Molecular Insight into the Effects of Clustering on the Dynamics of Ionomers in Solutions

Mohottalalage, Supun S.; Kosgallana, Chathurika; Senanayake, Manjula; Wijesinghe, Sidath; Osti, Naresh C.; Perahia, Dvora

doi:10.1021/acsmacrolett.3c00353

Title: Molecular Insight into the Effects of Clustering on the Dynamics of Ionomers in Solutions

Journal Article · Wed Jul 26 00:00:00 EDT 2023 · ACS Macro Letters

DOI:https://doi.org/10.1021/acsmacrolett.3c00353· OSTI ID:2301677

Mohottalalage, Supun S. ^[1]; Kosgallana, Chathurika ^[1]; Senanayake, Manjula ^[2]; Wijesinghe, Sidath ^[3];

^[4];

^[1]

Clemson Univ., SC (United States)
Clemson Univ., SC (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Clemson Univ., SC (United States); Appalachian State University, Boone, NC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Ionizable groups tethered to polymers enable their many current and potential applications. However, these functionalities drive the formation of physical networks through clustering of the ionic groups, resulting in constrained dynamics of the macromolecules. Understanding the molecular origin of this hindrance remains a critical fundamental question, whose solution will directly impact the processing of ionizable polymers from molecules to viable materials. Here, in this work, using quasielastic neutron scattering accompanied by molecular dynamics simulations, segmental dynamics of slightly sulfonated polystyrene is studied in solutions as the cohesion of the ionic assemblies is tuned. We find that in cyclohexane the ionic assemblies act as centers of confinement, affecting dynamics both on macroscopic lengths and in the vicinity of the ionic assemblies. Addition of a small amount of ethanol affects the packing of the ionizable groups within the assemblies, which in turn enhances the chain dynamics.

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Research Organization:: Clemson Univ., SC (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

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

Contributing Organization:: Oak Ridge National Laboratory (ORNL)

Grant/Contract Number:: SC0019284; AC05-00OR22725; AC02-05CH11231; 89233218CNA000001; SC001984; NA0003525

OSTI ID:: 2301677

Alternate ID(s):: OSTI ID: 1993664

Journal Information:: ACS Macro Letters, Vol. 12, Issue 8; ISSN 2161-1653

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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