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Research Article

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

Xinji Zhang, Yafang Zhang, Shiyue Zhou, Jingchuan Dang( ), Chenye Wang, Wenjia Wu( ), Jingtao Wang
School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
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Graphical Abstract

A lamellar composite solid electrolyte with β-conformation polyvinylidene fluoride (PVDF) was prepared by confining PVDF in the interlayer channel of –NH2 modified vermiculite (Vr) lamellar framework, which imparts superior room-temperature ionic conductivity and lithium-ion transference number.

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 ( tLi+). 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 tLi+ 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 mAh·g−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.

Keywords

solid-state lithium metal batterylamellar composite solid electrolyteroom-temperature ionic conductivitylithium-ion transference numberβ-conformation polyvinylidene fluoride (PVDF)

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Nano Research
Volume 17 Issue 6,
June 2024
Pages 5159-5167
DOI: 10.1007/s12274-024-6439-2
Cite this article:
Zhang X, Zhang Y, Zhou S, et al. Formatted PVDF in lamellar composite solid electrolyte for solid-state lithium metal battery. Nano Research, 2024, 17(6): 5159-5167. https://doi.org/10.1007/s12274-024-6439-2
Topics:
Lithium batteries

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Received: 05 November 2023
Revised: 19 December 2023
Accepted: 21 December 2023
Published: 01 February 2024
© Tsinghua University Press 2024
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