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Title: Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions

Abstract

Solid electrolytes with sufficiently high conductivities and stabilities are the elusive answer to the inherent shortcomings of organic liquid electrolytes prevalent in today's rechargeable batteries. We recently revealed a novel fast-ion-conducting sodium salt, Na2B12H12, which contains large, icosahedral, divalent B12H122– anions that enable impressive superionic conductivity, albeit only above its 529 K phase transition. Its lithium congener, Li2B12H12, possesses an even more technologically prohibitive transition temperature above 600 K. Here we show that the chemically related LiCB11H12 and NaCB11H12 salts, which contain icosahedral, monovalent CB11H12– anions, both exhibit much lower transition temperatures near 400 K and 380 K, respectively, and truly stellar ionic conductivities (>0.1 S cm–1) unmatched by any other known polycrystalline materials at these temperatures. Furthermore with proper modifications, we are confident that room-temperature-stabilized superionic salts incorporating such large polyhedral anion building blocks are attainable, thus enhancing their future prospects as practical electrolyte materials in next-generation, all-solid-state batteries.

Authors:
 [1];  [2];  [3];  [4];  [2];  [3];  [2];  [3]
  1. National Institute of Standards and Technology, Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
  2. Tohoku Univ., Sendai (Japan)
  3. National Institute of Standards and Technology, Gaithersburg, MD (United States)
  4. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
OSTI Identifier:
1327910
Report Number(s):
SAND-2016-9600J
Journal ID: ISSN 1754-5692; EESNBY; 647755
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 8; Journal Issue: 12; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Tang, Wan Si, Unemoto, Atsushi, Zhou, Wei, Stavila, Vitalie, Matsuo, Motoaki, Wu, Hui, Orimo, Shin-ichi, and Udovic, Terrence J. Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions. United States: N. p., 2015. Web. doi:10.1039/c5ee02941d.
Tang, Wan Si, Unemoto, Atsushi, Zhou, Wei, Stavila, Vitalie, Matsuo, Motoaki, Wu, Hui, Orimo, Shin-ichi, & Udovic, Terrence J. Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions. United States. doi:10.1039/c5ee02941d.
Tang, Wan Si, Unemoto, Atsushi, Zhou, Wei, Stavila, Vitalie, Matsuo, Motoaki, Wu, Hui, Orimo, Shin-ichi, and Udovic, Terrence J. Thu . "Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions". United States. doi:10.1039/c5ee02941d. https://www.osti.gov/servlets/purl/1327910.
@article{osti_1327910,
title = {Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions},
author = {Tang, Wan Si and Unemoto, Atsushi and Zhou, Wei and Stavila, Vitalie and Matsuo, Motoaki and Wu, Hui and Orimo, Shin-ichi and Udovic, Terrence J.},
abstractNote = {Solid electrolytes with sufficiently high conductivities and stabilities are the elusive answer to the inherent shortcomings of organic liquid electrolytes prevalent in today's rechargeable batteries. We recently revealed a novel fast-ion-conducting sodium salt, Na2B12H12, which contains large, icosahedral, divalent B12H122– anions that enable impressive superionic conductivity, albeit only above its 529 K phase transition. Its lithium congener, Li2B12H12, possesses an even more technologically prohibitive transition temperature above 600 K. Here we show that the chemically related LiCB11H12 and NaCB11H12 salts, which contain icosahedral, monovalent CB11H12– anions, both exhibit much lower transition temperatures near 400 K and 380 K, respectively, and truly stellar ionic conductivities (>0.1 S cm–1) unmatched by any other known polycrystalline materials at these temperatures. Furthermore with proper modifications, we are confident that room-temperature-stabilized superionic salts incorporating such large polyhedral anion building blocks are attainable, thus enhancing their future prospects as practical electrolyte materials in next-generation, all-solid-state batteries.},
doi = {10.1039/c5ee02941d},
journal = {Energy & Environmental Science},
number = 12,
volume = 8,
place = {United States},
year = {2015},
month = {10}
}

