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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.
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):
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308; 1605528
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
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
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; batteries; solid electrolyte interphase; operando
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1461861