@article{35916,
  author = {Kara D Fong and Julian Self and Bryan D McCloskey and Kristin A Persson},
  title = {Ion Correlations and Their Impact on Transport in Polymer-Based Electrolytes},
  abstract = {<p><span>The development of next-generation polymer-based electrolytes for energy storage applications would greatly benefit from a deeper understanding of transport phenomena in these systems. In this Perspective, we argue that the Onsager transport equations provide an intuitive but underutilized framework for analyzing transport in polymer-based electrolytes. Unlike the ubiquitous Stefan{\textendash}Maxwell equations, the Onsager framework generates transport coefficients with clear physical interpretation at the atomistic level and can be computed easily from molecular simulations using Green{\textendash}Kubo relations. Herein we present an overview of the Onsager transport theory as it applies to polymer-based electrolytes and discuss its relation to experimentally measurable transport properties and the Stefan{\textendash}Maxwell equations. Using case studies from recent computational work, we demonstrate how this framework can clarify nonintuitive phenomena such as negative cation transference number, anticorrelated cation{\textendash}anion motion, and the dramatic failure of the Nernst{\textendash}Einstein approximation. We discuss how insights from such analysis can inform design rules for improved systems.</span></p>},
  year = {2021},
  booktitle = {Macromolecules},
  journal = {Macromolecules},
  series = {Macromolecules},
  volume = {54},
  pages = {2575 - 2591},
  month = {02/2021},
  issn = {0024-9297},
  url = {https://pubs.acs.org/doi/10.1021/acs.macromol.0c02545},
  doi = {10.1021/acs.macromol.0c02545},
  language = {eng},
}