Structure and mechanisms underlying ion transport in ternary polymer electrolytes containing ionic liquids

Abstract

We use all atom molecular dynamics simulations to investigate the influence of 1-butyl-3-methylimidazolium hexafluorophosphate (BMIMPF6) ionic liquid on the structure and transport properties of poly(ethylene oxide) (PEO) polymer electrolytes doped with LiPF6 salt. We observe enhanced diffusivities of the Li+, PF6−, and BMIM+ ions with increasing loading of the ionic liquid. Interplay between the different ion-ion and ion-polymer interactions is seen to lead to a destabilization of the Li–PF6 coordination and increase in the strength of association between the Li+ cations and the polymer backbone. As a consequence, the polymer segmental relaxation times are shown to be only moderately affected by the addition of ionic liquids. The ionic-liquid induced changes in the mobilities of Li+ ions are seen to be correlated to polymer segmental relaxation times. However, the mobilities of BMIM+ ions are seen to be more strongly correlated to the BMIM–PF6 ion-pair relaxation times.

Document Details

Document Type
Pub Defense Publication
Publication Date
Feb 17, 2017
Source ID
10.1063/1.4976131

Entities

People

  • Santosh Mogurampelly
  • Venkat Ganesan

Organizations

  • Army Research Office
  • National Science Foundation
  • Robert A. Welch Foundation
  • University of Texas at Austin

Tags

Fields of Study

  • Materials science

Readers

  • Materials Science and Engineering.
  • Polymer Science and Engineering.
  • Quantum Chemistry