Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 18, Pages 20605-20612Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c06194
Keywords
LLZO; all-solid-state battery; lithium-ion battery; garnets; interfacial resistance
Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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The impact of liquid electrolyte soaking on the interfacial resistance between the garnet-structured Li7La3Zr2O12(LLZO) solid electrolyte and metallic lithium has been studied. Lithium carbonate (Li2CO3) formed by inadvertent exposure of LLZO to ambient conditions is generally known to increase interfacial impedance and decrease lithium wettability. Soaking LLZO powders and pellets in the electrolyte containing lithium tetrafluoroborate (LiBF4) shows a significantly reduced interfacial resistance and improved contact between lithium and LLZO. Raman spectroscopy, X-ray diffraction, and soft X-ray absorption spectroscopy reveal how Li2CO3 is continuously removed with increasing soaking time. On-line mass spectrometry and free energy calculations show how LiBF4 reacts with surface carbonate to form carbon dioxide. Using a very simple and scalable process that does not involve heat-treatment and expensive coating techniques, we show that the Li-LLZO interfacial resistance can be reduced by an order of magnitude.
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