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

Fengyu Shen; Marm B. Dixit; Xianghui Xiao; Kelsey B. Hatzell

doi:10.1021/acsenergylett.8b00249

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

Fengyu Shen, Marm B. Dixit, Xianghui Xiao, Kelsey B. Hatzell

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

290 Scopus citations

Abstract

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 processing-structure relationships for practical design of solid electrolytes, the present study tracks structural transformations in solid electrolytes processed at three different temperatures (1050, 1100, and 1150 °C) using synchrotron X-ray tomography. A subvolume 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. Solid electrolytes with interconnected pores short circuit at lower critical current densities than samples with less connected pores.

Original language	English
Pages (from-to)	1056-1061
Number of pages	6
Journal	ACS Energy Letters
Volume	3
Issue number	4
DOIs	https://doi.org/10.1021/acsenergylett.8b00249
State	Published - Apr 13 2018
Externally published	Yes

Funding

This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Experiments were conducted on the synchrotron beamline 2-BM. K.B.H and M.D. were supported by the National Science Foundation under Grant No. 1727863. F.S. acknowledges support from Vanderbilt School of Engineering Start-Up Grants. The authors acknowledge the Vanderbilt Institute of Nanoscience and Engineering (VINSE) for access to their shared characterization facilities.

Funders	Funder number
DOE Office of Science
Vanderbilt School of Engineering
National Science Foundation	1727863
U.S. Department of Energy
Office of Science
Argonne National Laboratory

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title = "Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography",

abstract = "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 processing-structure relationships for practical design of solid electrolytes, the present study tracks structural transformations in solid electrolytes processed at three different temperatures (1050, 1100, and 1150 °C) using synchrotron X-ray tomography. A subvolume 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. Solid electrolytes with interconnected pores short circuit at lower critical current densities than samples with less connected pores.",

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AU - Shen, Fengyu

AU - Dixit, Marm B.

AU - Xiao, Xianghui

AU - Hatzell, Kelsey B.

PY - 2018/4/13

Y1 - 2018/4/13

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AB - 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 processing-structure relationships for practical design of solid electrolytes, the present study tracks structural transformations in solid electrolytes processed at three different temperatures (1050, 1100, and 1150 °C) using synchrotron X-ray tomography. A subvolume 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. Solid electrolytes with interconnected pores short circuit at lower critical current densities than samples with less connected pores.

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

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