Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets

Chen, Yan; Rangasamy, Ezhiylmurugan; Liang, Chengdu; An, Ke

doi:10.1021/acs.chemmater.5b02521

Title: Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets

Abstract

Substitution of a native ion in the crystals with a foreign ion that differs in valence (aliovalent doping) has been widely attempted to upgrade solid-state ionic conductors for various charge carriers including O²⁻, H⁺, Li⁺, Na⁺, etc. The doping helps promote the high-conductive framework and dredge the tunnel for fast ion transport. The garnet-type Li₇La₃Zr₂O₁₂ (LLZO) is a fast Li⁺ solid conductor, which received much attention as an electrolyte candidate for all-solid-state lithium ion batteries, showing great potential to offer high energy density and minimize battery safety concerns to meet extensive applications in large energy storage systems such as those for electric vehicles and aerospace. In the Li-stuffed garnet framework of LLZO, the 3D pathway formed by the incompletely occupied tetrahedral sites bridged by a single octahedron enables the superior Li⁺ conductivity. For optimal performance, many aliovalent-doping efforts have been made throughout metal elements (Al³⁺, Ta⁵⁺) and metalloid elements (Ga³⁺, Te⁶⁺) in the periodic table with various valences to stabilize the high-conductive phase and increase the Li vacancy concentration.

Authors:

Chen, Yan ^[1]; Rangasamy, Ezhiylmurugan ^[1]; Liang, Chengdu ^[1]; An, Ke ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Thu Aug 06 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Laboratory (ORNL). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1213330

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Chemistry of Materials

Additional Journal Information:: Journal Volume: 27; Journal Issue: 16; Journal ID: ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Chen, Yan, Rangasamy, Ezhiylmurugan, Liang, Chengdu, and An, Ke. Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets.  United States: N. p., 2015. 
Web.  doi:10.1021/acs.chemmater.5b02521.

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                    Chen, Yan, Rangasamy, Ezhiylmurugan, Liang, Chengdu, & An, Ke. Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets.  United States.  https://doi.org/10.1021/acs.chemmater.5b02521

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                    Chen, Yan, Rangasamy, Ezhiylmurugan, Liang, Chengdu, and An, Ke. Thu .  
"Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets".  United States.  https://doi.org/10.1021/acs.chemmater.5b02521.  https://www.osti.gov/servlets/purl/1213330.

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@article{osti_1213330,

  title        = {Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets},

  author       = {Chen, Yan and Rangasamy, Ezhiylmurugan and Liang, Chengdu and An, Ke},

  abstractNote = {Substitution of a native ion in the crystals with a foreign ion that differs in valence (aliovalent doping) has been widely attempted to upgrade solid-state ionic conductors for various charge carriers including O²⁻, H⁺, Li⁺, Na⁺, etc. The doping helps promote the high-conductive framework and dredge the tunnel for fast ion transport. The garnet-type Li₇La₃Zr₂O₁₂ (LLZO) is a fast Li⁺ solid conductor, which received much attention as an electrolyte candidate for all-solid-state lithium ion batteries, showing great potential to offer high energy density and minimize battery safety concerns to meet extensive applications in large energy storage systems such as those for electric vehicles and aerospace. In the Li-stuffed garnet framework of LLZO, the 3D pathway formed by the incompletely occupied tetrahedral sites bridged by a single octahedron enables the superior Li⁺ conductivity. For optimal performance, many aliovalent-doping efforts have been made throughout metal elements (Al³⁺, Ta⁵⁺) and metalloid elements (Ga³⁺, Te⁶⁺) in the periodic table with various valences to stabilize the high-conductive phase and increase the Li vacancy concentration.},

  doi          = {10.1021/acs.chemmater.5b02521},

  journal      = {Chemistry of Materials},

  number       = 16,

  volume       = 27,

  place        = {United States},

  year         = {Thu Aug 06 00:00:00 EDT 2015},

  month        = {Thu Aug 06 00:00:00 EDT 2015}

}

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Abstract

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Microwave assisted reactive sintering for Al doped Li 7 La 3 Zr 2 O 12 lithium ion solid state electrolyte journal, December 2019

Lithium diffusion in L i 2 X ( X = O , S, and Se): Ab initio simulations and inelastic neutron scattering measurements journal, June 2019

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

Fast Lithium Ion Conduction in Lithium Phosphidoaluminates journal, January 2020

Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li7La3Zr2O12 Substituted with Iron text, January 2019

Lattice-Geometry Effects in Garnet Solid Electrolytes: A Lattice-Gas Monte Carlo Simulation Study preprint, January 2017

Intermediate temperature solid oxide fuel cells
journal, January 2008

Novel Chemically Stable Ba ₃ Ca _1.18 Nb _{1.82– x} Y _x O _9−δ Proton Conductor: Improved Proton Conductivity through Tailored Cation Ordering
journal, March 2014

Inorganic solid Li ion conductors: An overview
journal, June 2009

Ion transport in sodium ion conducting solid electrolytes
journal, October 2012

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

A preliminary investigation of fracture toughness of Li7La3Zr2O12 and its comparison to other solid Li-ionconductors
journal, April 2013

