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

Journal Article · · ACS Energy Letters
 [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
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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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1475558
Journal Information:
ACS Energy Letters, Vol. 3, Issue 4; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 208 works
Citation information provided by
Web of Science

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Cited By (16)

Dopant‐Dependent Stability of Garnet Solid Electrolyte Interfaces with Lithium Metal journal January 2019
Composite Electrode Ink Formulation for All Solid-State Batteries journal January 2019
Sur-/interfacial regulation in all-solid-state rechargeable Li-ion batteries based on inorganic solid-state electrolytes: advances and perspectives journal January 2019
Probing into the origin of an electronic conductivity surge in a garnet solid-state electrolyte journal January 2019
Managing transport properties in composite electrodes/electrolytes for all-solid-state lithium-based batteries journal January 2019
Oriented porous LLZO 3D structures obtained by freeze casting for battery applications journal January 2019
Deconstructing electrode pore network to learn transport distortion journal December 2019
Ultra-fine surface solid-state electrolytes for long cycle life all-solid-state lithium–air batteries journal January 2018
An efficient multi-doping strategy to enhance Li-ion conductivity in the garnet-type solid electrolyte Li 7 La 3 Zr 2 O 12 journal January 2019
Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries journal January 2019
Fundamentals of inorganic solid-state electrolytes for batteries journal August 2019
Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure journal October 2019
Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport? journal November 2019
Elastic and Li-ion–percolating hybrid membrane stabilizes Li metal plating journal November 2018
Solid‐State Lithium Batteries: Bipolar Design, Fabrication, and Electrochemistry journal May 2019
7Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries. journalarticle January 2019

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