Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes

María Abreu-Sepúlveda; Dominique E. Williams; Ashfia Huq; Chetan Dhital; Yunchao Li; M. Parans Paranthaman; Karim Zaghib; A. Manivannan

doi:10.1007/s11581-015-1556-2

Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes

María Abreu-Sepúlveda, Dominique E. Williams, Ashfia Huq, Chetan Dhital, Yunchao Li, M. Parans Paranthaman, Karim Zaghib, A. Manivannan

Nanomaterials Chemistry Group

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

Titanium, tantalum-substituted Li₇La₃Zr_2-xA_xO₁₂ (LLZO, A=Ta, Ti) garnets, and chromium-substituted La_(2/3)-xLi_3xTi_1-yCr_yO₃ (LLTO) perovskites were prepared by a conventional solid-state reaction and the Pechini processes. The desired crystal phases were obtained by varying the calcination temperature and time, as well as the substitution concentration. All samples indicated decomposition of the precursors when heated above 750 °C and formation of the desired phase after heat treatment at higher temperatures. Neutron diffraction data shows the formation of a predominant cubic phase in the case of Ta-LLZO, and monoclinic phase with minor impurity phases for Cr-LLTO. Ionic conductivity for Ti-LLZO (L i₇ L a₃ Z r_{1. 4} T i_{0. 6} O_{1 2}), Ta-LLZO (Li_6.03La₃Zr_1.533Ta_0.46O₁₂), and Cr-LLTO (La_(2/3)-xLi_3xTi_0.9Cr_0.1O₃) at room temperature were found to be 5.21×10⁻⁶, 1.01×10⁻⁶, and 1.2×10⁻⁴ S cm⁻¹, respectively. The activation energies of the compounds were determined from the Arrhenius plot and were 0.44 eV (Ti_0.6-LLZO), 0.54 eV (Ta_0.5-LLZO), and 0.20 eV (Cr_0.1-LLTO).

Original language	English
Pages (from-to)	317-325
Number of pages	9
Journal	Ionics
Volume	22
Issue number	3
DOIs	https://doi.org/10.1007/s11581-015-1556-2
State	Published - Sep 30 2015

Funding

This work was supported by the Vehicle Technology Program (EERE), Oak Ridge Institute for Science and Education (ORISE), and Mickey Leland Energy Fellowship (MLEF) programs. A portion of this research at ORNL?s Spallation Neutron Source was sponsored by the US Department of Energy, Office of Basic Energy Sciences Scientific User Facilities Division. Support (MPP and YL) for Neutron characterizations and impedance measurements was provided by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences, and Engineering Division.

Keywords

Garnet
Lithium-ion conduction
Perovskite
Solid electrolytes
Solid-state lithium-ion battery

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1007/s11581-015-1556-2

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@article{74cdad5d7bb3470091f717416999118f,

title = "Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes",

abstract = "Titanium, tantalum-substituted Li7La3Zr2-xAxO12 (LLZO, A=Ta, Ti) garnets, and chromium-substituted La(2/3)-xLi3xTi1-yCryO3 (LLTO) perovskites were prepared by a conventional solid-state reaction and the Pechini processes. The desired crystal phases were obtained by varying the calcination temperature and time, as well as the substitution concentration. All samples indicated decomposition of the precursors when heated above 750 °C and formation of the desired phase after heat treatment at higher temperatures. Neutron diffraction data shows the formation of a predominant cubic phase in the case of Ta-LLZO, and monoclinic phase with minor impurity phases for Cr-LLTO. Ionic conductivity for Ti-LLZO (L i7 L a3 Z r1. 4 T i0. 6 O1 2), Ta-LLZO (Li6.03La3Zr1.533Ta0.46O12), and Cr-LLTO (La(2/3)-xLi3xTi0.9Cr0.1O3) at room temperature were found to be 5.21×10−6, 1.01×10−6, and 1.2×10−4 S cm−1, respectively. The activation energies of the compounds were determined from the Arrhenius plot and were 0.44 eV (Ti0.6-LLZO), 0.54 eV (Ta0.5-LLZO), and 0.20 eV (Cr0.1-LLTO).",

keywords = "Garnet, Lithium-ion conduction, Perovskite, Solid electrolytes, Solid-state lithium-ion battery",

