Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12

Wang, Yingqi; Lü, Xujie; Zheng, Chong; Liu, Xiang; Chen, Zonghai; Yang, Wenge; Lin, Jianhua; Huang, Fuqiang

doi:10.1002/ange.201901739

Title: Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li ₄ Cu ₈ Ge ₃ S ₁₂

Abstract

Abstract Sulfide‐based superionic conductors with high ionic conductivity have been explored as candidates for solid‐state Li batteries. However, moisture hypersensitivity has made their manufacture complicated and costly and also impeded applications in batteries. Now, a sulfide‐based superionic conductor Li ₄ Cu ₈ Ge ₃ S ₁₂ with superior stability was developed based on the hard/soft acid–base theory. The compound is stable in both moist air and aqueous LiOH aqueous solution. The electrochemical stability window was up to 1.5 V. An ionic conductivity of 0.9×10 ⁻⁴ S cm with low activation energy of 0.33 eV was achieved without any optimization. The material features a rigid Cu‐Ge‐S open framework that increases its stability. Meanwhile, the weak bonding between Li ⁺ and the framework promotes ionic conductivity. This work provides a structural configuration in which weak Li bonding in the rigid framework promotes an environment for highly conductive and stable solid‐state electrolytes.

Authors:

Wang, Yingqi ^[1];

^[1]; Zheng, Chong ^[2]; Liu, Xiang ^[3]; Chen, Zonghai ^[3]; Yang, Wenge ^[1]; Lin, Jianhua ^[4]; Huang, Fuqiang ^[5]

Center for High Pressure Science &, Technology Advanced Research Shanghai 206203 P. R. China
Department of Chemistry and Biochemistry Northern Illinois University DeKalb IL 60115 USA
Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA
State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China
State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China, CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 P. R. China

Publication Date:: Mon Apr 29 00:00:00 EDT 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1509751

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 131 Journal Issue: 23; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Wang, Yingqi, Lü, Xujie, Zheng, Chong, Liu, Xiang, Chen, Zonghai, Yang, Wenge, Lin, Jianhua, and Huang, Fuqiang. Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12.  Germany: N. p., 2019. 
Web.  doi:10.1002/ange.201901739.

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                    Wang, Yingqi, Lü, Xujie, Zheng, Chong, Liu, Xiang, Chen, Zonghai, Yang, Wenge, Lin, Jianhua, & Huang, Fuqiang. Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12.  Germany.  https://doi.org/10.1002/ange.201901739

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                    Wang, Yingqi, Lü, Xujie, Zheng, Chong, Liu, Xiang, Chen, Zonghai, Yang, Wenge, Lin, Jianhua, and Huang, Fuqiang. Mon .  
"Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12".  Germany.  https://doi.org/10.1002/ange.201901739.

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@article{osti_1509751,

  title        = {Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12},

  author       = {Wang, Yingqi and Lü, Xujie and Zheng, Chong and Liu, Xiang and Chen, Zonghai and Yang, Wenge and Lin, Jianhua and Huang, Fuqiang},

  abstractNote = {Abstract Sulfide‐based superionic conductors with high ionic conductivity have been explored as candidates for solid‐state Li batteries. However, moisture hypersensitivity has made their manufacture complicated and costly and also impeded applications in batteries. Now, a sulfide‐based superionic conductor Li 4 Cu 8 Ge 3 S 12 with superior stability was developed based on the hard/soft acid–base theory. The compound is stable in both moist air and aqueous LiOH aqueous solution. The electrochemical stability window was up to 1.5 V. An ionic conductivity of 0.9×10 −4  S cm with low activation energy of 0.33 eV was achieved without any optimization. The material features a rigid Cu‐Ge‐S open framework that increases its stability. Meanwhile, the weak bonding between Li + and the framework promotes ionic conductivity. This work provides a structural configuration in which weak Li bonding in the rigid framework promotes an environment for highly conductive and stable solid‐state electrolytes.},

  doi          = {10.1002/ange.201901739},

  journal      = {Angewandte Chemie},

  number       = 23,

  volume       = 131,

  place        = {Germany},

  year         = {Mon Apr 29 00:00:00 EDT 2019},

  month        = {Mon Apr 29 00:00:00 EDT 2019}

}

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Title: Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li 4 Cu 8 Ge 3 S 12

Abstract

Citation Formats

Ionic conductivity of LISICON solid solutions, Li2+2xZn1−xGeO4 journal, October 1982

Crystal structure of a superionic conductor, Li7P3S11 journal, June 2007

A high conductivity oxide–sulfide composite lithium superionic conductor journal, January 2014

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries journal, December 2016

Li-rich antiperovskite superionic conductors based on cluster ions journal, October 2017

Materials Design Rules for Multivalent Ion Mobility in Intercalation Structures journal, August 2015

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On the Location of Li+ Cations in the Fast Li-Cation Conductor La0.5Li0.5TiO3 Perovskite journal, February 2000

Fluorine-Doped Antiperovskite Electrolyte for All-Solid-State Lithium-Ion Batteries journal, June 2016

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

Proton Conduction with Metal-Organic Frameworks journal, July 2013

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

Proton-conducting crystalline porous materials journal, January 2017

Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations journal, October 2015

High magnesium mobility in ternary spinel chalcogenides journal, November 2017

On the Location of Li+ Cations in the Fast Li-Cation Conductor La0.5Li0.5TiO3 Perovskite journal, February 2000

X-ray Crystal Structure Analysis of Sodium-Ion Conductivity in 94 Na 3 PS 4 ⋅6 Na 4 SiS 4 Glass-Ceramic Electrolytes journal, June 2014

