Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂
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...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/156482 |
| _version_ | 1826123980073861120 |
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| author | 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 |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering 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 |
| author_sort | Oruea, Ander |
| collection | NTU |
| description | 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. |
| first_indexed | 2024-10-01T06:13:30Z |
| format | Journal Article |
| id | ntu-10356/156482 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:13:30Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1564822022-04-23T20:11:18Z Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ 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 School of Materials Science and Engineering Energy Research Institute @ NTU (ERI@N) Engineering::Materials Active Material Solid-State Batteries 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. National Research Foundation (NRF) Submitted/Accepted version W. M. and M. S. are thankful for the financial support from the National Research Foundation of Singapore (NRF) under Investigatorship Award Number NRFI2017-08. 2022-04-20T07:18:03Z 2022-04-20T07:18:03Z 2022 Journal Article 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. https://dx.doi.org/10.1039/D1TA08362G 2050-7488 https://hdl.handle.net/10356/156482 10.1039/D1TA08362G 5 10 2352 2361 en NRFI2017-08 Journal of Materials Chemistry A © 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. application/pdf |
| spellingShingle | Engineering::Materials Active Material Solid-State Batteries 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 Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title | Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title_full | Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title_fullStr | Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title_full_unstemmed | Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title_short | Enhancing the polymer electrolyte – Li metal interface on highvoltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li₇La₃Zr₂O₁₂ |
| title_sort | enhancing the polymer electrolyte li metal interface on highvoltage solid state batteries with li based additives inspired by the surface chemistry of li₇la₃zr₂o₁₂ |
| topic | Engineering::Materials Active Material Solid-State Batteries |
| url | https://hdl.handle.net/10356/156482 |
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