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Title: Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography

Abstract

Li 7La 3Zr 2O 12 (LLZO) is a garnet type material that demonstrates promising characteristics for all solid-state battery applications due to its high Li-ion conductivity and its compatibility with Li metal. The primary limitation of LLZO is the propensity for short-circuiting at low current densities. Microstructure features such as grain boundaries, pore character, and density all contribute to this shorting phenomenon. Toward the goal of understanding structure-processing relationships for practical design of solid electrolytes, the present study tracks structural transformations in solid electrolytes processed at three different temperatures (1000, 1050 and 1150 °C) using synchrotron x-ray tomography. A sub volume of 300 μm 3 captures the heterogeneity of the solid electrolyte microstructure while minimizing the computational intensity associated with 3D reconstructions. While the porosity decreases with increasing temperature, the underlying connectivity of the pore region increases. In conclusion, solid electrolytes with interconnected pores short circuit at lower critical current densities than samples with less connected pores.

Authors:
 [1];  [2];  [3]; ORCiD logo [4]
  1. Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Dept. of Material Science; Vanderbilt Univ., Nashville, TN (United States). Dept. of Mechanical Engineering
  2. Vanderbilt Univ., Nashville, TN (United States). Dept. of Mechanical Engineering
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division
  4. Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Dept. of Material Science; Vanderbilt Univ., Nashville, TN (United States). Dept. of Mechanical Engineering; Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1475558
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Shen, Fengyu, Dixit, Marm B., Xiao, Xianghui, and Hatzell, Kelsey B. Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00249.
Shen, Fengyu, Dixit, Marm B., Xiao, Xianghui, & Hatzell, Kelsey B. Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography. United States. doi:10.1021/acsenergylett.8b00249.
Shen, Fengyu, Dixit, Marm B., Xiao, Xianghui, and Hatzell, Kelsey B. Fri . "Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography". United States. doi:10.1021/acsenergylett.8b00249. https://www.osti.gov/servlets/purl/1475558.
@article{osti_1475558,
title = {Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography},
author = {Shen, Fengyu and Dixit, Marm B. and Xiao, Xianghui and Hatzell, Kelsey B.},
abstractNote = {Li7La3Zr2O12 (LLZO) is a garnet type material that demonstrates promising characteristics for all solid-state battery applications due to its high Li-ion conductivity and its compatibility with Li metal. The primary limitation of LLZO is the propensity for short-circuiting at low current densities. Microstructure features such as grain boundaries, pore character, and density all contribute to this shorting phenomenon. Toward the goal of understanding structure-processing relationships for practical design of solid electrolytes, the present study tracks structural transformations in solid electrolytes processed at three different temperatures (1000, 1050 and 1150 °C) using synchrotron x-ray tomography. A sub volume of 300 μm3 captures the heterogeneity of the solid electrolyte microstructure while minimizing the computational intensity associated with 3D reconstructions. While the porosity decreases with increasing temperature, the underlying connectivity of the pore region increases. In conclusion, solid electrolytes with interconnected pores short circuit at lower critical current densities than samples with less connected pores.},
doi = {10.1021/acsenergylett.8b00249},
journal = {ACS Energy Letters},
number = 4,
volume = 3,
place = {United States},
year = {2018},
month = {3}
}

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Cited by: 19 works
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Works referencing / citing this record:

Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries
journal, January 2019

  • Zaman, Wahid; Hortance, Nicholas; Dixit, Marm B.
  • Journal of Materials Chemistry A, Vol. 7, Issue 41
  • DOI: 10.1039/c9ta05118j