Excellent Stability of a Lithium-Ion-Conducting Solid Electrolyte upon Reversible Li + /H + Exchange in Aqueous Solutions journal, October 2014

An Air-Stable Na 3 SbS 4 Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure journal, June 2016

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Hard and soft acids and bases, HSAB, part 1: Fundamental principles journal, September 1968

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Elucidating lithium-ion and proton dynamics in anti-perovskite solid electrolytes journal, January 2018

Fluorine-Doped Antiperovskite Electrolyte for All-Solid-State Lithium-Ion Batteries journal, June 2016

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

Excellent Stability of a Lithium-Ion-Conducting Solid Electrolyte upon Reversible Li + /H + Exchange in Aqueous Solutions journal, October 2014

Proton conduction in crystalline and porous covalent organic frameworks journal, April 2016

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries journal, December 2016

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

Li 3 BO 3 –Li 2 CO 3 : Rationally Designed Buffering Phase for Sulfide All-Solid-State Li-Ion Batteries journal, October 2018

A chemistry and material perspective on lithium redox flow batteries towards high-density electrical energy storage journal, January 2015

Antiperovskite Li 3 OCl Superionic Conductor Films for Solid-State Li-Ion Batteries journal, February 2016

A solid lithium superionic conductor Li 11 AlP 2 S 12 with a thio-LISICON analogous structure journal, January 2016

Na 3 PSe 4 : A Novel Chalcogenide Solid Electrolyte with High Ionic Conductivity journal, October 2015

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Structural and Electronic-State Changes of a Sulfide Solid Electrolyte during the Li Deinsertion–Insertion Processes journal, May 2017

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The Li-Ion Rechargeable Battery: A Perspective journal, January 2013

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Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction journal, December 2015

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Title: Chemistry Design Towards a Stable Sulfide‐Based Superionic Conductor Li ₄ Cu ₈ Ge ₃ S ₁₂

Ionic conductivity of LISICON solid solutions, Li2+2xZn1−xGeO4
journal, October 1982

Crystal structure of a superionic conductor, Li7P3S11
journal, June 2007

A high conductivity oxide–sulfide composite lithium superionic conductor
journal, January 2014

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016

Li-rich antiperovskite superionic conductors based on cluster ions
journal, October 2017

Materials Design Rules for Multivalent Ion Mobility in Intercalation Structures
journal, August 2015

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

On the Location of Li+ Cations in the Fast Li-Cation Conductor La0.5Li0.5TiO3 Perovskite
journal, February 2000

Fluorine-Doped Antiperovskite Electrolyte for All-Solid-State Lithium-Ion Batteries
journal, June 2016

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Proton Conduction with Metal-Organic Frameworks
journal, July 2013

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

Proton-conducting crystalline porous materials
journal, January 2017

Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations
journal, October 2015

High magnesium mobility in ternary spinel chalcogenides
journal, November 2017

On the Location of Li+ Cations in the Fast Li-Cation Conductor La0.5Li0.5TiO3 Perovskite
journal, February 2000

X-ray Crystal Structure Analysis of Sodium-Ion Conductivity in 94 Na ₃ PS ₄ ⋅6 Na ₄ SiS ₄ Glass-Ceramic Electrolytes
journal, June 2014

Excellent Stability of a Lithium-Ion-Conducting Solid Electrolyte upon Reversible Li ⁺ /H ⁺ Exchange in Aqueous Solutions
journal, October 2014

An Air-Stable Na ₃ SbS ₄ Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure
journal, June 2016

Air-stable, high-conduction solid electrolytes of arsenic-substituted Li ₄ SnS ₄
journal, January 2014

Hard and soft acids and bases, HSAB, part 1: Fundamental principles
journal, September 1968

Protonenleitung in Metall-organischen Gerüsten und verwandten modularen porösen Festkörpern
journal, January 2013

Elucidating lithium-ion and proton dynamics in anti-perovskite solid electrolytes
journal, January 2018

Fluorine-Doped Antiperovskite Electrolyte for All-Solid-State Lithium-Ion Batteries
journal, June 2016

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

Excellent Stability of a Lithium-Ion-Conducting Solid Electrolyte upon Reversible Li ⁺ /H ⁺ Exchange in Aqueous Solutions
journal, October 2014

Proton conduction in crystalline and porous covalent organic frameworks
journal, April 2016

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016

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

Li ₃ BO ₃ –Li ₂ CO ₃ : Rationally Designed Buffering Phase for Sulfide All-Solid-State Li-Ion Batteries
journal, October 2018

A chemistry and material perspective on lithium redox flow batteries towards high-density electrical energy storage
journal, January 2015

Antiperovskite Li ₃ OCl Superionic Conductor Films for Solid-State Li-Ion Batteries
journal, February 2016

A solid lithium superionic conductor Li ₁₁ AlP ₂ S ₁₂ with a thio-LISICON analogous structure
journal, January 2016

Na ₃ PSe ₄ : A Novel Chalcogenide Solid Electrolyte with High Ionic Conductivity
journal, October 2015

Electrochemical Stability of Li ₁₀ GeP ₂ S ₁₂ and Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolytes
journal, January 2016

Structural and Electronic-State Changes of a Sulfide Solid Electrolyte during the Li Deinsertion–Insertion Processes
journal, May 2017

An Air-Stable Na ₃ SbS ₄ Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure
journal, June 2016

The Li-Ion Rechargeable Battery: A Perspective
journal, January 2013

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

Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction
journal, December 2015

Lithium battery chemistries enabled by solid-state electrolytes
journal, February 2017

Proton Conduction in Metal-Organic Frameworks and Related Modularly Built Porous Solids
journal, January 2013

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