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The leakage of liquid electrolyte and the formation of lithium dendrites pose challenges to safety and stability of lithium metal batteries (LMBs). The appearance of gel polymer electrolyte (GPE) has obviously improved the safety of traditional LMBs. However, the limited inhibition of GPE on lithium dendrites is detrimental to the safety of LMBs. Herein, a kind of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/gelatin (GN) GPE with high ionic conductivity, high-temperature resistance, and flame-retardancy, was prepared by electrospinning and soaking method. Utilizing the electrospinning network of PVDF-HFP, its affinity to liquid electrolytes, makes this GPE more beneficial to ions transport and the formation of gel. And, the GN with sol–gel properties, enhances the mechanical property (13.5 MPa) of HFP-GN GPE. Meanwhile, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) suggest that the attraction of polar groups of GN to Li+ can regulate the distribution of Li+ and protect Li anodes. Consequently, the application of HFP-GN GPEs to LMBs with cathodes of LiFePO4 and LiCoO2 deliver excellent electrochemical performances: after 300 cycles, the LiFePO4/HFP-GN GPE/Li battery keeps a low capacity decay rate of 0.09% at 5 C; after 400 cycles at 2 C, the LiCoO2/HFP-GN GPE/Li cell retains a high capacity retention of 74%. This GPE is demonstrated for the application prospect of safe LMBs.


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A functional gel polymer electrolyte based on PVDF-HFP/gelatin toward dendrite-free lithium metal batteries

Show Author's information Xiaoyi Hu1,2Kangli Liu1,2Shijie Zhang1,2Guosheng Shao1,2( )S. Ravi P. Silva3Peng Zhang1,2( )
State Center for International Cooperation on Designer Low-carbon and Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
Zhengzhou Materials Genome Institute (ZMGI), Zhongyuanzhigu, Xingyang 450100, China
Nanoelectronics Center, Advanced Technology Institute, University of Surrey, Guildford, GU2 7XH, UK

Abstract

The leakage of liquid electrolyte and the formation of lithium dendrites pose challenges to safety and stability of lithium metal batteries (LMBs). The appearance of gel polymer electrolyte (GPE) has obviously improved the safety of traditional LMBs. However, the limited inhibition of GPE on lithium dendrites is detrimental to the safety of LMBs. Herein, a kind of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/gelatin (GN) GPE with high ionic conductivity, high-temperature resistance, and flame-retardancy, was prepared by electrospinning and soaking method. Utilizing the electrospinning network of PVDF-HFP, its affinity to liquid electrolytes, makes this GPE more beneficial to ions transport and the formation of gel. And, the GN with sol–gel properties, enhances the mechanical property (13.5 MPa) of HFP-GN GPE. Meanwhile, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) suggest that the attraction of polar groups of GN to Li+ can regulate the distribution of Li+ and protect Li anodes. Consequently, the application of HFP-GN GPEs to LMBs with cathodes of LiFePO4 and LiCoO2 deliver excellent electrochemical performances: after 300 cycles, the LiFePO4/HFP-GN GPE/Li battery keeps a low capacity decay rate of 0.09% at 5 C; after 400 cycles at 2 C, the LiCoO2/HFP-GN GPE/Li cell retains a high capacity retention of 74%. This GPE is demonstrated for the application prospect of safe LMBs.

Keywords: lithium dendrite, lithium metal battery, gelatin, polar groups, poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)

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Publication history
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Acknowledgements

Publication history

Received: 09 August 2023
Revised: 15 September 2023
Accepted: 24 September 2023
Published: 18 November 2023
Issue date: April 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

The work was supported by the National Natural Science Foundation of China (Nos. 51502269, 51972287, and U2004172), Natural Science Foundation of Henan Province (Nos. 202300410368 and 222301420039), the Foundation for University Key Teachers of Henan Province (No. 2020GGJS009), and sponsored by Program for Science&Technology Innovation Talents in Universities of Henan Province (No. 23HASTIT001).

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