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Initial SEI formation in LiBOB-, LiDFOB- and LiBF4-containing PEO electrolytes
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.ORCID iD: 0000-0003-1785-8364
Natl Taiwan Univ Sci & Technol, Dept Chem Engn, Taipei 106, Taiwan..ORCID iD: 0000-0002-4093-9093
Dipartimento Chim Materiali & Ingn Chim Giulio Nat, Dipartimento Chim Mat & Ingn Chim Giulio Natta, Via Luigi Mancinelli 7, I-20131 Milan, Italy..
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.ORCID iD: 0000-0002-8676-8605
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2024 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 12, no 15, p. 9184-9199Article in journal (Refereed) Published
Abstract [en]

A limiting factor for solid polymer electrolyte (SPE)-based Li-batteries is the functionality of the electrolyte decomposition layer that is spontaneously formed at the Li metal anode. A deeper understanding of this layer will facilitate its improvement. This study investigates three SPEs – polyethylene oxide:lithium tetrafluoroborate (PEO:LiBF4), polyethylene oxide:lithium bis(oxalate)borate (PEO:LiBOB), and polyethylene oxide:lithium difluoro(oxalato)borate (PEO:LiDFOB) – using a combination of electrochemical impedance spectroscopy (EIS), galvanostatic cycling, in situ Li deposition photoelectron spectroscopy (PES), and ab initio molecular dynamics (AIMD) simulations. Through this combination, the cell performance of PEO:LiDFOB can be connected to the initial SPE decomposition at the anode interface. It is found that PEO:LiDFOB had the highest capacity retention, which is correlated to having the least decomposition at the interface. This indicates that the lower SPE decomposition at the interface still creates a more effective decomposition layer, which is capable of preventing further electrolyte decomposition. Moreover, the PES results indicate formation of polyethylene in the SEI in cells based on PEO electrolytes. This is supported by AIMD that shows a polyethylene formation pathway through free-radical polymerization of ethylene.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2024. Vol. 12, no 15, p. 9184-9199
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Materials Chemistry Physical Chemistry Polymer Technologies
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URN: urn:nbn:se:uu:diva-528371DOI: 10.1039/d3ta07175hISI: 001187317000001PubMedID: 38633215OAI: oai:DiVA.org:uu-528371DiVA, id: diva2:1859351
Funder
StandUpSwedish Foundation for Strategic Research, 139501338EU, Horizon 2020, 860403EU, Horizon 2020, 772777Swedish Energy Agency, P2021-90225Available from: 2024-05-21 Created: 2024-05-21 Last updated: 2024-05-21Bibliographically approved

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Andersson, Edvin K. W.Weng, Yi-ChenFriesen, DanielElbouazzaoui, KenzaBrandell, DanielMindemark, JonasHahlin, Maria

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Andersson, Edvin K. W.Wu, Liang-TingWeng, Yi-ChenFriesen, DanielElbouazzaoui, KenzaGiangrisostomi, ErikaBrandell, DanielMindemark, JonasHahlin, Maria
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Structural ChemistryCondensed Matter Physics of Energy MaterialsDepartment of Chemistry - Ångström
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