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Formatted PVDF in lamellar composite solid electrolyte for solid-state lithium metal battery

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Abstract

Solid polymer electrolytes (SPEs) hold great application potential for solid-state lithium metal battery because of the excellent interfacial contact and processibility, but being hampered by the poor room-temperature conductivity (∼ 10−7 S·cm−1) and low lithium-ion transference number \(({t_{{\rm{L}}{{\rm{i}}^ + }}})\). Here, a lamellar composite solid electrolyte (Vr-NH2@polyvinylidene fluoride (PVDF) LCSE) with β-conformation PVDF is fabricated by confining PVDF in the interlayer channel of -NH2 modified vermiculite lamellar framework. We demonstrate that the conformation of PVDF can be manipulated by the nanoconfinement effect and the interaction from channel wall. The presence of -NH2 groups could induce the formation of β-conformation PVDF through electrostatic interaction, which serves as continuous and rapid lithium-ion transfer pathway. As a result, a high room-temperature ionic conductivity of 1.77 × 10−4 S·cm−1 is achieved, 1–2 orders of magnitude higher than most SPEs. Furthermore, Vr-NH2@PVDF LCSE shows a high \({t_{{\rm{L}}{{\rm{i}}^ + }}}\) of 0.68 because of the high dielectric constant, ∼ 3 times of that of PVDF SPE, and surpassing most of reported SPEs. The LiNi0.8Co0.1Mn0.1O2∥Li cell assembled by Vr-NH2@PVDF LCSE obtains a discharge specific capacity of 137.1 mA·hg−1 after 150 cycles with a capacity retention rate of 93% at 1 C and 25 °C. This study may pave a new avenue for high-performance SPEs.

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Acknowledgements

The authors would like to acknowledge financial support from National Natural Science Foundation of China (No. U2004199), Joint Foundation for Science and Technology Research & Development Plan of Henan Province (Nos. 222301420003 and 232301420038), China Postdoctoral Science Foundation (No. 2022TQ0293), and Key Science and Technology Project of Henan Province (No. 221100240200-06). Center for advanced analysis and computational science, Zhengzhou University is also highly acknowledged.

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  1. School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Xinji Zhang, Yafang Zhang, Shiyue Zhou, Jingchuan Dang, Chenye Wang, Wenjia Wu & Jingtao Wang

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  1. Xinji Zhang
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Correspondence to Jingchuan Dang or Wenjia Wu.

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Zhang, X., Zhang, Y., Zhou, S. et al. Formatted PVDF in lamellar composite solid electrolyte for solid-state lithium metal battery. Nano Res. 17, 5159–5167 (2024). https://doi.org/10.1007/s12274-024-6439-2

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