Electroanalytical Measurement of Interphase Formation at a Li Metal-Solid Electrolyte Interface

Andrew S. Westover; Robert L. Sacci; Nancy Dudney

doi:10.1021/acsenergylett.0c01840

Electroanalytical Measurement of Interphase Formation at a Li Metal-Solid Electrolyte Interface

Andrew S. Westover, Robert L. Sacci, Nancy Dudney

Energy Storage & Conversion

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

18 Scopus citations

Abstract

The interphase between Li metal and solid electrolytes dictates performance in Li metal batteries. For the solid electrolyte Lipon, we electroanalytically measure a capacity loss of 1.03 ± 0.16 μAh/cm2 when Lipon first contacts Li metal. Assuming this capacity is all lost to interphase formation, this corresponds to a maximum Li consumption of 5.0 ± 0.8 nm to form an interphase ∼4.7 nm thick. From dynamic electrochemical impedance spectroscopy (dEIS) during Li plating, we determine that nonlinear chaotic spectra demark this interphase formation and that this occurs immediately upon initiation of Li plating. dEIS also reveals interfacial resistance during both plating and stripping that decreases as the amount of plated Li increases.

Original language	English
Pages (from-to)	3860-3867
Number of pages	8
Journal	ACS Energy Letters
Volume	5
Issue number	12
DOIs	https://doi.org/10.1021/acsenergylett.0c01840
State	Published - Dec 11 2020

Funding

We acknowledge useful conversation and discussions with Paul Albertus and Scott Litzelman at ARPA-E as well as Frank Delnick and Andrew Kercher at ORNL. We would also like to acknowledge Jaymee Westover for help with the statistical analysis. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This work was initiated with funding from ARPA-E award No. DE-AR0000775 and completed with funding from the Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s US-German Cooperation on Energy Storage: Interfaces and Interphases In Rechargeable Li-metal based Batteries Program.

Funders	Funder number
US Department of Energy
U.S. Department of Energy
Advanced Research Projects Agency - Energy	DE-AR0000775
Office of Energy Efficiency and Renewable Energy

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abstract = "The interphase between Li metal and solid electrolytes dictates performance in Li metal batteries. For the solid electrolyte Lipon, we electroanalytically measure a capacity loss of 1.03 ± 0.16 μAh/cm2 when Lipon first contacts Li metal. Assuming this capacity is all lost to interphase formation, this corresponds to a maximum Li consumption of 5.0 ± 0.8 nm to form an interphase ∼4.7 nm thick. From dynamic electrochemical impedance spectroscopy (dEIS) during Li plating, we determine that nonlinear chaotic spectra demark this interphase formation and that this occurs immediately upon initiation of Li plating. dEIS also reveals interfacial resistance during both plating and stripping that decreases as the amount of plated Li increases.",

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N2 - The interphase between Li metal and solid electrolytes dictates performance in Li metal batteries. For the solid electrolyte Lipon, we electroanalytically measure a capacity loss of 1.03 ± 0.16 μAh/cm2 when Lipon first contacts Li metal. Assuming this capacity is all lost to interphase formation, this corresponds to a maximum Li consumption of 5.0 ± 0.8 nm to form an interphase ∼4.7 nm thick. From dynamic electrochemical impedance spectroscopy (dEIS) during Li plating, we determine that nonlinear chaotic spectra demark this interphase formation and that this occurs immediately upon initiation of Li plating. dEIS also reveals interfacial resistance during both plating and stripping that decreases as the amount of plated Li increases.

AB - The interphase between Li metal and solid electrolytes dictates performance in Li metal batteries. For the solid electrolyte Lipon, we electroanalytically measure a capacity loss of 1.03 ± 0.16 μAh/cm2 when Lipon first contacts Li metal. Assuming this capacity is all lost to interphase formation, this corresponds to a maximum Li consumption of 5.0 ± 0.8 nm to form an interphase ∼4.7 nm thick. From dynamic electrochemical impedance spectroscopy (dEIS) during Li plating, we determine that nonlinear chaotic spectra demark this interphase formation and that this occurs immediately upon initiation of Li plating. dEIS also reveals interfacial resistance during both plating and stripping that decreases as the amount of plated Li increases.

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Electroanalytical Measurement of Interphase Formation at a Li Metal-Solid Electrolyte Interface

Abstract

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