author = "Mar{\'i}a Abreu-Sep{\'u}lveda and Williams, {Dominique E.} and Ashfia Huq and Chetan Dhital and Yunchao Li and Paranthaman, {M. Parans} and Karim Zaghib and A. Manivannan",

note = "Publisher Copyright: {\textcopyright} Springer-Verlag Berlin Heidelberg (outside the USA) 2015.",

year = "2015",

month = sep,

day = "30",

doi = "10.1007/s11581-015-1556-2",

language = "English",

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TY - JOUR

T1 - Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes

AU - Abreu-Sepúlveda, María

AU - Williams, Dominique E.

AU - Huq, Ashfia

AU - Dhital, Chetan

AU - Li, Yunchao

AU - Paranthaman, M. Parans

AU - Zaghib, Karim

AU - Manivannan, A.

N1 - Publisher Copyright: © Springer-Verlag Berlin Heidelberg (outside the USA) 2015.

PY - 2015/9/30

Y1 - 2015/9/30

N2 - Titanium, tantalum-substituted Li7La3Zr2-xAxO12 (LLZO, A=Ta, Ti) garnets, and chromium-substituted La(2/3)-xLi3xTi1-yCryO3 (LLTO) perovskites were prepared by a conventional solid-state reaction and the Pechini processes. The desired crystal phases were obtained by varying the calcination temperature and time, as well as the substitution concentration. All samples indicated decomposition of the precursors when heated above 750 °C and formation of the desired phase after heat treatment at higher temperatures. Neutron diffraction data shows the formation of a predominant cubic phase in the case of Ta-LLZO, and monoclinic phase with minor impurity phases for Cr-LLTO. Ionic conductivity for Ti-LLZO (L i7 L a3 Z r1. 4 T i0. 6 O1 2), Ta-LLZO (Li6.03La3Zr1.533Ta0.46O12), and Cr-LLTO (La(2/3)-xLi3xTi0.9Cr0.1O3) at room temperature were found to be 5.21×10−6, 1.01×10−6, and 1.2×10−4 S cm−1, respectively. The activation energies of the compounds were determined from the Arrhenius plot and were 0.44 eV (Ti0.6-LLZO), 0.54 eV (Ta0.5-LLZO), and 0.20 eV (Cr0.1-LLTO).

AB - Titanium, tantalum-substituted Li7La3Zr2-xAxO12 (LLZO, A=Ta, Ti) garnets, and chromium-substituted La(2/3)-xLi3xTi1-yCryO3 (LLTO) perovskites were prepared by a conventional solid-state reaction and the Pechini processes. The desired crystal phases were obtained by varying the calcination temperature and time, as well as the substitution concentration. All samples indicated decomposition of the precursors when heated above 750 °C and formation of the desired phase after heat treatment at higher temperatures. Neutron diffraction data shows the formation of a predominant cubic phase in the case of Ta-LLZO, and monoclinic phase with minor impurity phases for Cr-LLTO. Ionic conductivity for Ti-LLZO (L i7 L a3 Z r1. 4 T i0. 6 O1 2), Ta-LLZO (Li6.03La3Zr1.533Ta0.46O12), and Cr-LLTO (La(2/3)-xLi3xTi0.9Cr0.1O3) at room temperature were found to be 5.21×10−6, 1.01×10−6, and 1.2×10−4 S cm−1, respectively. The activation energies of the compounds were determined from the Arrhenius plot and were 0.44 eV (Ti0.6-LLZO), 0.54 eV (Ta0.5-LLZO), and 0.20 eV (Cr0.1-LLTO).

KW - Garnet

KW - Lithium-ion conduction

KW - Perovskite

KW - Solid electrolytes

KW - Solid-state lithium-ion battery

UR - http://www.scopus.com/inward/record.url?scp=85028269969&partnerID=8YFLogxK

U2 - 10.1007/s11581-015-1556-2

DO - 10.1007/s11581-015-1556-2

M3 - Article

AN - SCOPUS:85028269969

SN - 0947-7047

VL - 22

SP - 317

EP - 325

JO - Ionics

JF - Ionics

IS - 3

ER -

Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes

Abstract

Funding

Keywords

UN SDGs

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