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Cited by: 43 works
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Works referenced in this record:

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    Works referencing / citing this record:

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    dataset, September 2018


    Complex Hydrides for Electrochemical Energy Storage
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    • Unemoto, Atsushi; Matsuo, Motoaki; Orimo, Shin-ichi
    • Advanced Functional Materials, Vol. 24, Issue 16
    • DOI: 10.1002/adfm.201303147

    New, Highly Ion-Conductive Crystals Precipitated from Li2S-P2S5 Glasses
    journal, April 2005

    • Mizuno, F.; Hayashi, A.; Tadanaga, K.
    • Advanced Materials, Vol. 17, Issue 7, p. 918-921
    • DOI: 10.1002/adma.200401286

    Exceptional Superionic Conductivity in Disordered Sodium Decahydro- closo -decaborate
    journal, October 2014

    • Udovic, Terrence J.; Matsuo, Motoaki; Tang, Wan Si
    • Advanced Materials, Vol. 26, Issue 45
    • DOI: 10.1002/adma.201403157

    Lithium Fast-Ionic Conduction in Complex Hydrides: Review and Prospects
    journal, January 2011


    Fast Lithium Ion Conduction in Garnet-Type Li7La3Zr2O12
    journal, October 2007

    • Murugan, Ramaswamy; Thangadurai, Venkataraman; Weppner, Werner
    • Angewandte Chemie International Edition, Vol. 46, Issue 41, p. 7778-7781
    • DOI: 10.1002/anie.200701144

    Superhalogens as Building Blocks of Halogen-Free Electrolytes in Lithium-Ion Batteries
    journal, October 2014

    • Giri, Santanab; Behera, Swayamprabha; Jena, Puru
    • Angewandte Chemie International Edition, Vol. 53, Issue 50
    • DOI: 10.1002/anie.201408648

    An Efficient Halogen-Free Electrolyte for Use in Rechargeable Magnesium Batteries
    journal, May 2015

    • Tutusaus, Oscar; Mohtadi, Rana; Arthur, Timothy S.
    • Angewandte Chemie International Edition, Vol. 54, Issue 27
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    • Solid State Communications, Vol. 86, Issue 10, p. 689-693
    • DOI: 10.1016/0038-1098(93)90841-a

    AgI-type solid electrolytes
    journal, January 1976


    Recent advances in magnetic structure determination by neutron powder diffraction
    journal, October 1993


    Alkali and alkaline-earth metal dodecahydro-closo-dodecaborates: Probing structural variations via neutron vibrational spectroscopy
    journal, September 2011


    Altering the structural properties of A2B12H12 compounds via cation and anion modifications
    journal, October 2015


    Evidence of a transition to reorientational disorder in the cubic alkali-metal dodecahydro-closo-dodecaborates
    journal, November 2011


    Complex high-temperature phase transitions in Li2B12H12 and Na2B12H12
    journal, April 2014


    The design of a bismuth-based auxiliary filter for the removal of spurious background scattering associated with filter-analyzer neutron spectrometers
    journal, April 2008

    • Udovic, T. J.; Brown, C. M.; Leão, J. B.
    • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 588, Issue 3
    • DOI: 10.1016/j.nima.2008.02.006

    Conductivity measurements on nasicon and nasicon-modified materials
    journal, July 1999


    Structure and dynamics from combined neutron scattering and first-principles studies
    journal, November 2000


    The Disk Chopper Spectrometer at NIST: a new instrument for quasielastic neutron scattering studies
    journal, August 2003


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    journal, March 2015

    • Wu, Hui; Tang, Wan Si; Stavila, Vitalie
    • The Journal of Physical Chemistry C, Vol. 119, Issue 12
    • DOI: 10.1021/acs.jpcc.5b00533

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    journal, August 2013

    • Douvris, Christos; Michl, Josef
    • Chemical Reviews, Vol. 113, Issue 10
    • DOI: 10.1021/cr400059k

