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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

  • 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
  • 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
  • Shigeyuki Takagi
    Shigeyuki Takagi
    Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
  • 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
  • , and 
  • 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
Cite this: ACS Appl. Energy Mater. 2020, 3, 5, 4831–4839
Publication Date (Web):April 21, 2020
https://doi.org/10.1021/acsaem.0c00433
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.

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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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