Controlling the Supramolecular Architecture Enables High Lithium Cationic Conductivity and High Electrochemical Stability for Solid Polymer Electrolytes

Ke Xie; Qiang Fu; Fangfang Chen; Haijin Zhu; Xiaoen Wang; Gongyue Huang; Hualin Zhan; Qinghua Liang; Cara M. Doherty; Dawei Wang; Greg G. Qiao; Dan Li

doi:10.1002/adfm.202315495

Controlling the Supramolecular Architecture Enables High Lithium Cationic Conductivity and High Electrochemical Stability for Solid Polymer Electrolytes

Ke Xie, Qiang Fu^*, Fangfang Chen^*, Haijin Zhu, Xiaoen Wang, Gongyue Huang, Hualin Zhan, Qinghua Liang, Cara M. Doherty, Dawei Wang, Greg G. Qiao, Dan Li^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

18 Scopus citations

Abstract

Solid polymer electrolytes (SPEs) are long sought after for versatile applications due to their low cost, light weight, flexibility, ease of scale-up, and low interfacial impedance. However, obtaining SPEs with high Li⁺ conductivity (σ₊) and high voltage stability to avoid concentrated polarization and premature capacity loss has proven challenging. Here a stretchable dry-SPE is reported with a semi-interpenetrating, supermolecular architecture consisting of a cross-linked polyethylene oxide (PEO) tetra-network and an alternating copolymer poly(ethylene oxide-alt-butylene terephthalate). Such a unique supermolecular architecture suppresses the formation of Li⁺/PEO intermolecular complex and enhances the oxidation stability of PEO-based electrolyte, thus maintaining high chain segmental motion even with high salt loading (up to 50 wt%) and achieving a wide electrochemical stability window of 5.3 V. These merits enable the simultaneous accomplishment of high ionic conductivity and high Li⁺ transference number (t₊) to enhance the energy efficiency of energy storage device, and electrochemical stability.

Original language	English (US)
Article number	2315495
Journal	Advanced Functional Materials
Volume	34
Issue number	17
DOIs	https://doi.org/10.1002/adfm.202315495
State	Published - Apr 25 2024

Funding

Q.F. acknowledges the Australian Research Council (ARC) under the Future Fellowship (FT180100312). F.C. acknowledges the Australian Research Council for funding via the Australian Centre for Electro materials Science (CE140100012) and computational resources provided at the NCI National Facility systems at the Australian National University through the National Computational Merit Allocation Scheme supported by the Australian Government. Q. Liang acknowledges the financial support from the ARC (DE190100445). D.L. was grateful for the financial support from the ARC (FL180100029) and the University of Melbourne.

Keywords

Vogel–Tammann–Fulcher theory
electrochemical stability window
ionic conductivity
solid-state electrolyte
supramolecular architecture
transference number

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Chemistry
Biomaterials
General Materials Science
Condensed Matter Physics
Electrochemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/adfm.202315495

Cite this

Xie, K., Fu, Q., Chen, F., Zhu, H., Wang, X., Huang, G., Zhan, H., Liang, Q., Doherty, C. M., Wang, D., Qiao, G. G., & Li, D. (2024). Controlling the Supramolecular Architecture Enables High Lithium Cationic Conductivity and High Electrochemical Stability for Solid Polymer Electrolytes. Advanced Functional Materials, 34(17), Article 2315495. https://doi.org/10.1002/adfm.202315495

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abstract = "Solid polymer electrolytes (SPEs) are long sought after for versatile applications due to their low cost, light weight, flexibility, ease of scale-up, and low interfacial impedance. However, obtaining SPEs with high Li+ conductivity (σ+) and high voltage stability to avoid concentrated polarization and premature capacity loss has proven challenging. Here a stretchable dry-SPE is reported with a semi-interpenetrating, supermolecular architecture consisting of a cross-linked polyethylene oxide (PEO) tetra-network and an alternating copolymer poly(ethylene oxide-alt-butylene terephthalate). Such a unique supermolecular architecture suppresses the formation of Li+/PEO intermolecular complex and enhances the oxidation stability of PEO-based electrolyte, thus maintaining high chain segmental motion even with high salt loading (up to 50 wt%) and achieving a wide electrochemical stability window of 5.3 V. These merits enable the simultaneous accomplishment of high ionic conductivity and high Li+ transference number (t+) to enhance the energy efficiency of energy storage device, and electrochemical stability.",

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AU - Wang, Xiaoen

AU - Huang, Gongyue

AU - Zhan, Hualin

AU - Liang, Qinghua

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AU - Qiao, Greg G.

AU - Li, Dan

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N2 - Solid polymer electrolytes (SPEs) are long sought after for versatile applications due to their low cost, light weight, flexibility, ease of scale-up, and low interfacial impedance. However, obtaining SPEs with high Li+ conductivity (σ+) and high voltage stability to avoid concentrated polarization and premature capacity loss has proven challenging. Here a stretchable dry-SPE is reported with a semi-interpenetrating, supermolecular architecture consisting of a cross-linked polyethylene oxide (PEO) tetra-network and an alternating copolymer poly(ethylene oxide-alt-butylene terephthalate). Such a unique supermolecular architecture suppresses the formation of Li+/PEO intermolecular complex and enhances the oxidation stability of PEO-based electrolyte, thus maintaining high chain segmental motion even with high salt loading (up to 50 wt%) and achieving a wide electrochemical stability window of 5.3 V. These merits enable the simultaneous accomplishment of high ionic conductivity and high Li+ transference number (t+) to enhance the energy efficiency of energy storage device, and electrochemical stability.

AB - Solid polymer electrolytes (SPEs) are long sought after for versatile applications due to their low cost, light weight, flexibility, ease of scale-up, and low interfacial impedance. However, obtaining SPEs with high Li+ conductivity (σ+) and high voltage stability to avoid concentrated polarization and premature capacity loss has proven challenging. Here a stretchable dry-SPE is reported with a semi-interpenetrating, supermolecular architecture consisting of a cross-linked polyethylene oxide (PEO) tetra-network and an alternating copolymer poly(ethylene oxide-alt-butylene terephthalate). Such a unique supermolecular architecture suppresses the formation of Li+/PEO intermolecular complex and enhances the oxidation stability of PEO-based electrolyte, thus maintaining high chain segmental motion even with high salt loading (up to 50 wt%) and achieving a wide electrochemical stability window of 5.3 V. These merits enable the simultaneous accomplishment of high ionic conductivity and high Li+ transference number (t+) to enhance the energy efficiency of energy storage device, and electrochemical stability.

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Controlling the Supramolecular Architecture Enables High Lithium Cationic Conductivity and High Electrochemical Stability for Solid Polymer Electrolytes

Abstract

Funding

Keywords

ASJC Scopus subject areas

UN SDGs

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