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Density Functional Theory Studies on Sulfur-Polyacrylonitrile as a Cathode Host Material for Lithium-Sulfur Batteries

Bertolini, Samuel; Jacob, Timo 1
1 Center for Electrochemical Energy Storage Ulm & Karlsruhe (CELEST), Karlsruher Institut für Technologie (KIT)


Cyclized polyacrylonitrile, which can be obtained by vulcanization of polyacrylonitrile with sulfur, is an electron-conductive polymer that can be used as a host material in lithium–sulfur batteries. Using density functional theory, we investigated the interaction between a surrounding electrolyte and the polymeric sulfur–polyacrylonitrile (SPAN) electrode. In particular, we focused on different configurations, where the system contains 1,3-dioxane as a solvent and can have (i) polysulfide (PS) solvated in the electrolyte, (ii) a PS attached to the polymer backbone, (iii) lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as a salt dissolved in the electrolyte, and (iv) both PS and LiTFSI dissolved in the electrolyte. We found that the polymer, when having a hydrogen vacancy at a carbon atom (undercoordinated carbon) of the polymer backbone, is able to not only capture a PS from the electrolyte but also decompose and bind to the solvent and/or remove lithium from the PS. During this capturing process, the polysulfide might undergo S–S bond cleavage and recombination, accompanied by a charge transfer between the polysulfide and polymer. ... mehr

Verlagsausgabe §
DOI: 10.5445/IR/1000132626
Veröffentlicht am 12.05.2021
DOI: 10.1021/acsomega.0c06240
Zitationen: 12
Web of Science
Zitationen: 11
Zitationen: 11
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Post Lithium Storage (POLiS)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2021
Sprache Englisch
Identifikator ISSN: 2470-1343
KITopen-ID: 1000132626
HGF-Programm 38.02.02 (POF IV, LK 01) Components and Cells
Erschienen in ACS Omega
Verlag American Chemical Society (ACS)
Band 6
Heft 14
Seiten 9700-9708
Nachgewiesen in Web of Science
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