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<p>Composite solid electrolytes (CSEs) combine the advantages of solid polymer electrolytes and inorganic solid electrolytes, making them promising candidates for all-solid-state lithium metal batteries. However, current CSEs exhibit deficiencies such as low ionic conductivity, lithium dendrite growth, and susceptibility to damage of the electrolyte membrane, which hinder their practical applications. Therefore, designing composite solid electrolytes with novel structures is crucial for enhancing the overall performance of batteries. In this study, PVDF-HFP was chosen as the polymer electrolyte matrix, while a network structure filled with two-dimensional MOF (UMCM-309a) served as the skeleton. The composite solid electrolyte (CSE) was prepared using a simple solution casting method, incorporating PVDF-HFP, lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), and two-dimensional MOF (UMCM-309a). The developed PVDF-HFP/LiTFSI/MOF (PLM) electrolyte demonstrates remarkable ionic conductivity of 5.7 × 10<sup>−4</sup> S cm<sup>−1</sup> at 60&#xa0;°C, along with an extensive electrochemical stability window of 4.8&#xa0;V. The Li|10% PLM CSE|LiFePO<sub>4</sub> cell exhibits exceptional cycling performance and longevity, maintaining 95% capacity retention after 1000 cycles of stable operation at 60&#xa0;°C and a rate of 1 C. Furthermore, the Li | Li symmetric cell illustrates strong interfacial compatibility, achieving stable cycling for 1100&#xa0;h at a current density of 0.1&#xa0;mA&#xa0;cm<sup>−2</sup>. Therefore, the PLM CSE composite provides a straightforward and effective approach for achieving high-performance lithium batteries, facilitating ultra-stable operation in solid-state lithium metal batteries.</p> Graphical Abstract <p></p>

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Incorporating lithium salts into two-dimensional metal–organic frameworks (MOFs) to create high-performance solid-state lithium metal batteries

  • 期刊论文

  • 发表日期：

    2025年8月8日

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  • Ning Yin,
  • Qiaoxia Li,
  • Fuming Wang,
  • Yulin Min,
  • Qunjie Xu

摘要

Composite solid electrolytes (CSEs) combine the advantages of solid polymer electrolytes and inorganic solid electrolytes, making them promising candidates for all-solid-state lithium metal batteries. However, current CSEs exhibit deficiencies such as low ionic conductivity, lithium dendrite growth, and susceptibility to damage of the electrolyte membrane, which hinder their practical applications. Therefore, designing composite solid electrolytes with novel structures is crucial for enhancing the overall performance of batteries. In this study, PVDF-HFP was chosen as the polymer electrolyte matrix, while a network structure filled with two-dimensional MOF (UMCM-309a) served as the skeleton. The composite solid electrolyte (CSE) was prepared using a simple solution casting method, incorporating PVDF-HFP, lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), and two-dimensional MOF (UMCM-309a). The developed PVDF-HFP/LiTFSI/MOF (PLM) electrolyte demonstrates remarkable ionic conductivity of 5.7 × 10−4 S cm−1 at 60 °C, along with an extensive electrochemical stability window of 4.8 V. The Li|10% PLM CSE|LiFePO4 cell exhibits exceptional cycling performance and longevity, maintaining 95% capacity retention after 1000 cycles of stable operation at 60 °C and a rate of 1 C. Furthermore, the Li | Li symmetric cell illustrates strong interfacial compatibility, achieving stable cycling for 1100 h at a current density of 0.1 mA cm−2. Therefore, the PLM CSE composite provides a straightforward and effective approach for achieving high-performance lithium batteries, facilitating ultra-stable operation in solid-state lithium metal batteries.

Graphical Abstract