    Crystal Structure of Li 2 B 12 H 12 : a Possible Intermediate Species in the Decomposition of LiBH 4
    journal, November 2008

    • Her, Jae-Hyuk; Yousufuddin, Muhammed; Zhou, Wei
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    • DOI: 10.1021/ic801345h

    The least coordinating anion
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    • Shelly, Kenneth.; Reed, Christopher A.; Lee, Young Ja.
    • Journal of the American Chemical Society, Vol. 108, Issue 11
    • DOI: 10.1021/ja00271a058

    Metal Cation−Methyl Interactions in CB 11 Me 12 - Salts of Me 3 Ge + , Me 3 Sn + , and Me 3 Pb +
    journal, September 2004

    • Zharov, Ilya; Weng, Tsu-Chien; Orendt, Anita M.
    • Journal of the American Chemical Society, Vol. 126, Issue 38
    • DOI: 10.1021/ja0475205

    Anionic Oligomerization of Li 2 [B 12 H 12 ] and Li[CB 11 H 12 ]: An Experimental and Computational Study
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    • The Journal of Physical Chemistry C, Vol. 117, Issue 3
    • DOI: 10.1021/jp3102354

    Nuclear Magnetic Resonance Study of Atomic Motion in A 2 B 12 H 12 (A = Na, K, Rb, Cs): Anion Reorientations and Na + Mobility
    journal, November 2013

    • Skripov, Alexander V.; Babanova, Olga A.; Soloninin, Alexei V.
    • The Journal of Physical Chemistry C, Vol. 117, Issue 49
    • DOI: 10.1021/jp4106585

    Nuclear Magnetic Resonance Study of Atomic Motion in the Mixed Borohydride–Amide Na 2 (BH 4 )(NH 2 )
    journal, June 2014

    • Soloninin, Alexei V.; Babanova, Olga A.; Medvedev, Evgeny Y.
    • The Journal of Physical Chemistry C, Vol. 118, Issue 27
    • DOI: 10.1021/jp503451d

    Anion Reorientations in the Superionic Conducting Phase of Na 2 B 12 H 12
    journal, July 2014

    • Verdal, Nina; Udovic, Terrence J.; Stavila, Vitalie
    • The Journal of Physical Chemistry C, Vol. 118, Issue 31
    • DOI: 10.1021/jp506252c

    Role of Cation Size on the Structural Behavior of the Alkali-Metal Dodecahydro- closo -Dodecaborates
    journal, June 2009

    • Her, Jae-Hyuk; Zhou, Wei; Stavila, Vitalie
    • The Journal of Physical Chemistry C, Vol. 113, Issue 26
    • DOI: 10.1021/jp904980m

    Superionic glass-ceramic electrolytes for room-temperature rechargeable sodium batteries
    journal, January 2012

    • Hayashi, Akitoshi; Noi, Kousuke; Sakuda, Atsushi
    • Nature Communications, Vol. 3, Issue 1
    • DOI: 10.1038/ncomms1843

    A lithium superionic conductor
    journal, July 2011

    • Kamaya, Noriaki; Homma, Kenji; Yamakawa, Yuichiro
    • Nature Materials, Vol. 10, Issue 9, p. 682-686
    • DOI: 10.1038/nmat3066

    Sodium superionic conduction in Na 2 B 12 H 12
    journal, January 2014

    • Udovic, Terrence J.; Matsuo, Motoaki; Unemoto, Atsushi
    • Chem. Commun., Vol. 50, Issue 28
    • DOI: 10.1039/c3cc49805k

    First-order phase transition in the Li2B12H12 system
    journal, January 2013

    • Paskevicius, Mark; Pitt, Mark P.; Brown, David H.
    • Physical Chemistry Chemical Physics, Vol. 15, Issue 38
    • DOI: 10.1039/c3cp53090f

    High temperature sodium batteries: status, challenges and future trends
    journal, January 2013

    • Hueso, Karina B.; Armand, Michel; Rojo, Teófilo
    • Energy & Environmental Science, Vol. 6, Issue 3
    • DOI: 10.1039/c3ee24086j

