25 mA cm(-2) at 60 degrees C and 0.5 mA cm(-2) at 80 degrees C under a relatively low stack-pressure of 1 MPa. Increasing the stack-pressure to 5 MPa and temperature to 80 degrees 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 degrees 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.

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