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Title: Enhanced lithium ion transport in garnet-type solid state electrolytes

Abstract

Al-substituted Li7La3Zr2O12 samples processed under argon show enhanced Li-ion transport and interfacial properties in symmetrical cells with lithium electrodes, compared to those prepared in air. In particular, the samples prepared under argon have higher ionic conductivities and lower interfacial impedances in symmetrical lithium cells, and show better DC cycling characteristics. The electronic conductivities are also somewhat higher. Pellets subjected to thermal treatment under the two types of atmospheres have different colors but exhibit similar microstructures. X-ray diffraction experiments suggest that there are slight structural differences between the two types of samples, but few dissimilarities were observed in elemental composition, distribution of ions, oxidation states, or bond lengths using laser-induced breakdown spectroscopy (LIBS), x-ray photoelectron spectroscopy (XPS), and extended x-ray absorption fine structure spectroscopy (EXAFS) to analyze the materials. Additionally, there was no evidence that La or Zr were reduced during the processing under Ar. Possible explanations for the improved electrochemical properties of the sample prepared under Ar compared to the one prepared in air include differences in grain boundary chemistries and conductivities and/or a small concentration of oxygen vacancies in the former.

Authors:
 [1];  [2];  [3];  [3];  [4];  [3];  [4]; ORCiD logo [3]
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  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); The Peac Inst. of Multiscale Sciences, Chengdu (China)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1532252
Grant/Contract Number:  
AC02-05CH11231; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Electroceramics
Additional Journal Information:
Journal Volume: 38; Journal Issue: 2-4; Journal ID: ISSN 1385-3449
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; All solid state batteries; Solid electrolytes; Li7La3Zr2O12; Garnet

Citation Formats

Cheng, Lei, Hou, Huaming, Lux, Simon, Kostecki, Robert, Davis, Ryan, Zorba, Vassilia, Mehta, Apurva, and Doeff, Marca. Enhanced lithium ion transport in garnet-type solid state electrolytes. United States: N. p., 2017. Web. doi:10.1007/s10832-017-0080-3.
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Cheng, Lei, Hou, Huaming, Lux, Simon, Kostecki, Robert, Davis, Ryan, Zorba, Vassilia, Mehta, Apurva, & Doeff, Marca. Enhanced lithium ion transport in garnet-type solid state electrolytes. United States. https://doi.org/10.1007/s10832-017-0080-3
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Cheng, Lei, Hou, Huaming, Lux, Simon, Kostecki, Robert, Davis, Ryan, Zorba, Vassilia, Mehta, Apurva, and Doeff, Marca. Wed . "Enhanced lithium ion transport in garnet-type solid state electrolytes". United States. https://doi.org/10.1007/s10832-017-0080-3. https://www.osti.gov/servlets/purl/1532252.
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@article{osti_1532252,
title = {Enhanced lithium ion transport in garnet-type solid state electrolytes},
author = {Cheng, Lei and Hou, Huaming and Lux, Simon and Kostecki, Robert and Davis, Ryan and Zorba, Vassilia and Mehta, Apurva and Doeff, Marca},
abstractNote = {Al-substituted Li7La3Zr2O12 samples processed under argon show enhanced Li-ion transport and interfacial properties in symmetrical cells with lithium electrodes, compared to those prepared in air. In particular, the samples prepared under argon have higher ionic conductivities and lower interfacial impedances in symmetrical lithium cells, and show better DC cycling characteristics. The electronic conductivities are also somewhat higher. Pellets subjected to thermal treatment under the two types of atmospheres have different colors but exhibit similar microstructures. X-ray diffraction experiments suggest that there are slight structural differences between the two types of samples, but few dissimilarities were observed in elemental composition, distribution of ions, oxidation states, or bond lengths using laser-induced breakdown spectroscopy (LIBS), x-ray photoelectron spectroscopy (XPS), and extended x-ray absorption fine structure spectroscopy (EXAFS) to analyze the materials. Additionally, there was no evidence that La or Zr were reduced during the processing under Ar. Possible explanations for the improved electrochemical properties of the sample prepared under Ar compared to the one prepared in air include differences in grain boundary chemistries and conductivities and/or a small concentration of oxygen vacancies in the former.},
doi = {10.1007/s10832-017-0080-3},
journal = {Journal of Electroceramics},
number = 2-4,
volume = 38,
place = {United States},
year = {2017},
month = {3}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1007/s10832-017-0080-3
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Citation Metrics:
Cited by: 12 works
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Figures / Tables:

Table 1 Table 1: Properties of LLZO pellets.
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Works referenced in this record:

Structural and Electrochemical Consequences of Al and Ga Cosubstitution in Li 7 La 3 Zr 2 O 12 Solid Electrolytes
journal, March 2016

