TY - JOUR
T1 - Revealing the role of liquid electrolytes in cycling of garnet-based solid-state lithium-metal batteries
AU - Yan, Shuo
AU - Abouali, Sara
AU - Yim, Chae Ho
AU - Zhou, Jigang
AU - Wang, Jian
AU - Baranova, Elena A.
AU - Weck, Arnaud
AU - Thangadurai, Venkataraman
AU - Merati, Ali
AU - Abu-Lebdeh, Yaser
N1 - The authors gratefully acknowledge financial support from the National Research Council of Canada (NRC) under the Low Emission Aviation Program (LEAP, A1-026222) and the Office of Energy Research & Development (OERD). They also specially thank James Sturman for the proofreading of the manuscript.
PY - 2022/8/25
Y1 - 2022/8/25
N2 - Solid-state lithium-metal batteries (SS-LMBs) suffer from the very high resistance at the garnet electrolyte/cathode interface that hampers their commercialization. Herein, a carbonate-based liquid electrolyte (LE) is introduced at the interface of a Li6.5La2.9Ba0.1Zr1.4Ta0.6O12 (LLBZTO) garnet/LiNi0.6Mn0.2Co0.2O2 (NMC 622) cathode to lower the interfacial resistance and improve the battery performance. In this work, we conducted a thorough study on the role of liquid electrolytes at the interface using scanning transmission X-ray microscopy (STXM) associated with X-ray absorption spectroscopy (XAS). As a result, we have shown new data related to the formation and the chemical composition of the two formed interphases: A solid-liquid electrolyte interphase (SLEI) and the cathode-electrolyte interphase (CEI). Furthermore, we have presented evidence that LE decomposes during cycling into fluoride species including LiF and LaF3, oxides like Li2O, and carbonates (i.e., Li2CO3) as the main components of in situ-formed SLEI. Based on the synergy between SLEI and CEI, we demonstrate Li|garnet|LE|NMC 622 cells cycled with an initial discharge capacity of 168 mAh g-1 and a capacity retention of ∼82% after 28 cycles. We expect that our study of SLEI will accelerate the implementation of a new hybrid electrolyte (solid garnet and liquid electrolyte) approach in SS-LMBs.
AB - Solid-state lithium-metal batteries (SS-LMBs) suffer from the very high resistance at the garnet electrolyte/cathode interface that hampers their commercialization. Herein, a carbonate-based liquid electrolyte (LE) is introduced at the interface of a Li6.5La2.9Ba0.1Zr1.4Ta0.6O12 (LLBZTO) garnet/LiNi0.6Mn0.2Co0.2O2 (NMC 622) cathode to lower the interfacial resistance and improve the battery performance. In this work, we conducted a thorough study on the role of liquid electrolytes at the interface using scanning transmission X-ray microscopy (STXM) associated with X-ray absorption spectroscopy (XAS). As a result, we have shown new data related to the formation and the chemical composition of the two formed interphases: A solid-liquid electrolyte interphase (SLEI) and the cathode-electrolyte interphase (CEI). Furthermore, we have presented evidence that LE decomposes during cycling into fluoride species including LiF and LaF3, oxides like Li2O, and carbonates (i.e., Li2CO3) as the main components of in situ-formed SLEI. Based on the synergy between SLEI and CEI, we demonstrate Li|garnet|LE|NMC 622 cells cycled with an initial discharge capacity of 168 mAh g-1 and a capacity retention of ∼82% after 28 cycles. We expect that our study of SLEI will accelerate the implementation of a new hybrid electrolyte (solid garnet and liquid electrolyte) approach in SS-LMBs.
U2 - 10.1021/acs.jpcc.2c02074
DO - 10.1021/acs.jpcc.2c02074
M3 - Article
AN - SCOPUS:85136715497
SN - 1932-7447
VL - 126
SP - 14027
EP - 14035
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 33
ER -