Characterization of the interface between LiCoO2 and Li7La3Zr2O12 in an all-solid-state rechargeable lithium battery
journal, January 2011

Compatibility of Li[sub 7]La[sub 3]Zr[sub 2]O[sub 12] Solid Electrolyte to All-Solid-State Battery Using Li Metal Anode
journal, January 2010

Lithium Distribution in Aluminum-Free Cubic Li ₇ La ₃ Zr ₂ O ₁₂
journal, August 2011

Crystal Chemistry and Stability of “Li₇La₃Zr₂O₁₂ ” Garnet: A Fast Lithium-Ion Conductor
journal, February 2011

High conductive yttrium doped Li7La3Zr2O12 cubic lithium garnet
journal, December 2011

Synthesis and high Li-ion conductivity of Ga-stabilized cubic Li7La3Zr2O12
journal, June 2012

Lithium metal electrode kinetics and ionic conductivity of the solid lithium ion conductors “Li7La3Zr2O12” and Li7−xLa3Zr2−xTaxO12 with garnet-type structure
journal, May 2012

Lithium ion transport properties of high conductive tellurium substituted Li7La3Zr2O12 cubic lithium garnets
journal, October 2013

The role of Al and Li concentration on the formation of cubic garnet solid electrolyte of nominal composition Li₇La₃Zr₂O₁₂
journal, January 2012

Synthesis and structure analysis of tetragonal Li₇La₃Zr₂O₁₂ with the garnet-related type structure
journal, August 2009

Mechanisms of Li $^{+}$ transport in garnet-type cubic Li $_{3 + x}$ La $_{3} M_{2}$ O $_{12}$ ( $M$ = Te, Nb, Zr)
journal, February 2012

First In Situ Lattice Strains Measurements Under Load at VULCAN
journal, October 2010

DFT Study of the Role of Al ³⁺ in the Fast Ion-Conductor Li _{7–3 x} Al ³⁺ _x La ₃ Zr ₂ O ₁₂ Garnet
journal, April 2014

High lithium ion conductivity of Li7La3Zr2O12 synthesized by solid state reaction
journal, May 2014

Structure and dynamics of the fast lithium ion conductor “Li7La3Zr2O12”
journal, January 2011

Concerted Migration Mechanism in the Li Ion Dynamics of Garnet-Type Li ₇ La ₃ Zr ₂ O ₁₂
journal, January 2013

Effects of Gallium Doping in Garnet-Type Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolytes
journal, April 2015

Garnet-type solid-state fast Li ion conductors for Li batteries: critical review
journal, January 2014

Ionic distribution and conductivity in lithium garnet Li7La3Zr2O12
journal, July 2012

Synthesis of garnet-type Li7−xLa3Zr2O12−1/2x and its stability in aqueous solutions
journal, February 2011

Effect of calcining and Al doping on structure and conductivity of Li 7 La 3 Zr 2 O 12
journal, November 2014

Low temperature synthesis of highly ion conductive Li7La3Zr2O12–Li3BO3 composites
journal, August 2013

Synthesis and Crystal Chemistry of the Fast Li-Ion Conductor Li ₇ La ₃ Zr ₂ O ₁₂ Doped with Fe
journal, July 2013

Tetragonal vs. cubic phase stability in Al – free Ta doped Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO)
journal, January 2014

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

Sur-/interfacial regulation in all-solid-state rechargeable Li-ion batteries based on inorganic solid-state electrolytes: advances and perspectives
journal, January 2019

Lithium ion micrometer diffusion in a garnet-type cubic Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO) studied using ⁷ Li NMR spectroscopy
journal, January 2017

Mechanistic understanding and strategies to design interfaces of solid electrolytes: insights gained from transmission electron microscopy
journal, May 2019

Electrochemical and mechanical stability of Li _x La _0.557 TiO _{3‐ δ} perovskite electrolyte at various voltages
journal, September 2018

Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li ₇ La ₃ Zr ₂ O ₁₂ Substituted with Iron
journal, January 2019

Tracing Phase Transformation and Lattice Evolution in a TRIP Sheet Steel under High-Temperature Annealing by Real-Time In Situ Neutron Diffraction
journal, September 2018

Lattice-geometry effects in garnet solid electrolytes: a lattice-gas Monte Carlo simulation study
journal, November 2017

Fast Lithium Ion Conduction in Lithium Phosphidoaluminates
journal, January 2020

An efficient multi-doping strategy to enhance Li-ion conductivity in the garnet-type solid electrolyte Li ₇ La ₃ Zr ₂ O ₁₂
journal, January 2019

Microwave assisted reactive sintering for Al doped Li ₇ La ₃ Zr ₂ O ₁₂ lithium ion solid state electrolyte
journal, December 2019

Lithium diffusion in $L i_{2} X$ ( $X = O$ , S, and Se): Ab initio simulations and inelastic neutron scattering measurements
journal, June 2019

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

Fast Lithium Ion Conduction in Lithium Phosphidoaluminates
journal, January 2020

Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li7La3Zr2O12 Substituted with Iron
text, January 2019

Lattice-Geometry Effects in Garnet Solid Electrolytes: A Lattice-Gas Monte Carlo Simulation Study
preprint, January 2017