Direct observation of lithium polysulfides in lithium–sulfur batteries using operando X-ray diffraction

Joanna Conder, Renaud Bouchet, Sigita Trabesinger, Cyril Marino, Lorenz Gubler and Claire Villevieille ()
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Joanna Conder: Paul Scherrer Institute, Electrochemistry Laboratory
Renaud Bouchet: Université Grenoble Alpes, Grenoble INP, LEPMI Laboratory
Sigita Trabesinger: Paul Scherrer Institute, Electrochemistry Laboratory
Cyril Marino: Paul Scherrer Institute, Electrochemistry Laboratory
Lorenz Gubler: Paul Scherrer Institute, Electrochemistry Laboratory
Claire Villevieille: Paul Scherrer Institute, Electrochemistry Laboratory

Nature Energy, 2017, vol. 2, issue 6, 1-7

Abstract: Abstract In the on going quest towards lithium-battery chemistries beyond the lithium-ion technology, the lithium–sulfur system is emerging as one of the most promising candidates. The major outstanding challenge on the route to commercialization is controlling the so-called polysulfide shuttle, which is responsible for the poor cycling efficiency of the current generation of lithium–sulfur batteries. However, the mechanistic understanding of the reactions underlying the polysulfide shuttle is still incomplete. Here we report the direct observation of lithium polysulfides in a lithium–sulfur cell during operation by means of operando X-ray diffraction. We identify signatures of polysulfides adsorbed on the surface of a glass-fibre separator and monitor their evolution during cycling. Furthermore, we demonstrate that the adsorption of the polysulfides onto SiO2 can be harnessed for buffering the polysulfide redox shuttle. The use of fumed silica as an electrolyte additive therefore significantly improves the specific charge and Coulombic efficiency of lithium–sulfur batteries.

Date: 2017
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DOI: 10.1038/nenergy.2017.69

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