    The structure of monoclinic Na 2 B 10 H 10 : a combined diffraction, spectroscopy, and theoretical approach
    journal, January 2015

    • Wu, Hui; Tang, Wan Si; Zhou, Wei
    • CrystEngComm, Vol. 17, Issue 18
    • DOI: 10.1039/c5ce00369e

    Lithium superionic conduction in lithium borohydride accompanied by structural transition
    journal, November 2007

    • Matsuo, Motoaki; Nakamori, Yuko; Orimo, Shin-ichi
    • Applied Physics Letters, Vol. 91, Issue 22
    • DOI: 10.1063/1.2817934

    Sodium ionic conduction in complex hydrides with [BH 4 ] and [NH 2 ] anions
    journal, May 2012

    • Matsuo, Motoaki; Kuromoto, Shingo; Sato, Toyoto
    • Applied Physics Letters, Vol. 100, Issue 20
    • DOI: 10.1063/1.4716021

    Development of bulk-type all-solid-state lithium-sulfur battery using LiBH 4 electrolyte
    journal, August 2014

    • Unemoto, Atsushi; Yasaku, Syun; Nogami, Genki
    • Applied Physics Letters, Vol. 105, Issue 8
    • DOI: 10.1063/1.4893666

    A study of the electrical properties of single-crystal and polycrystalline β-alumina using complex plane analysis
    journal, August 1977


    VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
    journal, October 2011


    A profile refinement method for nuclear and magnetic structures
    journal, June 1969


    Lithium Ionic Conductor Thio-LISICON: The Li2S-GeS2-P2S5 System
    journal, January 2001

    • Kanno, Ryoji; Murayama, Masahiro
    • Journal of The Electrochemical Society, Vol. 148, Issue 7, p. A742-A746
    • DOI: 10.1149/1.1379028

    Ab initio Force Constant Approach to Phonon Dispersion Relations of Diamond and Graphite
    journal, December 1995


    DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
    journal, November 2009

    • Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
    • Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
    • DOI: 10.6028/jres.114.025

    A 3D Analogue of Phenyllithium: Solution-Phase, Solid-State, and Computational Study of the Lithiacarborane [Li−CB 11 H 11 ] −
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    • Angewandte Chemie International Edition, Vol. 58, Issue 52
    • DOI: 10.1002/anie.201910568

    Chemistry Design Towards a Stable Sulfide-Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12
    journal, April 2019

    • Wang, Yingqi; Lü, Xujie; Zheng, Chong
    • Angewandte Chemie International Edition, Vol. 58, Issue 23
    • DOI: 10.1002/anie.201901739

    A 3D Analogue of Phenyllithium: Solution-Phase, Solid-State, and Computational Study of the Lithiacarborane [Li−CB 11 H 11 ] −
    journal, November 2019

    • Dontha, Rakesh; Zhu, Tian-Cheng; Shen, Yunjun
    • Angewandte Chemie International Edition, Vol. 58, Issue 52
    • DOI: 10.1002/anie.201910568

    Vacancies in functional materials for clean energy storage and harvesting: the perfect imperfection
    journal, January 2017

    • Li, Guowei; Blake, Graeme R.; Palstra, Thomas T. M.
    • Chemical Society Reviews, Vol. 46, Issue 6
    • DOI: 10.1039/c6cs00571c

    Borohydride-Scaffolded Li/Na/Mg Fast Ionic Conductors for Promising Solid-State Electrolytes
    journal, October 2018


    Complex Hydrides for Energy Storage, Conversion, and Utilization
    journal, July 2019


    Liquid‐Like Ionic Conduction in Solid Lithium and Sodium Monocarba‐ closo ‐Decaborates Near or at Room Temperature
    journal, February 2016

    • Tang, Wan Si; Matsuo, Motoaki; Wu, Hui
    • Advanced Energy Materials, Vol. 6, Issue 8
    • DOI: 10.1002/aenm.201502237

