Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries

Mingnan Li; Dmitrii A. Rakov; Yameng Fan; Caoyu Wang; Cheng Wang; Jodie A. Yuwono; Shuixin Xia; Jianfeng Mao; Zaiping Guo

doi:10.1002/anie.202513450

Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries

Mingnan Li (Co-first Author), Dmitrii A. Rakov (Co-first Author), Yameng Fan, Caoyu Wang, Cheng Wang, Jodie A. Yuwono, Shuixin Xia, Jianfeng Mao^*, Zaiping Guo^*

^*Corresponding author for this work

Department of Materials Science and Engineering

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

1 Citation (Scopus)

Abstract

Gel polymer electrolytes (GPEs) show practical potential in lithium metal batteries (LMBs), but their development is hindered by insufficient understanding of Li⁺ solvation chemistry and its impact on ion transport and solid electrolyte interphase (SEI) formation. By regulating the solvation abilities of polymer and solvent, this work explores the relationships between GPE composition, Li⁺ coordination structures, Li⁺ transference number, and interphase chemistry. The GPE combining weakly coordinated solvents with strongly coordinating polymer results in strong Li⁺-polymer attachment, leading to sluggish ion transport. Employing strongly chelating solvents causes complete Li⁺-polymer detachment, forming micelle structures that obstruct ion transport. The GPE with both weakly coordinated solvent fluoroethylene carbonate (FEC) and polymer 1H,1H,2H,2H-tridecafluoro-n-octyl acrylate (TFOA) enables optimal interactions between Li⁺ and polymer/solvent, facilitating partial Li⁺-polymer detachment and aggregates (AGGs) generation, avoiding micelle formation. This promotes efficient Li⁺ transport and anion-derived SEI generation. The resulting GPE achieves 99.2% Coulombic efficiency (CE) in Cu||Li cells and enables 4.5 V LiNi_0.8Mn_0.1Co_0.1O₂||Li to demonstrate 81% capacity retention after 140 cycles. These findings provide valuable insights for further advanced GPE design. © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Original language	English
Article number	e202513450
Number of pages	11
Journal	Angewandte Chemie International Edition
Volume	64
Issue number	41
Online published	19 Aug 2025
DOIs	https://doi.org/10.1002/anie.202513450
Publication status	Published - 6 Oct 2025

Funding

This work is financially supported by the Australian Research Council (FT230100598 and FL210100050). The simulation work was undertaken with the assistance of 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. M. L. acknowledges the Chinese Scholarship Council for scholarship support (No. 202106130006). Open access publishing facilitated by The University of Adelaide, as part of the Wiley - The University of Adelaide agreement via the Council of Australian University Librarians.

Research Keywords

Gel polymer electrolyte
Lithium metal batteries
Polymer
Solvated ability
Solvent

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This full text is made available under CC-BY-NC 4.0. https://creativecommons.org/licenses/by-nc/4.0/

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title = "Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries",

abstract = "Gel polymer electrolytes (GPEs) show practical potential in lithium metal batteries (LMBs), but their development is hindered by insufficient understanding of Li+ solvation chemistry and its impact on ion transport and solid electrolyte interphase (SEI) formation. By regulating the solvation abilities of polymer and solvent, this work explores the relationships between GPE composition, Li+ coordination structures, Li+ transference number, and interphase chemistry. The GPE combining weakly coordinated solvents with strongly coordinating polymer results in strong Li+-polymer attachment, leading to sluggish ion transport. Employing strongly chelating solvents causes complete Li+-polymer detachment, forming micelle structures that obstruct ion transport. The GPE with both weakly coordinated solvent fluoroethylene carbonate (FEC) and polymer 1H,1H,2H,2H-tridecafluoro-n-octyl acrylate (TFOA) enables optimal interactions between Li+ and polymer/solvent, facilitating partial Li+-polymer detachment and aggregates (AGGs) generation, avoiding micelle formation. This promotes efficient Li+ transport and anion-derived SEI generation. The resulting GPE achieves 99.2% Coulombic efficiency (CE) in Cu||Li cells and enables 4.5 V LiNi0.8Mn0.1Co0.1O2||Li to demonstrate 81% capacity retention after 140 cycles. These findings provide valuable insights for further advanced GPE design. {\textcopyright} 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

