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Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression

[Image: see text] Composite polymer electrolytes (CPEs) strike an effective balance between ionic conductivity and mechanical flexibility for lithium-ion solid-state batteries. Long-term performance, however, is limited by capacity fading after hundreds of charge and discharge cycles. The causes of...

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Autores principales: Yoon, Dan-il, Mulay, Nishad, Baltazar, Jericko, Cao, Dang Khoa, Perez, Valeria, Nelson Weker, Johanna, Lee, Min Hwan, Miller, Robert D., Oh, Dahyun, Lee, Sang-Joon John
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10538521/
https://www.ncbi.nlm.nih.gov/pubmed/37779902
http://dx.doi.org/10.1021/acsaem.3c01357
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author Yoon, Dan-il
Mulay, Nishad
Baltazar, Jericko
Cao, Dang Khoa
Perez, Valeria
Nelson Weker, Johanna
Lee, Min Hwan
Miller, Robert D.
Oh, Dahyun
Lee, Sang-Joon John
author_facet Yoon, Dan-il
Mulay, Nishad
Baltazar, Jericko
Cao, Dang Khoa
Perez, Valeria
Nelson Weker, Johanna
Lee, Min Hwan
Miller, Robert D.
Oh, Dahyun
Lee, Sang-Joon John
author_sort Yoon, Dan-il
collection PubMed
description [Image: see text] Composite polymer electrolytes (CPEs) strike an effective balance between ionic conductivity and mechanical flexibility for lithium-ion solid-state batteries. Long-term performance, however, is limited by capacity fading after hundreds of charge and discharge cycles. The causes of performance degradation include multiple contributing factors such as dendrite formation, physicochemical changes in electrolytes, and structural remodeling of porous electrodes. Among the many factors that contribute to performance degradation, the effect of stress specifically on the composite electrolyte is not well understood. This study examines the mechanical changes in a poly(ethylene oxide) electrolyte with bis(trifluoromethane) sulfonimide. Two different sizes of Li(6.4)La(3)Zr(1.4)Ta(0.6)O(12) particles (500 nm and 5 μm) are compared to evaluate the effect of the surface-to-volume ratio of the ion-conducting fillers within the composite. Cyclic compression was applied to mimic stress cycling in the electrolyte, which would be caused by asymmetric volume changes that occur during charging and discharging cycles. The electrolytes exhibited fatigue softening, whereby the compressive modulus gradually decreased with an increase in the number of cycles. When the electrolyte was tested for 500 cycles at 30% compressive strain, the compressive modulus of the electrolyte was reduced to approximately 80% of the modulus before cycling. While the extent of softening was similar regardless of particle size, CPEs with 500 nm particles exhibited a significant reduction in ionic conductivity after cyclic compression (1.4 × 10(–7) ± 2.3 × 10(–8) vs 1.1 × 10(–7) ± 2.0 × 10(–8) S/cm, mean ± standard deviation, n = 4), whereas there was no significant change in ionic conductivity for CPEs with 5 μm particles. These observations —performed deliberately in the absence of charge–discharge cycles —show that repetitive mechanical stresses can play a significant role in altering the performance of CPEs, thereby revealing another possible mechanism for performance degradation in all-solid-state batteries.
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spelling pubmed-105385212023-09-29 Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression Yoon, Dan-il Mulay, Nishad Baltazar, Jericko Cao, Dang Khoa Perez, Valeria Nelson Weker, Johanna Lee, Min Hwan Miller, Robert D. Oh, Dahyun Lee, Sang-Joon John ACS Appl Energy Mater [Image: see text] Composite polymer electrolytes (CPEs) strike an effective balance between ionic conductivity and mechanical flexibility for lithium-ion solid-state batteries. Long-term performance, however, is limited by capacity fading after hundreds of charge and discharge cycles. The causes of performance degradation include multiple contributing factors such as dendrite formation, physicochemical changes in electrolytes, and structural remodeling of porous electrodes. Among the many factors that contribute to performance degradation, the effect of stress specifically on the composite electrolyte is not well understood. This study examines the mechanical changes in a poly(ethylene oxide) electrolyte with bis(trifluoromethane) sulfonimide. Two different sizes of Li(6.4)La(3)Zr(1.4)Ta(0.6)O(12) particles (500 nm and 5 μm) are compared to evaluate the effect of the surface-to-volume ratio of the ion-conducting fillers within the composite. Cyclic compression was applied to mimic stress cycling in the electrolyte, which would be caused by asymmetric volume changes that occur during charging and discharging cycles. The electrolytes exhibited fatigue softening, whereby the compressive modulus gradually decreased with an increase in the number of cycles. When the electrolyte was tested for 500 cycles at 30% compressive strain, the compressive modulus of the electrolyte was reduced to approximately 80% of the modulus before cycling. While the extent of softening was similar regardless of particle size, CPEs with 500 nm particles exhibited a significant reduction in ionic conductivity after cyclic compression (1.4 × 10(–7) ± 2.3 × 10(–8) vs 1.1 × 10(–7) ± 2.0 × 10(–8) S/cm, mean ± standard deviation, n = 4), whereas there was no significant change in ionic conductivity for CPEs with 5 μm particles. These observations —performed deliberately in the absence of charge–discharge cycles —show that repetitive mechanical stresses can play a significant role in altering the performance of CPEs, thereby revealing another possible mechanism for performance degradation in all-solid-state batteries. American Chemical Society 2023-09-09 /pmc/articles/PMC10538521/ /pubmed/37779902 http://dx.doi.org/10.1021/acsaem.3c01357 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Yoon, Dan-il
Mulay, Nishad
Baltazar, Jericko
Cao, Dang Khoa
Perez, Valeria
Nelson Weker, Johanna
Lee, Min Hwan
Miller, Robert D.
Oh, Dahyun
Lee, Sang-Joon John
Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title_full Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title_fullStr Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title_full_unstemmed Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title_short Softening of PEO–LiTFSI/LLZTO Composite Polymer Electrolytes for Solid-State Batteries under Cyclic Compression
title_sort softening of peo–litfsi/llzto composite polymer electrolytes for solid-state batteries under cyclic compression
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10538521/
https://www.ncbi.nlm.nih.gov/pubmed/37779902
http://dx.doi.org/10.1021/acsaem.3c01357
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