Effect of Chain Rigidity on the Decoupling of Ion Motion from Segmental Relaxation in Polymerized Ionic Liquids: Ambient and Elevated Pressure Studies

Wojnarowska, Zaneta; Feng, Hongbo; Fu, Yao; Cheng, Shiwang; Carroll, Bobby; Kumar, Rajeev; Novikov, Vladimir N.; Kisliuk, Alexander M.; Saito, Tomonori; Kang, Nam-Goo; Mays, Jimmy W.; Sokolov, Alexei P.; Bocharova, Vera

doi:10.1021/acs.macromol.7b01217

Effect of Chain Rigidity on the Decoupling of Ion Motion from Segmental Relaxation in Polymerized Ionic Liquids: Ambient and Elevated Pressure Studies

Journal Article · Mon Aug 21 00:00:00 EDT 2017 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.7b01217· OSTI ID:1394356

^[1]; ^[2]; Fu, Yao ^[3]; ^[1]; Carroll, Bobby ^[2]; ^[4]; Novikov, Vladimir N. ^[2]; Kisliuk, Alexander M. ^[1]; ^[1]; ^[2]; Mays, Jimmy W. ^[5]; ^[6]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Univ. of Tennessee, Knoxville, TN (United States). Department of Chemistry
Univ. of Cincinnati, OH (United States). Department of Aerospace Engineering & Engineering Mechanics
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences and Computational Sciences & Engineering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Department of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Department of Chemistry and Department of Physics and Astronomy

Conductivity in polymer electrolytes has been generally discussed with the assumption that the segmental motions control charge transport. However, much less attention has been paid to the mechanism of ion conductivity where the motions of ions are less dependent (decoupled) on segmental dynamics. We present that this phenomenon is observed in ionic materials as they approach their glass transition temperature and becomes essential for design and development of highly conducting solid polymer electrolytes. In this paper, we study the effect of chain rigidity on the decoupling of ion transport from segmental motion in three polymerized ionic liquids (polyILs) containing the same cation–anion pair but differing in flexibility of the polymer backbones and side groups. Analysis of dielectric and rheology data reveals that decoupling is strong in vinyl-based rigid polymers while almost negligible in novel siloxane-based flexible polyILs. To explain this behavior, we investigated ion and chain dynamics at ambient and elevated pressure. Our results suggest that decoupling has a direct relationship to the frustration in chain packing and free volume. Finally, these conclusions are also supported by coarse-grained molecular dynamics simulations.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1394356

Alternate ID(s):: OSTI ID: 1408579

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 17 Vol. 50; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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