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Understanding Ion Dynamics in Closoborate-Type Lithium-Ion Conductors on Different Time-Scales

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    Physical Insights into Energy Science

    Understanding Ion Dynamics in Closoborate-Type Lithium-Ion Conductors on Different Time-Scales
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    • Arunkumar Dorai*
      Arunkumar Dorai
      Institute of Multidisciplinary Research for Advanced Materials (IMRAM), Tohoku University, Sendai, Miyagi 980-8577, Japan
      Institute of Materials Research (IMR), Tohoku University, Sendai, Miyagi 980-8577, Japan
      *Email: [email protected]
      More by Arunkumar Dorai
      Orcidhttps://orcid.org/0000-0001-5296-263X
    • Sangryun Kim*
      Sangryun Kim
      Institute of Materials Research (IMR), Tohoku University, Sendai, Miyagi 980-8577, Japan
      Graduate School of Energy Convergence, Gwangju Institute of Science and Technology (GIST), 123 Cheomdangwagi-ro, Gwangju 61005, Republic of Korea
      *Email: [email protected]
      More by Sangryun Kim
    • Naoaki Kuwata
      Naoaki Kuwata
      Institute of Multidisciplinary Research for Advanced Materials (IMRAM), Tohoku University, Sendai, Miyagi 980-8577, Japan
      National Institute of Materials Science, Tsukuba, Ibaraki 305-0047, Japan
      More by Naoaki Kuwata
      Orcidhttps://orcid.org/0000-0002-0736-6967
    • Junichi Kawamura
      Junichi Kawamura
      Institute of Multidisciplinary Research for Advanced Materials (IMRAM), Tohoku University, Sendai, Miyagi 980-8577, Japan
      More by Junichi Kawamura
    • Kazuaki Kisu
      Kazuaki Kisu
      Institute of Materials Research (IMR), Tohoku University, Sendai, Miyagi 980-8577, Japan
      College of Engineering, Shibaura Institute of Technology, Tokyo 108-8548, Japan
      More by Kazuaki Kisu
    • Shin-ichi Orimo*
      Shin-ichi Orimo
      Institute of Materials Research (IMR), Tohoku University, Sendai, Miyagi 980-8577, Japan
      Advanced Institute for Materials Research (AIMR), Tohoku University, Sendai, Miyagi 980-8577, Japan
      *Email: [email protected]
      More by Shin-ichi Orimo
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2024, 15, 18, 4864–4871
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    https://doi.org/10.1021/acs.jpclett.4c00754
    Published April 26, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    The lithium-ion transport mechanism in 0.7Li(CB9H10)–0.3Li(CB11H12) complex hydride solid electrolyte was studied over a wide time-scale (ns–ms) by choosing appropriate techniques for assessing ionic motion on the desired time-scale using nuclear magnetic resonance (NMR) relaxation, AC impedance, and pulsed field gradient-NMR (PFG-NMR) measurements. The 7Li NMR line width decreased with increasing temperature, and the spin–lattice relaxation time T1 for the cation and anions showed a minimum near 303 K, indicating that the lithium ions and the anions were highly mobile. The activation energy estimated from the analysis of the NMR relaxation time matched well with the values estimated from the AC impedance and PFG-NMR. This confirms that the lithium-ion motion in 0.7Li(CB9H10)–0.3Li(CB11H12) is the same over a wide time-scale, suggesting steady Li-ion motion over a wide transport range. This understanding offers insights into strategies for designing complex hydride lithium superionic conductors.

    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/acs.jpclett.4c00754.

    • Temperature dependence of the 1H, 11B NMR line width and correlation time (PDF)

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    This article is cited by 2 publications.

    1. Taehyun Kim, Taeseung Kim, Taegyoung Lee, Ye-Eun Park, Jeonghyun Kim, Seoungjae Kang, Hyerim Kim, Seokjae Hong, Naoki Matsui, Hyungsub Kim, Sangryun Kim. Hydride Ion Conductors with Polyanionic Complex Anions. Journal of the American Chemical Society 2025, 147 (17) , 14244-14253. https://doi.org/10.1021/jacs.4c17532
    2. Hyerim Kim, Taehyun Kim, Seunghee Joo, Jeonghyun Kim, Jaehyun Noh, Jiyoung Ma, Jung–Je Woo, Seungho Choi, KyungSu Kim, Woosuk Cho, Kazuaki Kisu, Shin–ichi Orimo, Sangryun Kim. Aqueous synthesis of lithium superionic-conducting complex hydride solid electrolytes. Journal of Materials Chemistry A 2024, 12 (46) , 32132-32139. https://doi.org/10.1039/D4TA05962J
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2024, 15, 18, 4864–4871
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.4c00754
    Published April 26, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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