Quantifying Single-Ion Transport in Percolated Ionic Aggregates of Polymer Melts

Bollinger, Jonathan A.; Stevens, Mark J.; Frischknecht, Amalie L.

doi:10.1021/acsmacrolett.0c00139

Quantifying Single-Ion Transport in Percolated Ionic Aggregates of Polymer Melts

Journal Article · Thu Apr 02 00:00:00 EDT 2020 · ACS Macro Letters

DOI:https://doi.org/10.1021/acsmacrolett.0c00139· OSTI ID:1614784

Bollinger, Jonathan A. ^[1]; Stevens, Mark J. ^[1]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Single-ion conducting polymers such as ionomers are promising battery electrolyte materials, but it is critical to understand how rates and mechanisms of free cation transport depend on the nanoscale aggregation of cations and polymer-bound anions. We perform coarse-grained molecular dynamics simulations of ionomer melts to understand cation mobility as a function of polymer architecture, background relative permittivity, and corresponding ionic aggregate morphology. In systems exhibiting percolated ionic aggregates, cations diffuse via stepping motions along the ionic aggregates. These diffusivities can be quantitatively predicted by calculating the lifetimes of continuous association between oppositely charged ions, which equal the time scales of the stepping (diffusive) motions. In contrast, predicting cation diffusivity for systems with isolated ionic aggregates requires another time scale. Finally, our results suggest that to improve conductivity the Coulombic interaction strength should be strong enough to favor percolated aggregates but weak enough to facilitate ion dissociation.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

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

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1614784

Report Number(s):: SAND--2020-3838J; 685182

Journal Information:: ACS Macro Letters, Journal Name: ACS Macro Letters Journal Issue: 4 Vol. 9; ISSN 2161-1653

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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