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Understanding the Role of Imide‐Based Salts and Borate‐Based Additives for Safe and High‐Performance Glyoxal‐Based Electrolytes in Ni‐Rich NMC$_{811}$ Cathodes for Li‐Ion Batteries

Klein, Michel; Binder, Markus 1,2; Koželj, Matjaž; Pierini, Adriano; Gouveia, Tom; Diemant, Thomas 1; Schür, Annika 1; Brutti, Sergio; Bodo, Enrico; Bresser, Dominic 1; Gómez-Urbano, Juan Luis ; Balducci, Andrea
1 Karlsruher Institut für Technologie (KIT)
2 Sicherheit und Umwelt (SUM), Karlsruher Institut für Technologie (KIT)

Abstract:

Herein, the design of novel and safe electrolyte formulations for high-
voltage Ni-rich cathodes is reported. The solvent mixture comprising
1,1,2,2-tetraethoxyethane and propylene carbonate not only displays
good transport properties, but also greatly enhances the overall safety
of the cell thanks to its low flammability. The influence of the conducting
salts, that is, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium
bis(fluorosulfonyl)imide (LiFSI), and of the additives lithium bis(oxalato)borate
(LiBOB) and lithium difluoro(oxalato)borate (LiDFOB) is examined. Molecular
dynamics simulations are carried out to gain insights into the local structure
of the different electrolytes and the lithium-ion coordination. Furthermore,
special emphasis is placed on the film-forming abilities of the salts to suppress
the anodic dissolution of the aluminum current collector and to create
a stable cathode electrolyte interphase (CEI). In this regard, the borate-based
additives significantly alleviate the intrinsic challenges associated
with the use of LiTFSI and LiFSI salts. It is worth remarking that a superior
cathode performance is achieved by using the LiFSI/LiDFOB electrolyte,
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Verlagsausgabe §
DOI: 10.5445/IR/1000171853
Veröffentlicht am 21.06.2024
Originalveröffentlichung
DOI: 10.1002/smll.202401610
Scopus
Zitationen: 1
Web of Science
Zitationen: 1
Dimensions
Zitationen: 1
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Karlsruher Institut für Technologie (KIT)
Sicherheit und Umwelt (SUM)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 10.2024
Sprache Englisch
Identifikator ISSN: 1613-6810, 1613-6829
KITopen-ID: 1000171853
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Small
Verlag John Wiley and Sons
Band 20
Heft 42
Seiten Art.-Nr.: 2401610
Vorab online veröffentlicht am 10.06.2024
Nachgewiesen in Scopus
Dimensions
Web of Science
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie
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