Ion transport mechanisms in lamellar phases of salt-doped PS–PEO block copolymer electrolytes

Handle URI:
http://hdl.handle.net/10754/626079
Title:
Ion transport mechanisms in lamellar phases of salt-doped PS–PEO block copolymer electrolytes
Authors:
Sethuraman, Vaidyanathan; Mogurampelly, Santosh ( 0000-0002-3145-4377 ) ; Ganesan, Venkat ( 0000-0003-3899-5843 )
Abstract:
We use a multiscale simulation strategy to elucidate, at an atomistic level, the mechanisms underlying ion transport in the lamellar phase of polystyrene–polyethylene oxide (PS–PEO) block copolymer (BCP) electrolytes doped with LiPF6 salts. Explicitly, we compare the results obtained for ion transport in the microphase separated block copolymer melts to those for salt-doped PEO homopolymer melts. In addition, we also present results for dynamics of the ions individually in the PEO and PS domains of the BCP melt, and locally as a function of the distance from the lamellar interfaces. When compared to the PEO homopolymer melt, ions were found to exhibit slower dynamics in both the block copolymer (overall) and in the PEO phase of the BCP melt. Such results are shown to arise from the effects of slower polymer segmental dynamics in the BCP melt and the coordination characteristics of the ions. Polymer backbone-ion residence times analyzed as a function of distance from the interface indicate that ions have a larger residence time near the interface compared to that near the bulk of lamella, and demonstrates the influence of the glassy PS blocks and microphase segregation on the ion transport properties. Ion transport mechanisms in BCP melts reveal that there exist five distinct mechanisms for ion transport along the backbone of the chain and exhibit qualitative differences from the behavior in homopolymer melts. We also present results as a function of salt concentration which show that the mean-squared displacements of the ions decrease with increasing salt concentration, and that the ion residence times near the polymer backbone increase with increasing salt concentration.
Citation:
Sethuraman V, Mogurampelly S, Ganesan V (2017) Ion transport mechanisms in lamellar phases of salt-doped PS–PEO block copolymer electrolytes. Soft Matter. Available: http://dx.doi.org/10.1039/c7sm01345k.
Publisher:
Royal Society of Chemistry (RSC)
Journal:
Soft Matter
KAUST Grant Number:
OSR-2016-CRG5-2993-1
Issue Date:
23-Oct-2017
DOI:
10.1039/c7sm01345k
Type:
Article
ISSN:
1744-683X; 1744-6848
Sponsors:
VG acknowledges funding in part by grants from the Robert A. Welch Foundation (Grant F1599), the National Science Foundation (DMR-1721512), and to King Abdullah University of Science and Technology (OSR-2016-CRG5-2993-1). Acknowledgment is also made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research (56715-ND9). The authors acknowledge the Texas Advanced Computing Center (TACC) for computing resources.
Appears in Collections:
Publications Acknowledging KAUST Support

Full metadata record

DC FieldValue Language
dc.contributor.authorSethuraman, Vaidyanathanen
dc.contributor.authorMogurampelly, Santoshen
dc.contributor.authorGanesan, Venkaten
dc.date.accessioned2017-11-01T08:19:12Z-
dc.date.available2017-11-01T08:19:12Z-
dc.date.issued2017-10-23en
dc.identifier.citationSethuraman V, Mogurampelly S, Ganesan V (2017) Ion transport mechanisms in lamellar phases of salt-doped PS–PEO block copolymer electrolytes. Soft Matter. Available: http://dx.doi.org/10.1039/c7sm01345k.en
dc.identifier.issn1744-683Xen
dc.identifier.issn1744-6848en
dc.identifier.doi10.1039/c7sm01345ken
dc.identifier.urihttp://hdl.handle.net/10754/626079-
dc.description.abstractWe use a multiscale simulation strategy to elucidate, at an atomistic level, the mechanisms underlying ion transport in the lamellar phase of polystyrene–polyethylene oxide (PS–PEO) block copolymer (BCP) electrolytes doped with LiPF6 salts. Explicitly, we compare the results obtained for ion transport in the microphase separated block copolymer melts to those for salt-doped PEO homopolymer melts. In addition, we also present results for dynamics of the ions individually in the PEO and PS domains of the BCP melt, and locally as a function of the distance from the lamellar interfaces. When compared to the PEO homopolymer melt, ions were found to exhibit slower dynamics in both the block copolymer (overall) and in the PEO phase of the BCP melt. Such results are shown to arise from the effects of slower polymer segmental dynamics in the BCP melt and the coordination characteristics of the ions. Polymer backbone-ion residence times analyzed as a function of distance from the interface indicate that ions have a larger residence time near the interface compared to that near the bulk of lamella, and demonstrates the influence of the glassy PS blocks and microphase segregation on the ion transport properties. Ion transport mechanisms in BCP melts reveal that there exist five distinct mechanisms for ion transport along the backbone of the chain and exhibit qualitative differences from the behavior in homopolymer melts. We also present results as a function of salt concentration which show that the mean-squared displacements of the ions decrease with increasing salt concentration, and that the ion residence times near the polymer backbone increase with increasing salt concentration.en
dc.description.sponsorshipVG acknowledges funding in part by grants from the Robert A. Welch Foundation (Grant F1599), the National Science Foundation (DMR-1721512), and to King Abdullah University of Science and Technology (OSR-2016-CRG5-2993-1). Acknowledgment is also made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research (56715-ND9). The authors acknowledge the Texas Advanced Computing Center (TACC) for computing resources.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.titleIon transport mechanisms in lamellar phases of salt-doped PS–PEO block copolymer electrolytesen
dc.typeArticleen
dc.identifier.journalSoft Matteren
dc.contributor.institutionDepartment of Chemical Engineering, University of Texas at Austin, Austin, USAen
kaust.grant.numberOSR-2016-CRG5-2993-1en
All Items in KAUST are protected by copyright, with all rights reserved, unless otherwise indicated.