    Solid-State Sodium Batteries
    journal, February 2018

    • Zhao, Chenglong; Liu, Lilu; Qi, Xingguo
    • Advanced Energy Materials, Vol. 8, Issue 17
    • DOI: 10.1002/aenm.201703012

    Sodium-Ion Battery Electrolytes: Modeling and Simulations
    journal, February 2018

    • Åvall, Gustav; Mindemark, Jonas; Brandell, Daniel
    • Advanced Energy Materials, Vol. 8, Issue 17
    • DOI: 10.1002/aenm.201703036

    Carbon Incorporation and Anion Dynamics as Synergistic Drivers for Ultrafast Diffusion in Superionic LiCB 11 H 12 and NaCB 11 H 12
    journal, February 2018

    • Dimitrievska, Mirjana; Shea, Patrick; Kweon, Kyoung E.
    • Advanced Energy Materials, Vol. 8, Issue 15
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    Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12
    journal, April 2019


    A 3D Analogue of Phenyllithium: Solution‐Phase, Solid‐State, and Computational Study of the Lithiacarborane [Li−CB 11 H 11 ]
    journal, November 2019

    • Dontha, Rakesh; Zhu, Tian‐Cheng; Shen, Yunjun
    • Angewandte Chemie, Vol. 131, Issue 52
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    Magnesium‐Based Clusters as Building Blocks of Electrolytes in Lithium‐Ion Batteries
    journal, July 2019


    The renaissance of hydrides as energy materials
    journal, December 2016


    A complex hydride lithium superionic conductor for high-energy-density all-solid-state lithium metal batteries
    journal, March 2019


    Fundamentals of inorganic solid-state electrolytes for batteries
    journal, August 2019

    • Famprikis, Theodosios; Canepa, Pieremanuele; Dawson, James A.
    • Nature Materials, Vol. 18, Issue 12
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    Dynamics of porous and amorphous magnesium borohydride to understand solid state Mg-ion-conductors
    journal, June 2020


    Metal borohydrides and derivatives – synthesis, structure and properties
    journal, January 2017

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    A highly stable sodium solid-state electrolyte based on a dodeca/deca-borate equimolar mixture
    journal, January 2017

    • Duchêne, L.; Kühnel, R. -S.; Rentsch, D.
    • Chemical Communications, Vol. 53, Issue 30
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    Superhalogen-based lithium superionic conductors
    journal, January 2017

    • Fang, Hong; Wang, Shuo; Liu, Junyi
    • Journal of Materials Chemistry A, Vol. 5, Issue 26
    • DOI: 10.1039/c7ta01648d

    Teaching an old dog new tricks: new directions in fundamental and applied closo -carborane anion chemistry
    journal, January 2019

    • Fisher, Steven P.; Tomich, Anton W.; Guo, Juchen
    • Chemical Communications, Vol. 55, Issue 12
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    Theoretical description of alkali metal closo -boranes – towards the crystal structure of MgB 12 H 12
    journal, January 2018

    • Maniadaki, Aristea E.; Łodziana, Zbigniew
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    Superatom chemistry: promising properties of near-spherical noble metal clusters
    journal, January 2018

    • Roduner, Emil
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    • DOI: 10.1039/c8cp04651d

    Novel and versatile room temperature ionic liquids for energy storage
    journal, January 2019

    • Kar, Mega; Tutusaus, Oscar; MacFarlane, Douglas R.
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    Combining proton and silaborane-based superhalogen anions – an effective route to new superacids as verified via systematic DFT calculations
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    Ultra stable superatomic structure of doubly magic Ga 13 and Ga 13 Li electrolyte
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    • Nanoscale, Vol. 12, Issue 1
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    Interatomic potential construction with self-learning and adaptive database
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    Reorientational motion and Li + -ion transport in Li 2 B 12 H 12 system: Molecular dynamics study
    journal, July 2019


    Lightweight complex metal hydrides for Li-, Na-, and Mg-based batteries
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    Complex Metal Hydrides for Hydrogen, Thermal and Electrochemical Energy Storage
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