On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering

Christian Prehal (), Jean-Marc Mentlen, Sara Drvarič Talian, Alen Vizintin, Robert Dominko, Heinz Amenitsch, Lionel Porcar, Stefan A. Freunberger () and Vanessa Wood ()
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Christian Prehal: ETH Zürich
Jean-Marc Mentlen: ETH Zürich
Sara Drvarič Talian: National Institute of Chemistry
Alen Vizintin: National Institute of Chemistry
Robert Dominko: National Institute of Chemistry
Heinz Amenitsch: Graz University of Technology
Lionel Porcar: Institut Laue–Langevin
Stefan A. Freunberger: Institute of Science and Technology Austria (ISTA)
Vanessa Wood: ETH Zürich

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: Abstract The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li2S) via soluble polysulfides (PSs) formation impedes the development of high-performance lithium-sulfur (Li-S) batteries with non-aqueous electrolyte solutions. Here, we use operando small and wide angle X-ray scattering and operando small angle neutron scattering (SANS) measurements to track the nucleation, growth and dissolution of solid deposits from atomic to sub-micron scales during real-time Li-S cell operation. In particular, stochastic modelling based on the SANS data allows quantifying the nanoscale phase evolution during battery cycling. We show that next to nano-crystalline Li2S the deposit comprises solid short-chain PSs particles. The analysis of the experimental data suggests that initially, Li2S2 precipitates from the solution and then is partially converted via solid-state electroreduction to Li2S. We further demonstrate that mass transport, rather than electron transport through a thin passivating film, limits the discharge capacity and rate performance in Li-S cells.

Date: 2022
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DOI: 10.1038/s41467-022-33931-4

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