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Elemental-sensitive Detection of the Chemistry in Batteries through Soft X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering
Published on: April 17, 2018
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Fingerprinting Mean Composition of Lithium Polysulfide Standard Solutions by Applying High-Energy Resolution
A Robba1,2, C Barchasz1, K Bučar3
1Univ. Grenoble Alpes, CEA, LITEN, DEHT, STB, 38000 Grenoble, France.
The Journal of Physical Chemistry Letters
|June 26, 2020
Summary
This study characterizes lithium polysulfides in lithium/sulfur batteries using X-ray scattering. The findings show a specific X-ray peak ratio reliably indicates polysulfide chain length, aiding battery analysis.
Area of Science:
- Materials Science
- Electrochemistry
- Analytical Chemistry
Background:
- Lithium/sulfur (Li/S) batteries offer high energy density but face challenges with sulfur dissolution.
- Understanding lithium polysulfide (Li₂Sₓ) intermediates is crucial for Li/S battery performance.
- Characterizing the mean polysulfide chain length is key to optimizing Li/S battery technology.
Purpose of the Study:
- To characterize lithium polysulfide (Li₂Sₓ) standard solutions using sulfur K-edge resonant inelastic X-ray scattering.
- To establish a reliable method for determining the mean polysulfide chain length in Li/S battery electrolytes.
- To validate the use of High-Energy Resolution Fluorescence Detected X-ray Absorption Spectroscopy (HERFD XAS) for operando analysis.
Main Methods:
- Sulfur K-edge resonant inelastic X-ray scattering (XRS) measurements.
- High-Energy Resolution Fluorescence Detected X-ray Absorption Spectroscopy (HERFD XAS).
- Analysis of spectral features, specifically the pre-edge absorption peak, to differentiate terminal and internal sulfur atoms.
Main Results:
- HERFD XAS enabled clear separation of pre-edge peaks (terminal sulfur) from main peaks (internal sulfur).
- The normalized area ratio of the pre-edge peak quantitatively correlates with polysulfide chain length.
- Experimental results align with theoretical predictions regarding polysulfide chain length determination.
Conclusions:
- The normalized pre-edge peak area serves as a reliable fingerprint for the mean lithium polysulfide chain length.
- Operando HERFD XAS is confirmed as a viable technique for differentiating polysulfide composition in Li/S cells.
- This method provides critical insights for advancing Li/S battery characterization and development.
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