Design and Fabrication of LiNbO3/PVDF Composite Solid Electrolytes and Their Electrochemical Properties

doi:10.15541/jim20260317

Abstract

Abstract: Composite solid electrolytes are key materials for enhancing the safety and energy density of solid-state lithium metal batteries, yet their low room-temperature ionic conductivity and poor interfacial stability remain critical challenges. In this study, lithium niobate(LiNbO₃, LN), a functional filler with both high dielectric constant and lithium-ion conduction capability, was introduced into poly(vinylidene fluoride) (PVDF) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) polymer matrices. Composite solid electrolyte membranes were prepared via solution casting, and the effects of LiNbO₃, content and matrix type on ion transport behavior, electrochemical stability window, and lithium anode interface stability were systematically compared. The optimal LiNbO₃, loading was found to be 30%(in mass) for both matrices. The PVDF/30LN electrolyte exhibited a room-temperature ionic conductivity of 9.0×10^-4 S∙cm^-1 and an electrochemical window extended to 4.6 V. In contrast, the PVDF-HFP/30LN electrolyte, benefited from the reduced polymer crystallinity and enlarged amorphous fraction imparted by the HFP units, achieved a higher ionic conductivity of 14.8×10^-4 S∙cm^-1 and a wider electrochemical window of 5.1 V, demonstrating superior lithium salt dissociation and high-voltage tolerance. However, due to the inherent high creep compliance of the amorphous chain segments in the PVDF-HFP matrix, this electrolyte showed slightly inferior performance in critical current density (0.52 mA∙cm^-2) and long-term cycling stability compared with its PVDF-based counterpart. This study reveals the distinct performance responses of the same ferroelectric active filler in polymer matrices with similar chemical structures but different crystallinity, providing experimental evidence for matrix material selection and interface engineering optimization in composite solid electrolytes.

Key words: composite solid electrolyte, lithium metal battery, LiNbO₃, PVDF, PVDF-HFP

CLC Number:

TM912

DENG Ting, WANG Long, YANG Haijun, FANG Ruyi, ZHANG Jun, XIA Yang, HUANG Hui, ZHANG Wenkui, XIA Xinhui. Design and Fabrication of LiNbO₃/PVDF Composite Solid Electrolytes and Their Electrochemical Properties[J]. Journal of Inorganic Materials, DOI: 10.15541/jim20260317.

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Design and Fabrication of LiNbO₃/PVDF Composite Solid Electrolytes and Their Electrochemical Properties

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