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Title: Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li 2S-P 2S 5 solid-state electrolytes

Solid-state electrolytes such as Li 2S-P 2S 5 compounds are promising materials that could enable Li metal anodes. However, many solid-state electrolytes are unstable against metallic lithium, and little is known about the chemical evolution of these interfaces during cycling, hindering the rational design of these materials. In this work, operando X-ray photoelectron spectroscopy and real-time in situ Auger electron spectroscopy mapping are developed to probe the formation and evolution of the Li/Li 2S-P 2S 5 solid-electrolyte interphase during electrochemical cycling, and to measure individual overpotentials associated with specific interphase constituents. Results for the Li/Li 2S-P 2S 5 system reveal that electrochemically driving Li + to the surface leads to phase decomposition into Li 2S and Li 3P. Additionally, oxygen contamination within the Li 2S-P 2S 5 leads initially to Li 3PO 4 phase segregation, and subsequently to Li 2O formation. The spatially non-uniform distribution of these phases, coupled with differences in their ionic conductivities, have important implications for the overall properties and performance of the solid-electrolyte interphase.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ; ORCiD logo [1] ;  [1] ;  [3] ;  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Colorado School of Mines, Golden, CO (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-71811
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308; 1605528
Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; batteries; solid electrolyte interphase; operando
OSTI Identifier:
1456254
Alternate Identifier(s):
OSTI ID: 1461861

Wood, Kevin N., Steirer, K. Xerxes, Hafner, Simon E., Ban, Chunmei, Santhanagopalan, Shriram, Lee, Se-Hee, and Teeter, Glenn. Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li2S-P2S5 solid-state electrolytes. United States: N. p., Web. doi:10.1038/s41467-018-04762-z.
Wood, Kevin N., Steirer, K. Xerxes, Hafner, Simon E., Ban, Chunmei, Santhanagopalan, Shriram, Lee, Se-Hee, & Teeter, Glenn. Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li2S-P2S5 solid-state electrolytes. United States. doi:10.1038/s41467-018-04762-z.
Wood, Kevin N., Steirer, K. Xerxes, Hafner, Simon E., Ban, Chunmei, Santhanagopalan, Shriram, Lee, Se-Hee, and Teeter, Glenn. 2018. "Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li2S-P2S5 solid-state electrolytes". United States. doi:10.1038/s41467-018-04762-z.
@article{osti_1456254,
title = {Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li2S-P2S5 solid-state electrolytes},
author = {Wood, Kevin N. and Steirer, K. Xerxes and Hafner, Simon E. and Ban, Chunmei and Santhanagopalan, Shriram and Lee, Se-Hee and Teeter, Glenn},
abstractNote = {Solid-state electrolytes such as Li2S-P2S5 compounds are promising materials that could enable Li metal anodes. However, many solid-state electrolytes are unstable against metallic lithium, and little is known about the chemical evolution of these interfaces during cycling, hindering the rational design of these materials. In this work, operando X-ray photoelectron spectroscopy and real-time in situ Auger electron spectroscopy mapping are developed to probe the formation and evolution of the Li/Li2S-P2S5 solid-electrolyte interphase during electrochemical cycling, and to measure individual overpotentials associated with specific interphase constituents. Results for the Li/Li2S-P2S5 system reveal that electrochemically driving Li+ to the surface leads to phase decomposition into Li2S and Li3P. Additionally, oxygen contamination within the Li2S-P2S5 leads initially to Li3PO4 phase segregation, and subsequently to Li2O formation. The spatially non-uniform distribution of these phases, coupled with differences in their ionic conductivities, have important implications for the overall properties and performance of the solid-electrolyte interphase.},
doi = {10.1038/s41467-018-04762-z},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}

Works referenced in this record:

Progress and prospective of solid-state lithium batteries
journal, February 2013

Ceramic and polymeric solid electrolytes for lithium-ion batteries
journal, August 2010

New, Highly Ion-Conductive Crystals Precipitated from Li2S-P2S5 Glasses
journal, April 2005
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