Dataset Information

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

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.

SUBMITTER: Wood KN

PROVIDER: S-EPMC6021442 | biostudies-literature | 2018 Jun

REPOSITORIES: biostudies-literature

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

Wood Kevin N KN Steirer K Xerxes KX Hafner Simon E SE Ban Chunmei C Santhanagopalan Shriram S Lee Se-Hee SH Teeter Glenn G

Nature communications 20180627 1

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 f ...[more]

PMID: 29950672

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Project description:Fluorinated electrolytes based on fluoroethylene carbonate (FEC) have been considered as promising alternative electrolytes for high-voltage and high-energy capacity lithium-ion batteries (LIBs). However, the compatibility of the fluorinated electrolytes with graphite negative electrodes is unclear. In this paper, we have systematically investigated, for the first time, the stability of fluorinated electrolytes with graphite negative electrodes, and the result shows that unlike the ethylene carbonate (EC)-based electrolyte, the FEC-based electrolyte (EC was totally replaced by FEC) is incapable of forming a protective and effective solid electrolyte interphase (SEI) that protects the electrolyte from runaway reduction on the graphite surface. The reason is that the lowest unoccupied molecular orbital energy levels are also lowered by the introduction of fluorine into the solvent, and the FEC solvent has poorer resistance against reduction, leading to instability on the graphite negative electrode. To tackle this problem, two lithium salts of lithium bis(oxalato)borate and lithium difluoro(oxalato)borate (LiDFOB) have been investigated as negative-electrode film-forming additives. Incorporation of only 0.5 wt % LiDFOB to a FEC-based electrolyte [1.0 M LiPF6 in 3:7 (FEC-ethyl methyl carbonate)] results in excellent cycling performance of the graphite negative electrode. This improved property originates from the generation of a thinner and better quality SEI film with little LiF by the sacrificial reduction of the LiDFOB additive on the graphite negative electrode surface. On the other hand, this additive can stabilize the electrolyte by scavenging HF. Meanwhile, the incorporated LiDFOB additive has positive influence on the interphase layer on the positive electrode surface and significantly decreases the amount of HF formation, finally leading to improved cycling stability and rate capability of LiNi0.5Mn1.5O4 electrodes at a high cutoff voltage of 5 V. The data demonstrate that the LiDFOB additive not only exhibits a superior compatibility with graphite but also improves the electrochemical properties of high-voltage spinel LiNi0.5Mn1.5O4 positive electrodes considerably, confirming its potential as a prospective, multifunctional additive for 5 V fluorinated electrolytes in high-energy capacity lithium-ion batteries (LIBs).

Dataset Information

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

Publications

Operando X-ray photoelectron spectroscopy of solid electrolyte interphase formation and evolution in Li<sub>2</sub>S-P<sub>2</sub>S<sub>5</sub> solid-state electrolytes.

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