  • Rettenwander, Daniel; Redhammer, Günther; Preishuber-Pflügl, Florian
  • Chemistry of Materials, Vol. 28, Issue 7
  • DOI: 10.1021/acs.chemmater.6b00579

A shortcut to garnet-type fast Li-ion conductors for all-solid state batteries
journal, January 2015

  • Afyon, Semih; Krumeich, Frank; Rupp, Jennifer L. M.
  • Journal of Materials Chemistry A, Vol. 3, Issue 36
  • DOI: 10.1039/c5ta03239c

Interface-Engineered All-Solid-State Li-Ion Batteries Based on Garnet-Type Fast Li + Conductors
journal, July 2016

  • van den Broek, Jan; Afyon, Semih; Rupp, Jennifer L. M.
  • Advanced Energy Materials, Vol. 6, Issue 19
  • DOI: 10.1002/aenm.201600736

Structure and Stoichiometry in Supervalent Doped Li 7 La 3 Zr 2 O 12
journal, May 2015

Electrochemical Methods for Determining Kinetic Properties of Solids
journal, August 1978

Highly Conductive Li Garnets by a Multielement Doping Strategy
journal, March 2015

Effects of Li source on microstructure and ionic conductivity of Al-contained Li6.75La3Zr1.75Ta0.25O12 ceramics
journal, February 2015

Recent Advances in Inorganic Solid Electrolytes for Lithium Batteries
journal, June 2014

Low temperature stabilization of cubic (Li7−xAlx/3)La3Zr2O12: role of aluminum during formation
journal, January 2013

  • Hubaud, Aude A.; Schroeder, David J.; Key, Baris
  • Journal of Materials Chemistry A, Vol. 1, Issue 31
  • DOI: 10.1039/c3ta11338h

Li 7 La 3 Zr 2 O 12 Interface Modification for Li Dendrite Prevention
journal, April 2016

  • Tsai, Chih-Long; Roddatis, Vladimir; Chandran, C. Vinod
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 16
  • DOI: 10.1021/acsami.6b00831

Cubic phases of garnet-type Li7La3Zr2O12: the role of hydration
journal, January 2013

  • Larraz, G.; Orera, A.; Sanjuán, M. L.
  • Journal of Materials Chemistry A, Vol. 1, Issue 37
  • DOI: 10.1039/c3ta11996c

Interrelationships among Grain Size, Surface Composition, Air Stability, and Interfacial Resistance of Al-Substituted Li 7 La 3 Zr 2 O 12 Solid Electrolytes
journal, August 2015

  • Cheng, Lei; Wu, Cheng Hao; Jarry, Angelique
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 32
  • DOI: 10.1021/acsami.5b02528

Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density
journal, January 2016

Rechargeable alkali-ion cathode-flow battery
journal, January 2011

  • Lu, Yuhao; Goodenough, John B.
  • Journal of Materials Chemistry, Vol. 21, Issue 27
  • DOI: 10.1039/c0jm04222f

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

  • Rettenwander, Daniel; Geiger, Charles A.; Amthauer, Georg
  • Inorganic Chemistry, Vol. 52, Issue 14
  • DOI: 10.1021/ic400589u

A Synthesis and Crystal Chemical Study of the Fast Ion Conductor Li 7–3 x Ga x La 3 Zr 2 O 12 with x = 0.08 to 0.84
journal, May 2014

  • Rettenwander, Daniel; Geiger, Charles A.; Tribus, Martina
  • Inorganic Chemistry, Vol. 53, Issue 12
  • DOI: 10.1021/ic500803h

Alternative Approach to Increasing Li Mobility in Li-La-Nb/Ta Garnet Electrolytes
journal, October 2010

  • Nyman, May; Alam, Todd M.; McIntyre, Sarah K.
  • Chemistry of Materials, Vol. 22, Issue 19
  • DOI: 10.1021/cm101438x

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

  • Thompson, Travis; Wolfenstine, Jeff; Allen, Jan L.
  • J. Mater. Chem. A, Vol. 2, Issue 33
  • DOI: 10.1039/c4ta02099e

Resolving the Grain Boundary and Lattice Impedance of Hot-Pressed Li 7 La 3 Zr 2 O 12 Garnet Electrolytes
journal, July 2013

  • Tenhaeff, Wyatt E.; Rangasamy, Ezhiyl; Wang, Yangyang
  • ChemElectroChem, Vol. 1, Issue 2
  • DOI: 10.1002/celc.201300022

Flame made nanoparticles permit processing of dense, flexible, Li + conducting ceramic electrolyte thin films of cubic-Li 7 La 3 Zr 2 O 12 (c-LLZO)
journal, January 2016

