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

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 ch...

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Main Authors: Jørgensen, M., Jensen, Steffen, Humphries, Terry, Rowles, Matthew, Sofianos, M. Veronica, Buckley, Craig, Jensen, T.R., Paskevicius, Mark
Format: Journal Article
Published: ACS 2020
Online Access:http://purl.org/au-research/grants/arc/FT160100303
http://hdl.handle.net/20.500.11937/82258
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author Jørgensen, M.
Jensen, Steffen
Humphries, Terry
Rowles, Matthew
Sofianos, M. Veronica
Buckley, Craig
Jensen, T.R.
Paskevicius, Mark
author_facet Jørgensen, M.
Jensen, Steffen
Humphries, Terry
Rowles, Matthew
Sofianos, M. Veronica
Buckley, Craig
Jensen, T.R.
Paskevicius, Mark
author_sort Jørgensen, M.
building Curtin Institutional Repository
collection Online Access
description 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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spelling curtin-20.500.11937-822582021-05-11T03:35:03Z Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity Jørgensen, M. Jensen, Steffen Humphries, Terry Rowles, Matthew Sofianos, M. Veronica Buckley, Craig Jensen, T.R. Paskevicius, Mark 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. 2020 Journal Article http://hdl.handle.net/20.500.11937/82258 10.1021/acs.jpcc.0c02523 http://purl.org/au-research/grants/arc/FT160100303 ACS fulltext
spellingShingle Jørgensen, M.
Jensen, Steffen
Humphries, Terry
Rowles, Matthew
Sofianos, M. Veronica
Buckley, Craig
Jensen, T.R.
Paskevicius, Mark
Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title_full Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title_fullStr Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title_full_unstemmed Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title_short Hydroxylated closo-Dodecaborates M2B12(OH)12 (M = Li, Na, K, and Cs); Structural Analysis, Thermal Properties, and Solid-State Ionic Conductivity
title_sort hydroxylated closo-dodecaborates m2b12(oh)12 (m = li, na, k, and cs); structural analysis, thermal properties, and solid-state ionic conductivity
url http://purl.org/au-research/grants/arc/FT160100303
http://hdl.handle.net/20.500.11937/82258