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丁二腈与勃姆石协同改性PEO基固态电解质的性能研究

Study on the performance of PEO-based solid-state electrolytes synergistically modified by succinonitrile and boehmite

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    摘要

  • 摘要: 针对聚环氧乙烷(PEO)基固态电解质室温离子电导率低和机械强度差的问题，本研究提出了一种勃姆石(BM)与丁二腈(SN)协同改性的策略。通过水热法调控合成了一系列不同晶粒尺寸的勃姆石，并采用溶液浇铸法制备了PEO-LiTFSI-SN-BM复合固态电解质。利用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)和电化学阻抗谱(EIS)等手段对电解质的结构与性能进行了系统表征。结果表明，SN与勃姆石的引入显著降低了PEO的结晶度，且勃姆石表面的羟基与聚合物链、锂盐阴离子之间存在相互作用，构建了良好的锂离子运输通道。当勃姆石水热温度为220℃、添加量为15wt.%，且SN与EO的摩尔比为1∶4时，所制备的复合电解质(PL24S4B15-220)在30℃下的离子电导率高达0.913×10−4 S·cm−1，比纯PEO电解质(1.16×10−6 S·cm−1)提升了近两个数量级，同时其机械强度和电化学稳定性也得到了显著增强。组装的LiFePO4|PL24S4B15-220|Li电池展现了良好的循环稳定性。本研究为开发高性能、低成本的聚合物基复合固态电解质提供了新思路。

     

    Abstract: To address the low room-temperature ionic conductivity and poor mechanical strength of poly(ethylene oxide) (PEO)-based solid-state electrolytes, this study proposes a synergistic modification strategy using boehmite (BM) and succinonitrile (SN). A series of boehmite samples with different grain sizes were synthesized via a hydrothermal method, and PEO-LiTFSI-SN-BM composite solid electrolytes were prepared by solution casting. The structure and properties of the electrolytes were systematically characterized using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS). The results show that the incorporation of SN and boehmite significantly reduces the crystallinity of PEO. Moreover, interactions between hydroxyl groups on the boehmite surface and the polymer chains as well as lithium salt anions establish favorable lithium-ion transport pathways. When the hydrothermal temperature of boehmite was 220℃ with an addition amount of 15wt.%, and the molar ratio of SN to ethylene oxide (EO) units was 1∶4, the obtained composite electrolyte (PL24S4B15-220) exhibited an ionic conductivity as high as 0.913×10−4 S·cm−1 at 30℃, approximately two orders of magnitude higher than that of the pure PEO electrolyte (1.16×10−6 S·cm−1). Simultaneously, its mechanical strength and electrochemical stability were significantly enhanced. Furthermore, the assembled LiFePO4|PL24S4B15-220|Li battery demonstrated good cycling stability. This study provides a new approach for developing high-performance, low-cost polymer-based composite solid electrolytes.

     

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