Journal Article

FZJ-2017-03792

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Improving the Lithium Ion Transport in Polymer Electrolytes by Functionalized Ionic-Liquid Additives: Simulations and Modeling

Diddens, D. (Corresponding author)FZJ* ; Paillard, E.-E.FZJ* ; Heuer, A.

2017
Electrochemical Soc. Pennington, NJ

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Please use a persistent id in citations: http://hdl.handle.net/2128/14551  doi:10.1149/2.0271711jes

Abstract: We present a theoretical study combining molecular dynamics (MD) simulations with an analytical lithium ion transport model [Maitra and Heuer, Phys. Rev. Lett. 2007, 98, 227802] to highlight a novel strategy to increase the lithium mobility in polymer electrolytes based on poly(ethylene oxide) (PEO). This is achieved by using a pyrrolidinium-based ionic liquid (IL) where the cation has been chemically functionalized by a short oligoether side chain [von Zamory et al., Phys. Chem. Chem. Phys. 2016, 18(31), 21539] as an additive. Since the oligoether moieties at the pyrrolidinium cations form pronounced coordinations to the lithium ions for sufficiently long side chains, the ions can be detached from the PEO backbone. In this way, a fundamentally new lithium ion transport mechanism is established (shuttling mechanism), in which the lithium dynamics is decoupled from the polymer dynamics, the latter typically being slow under experimental conditions. Based on our simulations, we incorporate this novel mechanism into our existing model, which accurately reproduces the observed lithium dynamics. We demonstrate that the use of oligoether-functionalized IL additives significantly increases the lithium diffusivity. Finally, we show that for experimentally relevant electrolytes containing long polymer chains, an even stronger increase of the lithium mobility can be expected.

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Contributing Institute(s):

1. Helmholtz-Institut Münster Ionenleiter für Energiespeicher (IEK-12)

Research Program(s):

1. 131 - Electrochemical Storage (POF3-131) (POF3-131)

Appears in the scientific report 2017

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Database coverage:
; ; ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; IF < 5 ; JCR ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection

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