  • Yi, Eongyu; Wang, Weimin; Kieffer, John
  • Journal of Materials Chemistry A, Vol. 4, Issue 33
  • DOI: 10.1039/c6ta04492a

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

  • Thangadurai, Venkataraman; Narayanan, Sumaletha; Pinzaru, Dana
  • Chemical Society Reviews, Vol. 43, Issue 13
  • DOI: 10.1039/c4cs00020j

The origin of high electrolyte–electrode interfacial resistances in lithium cells containing garnet type solid electrolytes
journal, January 2014

  • Cheng, Lei; Crumlin, Ethan J.; Chen, Wei
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 34
  • DOI: 10.1039/c4cp02921f

Synthesis and Raman micro-spectroscopy investigation of Li7La3Zr2O12
journal, January 2013

Effect of Al2O3 on the sintering of garnet-type Li6.5La3Zr1.5Ta0.5O12
journal, October 2016

Densification and ionic-conduction improvement of lithium garnet solid electrolytes by flowing oxygen sintering
journal, February 2014

Electrochemical properties of Li7La3Zr2O12 solid electrolyte prepared in argon atmosphere
journal, February 2012

Chemical stability of cubic Li7La3Zr2O12 with molten lithium at elevated temperature
journal, April 2013

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

Thin-film lithium and lithium-ion batteries
journal, November 2000

Al-doped Li7La3Zr2O12 synthesized by a polymerized complex method
journal, October 2011

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

  • Geiger, Charles A.; Alekseev, Evgeny; Lazic, Biljana
  • Inorganic Chemistry, Vol. 50, Issue 3, p. 1089-1097
  • DOI: 10.1021/ic101914e

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

  • Thompson, Travis; Wolfenstine, Jeff; Allen, Jan L.
  • J. Mater. Chem. A, Vol. 2, Issue 33
  • DOI: 10.1039/C4TA02099E

A shortcut to garnet-type fast Li-ion conductors for all-solid state batteries
journal, January 2015

  • Afyon, Semih; Krumeich, Frank; Rupp, Jennifer L. M.
  • Journal of Materials Chemistry A, Vol. 3, Issue 36
  • DOI: 10.1039/C5TA03239C

The origin of high electrolyte–electrode interfacial resistances in lithium cells containing garnet type solid electrolytes
journal, January 2014

  • Cheng, Lei; Crumlin, Ethan J.; Chen, Wei
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 34
  • DOI: 10.1039/C4CP02921F

Flame made nanoparticles permit processing of dense, flexible, Li + conducting ceramic electrolyte thin films of cubic-Li 7 La 3 Zr 2 O 12 (c-LLZO)
journal, January 2016

  • Yi, Eongyu; Wang, Weimin; Kieffer, John
  • Journal of Materials Chemistry A, Vol. 4, Issue 33
  • DOI: 10.1039/C6TA04492A

Fast microwave-assisted synthesis of Li-stuffed garnets and insights into Li diffusion from muon spin spectroscopy
journal, January 2016

  • Amores, Marco; Ashton, Thomas E.; Baker, Peter J.
  • Journal of Materials Chemistry A, Vol. 4, Issue 5
  • DOI: 10.1039/C5TA08107F
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    Works referencing / citing this record:

    Effect of Al-Mo codoping on the structure and ionic conductivity of sol-gel derived Li7La3Zr2O12 ceramics
    journal, March 2018

    Local Li-ion conductivity changes within Al stabilized Li 7 La 3 Zr 2 O 12 and their relationship to three-dimensional variations of the bulk composition
    journal, January 2019

    • Smetaczek, Stefan; Wachter-Welzl, Andreas; Wagner, Reinhard
    • Journal of Materials Chemistry A, Vol. 7, Issue 12
    • DOI: 10.1039/c9ta00356h

    Lithium Dissolution/Deposition Behavior of Al-Doped Li 7 La 3 Zr 2 O 12 Ceramics with Different Grain Sizes
    journal, January 2019

    • Matsuki, Yuma; Noi, Kousuke; Deguchi, Minako
    • Journal of The Electrochemical Society, Vol. 166, Issue 3
    • DOI: 10.1149/2.0661903jes
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      Figures / Tables found in this record:

      Table 1 (p. 22)table
      Figure 1 (p. 24)figure
      Figure 2 (p. 25)figure
      Figure 3 (p. 26)figure
      Figure 4 (p. 27)figure
      Figure 5 (p. 28)figure
      Figure 6 (p. 29)figure
      Figure 7 (p. 30)figure
      Figure 8 (p. 31)figure
      Figure 9 (p. 32)figure
      Figure 10 (p. 33)figure
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