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Complex Hydride Solid Electrolytes of the Li(CB9H10)–Li(CB11H12) Quasi-Binary System: Relationship between the Solid Solution and Phase Transition, and the Electrochemical Properties

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Energy Mater. 2020, 3, 5, 4831-4839
    Article

    Complex Hydride Solid Electrolytes of the Li(CB9H10)–Li(CB11H12) Quasi-Binary System: Relationship between the Solid Solution and Phase Transition, and the Electrochemical Properties
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    • Sangryun Kim*
      Sangryun Kim
      Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
      *E-mail: [email protected]
      More by Sangryun Kim
      Orcidhttp://orcid.org/0000-0001-8617-3022
    • Kazuaki Kisu
      Kazuaki Kisu
      WPI-Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
      More by Kazuaki Kisu
      Orcidhttp://orcid.org/0000-0002-1693-4225
    • Shigeyuki Takagi
      Shigeyuki Takagi
      Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
      More by Shigeyuki Takagi
    • Hiroyuki Oguchi
      Hiroyuki Oguchi
      WPI-Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
      New Industry Creation Hatchery Center (NICHe), Tohoku University, Sendai 980-8579, Japan
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    • Shin-ichi Orimo
      Shin-ichi Orimo
      Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
      WPI-Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2020, 3, 5, 4831–4839
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    https://doi.org/10.1021/acsaem.0c00433
    Published April 21, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Closo-type complex hydrides have recently received much attention as promising solid electrolyte systems for all-solid-state batteries, because of the high lithium ion conductivity of their high-temperature (high-T) phases, excellent stability against a lithium metal anode, and a highly deformable nature. However, the superionic conductivity of closo-type complex hydrides is achieved in only a few materials; therefore, an understanding of the material factors involved in the formation of the high-T phase at room temperature and experimental demonstration of their battery applications are required. Here, we report the relationship between the solid solution and formation of the high-T phase of the Li(CB9H10)–Li(CB11H12) quasi-binary system, and the electrochemical properties as a solid electrolyte for all-solid-state Li–TiS2 batteries. The single-phase solid solutions, Li(CB9H10)-based phase in which [CB9H10]− is partially substituted with [CB11H12]− and Li(CB11H12)-based phase in which [CB11H12]− is partially substituted with [CB9H10]−, are obtained at compositions with low- and high-x in the (1 – x)Li(CB9H10)–xLi(CB11H12) (0.1 ≤ x ≤ 0.9) system. The effect of the solid solution on structural changes is more noticeable at low x, whereby a superionic conducting phase is formed with an identical structural framework as that of the high-T phase of Li(CB9H10) at room temperature. In addition, the 0.7Li(CB9H10)–0.3Li(CB11H12) (x = 0.3) solid electrolyte exhibits high chemical/electrochemical stability against a TiS2 cathode, which leads to superior performance in the rate capability and cycle life of all-solid-state Li–TiS2 batteries. The results presented here offer insights into strategies for the design of complex hydride lithium superionic conductors and for the development of all-solid-state batteries with these solid electrolytes.

    Copyright © 2020 American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.0c00433.

    • Additional characterization data (XRD, lattice volume, Raman spectroscopy, DTA, EIS, and battery performance) (PDF)

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    Cited By

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    This article is cited by 34 publications.

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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2020, 3, 5, 4831–4839
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaem.0c00433
    Published April 21, 2020
    Copyright © 2020 American Chemical Society
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