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    Energy, Environmental, and Catalysis Applications

    Enhanced Free Li-Ion Mobility in Solid-State Electrolytes via Long-Range Assembly of Porous Materials
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    • Gi Hwan Kim
      Gi Hwan Kim
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
      More by Gi Hwan Kim
      Orcidhttps://orcid.org/0000-0002-1690-4202
    • Jinha Jang
      Jinha Jang
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
      More by Jinha Jang
    • Jiheong Kang*
      Jiheong Kang
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
      *Email: [email protected]
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 28, 36479–36488
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    https://doi.org/10.1021/acsami.4c07495
    Published July 1, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Metal–organic frameworks (MOFs), with their tunable pore sizes and high surface areas, are gaining prominence in Li metal battery applications, including their use as nanofillers in solid composite electrolytes (SCEs) for enhanced ionic conductivity. Yet, when used in SCEs, individual dispersed MOF particles in isolation as nanofillers can impede efficient ion transport in all-solid-state batteries due to the insufficient supply of ionic transport pathways within SCEs. Here, we introduced a continuous SCE nanofiller with long-range assembly interconnected porous MOFs (IMOF_SCE) for effective ion transport pathway supply along the interface between the nanofiller and the polymer matrix. IMOF_SCE achieved Li-ion conductivity (6.72 × 10–5 S cm–1 at 20 °C) and Li-ion transference number (tLi+ = 0.855), resulting in the improved electrochemical performance of Li metal batteries. Additionally, the Li/LiFePO4 full cell integrated with IMOF_SCE achieved an outstanding stable capacity retention of 98.8% in 300 cycles. This work offers insights into the design strategy of effective nanofillers for SCEs and can be adapted for other porous materials.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.4c07495.

    • SEM image of as-synthesized IMOF with different magnifications; comparison of MOF growth according to the type of substrate; STEM image of as-synthesized IMOF with different magnifications; HAADF-STEM and EDS elemental mapping images of the as-synthesized interconnected MOF nanofiller; flexible property of IMOF_SCE as the bending of the free-standing film; XRD patterns of MOF, BC, IMOF, and IMOF_SCE; Raman spectroscopy curves of MOF (UiO-66), IMOF_nanofiller, PEO + LiTFSI solid electrolyte, and IMOF_SCE; TGA curve of MOF powder, IMOF membrane, and IMOF_SCE in air atmosphere conditions; measured ionic conductivities of PEO, DMOF_SCE, and IMOF_SCE depending on temperatures; DSC curves of SCEs showing a glass transition temperature; current–time curve with polarization and the inset shows EIS Nyquist plots before and after polarization of the Li metal symmetric cell with IMOF_SCE; enlarged charge/discharge overpotentials curve of SCEs at 2 mA cm–1 current density; enlarged charge/discharge overpotentials curve of SCEs at 0.1 mA cm–1 current density after high current density cycles; LSV curves of each SCE at room temperature; enlarged charge/discharge overpotentials profile curve of SCEs around 1000 h with 0.1 mA cm–2 and 0.1 mAh cm–2 conditions; Coulombic efficiency data of the Li/Cu cell with SCEs under 0.1 mA cm–2 and 0.1 mAh cm–2 conditions; Coulombic efficiency measured by the Aurbach method of Li/Cu cells with different SCEs; galvanostatic charge/discharge voltage profiles of Li/LFP full cells using the PEO electrolyte at the first cycle of each of the different current densities; and comparison of the Li-ion transference numbers of previously reported MOF-utilized SCEs (PDF)

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    This article is cited by 1 publications.

    1. Shruti Suriyakumar, Rohit M. Manoj, Sreelakshmy K. Jayaprakash, Sreelakshmi Anil Kumar, Keerthy P. Sudhakaran, Vinesh Vijayan, Manikoth M. Shaijumon. Metal–organic frameworks as conductivity enhancers for all-solid-state lithium batteries. RSC Applied Interfaces 2024, 1 (6) , 1436-1442. https://doi.org/10.1039/D4LF00263F
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 28, 36479–36488
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.4c07495
    Published July 1, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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