Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li2S-P2S5 solid-state electrolytes

Kevin N. Wood (), K. Xerxes Steirer, Simon E. Hafner, Chunmei Ban, Shriram Santhanagopalan, Se-Hee Lee and Glenn Teeter ()
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Kevin N. Wood: National Renewable Energy Laboratory
K. Xerxes Steirer: Colorado School of Mines
Simon E. Hafner: University of Colorado
Chunmei Ban: National Renewable Energy Laboratory
Shriram Santhanagopalan: National Renewable Energy Laboratory
Se-Hee Lee: University of Colorado
Glenn Teeter: National Renewable Energy Laboratory

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract 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.

Date: 2018
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DOI: 10.1038/s41467-018-04762-z

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