Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material

Zhang, Yubin; Zheng, Zhangfeng; Liu, Xiaoming; Chi, Miaofang; Wang, Yan

doi:10.1149/2.0161904jes

Title: Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material

Abstract

All-solid-state Li-ion batteries (ASSLiB) attracted lots of attention mainly due to their higher safety compared with commercial Li-ion batteries. The research of solid electrolyte is critical for the development of ASSLiB, and among all the candidates of solid electrolyte materials, amorphous Lithium Lanthanum Titanate Oxide (LLTO) is promising because of its outstanding electrochemical stability up to 12V. However, the fundamental relationship among the ionic conductivity, microstructure, and mechanism of Li ion transport is still unrevealed. In this study, both amorphous LLTO thin film and LLTO powder were successfully prepared by sol-gel process. In order to determine the relationship between microstructure and ionic conductivity, various annealing time at 500°C were applied. This work shows that the ionic conductivity increases from 2.32 × 10^-8 S/cm to 9.01 × 10^-6 S/cm with the annealing time before LLTO starts to crystallize and decreases back to ~1.6 × 10^-9 S/cm after the formation of crystal phase. The absolute value of difference is close to 3 orders of magnitude. Furthermore, the morphology of the thin film changes accordingly, solvent evaporation, surface refinement and crystallization phases would occur sequentially, and this indicates that there is an optimal synthesis condition for the LLTO film. However, the changes ofmore »« less

Authors:

Zhang, Yubin ^[1]; Zheng, Zhangfeng ^[1]; Liu, Xiaoming ^[2]; Chi, Miaofang ^[2];

^[1]

Worcester Polytechnic Univ., Worcester, MA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Thu Feb 14 00:00:00 EST 2019

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1509535

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Volume: 166; Journal Issue: 4; Journal ID: ISSN 0013-4651

Publisher:: The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE

Citation Formats


                    Zhang, Yubin, Zheng, Zhangfeng, Liu, Xiaoming, Chi, Miaofang, and Wang, Yan. Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material.  United States: N. p., 2019. 
Web.  doi:10.1149/2.0161904jes.

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                    Zhang, Yubin, Zheng, Zhangfeng, Liu, Xiaoming, Chi, Miaofang, & Wang, Yan. Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material.  United States.  https://doi.org/10.1149/2.0161904jes

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                    Zhang, Yubin, Zheng, Zhangfeng, Liu, Xiaoming, Chi, Miaofang, and Wang, Yan. Thu .  
"Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material".  United States.  https://doi.org/10.1149/2.0161904jes.  https://www.osti.gov/servlets/purl/1509535.

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@article{osti_1509535,

  title        = {Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material},

  author       = {Zhang, Yubin and Zheng, Zhangfeng and Liu, Xiaoming and Chi, Miaofang and Wang, Yan},

  abstractNote = {All-solid-state Li-ion batteries (ASSLiB) attracted lots of attention mainly due to their higher safety compared with commercial Li-ion batteries. The research of solid electrolyte is critical for the development of ASSLiB, and among all the candidates of solid electrolyte materials, amorphous Lithium Lanthanum Titanate Oxide (LLTO) is promising because of its outstanding electrochemical stability up to 12V. However, the fundamental relationship among the ionic conductivity, microstructure, and mechanism of Li ion transport is still unrevealed. In this study, both amorphous LLTO thin film and LLTO powder were successfully prepared by sol-gel process. In order to determine the relationship between microstructure and ionic conductivity, various annealing time at 500°C were applied. This work shows that the ionic conductivity increases from 2.32 × 10-8 S/cm to 9.01 × 10-6 S/cm with the annealing time before LLTO starts to crystallize and decreases back to ~1.6 × 10-9 S/cm after the formation of crystal phase. The absolute value of difference is close to 3 orders of magnitude. Furthermore, the morphology of the thin film changes accordingly, solvent evaporation, surface refinement and crystallization phases would occur sequentially, and this indicates that there is an optimal synthesis condition for the LLTO film. However, the changes of structure, morphology and ionic conductivity does not affect activation energy. This will help researchers to find optimized synthesis condition of amorphous LLTO and potentially search for and design other solid electrolyte materials.},

  doi          = {10.1149/2.0161904jes},

  journal      = {Journal of the Electrochemical Society},

  number       = 4,

  volume       = 166,

  place        = {United States},

  year         = {Thu Feb 14 00:00:00 EST 2019},

  month        = {Thu Feb 14 00:00:00 EST 2019}

}

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Works referencing / citing this record:

A hybrid solid electrolyte Li _0.33 La _0.557 TiO ₃ /poly(acylonitrile) membrane infiltrated with a succinonitrile-based electrolyte for solid state lithium-ion batteries
journal, January 2020

Bi, Jiaying; Mu, Daobin; Wu, Borong
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Title: Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material

Abstract

Citation Formats

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Lithium Ion Transfer at the Interface between Lithium-Ion-Conductive Solid Crystalline Electrolyte and Polymer Electrolyte journal, January 2004

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

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Lithium-Ion Batteries: Solid Electrolyte: the Key for High-Voltage Lithium Batteries (Adv. Energy Mater. 4/2015)
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Structural, microstructural and transport properties study of lanthanum lithium titanium perovskite thin films grown by Pulsed Laser Deposition
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