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Research Article | Online first | Published: 07 March 2024

Dual-filler reinforced PVDF-HFP based polymer electrolyte enabling high-safety design of lithium metal batteries

Show Author's Information Chang Fang,§,  Kangsheng Huang,§,  Jing Zhao,  Shiqi Tian,  Hui Dou( ),  Xiaogang Zhang( )
Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China

§ Chang Fang and Kangsheng Huang contributed equally to this work.

Keywords:
long cycle life, polymer electrolyte, lithium metal battery, non-flammable, SiO2/Li6.4La3Zr1.4Ta0.6O12 (LLZTO) dual-filler
Topics:
Energy storageLithium batteries
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Fang C, Huang K, Zhao J, et al. Dual-filler reinforced PVDF-HFP based polymer electrolyte enabling high-safety design of lithium metal batteries. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6502-z
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Abstract Full text Electronic supplementary material About this article

Despite the high energy density of lithium metal batteries (LMBs), their application in rechargeable batteries is still hampered due to insufficient safety. Here, we present a novel flame-retardant solid-state electrolyte based on polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) with nano SiO2 aerogel as an inert filler but Li6.4La3Zr1.4Ta0.6O12 (LLZTO) as an auxiliary component to enhance the ion conductivity. The introduction of SiO2 aerogels imparts the polymer electrolyte with exceptional thermal stability and flame retardancy. Simultaneously, the interaction between hydroxyl groups of SiO2 particles and PVDF-HFP creates a strong cross-linking structure, enhancing the mechanical strength and stability of the electrolyte. Furthermore, the presence of SiO2 aerogel and LLZTO facilitates the dissociation of lithium salts through Lewis acid-base interactions, resulting in a high ionic conductivity of 1.01 × 10−3 S·cm−1 and a wide electrochemical window of ~ 5.0 V at room temperature for the prepared electrolytes. Remarkably, the assembled Li|Li cell demonstrates the excellent resistance to lithium dendrite and runs stablly for over 1500 h at a current density of 0.25 mA·cm−2. Thus, we prepare a pouch cell with high safety, which can work normally after short-circuiting under the external folding and cutting.


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About this article

Dual-filler reinforced PVDF-HFP based polymer electrolyte enabling high-safety design of lithium metal batteries

Show Author's information Chang Fang,§, Kangsheng Huang,§, Jing Zhao, Shiqi Tian, Hui Dou( ), Xiaogang Zhang( )
Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China

§ Chang Fang and Kangsheng Huang contributed equally to this work.

Abstract

Despite the high energy density of lithium metal batteries (LMBs), their application in rechargeable batteries is still hampered due to insufficient safety. Here, we present a novel flame-retardant solid-state electrolyte based on polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) with nano SiO2 aerogel as an inert filler but Li6.4La3Zr1.4Ta0.6O12 (LLZTO) as an auxiliary component to enhance the ion conductivity. The introduction of SiO2 aerogels imparts the polymer electrolyte with exceptional thermal stability and flame retardancy. Simultaneously, the interaction between hydroxyl groups of SiO2 particles and PVDF-HFP creates a strong cross-linking structure, enhancing the mechanical strength and stability of the electrolyte. Furthermore, the presence of SiO2 aerogel and LLZTO facilitates the dissociation of lithium salts through Lewis acid-base interactions, resulting in a high ionic conductivity of 1.01 × 10−3 S·cm−1 and a wide electrochemical window of ~ 5.0 V at room temperature for the prepared electrolytes. Remarkably, the assembled Li|Li cell demonstrates the excellent resistance to lithium dendrite and runs stablly for over 1500 h at a current density of 0.25 mA·cm−2. Thus, we prepare a pouch cell with high safety, which can work normally after short-circuiting under the external folding and cutting.

Keywords: long cycle life, polymer electrolyte, lithium metal battery, non-flammable, SiO2/Li6.4La3Zr1.4Ta0.6O12 (LLZTO) dual-filler

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Publication history
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Acknowledgements

Publication history

Received: 22 November 2023
Revised: 09 January 2024
Accepted: 18 January 2024
Published: 07 March 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Program Intergovernmental International Science and Technology Innovation Cooperation (No. 2022YFE0109400), Leading Edge Technology of Jiangsu Province (Nos. BK20202008 and BK20220009), and Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

We acknowledge the facilities in the Center for Microscopy and Analysis of Nanjing University of Aeronautics and Astronautics.

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