Cation Transport in Polymer Electrolytes: A Microscopic Approach

Maitra, Arijit; Heuer, Andreas

doi:10.1103/physrevlett.98.227802

Cited by 134 publications

(217 citation statements)

References 20 publications

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“…As discussed in Ref. [22] the diffusive behavior of the Li + ions for long chains is achieved via jumps between different PEO chains. The residence time of the cation with one chain is found to be τ Li ≈ 100 ns [22].…”

Section: Stolwijk-obeidi Modelmentioning

confidence: 99%

“…[22] the diffusive behavior of the Li + ions for long chains is achieved via jumps between different PEO chains. The residence time of the cation with one chain is found to be τ Li ≈ 100 ns [22]. Only for short chains (as in the present case) the timescale of Li + diffusion will be somewhat shorter because of the dominance of the center of mass diffusion of the polymer.…”

Section: Stolwijk-obeidi Modelmentioning

confidence: 99%

“…This led them to interpret that the ion-pairs are not coordinated with the ether oxygen atoms. In light of the insights from computer simulations where most of the cations (both free and those associated with anions) are structurally correlated and dynamically coupled to the ether oxygen atoms [22] the SO model can be extended to accommodate the scenario where the free ions and ion-pairs should display similar mobility.…”

Section: Introductionmentioning

confidence: 99%

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Understanding Correlation Effects for Ion Conduction in Polymer Electrolytes

Maitra

Heuer

2008

J. Phys. Chem. B

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Polymer electrolytes typically exhibit diminished ionic conductivity due to the presence of correlation effects between the cations and anions. Microscopically, transient ionic aggregates, e.g. Lett. 93, 125901, 2004]. The approximation parameters, which can be retrieved from simulations, point to the necessity of additional information in order to fully describe the correlation effects apart from merely the fraction of ion-pairs which apparently accounts for the correlations originating from only the nearest neighbor structural correlations. These parameters are close to but not exactly unity as assumed in the SO model. Finally, as an application of the extended SO model one is able to estimate the dynamics of the free and non-free ions as well as their fractions from the knowledge of the single particle diffusivities and the collective diffusivity of the ions. * Electronic address: arijitmaitra@uni-muenster.de,andheuer@uni-muenster.de

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Section: Stolwijk-obeidi Modelmentioning

confidence: 99%

Section: Stolwijk-obeidi Modelmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Understanding Correlation Effects for Ion Conduction in Polymer Electrolytes

Maitra

Heuer

2008

J. Phys. Chem. B

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“…Analytical model.-To rationalize our findings from the MD simulations, we employ an analytical lithium ion transport model, 29 which has already been successfully applied to ternary polymer electrolytes of the type PEO/LiTFSI/Pyr 13 TFSI. 17,18 This model is based on both Figure 2.…”

Section: Theoretical Backgroundmentioning

confidence: 99%

“…Sketch of the microscopic lithium transport mechanisms taken into account by the analytical model. 29 Each mechanism is quantified by a characteristic time scale.…”

Section: Theoretical Backgroundmentioning

confidence: 99%

Improving the Lithium Ion Transport in Polymer Electrolytes by Functionalized Ionic-Liquid Additives: Simulations and Modeling

Diddens

Paillard

Heuer

2017

J. Electrochem. Soc.

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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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Heterogeneous Nanodomain Electrolytes for Ultra‐Long‐Life All‐Solid‐State Lithium‐Metal Batteries

Yang

Luo

Zheng

et al. 2022

Adv Funct Materials

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Solid polymer electrolytes exhibit huge advantages but are hindered by insufficient mechanical strength and ionic conductivity in the applications of all‐solid‐state lithium‐metal batteries (ASSLBs). Herein, poly(ether‐block‐amide) (Pebax) strategies to construct heterogeneous nanodomain electrolytes (HNEs) for ultra‐long‐life ASSLBs are introduced. Pebax HNEs forms conductive nanodomains via phase separation, exhibiting interconnected and high Li+ conductive features. Compared with conventional PEO‐based electrolytes, the Pebax HNEs with controllable size and order can facilitate rapid Li+ transport with steerable transport channels, further enhancing the Li+ conductivity and inducing the uniform Li+ deposition. Furthermore, the obtained thin and dense hybrid SEI layer with potent mechanical strength can synergistically suppress the dendrite growth, and the as‐prepared ASSLBs exhibit a satisfactory capacity with a tiny capacity reduction of 0.013% per cycle over 1500 cycles. This work provides a brand‐new insight to construct a conductive structure in electrolytes for high‐performance ASSLBs.

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Cation Transport in Polymer Electrolytes: A Microscopic Approach

Cited by 134 publications

References 20 publications

Understanding Correlation Effects for Ion Conduction in Polymer Electrolytes

Understanding Correlation Effects for Ion Conduction in Polymer Electrolytes

Improving the Lithium Ion Transport in Polymer Electrolytes by Functionalized Ionic-Liquid Additives: Simulations and Modeling

Heterogeneous Nanodomain Electrolytes for Ultra‐Long‐Life All‐Solid‐State Lithium‐Metal Batteries

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