Polysulfide driven degradation in lithium–sulfur batteries during cycling – quantitative and high time-resolution operando X-ray absorption study for dissolved polysulfides probed at both electrode sides

dc.bibliographicCitation.firstPage10231eng
dc.bibliographicCitation.issue16eng
dc.bibliographicCitation.lastPage10239eng
dc.bibliographicCitation.volume9eng
dc.contributor.authorZech, Claudia
dc.contributor.authorHönicke, Philipp
dc.contributor.authorKayser, Yves
dc.contributor.authorRisse, Sebastian
dc.contributor.authorGrätz, Olga
dc.contributor.authorStamm, Manfred
dc.contributor.authorBeckhoff, Burkhard
dc.date.accessioned2022-03-22T11:00:02Z
dc.date.available2022-03-22T11:00:02Z
dc.date.issued2021
dc.description.abstractThe development of operando characterization techniques on realistic batteries is essential for an advanced mechanistic understanding in battery chemistry and, therefore, contributes to their further performance improvement. This manuscript presents operando Near-Edge X-ray Absorption Spectroscopy (NEXAFS) traceable to the SI units (SI is the abbreviation for the International System of Units) during multiple charge–discharge cycles on both electrodes of lithium–sulfur (Li/S) coin cells which enables an absolute quantification of dissolved polysulfides with no need for calibration samples or reference material. We could reveal that during the charging process, polysulfide (PS) movement from the negative to the positive electrode is inhibited. This leads to a steady increase of dissolved polysulfides at the anode side and, therefore, is one of the key points for capacity fading. We quantitatively track the polysulfides dissolved in the electrolyte and correlate for the first time their evolution with the capacity fading of the cell. We analyze the appearance of PS during cell operation at the cathode and anode side to characterize the transport mechanisms of the polysulfide shuttle phenomena and to reveal quantitative information about their evolution at different states of charge and states of health. Our cell design suppresses the contribution of cathodic sulfur, which is mandatory for reference-sample-free quantification in X-ray spectrometry and allows us to use only slightly modified standard coin cell batteries.eng
dc.description.versionpublishedVersioneng
dc.identifier.urihttps://oa.tib.eu/renate/handle/123456789/8317
dc.identifier.urihttps://doi.org/10.34657/7355
dc.language.isoengeng
dc.publisherLondon [u.a.] : RSCeng
dc.relation.doihttps://doi.org/10.1039/d0ta12011a
dc.relation.essn2050-7496
dc.relation.ispartofseriesJournal of materials chemistry : A, Materials for energy and sustainability 9 (2021), Nr. 16eng
dc.rights.licenseCC BY-NC 3.0 Unportedeng
dc.rights.urihttps://creativecommons.org/licenses/by-nc/3.0/eng
dc.subjectAnodeseng
dc.subjectDissolutioneng
dc.subjectElectric dischargeseng
dc.subjectElectrolyteseng
dc.subjectLithium batterieseng
dc.subjectLithium metallographyeng
dc.subjectMetric systemeng
dc.subjectPhotodegradationeng
dc.subjectPolysulfideseng
dc.subjectX ray absorption spectroscopyeng
dc.subjectAbsolute quantificationeng
dc.subjectCalibration sampleseng
dc.subjectHigh-time resolutioneng
dc.subjectNear edge x-ray absorption spectroscopieseng
dc.subjectPolysulfide shuttleseng
dc.subjectQuantitative informationeng
dc.subjectTransport mechanismeng
dc.subjectLithium sulfur batterieseng
dc.subject.ddc540eng
dc.subject.ddc530eng
dc.titlePolysulfide driven degradation in lithium–sulfur batteries during cycling – quantitative and high time-resolution operando X-ray absorption study for dissolved polysulfides probed at both electrode sideseng
dc.typearticleeng
dc.typeTexteng
dcterms.bibliographicCitation.journalTitleJournal of materials chemistry : A, Materials for energy and sustainabilityeng
tib.accessRightsopenAccesseng
wgl.contributorIPFeng
wgl.subjectChemieeng
wgl.typeZeitschriftenartikeleng
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