Polysulfide Speciation in Li–S Battery Electrolyte via In-Operando Optical Imaging and Ex-Situ UV-vis Spectra Analysis

Author(s)Taiwo, Gbenga S.
Author(s)Rashti, Ali
Author(s)Mishra, Mritunjay
Author(s)Yao, Koffi P. C.
Date Accessioned2022-09-14T19:24:52Z
Date Available2022-09-14T19:24:52Z
Publication Date2022-09-13
DescriptionThis article was originally published in Journal of The Electrochemical Society. The version of record is available at: https://doi.org/10.1149/1945-7111/ac8b3den_US
AbstractLithium sulfur (Li–S) batteries have received significant attention as one of the energy storage systems with excellent prospects for emerging applications due to their high energy density and low-cost. However, there are fundamental challenges impeding the commercialization of Li–S batteries. Notorious among those challenges is the "polysulfide shuttle" consisting of the dissolution into the electrolyte solvent and subsequent crossover to the anode of long-chain lithium polysulfides. Sparingly solvating electrolytes have been exploited as an approach to reduce the dissolution of polysulfides and thereby the shuttle effect. Using an optical in operando lithium-sulfur cell and ex situ UV–vis spectroscopy, we elucidate the speciation of polysulfides in fully and sparingly solvating electrolytes for Li–S batteries. Extensive literature meta-analysis reveals that the most unambiguous effect of sparingly solvating solvent is in improving the coulombic efficiency of sulfur-cells. Experimental optical imaging and UV–vis characterization elucidate a shift towards shorter-chain polysulfides in electrolytes with increasing lithium-salt concentration (more sparingly solvating). The shift to shorter-chain polysulfides corresponds to a reduction of polysulfide species participating in shuttling which corroborate the increased coulombic efficiency in sparingly-solvating electrolytes.en_US
SponsorThis research was funded by University of Delaware faculty start-up support for Koffi Yao. The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest. KPY is the principal investigator. GST performed the experiments and drafted the manuscript. MM did the fitting of the UV–vis spectra and interpretation of data. AR provided postdoctoral experimental guidance and suggestions during the experimentation phase.en_US
CitationTaiwo, Gbenga S., Ali Rashti, Mritunjay Mishra, and Koffi P. C. Yao. “Polysulfide Speciation in Li–S Battery Electrolyte via In-Operando Optical Imaging and Ex-Situ UV-Vis Spectra Analysis.” Journal of The Electrochemical Society 169, no. 9 (2022): 090518. https://doi.org/10.1149/1945-7111/ac8b3d.en_US
ISSN1945-7111
URLhttps://udspace.udel.edu/handle/19716/31360
Languageen_USen_US
PublisherJournal of The Electrochemical Societyen_US
TitlePolysulfide Speciation in Li–S Battery Electrolyte via In-Operando Optical Imaging and Ex-Situ UV-vis Spectra Analysisen_US
TypeArticleen_US
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