Superhalogen-based lithium superionic conductors

doi:10.1039/c7ta01648d

Title: Superhalogen-based lithium superionic conductors

Abstract

The development of cheap, durable, and safe inorganic solid electrolytes with superionic conductivity is the key for the next generation of all-solid metal-ion batteries. The recent discovery of antiperovskites with composition Li ₃OA (A = halogen) shows promise in this regard. Here, we demonstrate the potential of a new class of antiperovskites where halogens are replaced by BH ₄ superhalogens. In addition to maintaining the high ionic conductivity of Li ₃OA, Li ₃O(BH ₄) is lightweight, mechanically flexible, thermodynamically more stable, and electronically more insulating than Li ₃OA. By mixing BH ₄ with Cl to make Li ₃O(BH ₄) _0.5Cl _0.5, we further show that the conductivity will be doubled. The Li ⁺-ion conductivity of the new materials is of the order of 10 ^-4 to over 10 ^-3 S cm ^-1 at room temperature and will be well above 10 ^-2 S cm ^-1 at higher temperatures below the melting point. The conduction mechanism of the material is revealed by identifying the relationship between the orientational symmetry of the BH ^4- rotors and the potential surface felt by the lithium ions.

Authors:

^[1]; Wang, Shuo ^[2]; Liu, Junyi ^[2]; Sun, Qiang ^[3]; Jena, Puru ^[1]

Virginia Commonwealth Univ., Richmond, VA (United States). Dept. of Physics
Peking Univ., Beijing (China). Department of Materials Science and Engineering
Peking Univ., Beijing (China). Department of Materials Science and Engineering and Center for Applied Physics and Technology

Publication Date:: 2017-01-01

Research Org.:: Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

OSTI Identifier:: 1493600

DOE Contract Number:: FG02-96ER45579; AC02-05CH11231

Resource Type:: Journal Article

Journal Name:: Journal of Materials Chemistry. A

Additional Journal Information:: Journal Volume: 5; Journal Issue: 26; Journal ID: ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Citation Formats


                    Fang, Hong, Wang, Shuo, Liu, Junyi, Sun, Qiang, and Jena, Puru. Superhalogen-based lithium superionic conductors.  United States: N. p., 2017. 
        Web.  doi:10.1039/c7ta01648d.

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                    Fang, Hong, Wang, Shuo, Liu, Junyi, Sun, Qiang, & Jena, Puru. Superhalogen-based lithium superionic conductors.  United States.  doi:10.1039/c7ta01648d.

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                    Fang, Hong, Wang, Shuo, Liu, Junyi, Sun, Qiang, and Jena, Puru. Sun .  
        "Superhalogen-based lithium superionic conductors".  United States.  doi:10.1039/c7ta01648d.

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@article{osti_1493600,

  title        = {Superhalogen-based lithium superionic conductors},

  author       = {Fang, Hong and Wang, Shuo and Liu, Junyi and Sun, Qiang and Jena, Puru},

  abstractNote = {The development of cheap, durable, and safe inorganic solid electrolytes with superionic conductivity is the key for the next generation of all-solid metal-ion batteries. The recent discovery of antiperovskites with composition Li3OA (A = halogen) shows promise in this regard. Here, we demonstrate the potential of a new class of antiperovskites where halogens are replaced by BH4 superhalogens. In addition to maintaining the high ionic conductivity of Li3OA, Li3O(BH4) is lightweight, mechanically flexible, thermodynamically more stable, and electronically more insulating than Li3OA. By mixing BH4 with Cl to make Li3O(BH4)0.5Cl0.5, we further show that the conductivity will be doubled. The Li+-ion conductivity of the new materials is of the order of 10-4 to over 10-3 S cm-1 at room temperature and will be well above 10-2 S cm-1 at higher temperatures below the melting point. The conduction mechanism of the material is revealed by identifying the relationship between the orientational symmetry of the BH4- rotors and the potential surface felt by the lithium ions.},

  doi          = {10.1039/c7ta01648d},

  journal      = {Journal of Materials Chemistry. A},

  issn         = {2050-7488},

  number       = 26,

  volume       = 5,

  place        = {United States},

  year         = {2017},

  month        = {1}

}

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DOI: 10.1039/c7ta01648d

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Title: Superhalogen-based lithium superionic conductors

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

Superhalogens as building blocks of two-dimensional organic–inorganic hybrid perovskites for optoelectronics applications journal, January 2016

Fast Na+-ion transport in skeleton structures journal, February 1976

Design principles for solid-state lithium superionic conductors journal, August 2015

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Spectroscopic Studies of a Superionic Plastic Phase Crystal: Lithium Sulfate journal, January 1988

Structure and properties of complex hydride perovskite materials journal, December 2014

Super-ion inspired colorful hybrid perovskite solar cells journal, January 2016

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Phonons, Localization, and Thermal Conductivity of Diamond Nanothreads and Amorphous Graphene journal, July 2016

Intrinsic and Extrinsic Charge Transport in CH3NH3PbI3 Perovskites Predicted from First-Principles journal, January 2016

A lithium superionic conductor journal, July 2011

Generalized Debye-Peierls/Allen-Feldman model for the lattice thermal conductivity of low-dimensional and disordered materials journal, April 2016

High-pressure lattice dynamic and thermodynamic properties of Ir by first-principles calculation journal, January 2010

