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    Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity

    82300.pdf (1.030Mb)
    Access Status
    Open access
    Authors
    Jørgensen, M.
    Jensen, Steffen
    Humphries, Terry
    Rowles, Matthew
    Sofianos, M. Veronica
    Buckley, Craig
    Jensen, T.R.
    Paskevicius, Mark
    Date
    2020
    Type
    Journal Article
    
    Metadata
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    Citation
    Jørgensen, M. and Jensen, S.R.H. and Humphries, T.D. and Rowles, M.R. and Sofianos, M.V. and Buckley, C.E. and Jensen, T.R. et al. 2020. Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity. Journal of Physical Chemistry C. 124 (21): pp. 11340-11349.
    Source Title
    Journal of Physical Chemistry C
    DOI
    10.1021/acs.jpcc.0c02523
    ISSN
    1932-7447
    Faculty
    Faculty of Science and Engineering
    School
    John de Laeter Centre (JdLC)
    School of Electrical Engineering, Computing and Mathematical Sciences (EECMS)
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/FT160100303
    URI
    http://hdl.handle.net/20.500.11937/82258
    Collection
    • Curtin Research Publications
    Abstract

    Copyright © 2020 American Chemical Society.

    Closo-borates and derivatives thereof have shown great potential as electrolyte materials for all-solid-state batteries owing to their exceptional ionic conductivity and high thermal and chemical stability. However, because of the myriad of possible chemical modifications of the large, complex anion, only a fraction of closo-borate derivatives has so far been investigated as electrolyte materials. Here, the crystal structures, thermal properties, and ionic conductivities of M2B12(OH)12 (M = Li, Na, K, and Cs) are investigated with a focus on their possible utilization as new solid-state ion conductors for solid-state batteries. The compounds generally show rich thermal polymorphism, with eight identified polymorphs among the four dehydrated compounds. Both Li2B12(OH)12 and Na2B12(OH)12 undergo a first-order transition, in which the cation sublattices become disordered, resulting in an order of magnitude jump in ionic conductivity for Na2B12(OH)12. K2B12(OH)12 undergoes a second-order polymorphic transition driven by a change in the anion-cation interaction, with no evidence of dynamic disorder. The ionic conductivities of M2B12(OH)12 range from 1.60 × 10-8 to 5.97 × 10-5 S cm-1 at 250 °C for M = Cs and Li, respectively, showing decreasing conductivity with increasing cation size. Compared with the analogous M2B12H12 compounds, such relatively low conductivities are suggested to be a consequence of strong and directional anion-cation interactions, resulting in a more static anion framework.

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