TY - JOUR
T1 - Revisiting the LiPON/Li thin film as a bifunctional interlayer for NASICON solid electrolyte-based lithium metal batteries
AU - Lee, Seunghwan
AU - Jung, Sehun
AU - Yang, Sungeun
AU - Lee, Jong Ho
AU - Shin, Hyunjung
AU - Kim, Joosun
AU - Park, Sangbaek
N1 - Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/6/1
Y1 - 2022/6/1
N2 - Emerging solid-state lithium batteries demand a stable solid electrolyte against both Li anodes and high-voltage cathodes. The NASICON-type Li1.5Al0.5Ge1.5(PO4)3 (LAGP) solid electrolyte is highly tolerant to high-voltage operation and air environments, but it suffers from poor interfacial compatibility with Li anodes. Herein, we revisit the Li/LiPON bilayer thin-film in mature and ultrastable thin-film batteries as a bifunctional interlayer that can resolve both chemical and mechanical interfacial problems between Li anodes and LAGP. Interestingly, defect-free contact of the Li thin film onto LiPON/LAGP dramatically reduces the anode interface impedance between LAGP and Li foil, which eliminates the step for Li foil heating. As a result, it delivers a high capacity and rate capability with a long cycle in all-solid-state Li-O2 batteries. Moreover, by virtue of a systematic thin-film configuration, a model study with different interlayer combinations as well as LiPON thicknesses clearly distinguishes two degradation mechanisms in LAGP-based cells: chemical reduction of Ge at the anode interface and mechanical contact loss by nonuniform Li stripping/plating upon cycling. Thanks to its exceptional electrochemical stability window, this Li/LiPON-modified LAGP will help to achieve the commercialization of safe and long-lasting solid-state lithium batteries.
AB - Emerging solid-state lithium batteries demand a stable solid electrolyte against both Li anodes and high-voltage cathodes. The NASICON-type Li1.5Al0.5Ge1.5(PO4)3 (LAGP) solid electrolyte is highly tolerant to high-voltage operation and air environments, but it suffers from poor interfacial compatibility with Li anodes. Herein, we revisit the Li/LiPON bilayer thin-film in mature and ultrastable thin-film batteries as a bifunctional interlayer that can resolve both chemical and mechanical interfacial problems between Li anodes and LAGP. Interestingly, defect-free contact of the Li thin film onto LiPON/LAGP dramatically reduces the anode interface impedance between LAGP and Li foil, which eliminates the step for Li foil heating. As a result, it delivers a high capacity and rate capability with a long cycle in all-solid-state Li-O2 batteries. Moreover, by virtue of a systematic thin-film configuration, a model study with different interlayer combinations as well as LiPON thicknesses clearly distinguishes two degradation mechanisms in LAGP-based cells: chemical reduction of Ge at the anode interface and mechanical contact loss by nonuniform Li stripping/plating upon cycling. Thanks to its exceptional electrochemical stability window, this Li/LiPON-modified LAGP will help to achieve the commercialization of safe and long-lasting solid-state lithium batteries.
KW - All-solid-state batteries
KW - Bifunctional thin film interlayer
KW - LiPON
KW - Oxide solid electrolyte
KW - Solid interface
UR - https://www.scopus.com/pages/publications/85124697142
U2 - 10.1016/j.apsusc.2022.152790
DO - 10.1016/j.apsusc.2022.152790
M3 - Article
AN - SCOPUS:85124697142
SN - 0169-4332
VL - 586
JO - Applied Surface Science
JF - Applied Surface Science
M1 - 152790
ER -
