Home > Publications database > Controlling Li + transport in ionic liquid electrolytes through salt content and anion asymmetry: a mechanistic understanding gained from molecular dynamics simulations > print

001     1024592
005     20240712113117.0
024 7 _ |a 10.1039/D1CP04830A
|2 doi
024 7 _ |a 1463-9076
|2 ISSN
024 7 _ |a 1463-9084
|2 ISSN
024 7 _ |a 10.34734/FZJ-2024-02266
|2 datacite_doi
024 7 _ |a 35212346
|2 pmid
024 7 _ |a WOS:000760909900001
|2 WOS
037 _ _ |a FZJ-2024-02266
082 _ _ |a 540
100 1 _ |a Wettstein, Alina
|0 0000-0003-2693-3653
|b 0
245 _ _ |a Controlling Li + transport in ionic liquid electrolytes through salt content and anion asymmetry: a mechanistic understanding gained from molecular dynamics simulations
260 _ _ |a Cambridge
|c 2022
|b RSC Publ.
336 7 _ |a article
|2 DRIVER
336 7 _ |a Output Types/Journal article
|2 DataCite
336 7 _ |a Journal Article
|b journal
|m journal
|0 PUB:(DE-HGF)16
|s 1712837718_16170
|2 PUB:(DE-HGF)
336 7 _ |a ARTICLE
|2 BibTeX
336 7 _ |a JOURNAL_ARTICLE
|2 ORCID
336 7 _ |a Journal Article
|0 0
|2 EndNote
500 _ _ |a Unterstützt durch den MWIDE Grant: “GrEEn” project (funding code: 313-W044A)
520 _ _ |a In this work, we report the results from molecular dynamics simulations of lithium salt-ionic liquid electrolytes (ILEs) based either on the symmetric bis[(trifluoromethyl)sulfonyl]imide (TFSI−) anion or its asymmetric analogue 2,2,2-(trifluoromethyl)sulfonyl-N-cyanoamide (TFSAM−). Relating lithium's coordination environment to anion mean residence times and diffusion constants confirms the remarkable transport behaviour of the TFSAM−-based ILEs that has been observed in recent experiments: for increased salt doping, the lithium ions must compete for the more attractive cyano over oxygen coordination and a fragmented landscape of solvation geometries emerges, in which lithium appears to be less strongly bound. We present a novel, yet statistically straightforward methodology to quantify the extent to which lithium and its solvation shell are dynamically coupled. By means of a Lithium Coupling Factor (LCF) we demonstrate that the shell anions do not constitute a stable lithium vehicle, which suggests for this electrolyte material the commonly termed “vehicular” lithium transport mechanism could be more aptly pictured as a correlated, flow-like motion of lithium and its neighbourhood. Our analysis elucidates two separate causes why lithium and shell dynamics progressively decouple with higher salt content: on the one hand, an increased sharing of anions between lithium limits the achievable LCF of individual lithium-anion pairs. On the other hand, weaker binding configurations naturally entail a lower dynamic stability of the lithium-anion complex, which is particularly relevant for the TFSAM−-containing ILEs.
536 _ _ |a 1221 - Fundamentals and Materials (POF4-122)
|0 G:(DE-HGF)POF4-1221
|c POF4-122
|f POF IV
|x 0
588 _ _ |a Dataset connected to CrossRef, Journals: juser.fz-juelich.de
700 1 _ |a Diddens, Diddo
|0 P:(DE-Juel1)169877
|b 1
700 1 _ |a Heuer, Andreas
|0 P:(DE-Juel1)176646
|b 2
|e Corresponding author
773 _ _ |a 10.1039/D1CP04830A
|g Vol. 24, no. 10, p. 6072 - 6086
|0 PERI:(DE-600)1476244-4
|n 10
|p 6072 - 6086
|t Physical chemistry, chemical physics
|v 24
|y 2022
|x 1463-9076
856 4 _ |y OpenAccess
|u https://juser.fz-juelich.de/record/1024592/files/2110.11278.pdf
856 4 _ |y OpenAccess
|x icon
|u https://juser.fz-juelich.de/record/1024592/files/2110.11278.gif?subformat=icon
856 4 _ |y OpenAccess
|x icon-1440
|u https://juser.fz-juelich.de/record/1024592/files/2110.11278.jpg?subformat=icon-1440
856 4 _ |y OpenAccess
|x icon-180
|u https://juser.fz-juelich.de/record/1024592/files/2110.11278.jpg?subformat=icon-180
856 4 _ |y OpenAccess
|x icon-640
|u https://juser.fz-juelich.de/record/1024592/files/2110.11278.jpg?subformat=icon-640
909 C O |o oai:juser.fz-juelich.de:1024592
|p openaire
|p open_access
|p VDB
|p driver
|p dnbdelivery
910 1 _ |a External Institute
|0 I:(DE-HGF)0
|k Extern
|b 0
|6 0000-0003-2693-3653
910 1 _ |a Forschungszentrum Jülich
|0 I:(DE-588b)5008462-8
|k FZJ
|b 1
|6 P:(DE-Juel1)169877
910 1 _ |a Forschungszentrum Jülich
|0 I:(DE-588b)5008462-8
|k FZJ
|b 2
|6 P:(DE-Juel1)176646
913 1 _ |a DE-HGF
|b Forschungsbereich Energie
|l Materialien und Technologien für die Energiewende (MTET)
|1 G:(DE-HGF)POF4-120
|0 G:(DE-HGF)POF4-122
|3 G:(DE-HGF)POF4
|2 G:(DE-HGF)POF4-100
|4 G:(DE-HGF)POF
|v Elektrochemische Energiespeicherung
|9 G:(DE-HGF)POF4-1221
|x 0
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)0200
|2 StatID
|b SCOPUS
|d 2023-10-21
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)0160
|2 StatID
|b Essential Science Indicators
|d 2023-10-21
915 _ _ |a JCR
|0 StatID:(DE-HGF)0100
|2 StatID
|b PHYS CHEM CHEM PHYS : 2022
|d 2023-10-21
915 _ _ |a WoS
|0 StatID:(DE-HGF)0113
|2 StatID
|b Science Citation Index Expanded
|d 2023-10-21
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)0150
|2 StatID
|b Web of Science Core Collection
|d 2023-10-21
915 _ _ |a IF < 5
|0 StatID:(DE-HGF)9900
|2 StatID
|d 2023-10-21
915 _ _ |a OpenAccess
|0 StatID:(DE-HGF)0510
|2 StatID
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)1150
|2 StatID
|b Current Contents - Physical, Chemical and Earth Sciences
|d 2023-10-21
915 _ _ |a National-Konsortium
|0 StatID:(DE-HGF)0430
|2 StatID
|d 2023-10-21
|w ger
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)0300
|2 StatID
|b Medline
|d 2023-10-21
915 _ _ |a DBCoverage
|0 StatID:(DE-HGF)0199
|2 StatID
|b Clarivate Analytics Master Journal List
|d 2023-10-21
920 1 _ |0 I:(DE-Juel1)IEK-12-20141217
|k IEK-12
|l Helmholtz-Institut Münster Ionenleiter für Energiespeicher
|x 0
980 1 _ |a FullTexts
980 _ _ |a journal
980 _ _ |a VDB
980 _ _ |a UNRESTRICTED
980 _ _ |a I:(DE-Juel1)IEK-12-20141217
981 _ _ |a I:(DE-Juel1)IMD-4-20141217

LibraryCollectionCLSMajorCLSMinorLanguageAuthor
Marc 21