Volume Effect or Paddle-Wheel Mechanism—Fast Alkali-Metal Ionic Conduction in Solids with Rotationally Disordered Complex Anions journal, December 1991

A Stable Thin-Film Lithium Electrolyte: Lithium Phosphorus Oxynitride journal, January 1997

Phase Stability and Transport Mechanisms in Antiperovskite Li 3 OCl and Li 3 OBr Superionic Conductors journal, November 2013

Semiempirical GGA-type density functional constructed with a long-range dispersion correction journal, January 2006

Ag–Ag dispersive interaction and physical properties of Ag 3 Co ( CN ) 6 journal, August 2014

Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions journal, January 2015

Plane-wave pseudopotential study for the structural stability of Hf: The role of spin–orbit interaction journal, April 2011

High ionic conductivity in lithium lanthanum titanate journal, June 1993

The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces journal, January 2005

The A-C Conductivity of Polycrystalline LISICON, Li[sub 2+2x]Zn[sub 1−x]GeO[sub 4], and a Model for Intergranular Constriction Resistances journal, January 1983

Orientational order in ionic crystals containing tetrahedral ions journal, December 1983

Ab initio study of the stabilities of and mechanism of superionic transport in lithium-rich antiperovskites journal, April 2013

Ionic Conductivity of Solid Electrolytes Based on Lithium Titanium Phosphate journal, January 1990

Tetragonal Li10GeP2S12 and Li7GePS8 – exploring the Li ion dynamics in LGPS Li electrolytes journal, January 2013

Li-rich anti-perovskite Li 3 OCl films with enhanced ionic conductivity journal, January 2014

Defect chemistry and lithium transport in Li 3 OCl anti-perovskite superionic conductors journal, January 2015

Hydrogen storage properties of LiBH4 journal, August 2003

Superionic Conduction of Sodium and Lithium in Anion-Mixed Hydroborates Na 3 BH 4 B 12 H 12 and (Li 0.7 Na 0.3 ) 3 BH 4 B 12 H 12 journal, August 2015

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

Superionic Conductivity in Lithium-Rich Anti-Perovskites journal, August 2012

Generalized Gradient Approximation Made Simple
journal, October 1996

Superhalogens as building blocks of two-dimensional organic–inorganic hybrid perovskites for optoelectronics applications
journal, January 2016

Fast Na+-ion transport in skeleton structures
journal, February 1976

Design principles for solid-state lithium superionic conductors
journal, August 2015

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Spectroscopic Studies of a Superionic Plastic Phase Crystal: Lithium Sulfate
journal, January 1988

Structure and properties of complex hydride perovskite materials
journal, December 2014

Super-ion inspired colorful hybrid perovskite solar cells
journal, January 2016

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Phonons, Localization, and Thermal Conductivity of Diamond Nanothreads and Amorphous Graphene
journal, July 2016

Intrinsic and Extrinsic Charge Transport in CH3NH3PbI3 Perovskites Predicted from First-Principles
journal, January 2016

A lithium superionic conductor
journal, July 2011

Generalized Debye-Peierls/Allen-Feldman model for the lattice thermal conductivity of low-dimensional and disordered materials
journal, April 2016

High-pressure lattice dynamic and thermodynamic properties of Ir by first-principles calculation
journal, January 2010

Volume Effect or Paddle-Wheel Mechanism—Fast Alkali-Metal Ionic Conduction in Solids with Rotationally Disordered Complex Anions
journal, December 1991

A Stable Thin-Film Lithium Electrolyte: Lithium Phosphorus Oxynitride
journal, January 1997

Phase Stability and Transport Mechanisms in Antiperovskite Li ₃ OCl and Li ₃ OBr Superionic Conductors
journal, November 2013

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

Ag–Ag dispersive interaction and physical properties of ${Ag}_{3} Co (CN)_{6}$
journal, August 2014

Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions
journal, January 2015

Plane-wave pseudopotential study for the structural stability of Hf: The role of spin–orbit interaction
journal, April 2011

High ionic conductivity in lithium lanthanum titanate
journal, June 1993

The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces
journal, January 2005

The A-C Conductivity of Polycrystalline LISICON, Li[sub 2+2x]Zn[sub 1−x]GeO[sub 4], and a Model for Intergranular Constriction Resistances
journal, January 1983

Orientational order in ionic crystals containing tetrahedral ions
journal, December 1983

Ab initio study of the stabilities of and mechanism of superionic transport in lithium-rich antiperovskites
journal, April 2013

Ionic Conductivity of Solid Electrolytes Based on Lithium Titanium Phosphate
journal, January 1990

Tetragonal Li10GeP2S12 and Li7GePS8 – exploring the Li ion dynamics in LGPS Li electrolytes
journal, January 2013

Li-rich anti-perovskite Li ₃ OCl films with enhanced ionic conductivity
journal, January 2014

Defect chemistry and lithium transport in Li ₃ OCl anti-perovskite superionic conductors
journal, January 2015

Hydrogen storage properties of LiBH4
journal, August 2003

Superionic Conduction of Sodium and Lithium in Anion-Mixed Hydroborates Na ₃ BH ₄ B ₁₂ H ₁₂ and (Li _0.7 Na _0.3 ) ₃ BH ₄ B ₁₂ H ₁₂
journal, August 2015

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

Superionic Conductivity in Lithium-Rich Anti-Perovskites
journal, August 2012