Abstract
Bottom-up understanding of transport describes how molecular changes alter species concentrations and electrolyte voltage drops in operating batteries. Such an understanding is essential to predictively design electrolytes for desired transport behavior. We herein advocate building a structure-property-performance relationship as a systematic approach to accurate bottom-up understanding. To ensure generalization across salt concentrations as well as different electrolyte types and cell configurations, the property-performance relation must be described using Newman's concentrated solution theory. It uses Stefan-Maxwell diffusivity, ij, to describe the role of molecular motions at the continuum scale. The key challenge is to connect ij to the structure. We discuss existing methods for making such a connection, their peculiarities, and future directions to advance our understanding of electrolyte transport.
| Original language | English |
|---|---|
| Pages (from-to) | 880-890 |
| Number of pages | 11 |
| Journal | ACS Central Science |
| Volume | 8 |
| Issue number | 7 |
| DOIs | |
| State | Published - Jul 27 2022 |
| Externally published | Yes |
Funding
This work was supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES). The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan, http://energy.gov/downloads/doe-public-access-plan . A.M., B.L.P., and V.S. appreciate discussions with Dean Wheeler about his approach to calculating the Stefan–Maxwell diffusivities from Molecular Dynamics calculations.