skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electro-chemo-mechanical evolution of sulfide solid electrolyte/Li metal interfaces: operando analysis and ALD interlayer effects

Abstract

Sulfide solid electrolytes (SE) show promise for high-performance solid-state batteries because of their high ionic conductivity and ease of processing. However, sulfide electrolytes have suffered from chemical and electrochemical instability against Li metal anodes. In this paper, we use a suite of in situ/operando microscopy and spectroscopy techniques to demonstrate that Al2O3 interlayers deposited using atomic layer deposition (ALD) delay degradation at the Li/LGPS interface by modifying the solid electrolyte interphase (SEI) chemistry and morphology. Optical and scanning electron microscopy are used to rationalize the electrochemical response of the system, which is attributed to a delayed onset of mechanical degradation at the interface when ALD interlayers are used. Operando X-ray photoelectron spectroscopy demonstrates that the dynamic evolution of SEI chemistry is impacted by the presence of the ALD interlayer. In situ Auger spectroscopy and operando optical microscopy provide visual evidence of spatial heterogeneity of Li plating, which is attributed to the chemo-mechanical degradation of the ALD interphase. The implications of these observations provide valuable insights toward the development of robust interlayers for solid-state batteries.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1];  [1];  [3];  [1]; ORCiD logo [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); San Diego State Univ., CA (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
OSTI Identifier:
1659923
Alternate Identifier(s):
OSTI ID: 1605610
Report Number(s):
NREL/JA-5K00-75158
Journal ID: ISSN 2050-7488; MainId:6951;UUID:d4e01ca9-7feb-e911-9c29-ac162d87dfe5;MainAdminID:13648
Grant/Contract Number:  
AC36-08GO28308; DGE 1256260
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 8; Journal Issue: 13; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; operando XPS; solid electrolyte

Citation Formats

Davis, Andrew L., Garcia-Mendez, Regina, Wood, Kevin N., Kazyak, Eric, Chen, Kuan-Hung, Teeter, Glenn, Sakamoto, Jeff, and Dasgupta, Neil P.. Electro-chemo-mechanical evolution of sulfide solid electrolyte/Li metal interfaces: operando analysis and ALD interlayer effects. United States: N. p., 2020. Web. https://doi.org/10.1039/c9ta11508k.
Davis, Andrew L., Garcia-Mendez, Regina, Wood, Kevin N., Kazyak, Eric, Chen, Kuan-Hung, Teeter, Glenn, Sakamoto, Jeff, & Dasgupta, Neil P.. Electro-chemo-mechanical evolution of sulfide solid electrolyte/Li metal interfaces: operando analysis and ALD interlayer effects. United States. https://doi.org/10.1039/c9ta11508k
Davis, Andrew L., Garcia-Mendez, Regina, Wood, Kevin N., Kazyak, Eric, Chen, Kuan-Hung, Teeter, Glenn, Sakamoto, Jeff, and Dasgupta, Neil P.. Fri . "Electro-chemo-mechanical evolution of sulfide solid electrolyte/Li metal interfaces: operando analysis and ALD interlayer effects". United States. https://doi.org/10.1039/c9ta11508k. https://www.osti.gov/servlets/purl/1659923.
@article{osti_1659923,
title = {Electro-chemo-mechanical evolution of sulfide solid electrolyte/Li metal interfaces: operando analysis and ALD interlayer effects},
author = {Davis, Andrew L. and Garcia-Mendez, Regina and Wood, Kevin N. and Kazyak, Eric and Chen, Kuan-Hung and Teeter, Glenn and Sakamoto, Jeff and Dasgupta, Neil P.},
abstractNote = {Sulfide solid electrolytes (SE) show promise for high-performance solid-state batteries because of their high ionic conductivity and ease of processing. However, sulfide electrolytes have suffered from chemical and electrochemical instability against Li metal anodes. In this paper, we use a suite of in situ/operando microscopy and spectroscopy techniques to demonstrate that Al2O3 interlayers deposited using atomic layer deposition (ALD) delay degradation at the Li/LGPS interface by modifying the solid electrolyte interphase (SEI) chemistry and morphology. Optical and scanning electron microscopy are used to rationalize the electrochemical response of the system, which is attributed to a delayed onset of mechanical degradation at the interface when ALD interlayers are used. Operando X-ray photoelectron spectroscopy demonstrates that the dynamic evolution of SEI chemistry is impacted by the presence of the ALD interlayer. In situ Auger spectroscopy and operando optical microscopy provide visual evidence of spatial heterogeneity of Li plating, which is attributed to the chemo-mechanical degradation of the ALD interphase. The implications of these observations provide valuable insights toward the development of robust interlayers for solid-state batteries.},
doi = {10.1039/c9ta11508k},
journal = {Journal of Materials Chemistry. A},
number = 13,
volume = 8,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share: