Electrochemical Healing of Dendrites in Garnet-Based Solid Electrolytes

Anand Parejiya; Ruhul Amin; Rachid Essehli; David L. Wood; Ilias Belharouak

doi:10.1021/acsenergylett.0c01896

Electrochemical Healing of Dendrites in Garnet-Based Solid Electrolytes

Anand Parejiya, Ruhul Amin, Rachid Essehli, David L. Wood, Ilias Belharouak

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

36 Scopus citations

Abstract

Garnet oxides are a promising material family for solid-state batteries (SSBs). Dendrite formation in solid electrolytes critically limits the applicability of SSBs because of limiting Coulombic efficiency and power capability. Herein, the authors report operando electrochemical healing of dendrites in a garnet-based solid electrolyte (SE). Dendrites were deliberately formed at high operational current density (2 mA cm-2) beyond the critical current density (0.55 mA cm-2) of the used garnet SE. Electrochemical impedance spectroscopy and scanning electron microscopy were used to confirm dendrite growth in the SE. Dendrites were subsequently healed electrochemically via plating and stripping at 20 and 1 μA cm-2 current densities. Removal of dendrites was shown by an increase in bulk and interfacial resistance and a progressive increase in polarization during galvanostatic plating and stripping. High local current density at the dendrite tips was identified as the mechanism for preferentially removing dendrites electrochemically. The dendrite detection and healing methods discussed here are crucial for extending the life of SSBs.

Original language	English
Pages (from-to)	3368-3373
Number of pages	6
Journal	ACS Energy Letters
Volume	5
Issue number	11
DOIs	https://doi.org/10.1021/acsenergylett.0c01896
State	Published - Nov 13 2020

Funding

This research at the Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC05-00OR22725, was sponsored by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory, and the Office of Energy Efficiency and Renewable Energy Vehicle Technologies Office (Deputy Director: David Howell) Applied Battery Research Program (Program Manager: Peter Faguy). A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

Funders	Funder number
Office of Energy Efficiency and Renewable Energy Vehicle Technologies Office
U.S. Department of Energy	DE-AC05-00OR22725
Oak Ridge National Laboratory
UT-Battelle

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10.1021/acsenergylett.0c01896

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title = "Electrochemical Healing of Dendrites in Garnet-Based Solid Electrolytes",

abstract = "Garnet oxides are a promising material family for solid-state batteries (SSBs). Dendrite formation in solid electrolytes critically limits the applicability of SSBs because of limiting Coulombic efficiency and power capability. Herein, the authors report operando electrochemical healing of dendrites in a garnet-based solid electrolyte (SE). Dendrites were deliberately formed at high operational current density (2 mA cm-2) beyond the critical current density (0.55 mA cm-2) of the used garnet SE. Electrochemical impedance spectroscopy and scanning electron microscopy were used to confirm dendrite growth in the SE. Dendrites were subsequently healed electrochemically via plating and stripping at 20 and 1 μA cm-2 current densities. Removal of dendrites was shown by an increase in bulk and interfacial resistance and a progressive increase in polarization during galvanostatic plating and stripping. High local current density at the dendrite tips was identified as the mechanism for preferentially removing dendrites electrochemically. The dendrite detection and healing methods discussed here are crucial for extending the life of SSBs.",

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AU - Parejiya, Anand

AU - Amin, Ruhul

AU - Essehli, Rachid

AU - Wood, David L.

AU - Belharouak, Ilias

PY - 2020/11/13

Y1 - 2020/11/13

N2 - Garnet oxides are a promising material family for solid-state batteries (SSBs). Dendrite formation in solid electrolytes critically limits the applicability of SSBs because of limiting Coulombic efficiency and power capability. Herein, the authors report operando electrochemical healing of dendrites in a garnet-based solid electrolyte (SE). Dendrites were deliberately formed at high operational current density (2 mA cm-2) beyond the critical current density (0.55 mA cm-2) of the used garnet SE. Electrochemical impedance spectroscopy and scanning electron microscopy were used to confirm dendrite growth in the SE. Dendrites were subsequently healed electrochemically via plating and stripping at 20 and 1 μA cm-2 current densities. Removal of dendrites was shown by an increase in bulk and interfacial resistance and a progressive increase in polarization during galvanostatic plating and stripping. High local current density at the dendrite tips was identified as the mechanism for preferentially removing dendrites electrochemically. The dendrite detection and healing methods discussed here are crucial for extending the life of SSBs.

AB - Garnet oxides are a promising material family for solid-state batteries (SSBs). Dendrite formation in solid electrolytes critically limits the applicability of SSBs because of limiting Coulombic efficiency and power capability. Herein, the authors report operando electrochemical healing of dendrites in a garnet-based solid electrolyte (SE). Dendrites were deliberately formed at high operational current density (2 mA cm-2) beyond the critical current density (0.55 mA cm-2) of the used garnet SE. Electrochemical impedance spectroscopy and scanning electron microscopy were used to confirm dendrite growth in the SE. Dendrites were subsequently healed electrochemically via plating and stripping at 20 and 1 μA cm-2 current densities. Removal of dendrites was shown by an increase in bulk and interfacial resistance and a progressive increase in polarization during galvanostatic plating and stripping. High local current density at the dendrite tips was identified as the mechanism for preferentially removing dendrites electrochemically. The dendrite detection and healing methods discussed here are crucial for extending the life of SSBs.

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Electrochemical Healing of Dendrites in Garnet-Based Solid Electrolytes

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