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Fingerprinting mean composition of lithium polysulfide standard solutions by applying high energy resolution fluorescence detected X-ray Absorption Spectroscopy

J. Phys. Chem. Lett.

Mis à jour le 27 juillet 2020
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A. Robba, C. Barchasz, K. Bucard, M. Petricd, M. Žitnikd, K. Kvashninae, G. Vaughan, R. Bouchet, F. Alloin, M. Kavcic

Annotation 2020-07-27 220308.jpg

Annotation 2020-07-27 220308.jpg

In a lithium/sulfur (Li/S) battery, the reduction of sulfur during discharge involves a particular mechanism, where the active material successively dissolves into the electrolyte to form lithium polysulfide intermediate species (Li2Sx), with x being a function of the state of charge. In this work, sulfur K-edge resonant inelastic X-ray scattering measurements were performed for the characterization of different Li2Sx polysulfide standard solutions. High-energy resolution fluorescence detected X-ray absorption spectroscopy allowed clear separation the pre-edge absorption peak corresponding to terminal sulfur atoms from the main absorption peak due to internal atoms and allowed quantitative evaluation of the evolution of the peak area ratio as a function of the polysulfide chain length. Results of this experimental work demonstrate that the normalized area of the pre-edge is a reliable fingerprint of the Li2Sx mean chain length in agreement with recent theoretical predictions. As a perspective, this work confirms that operando HERFD XAS can be used to differentiate mean polysulfide composition, which is key issue in the characterization of Li/S cells.
doi.org/10.1021/acs.jpclett.0c01120
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mise à jour le 27 juillet 2020

Université Grenoble Alpes