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author = "Mingnan Li and Rakov, {Dmitrii A.} and Yameng Fan and Caoyu Wang and Cheng Wang and Yuwono, {Jodie A.} and Shuixin Xia and Jianfeng Mao and Zaiping Guo",

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Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries. / Li, Mingnan (Co-first Author); Rakov, Dmitrii A. (Co-first Author); Fan, Yameng et al.
In: Angewandte Chemie International Edition, Vol. 64, No. 41, e202513450, 06.10.2025.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries

AU - Li, Mingnan

AU - Rakov, Dmitrii A.

AU - Fan, Yameng

AU - Wang, Caoyu

AU - Wang, Cheng

AU - Yuwono, Jodie A.

AU - Xia, Shuixin

AU - Mao, Jianfeng

AU - Guo, Zaiping

PY - 2025/10/6

Y1 - 2025/10/6

N2 - Gel polymer electrolytes (GPEs) show practical potential in lithium metal batteries (LMBs), but their development is hindered by insufficient understanding of Li+ solvation chemistry and its impact on ion transport and solid electrolyte interphase (SEI) formation. By regulating the solvation abilities of polymer and solvent, this work explores the relationships between GPE composition, Li+ coordination structures, Li+ transference number, and interphase chemistry. The GPE combining weakly coordinated solvents with strongly coordinating polymer results in strong Li+-polymer attachment, leading to sluggish ion transport. Employing strongly chelating solvents causes complete Li+-polymer detachment, forming micelle structures that obstruct ion transport. The GPE with both weakly coordinated solvent fluoroethylene carbonate (FEC) and polymer 1H,1H,2H,2H-tridecafluoro-n-octyl acrylate (TFOA) enables optimal interactions between Li+ and polymer/solvent, facilitating partial Li+-polymer detachment and aggregates (AGGs) generation, avoiding micelle formation. This promotes efficient Li+ transport and anion-derived SEI generation. The resulting GPE achieves 99.2% Coulombic efficiency (CE) in Cu||Li cells and enables 4.5 V LiNi0.8Mn0.1Co0.1O2||Li to demonstrate 81% capacity retention after 140 cycles. These findings provide valuable insights for further advanced GPE design. © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.

AB - Gel polymer electrolytes (GPEs) show practical potential in lithium metal batteries (LMBs), but their development is hindered by insufficient understanding of Li+ solvation chemistry and its impact on ion transport and solid electrolyte interphase (SEI) formation. By regulating the solvation abilities of polymer and solvent, this work explores the relationships between GPE composition, Li+ coordination structures, Li+ transference number, and interphase chemistry. The GPE combining weakly coordinated solvents with strongly coordinating polymer results in strong Li+-polymer attachment, leading to sluggish ion transport. Employing strongly chelating solvents causes complete Li+-polymer detachment, forming micelle structures that obstruct ion transport. The GPE with both weakly coordinated solvent fluoroethylene carbonate (FEC) and polymer 1H,1H,2H,2H-tridecafluoro-n-octyl acrylate (TFOA) enables optimal interactions between Li+ and polymer/solvent, facilitating partial Li+-polymer detachment and aggregates (AGGs) generation, avoiding micelle formation. This promotes efficient Li+ transport and anion-derived SEI generation. The resulting GPE achieves 99.2% Coulombic efficiency (CE) in Cu||Li cells and enables 4.5 V LiNi0.8Mn0.1Co0.1O2||Li to demonstrate 81% capacity retention after 140 cycles. These findings provide valuable insights for further advanced GPE design. © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.

KW - Gel polymer electrolyte

KW - Lithium metal batteries

KW - Polymer

KW - Solvated ability

KW - Solvent

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DO - 10.1002/anie.202513450

M3 - RGC 21 - Publication in refereed journal

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SN - 1433-7851

VL - 64

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

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M1 - e202513450

ER -

Balancing Solvation Ability of Polymer and Solvent in Gel Polymer Electrolytes for Efficient Lithium Metal Batteries

Abstract

Funding

Research Keywords

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