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Effect of Liquid Electrolyte Soaking on the Interfacial Resistance of Li7La3Zr2O12 for All-Solid-State Lithium Batteries
Author(s) -
Münir M. Besli,
Camille Usubelli,
Michael Metzger,
Vikram Pande,
Katherine Harry,
Dennis Nordlund,
Sami Sainio,
Jake Christensen,
Marca M. Doeff,
Saravanan Kuppan
Publication year - 2020
Publication title -
acs applied materials and interfaces
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.535
H-Index - 228
eISSN - 1944-8252
pISSN - 1944-8244
DOI - 10.1021/acsami.0c06194
Subject(s) - materials science , lithium (medication) , electrolyte , solid state , chemical engineering , inorganic chemistry , chemistry , electrode , medicine , engineering , endocrinology
The impact of liquid electrolyte soaking on the interfacial resistance between the garnet-structured Li 7 La 3 Zr 2 O 12 (LLZO) solid electrolyte and metallic lithium has been studied. Lithium carbonate (Li 2 CO 3 ) 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 (LiBF 4 ) 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 Li 2 CO 3 is continuously removed with increasing soaking time. On-line mass spectrometry and free energy calculations show how LiBF 4 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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