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

Author

Listed:
  • 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
    Faculty of Chemistry and Chemical Technology University of Ljubljana)

  • 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)

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.

Suggested Citation

  • Christian Prehal & Jean-Marc Mentlen & Sara Drvarič Talian & Alen Vizintin & Robert Dominko & Heinz Amenitsch & Lionel Porcar & Stefan A. Freunberger & Vanessa Wood, 2022. "On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33931-4
    DOI: 10.1038/s41467-022-33931-4
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    References listed on IDEAS

    as
    1. Quan Pang & Xiao Liang & Chun Yuen Kwok & Linda F. Nazar, 2016. "Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes," Nature Energy, Nature, vol. 1(9), pages 1-11, September.
    2. Christian Prehal & Harald Fitzek & Gerald Kothleitner & Volker Presser & Bernhard Gollas & Stefan A. Freunberger & Qamar Abbas, 2020. "Author Correction: Persistent and reversible solid iodine electrodeposition in nanoporous carbons," Nature Communications, Nature, vol. 11(1), pages 1-1, December.
    3. Christian Prehal & Harald Fitzek & Gerald Kothleitner & Volker Presser & Bernhard Gollas & Stefan A. Freunberger & Qamar Abbas, 2020. "Persistent and reversible solid iodine electrodeposition in nanoporous carbons," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    4. Joanna Conder & Renaud Bouchet & Sigita Trabesinger & Cyril Marino & Lorenz Gubler & Claire Villevieille, 2017. "Direct observation of lithium polysulfides in lithium–sulfur batteries using operando X-ray diffraction," Nature Energy, Nature, vol. 2(6), pages 1-7, June.
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