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Title: Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂
Authors: Oruea, Ander
Arrese-Igor, Mikel
Cid, Rosalia
Júdez, Xabier
Gómez, Nuria
López del Amo, Juan Miguel
Manalastas, William
Srinivasan, Madhavi
Rojviriya, Catleya
Armand, Michel
Aguesse, Frédéric
López-Aranguren, Pedro
Keywords: Engineering::Materials
Issue Date: 2022
Source: Oruea, A., Arrese-Igor, M., Cid, R., Júdez, X., Gómez, N., López del Amo, J. M., Manalastas, W., Srinivasan, M., Rojviriya, C., Armand, M., Aguesse, F. & López-Aranguren, P. (2022). Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂. Journal of Materials Chemistry A, 10(5), 2352-2361.
Project: NRFI2017-08 
Journal: Journal of Materials Chemistry A 
Abstract: High-voltage Li metal solid-state batteries are in the spotlight of high energy and power density devices for the next generation of batteries. However, the lack of robust solid-electrolyte interfaces (SEI) and the propagation of Li dendrites still need to be addressed for practical application with extended cyclability. In the present work, high-voltage Li metal cells with LiNi0.6Mn0.2Co0.2O2 active material were assembled with a polyethylene(oxide) based electrolyte mixed with bis(fluorosulfonyl)imide (LiFSI) salt. The addition of Li7La3Zr2012 garnet to form a composite electrolyte demonstrated the beneficial effect for cell cycling stability. Inspired by the improved interface of ceramic Li7La3Zr2012 garnet and Li metal, as well as by previous knowledge on favorable SEI forming species, various additive candidates were selected to optimize its electrolyte composition. Among them, lithium hydroxide (LiOH) is a key favorable specie that shows a relevant improvement on the cyclability of the cells. X-ray photoelectron spectroscopy showed that the SEI layer is composed mainly by chemical species arising from the reduction of the Li salt, being the lithium fluoride (LiF) the main product. In addition, solid-state nuclear magnetic resonance proved that LiOH induces the cleavage of the labile S-F bond, increasing the concentration of LiF. Herein, we highlight that SEI-forming additives need to be considered for the interfacial engineering design of stable SEI to expand the performance boundary of SSBs.
ISSN: 2050-7488
DOI: 10.1039/D1TA08362G
Schools: School of Materials Science and Engineering 
Research Centres: Energy Research Institute @ NTU (ERI@N) 
Rights: © 2022 The Royal Society of Chemistry. All rights reserved. This paper was published in Journal of Materials Chemistry A and is made available with permission of The Royal Society of Chemistry.
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:ERI@N Journal Articles
MSE Journal Articles

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