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Title: Electrochemical Stability of Li10GeP2S12 and Li7La3Zr2O12 Solid Electrolytes

Abstract

The electrochemical stability window of solid electrolyte is overestimated by the conventional experimental method using a Li/electrolyte/inert metal semiblocking electrode because of the limited contact area between solid electrolyte and inert metal. Since the battery is cycled in the overestimated stability window, the decomposition of the solid electrolyte at the interfaces occurs but has been ignored as a cause for high interfacial resistances in previous studies, limiting the performance improvement of the bulk-type solid-state battery despite the decades of research efforts. Thus, there is an urgent need to identify the intrinsic stability window of the solid electrolyte. The thermodynamic electrochemical stability window of solid electrolytes is calculated using first principles computation methods, and an experimental method is developed to measure the intrinsic electrochemical stability window of solid electrolytes using a Li/electrolyte/electrolyte-carbon cell. The most promising solid electrolytes, Li10GeP2S12 and cubic Li-garnet Li7La3Zr2O12, are chosen as the model materials for sulfide and oxide solid electrolytes, respectively. The results provide valuable insights to address the most challenging problems of the interfacial stability and resistance in high-performance solid-state batteries.

Authors:
 [1];  [2];  [2];  [2];  [1]
  1. Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
  2. Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); US Army Research Office (ARO)
OSTI Identifier:
1433676
Alternate Identifier(s):
OSTI ID: 1433674
Grant/Contract Number:  
EE0006860; 1235719; TG-DMR130142; W911NF1510187
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 8; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; all-solid-state batteries; electrochemical stability windows; first-principles computation; interfaces; solid electrolytes

Citation Formats

Han, Fudong, Zhu, Yizhou, He, Xingfeng, Mo, Yifei, and Wang, Chunsheng. Electrochemical Stability of Li10GeP2S12 and Li7La3Zr2O12 Solid Electrolytes. United States: N. p., 2016. Web. doi:10.1002/aenm.201501590.
Han, Fudong, Zhu, Yizhou, He, Xingfeng, Mo, Yifei, & Wang, Chunsheng. Electrochemical Stability of Li10GeP2S12 and Li7La3Zr2O12 Solid Electrolytes. United States. doi:10.1002/aenm.201501590.
Han, Fudong, Zhu, Yizhou, He, Xingfeng, Mo, Yifei, and Wang, Chunsheng. Thu . "Electrochemical Stability of Li10GeP2S12 and Li7La3Zr2O12 Solid Electrolytes". United States. doi:10.1002/aenm.201501590. https://www.osti.gov/servlets/purl/1433676.
@article{osti_1433676,
title = {Electrochemical Stability of Li10GeP2S12 and Li7La3Zr2O12 Solid Electrolytes},
author = {Han, Fudong and Zhu, Yizhou and He, Xingfeng and Mo, Yifei and Wang, Chunsheng},
abstractNote = {The electrochemical stability window of solid electrolyte is overestimated by the conventional experimental method using a Li/electrolyte/inert metal semiblocking electrode because of the limited contact area between solid electrolyte and inert metal. Since the battery is cycled in the overestimated stability window, the decomposition of the solid electrolyte at the interfaces occurs but has been ignored as a cause for high interfacial resistances in previous studies, limiting the performance improvement of the bulk-type solid-state battery despite the decades of research efforts. Thus, there is an urgent need to identify the intrinsic stability window of the solid electrolyte. The thermodynamic electrochemical stability window of solid electrolytes is calculated using first principles computation methods, and an experimental method is developed to measure the intrinsic electrochemical stability window of solid electrolytes using a Li/electrolyte/electrolyte-carbon cell. The most promising solid electrolytes, Li10GeP2S12 and cubic Li-garnet Li7La3Zr2O12, are chosen as the model materials for sulfide and oxide solid electrolytes, respectively. The results provide valuable insights to address the most challenging problems of the interfacial stability and resistance in high-performance solid-state batteries.},
doi = {10.1002/aenm.201501590},
journal = {Advanced Energy Materials},
number = 8,
volume = 6,
place = {United States},
year = {2016},
month = {1}
}

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    Oxysulfide LiAlSO: A Lithium Superionic Conductor from First Principles
    journal, May 2017


    Dense freeze-cast Li 7 La 3 Zr 2 O 12 solid electrolytes with oriented open porosity and contiguous ceramic scaffold
    journal, August 2018

    • Buannic, Lucienne; Naviroj, Maninpat; Miller, Sarah M.
    • Journal of the American Ceramic Society, Vol. 102, Issue 3
    • DOI: 10.1111/jace.15938

    An Interdisciplinary View of Interfaces: Perspectives Regarding Emergent Phase Formation
    journal, October 2017

    • Brinkman, Kyle S.
    • Journal of Electrochemical Energy Conversion and Storage, Vol. 15, Issue 1
    • DOI: 10.1115/1.4037583

    Highly efficient electrochemical reforming of CH 4 /CO 2 in a solid oxide electrolyser
    journal, March 2018


    Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery
    journal, December 2018


    Communication—Li/Li 7 La 3 Zr 2 O 12 Interfacial Modification by Constructing a Layer of Cu-Li Alloy
    journal, January 2019

    • Xiang, Xing; Cao, Shiyu; Chen, Fei
    • Journal of The Electrochemical Society, Vol. 166, Issue 13
    • DOI: 10.1149/2.0651913jes