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

Autor: Prehal C; Department of Information Technology and Electrical Engineering, ETH Zürich, Gloriastrasse 35, 8092, Zürich, Switzerland. cprehal@ethz.ch., von Mentlen JM; Department of Information Technology and Electrical Engineering, ETH Zürich, Gloriastrasse 35, 8092, Zürich, Switzerland., Drvarič Talian S; Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000, Ljubljana, Slovenia., Vizintin A; Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000, Ljubljana, Slovenia., Dominko R; Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000, Ljubljana, Slovenia.; Faculty of Chemistry and Chemical Technology University of Ljubljana, Večna pot 113, 1000, Ljubljana, Slovenia., Amenitsch H; Institute for Inorganic Chemistry, Graz University of Technology, Stremayrgasse 9, 8010, Graz, Austria., Porcar L; Institut Laue-Langevin, 71 Avenue des Martyrs, Grenoble, 38042, France., Freunberger SA; Institute of Science and Technology Austria (ISTA), Am Campus 1, 3400, Klosterneuburg, Austria. stefan.freunberger@ist.ac.at., Wood V; Department of Information Technology and Electrical Engineering, ETH Zürich, Gloriastrasse 35, 8092, Zürich, Switzerland. vwood@ethz.ch.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2022 Oct 24; Vol. 13 (1), pp. 6326. Date of Electronic Publication: 2022 Oct 24.
DOI: 10.1038/s41467-022-33931-4
Abstrakt: The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li 2 S) 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 Li 2 S the deposit comprises solid short-chain PSs particles. The analysis of the experimental data suggests that initially, Li 2 S 2 precipitates from the solution and then is partially converted via solid-state electroreduction to Li 2 S. 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.
(© 2022. The Author(s).)
Databáze: MEDLINE
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