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Peer-reviewedCC BY 4.0Polymers

Recent Progress in Gel Polymer Electrolytes for Lithium-Based Batteries: Design Strategies and Practical Applications

  1. 1Department of Mechanical, Smart, and Industrial Engineering (Mechanical Engineering Major), Gachon University, 1342, Seongnam-daero, Sujeong-gu, Seongnam-si 13120, Republic of Korea

Abstract

Gel polymer electrolytes are attractive quasi-solid electrolyte systems that combine the high ionic mobility and electrode wetting of liquid electrolytes with the dimensional stability and reduced leakage of polymer networks. Their value for high-performance lithium-ion batteries is increasingly determined not only by bulk ionic conductivity, but also by Li+ selectivity, solvent retention, mechanical integrity, electrochemical stability, and the ability to form stable interfaces with high-voltage cathodes and practical graphite and Si-containing anodes. This review critically summarizes recent progress in GPEs through a structure, transport, interface-performance framework, with particular emphasis on developments reported in recent years while retaining foundational studies that established the field. Representative polymer hosts, including PVDF/PVDF-HFP, PEO, PAN, PMMA and methacrylate networks, cellulose-derived matrices, and emerging functional polymers, are compared according to their molecular functionality and practical limitations. Major performance-enhancement strategies-including blending, crosslinking, inorganic or nanostructured fillers, functional additives, nonflammable components, self-healing chemistries, and in situ polymerization-are then evaluated in terms of how they regulate ion transport, interphase chemistry, mechanical behavior, thermal safety, and manufacturability. Recent demonstrations in NCM/graphite and NCM/Si graphite pouch cells show that conformal in situ gelation, LiF-rich interphases, adaptive network mechanics, and low-reactivity liquid phases can translate materials-level improvements into high-rate cycling, long life, and improved abuse tolerance. Remaining challenges include conductivity, mechanical strength, high-voltage oxidation and wide-temperature operation. Future GPE development will therefore require integrated molecular, interfacial, and cell-level design rather than optimization of isolated membrane properties.

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BibTeX
@article{bhuyan2026recent,
  title = {{Recent Progress in Gel Polymer Electrolytes for Lithium-Based Batteries: Design Strategies and Practical Applications}},
  author = {Md Murshed Bhuyan and Kyungjun Lee},
  journal = {Polymers},
  year = {2026},
  month = nov,
  doi = {10.3390/polym18212779},
  url = {https://www.mdpi.com/2073-4360/18/21/2779},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Recent Progress in Gel Polymer Electrolytes for Lithium-Based Batteries: Design Strategies and Practical Applications
AU  - Md Murshed Bhuyan
AU  - Kyungjun Lee
PY  - 2026
DA  - 2026/11/07
JO  - Polymers
DO  - 10.3390/polym18212779
UR  - https://www.mdpi.com/2073-4360/18/21/2779
AB  - Gel polymer electrolytes are attractive quasi-solid electrolyte systems that combine the high ionic mobility and electrode wetting of liquid electrolytes with the dimensional stability and reduced leakage of polymer networks. Their value for high-performance lithium-ion batteries is increasingly determined not only by bulk ionic conductivity, but also by Li+ selectivity, solvent retention, mechanical integrity, electrochemical stability, and the ability to form stable interfaces with high-voltage cathodes and practical graphite and Si-containing anodes. This review critically summarizes recent progress in GPEs through a structure, transport, interface-performance framework, with particular emphasis on developments reported in recent years while retaining foundational studies that established the field. Representative polymer hosts, including PVDF/PVDF-HFP, PEO, PAN, PMMA and methacrylate networks, cellulose-derived matrices, and emerging functional polymers, are compared according to their molecular functionality and practical limitations. Major performance-enhancement strategies-including blending, crosslinking, inorganic or nanostructured fillers, functional additives, nonflammable components, self-healing chemistries, and in situ polymerization-are then evaluated in terms of how they regulate ion transport, interphase chemistry, mechanical behavior, thermal safety, and manufacturability. Recent demonstrations in NCM/graphite and NCM/Si graphite pouch cells show that conformal in situ gelation, LiF-rich interphases, adaptive network mechanics, and low-reactivity liquid phases can translate materials-level improvements into high-rate cycling, long life, and improved abuse tolerance. Remaining challenges include conductivity, mechanical strength, high-voltage oxidation and wide-temperature operation. Future GPE development will therefore require integrated molecular, interfacial, and cell-level design rather than optimization of isolated membrane properties.
SN  - 2073-4360
ER  -