(Invited) Molecular Modeling of Lithium and Zinc Electrolytes

Abstract

In this presentation I will update on the recent progress towards obtaining fundamental understanding and improving three classes of electrolytes: 1) aqueous and hybrid electrolytes for lithium ion batteries including superconcentrated electrolytes; 2) non-aqueous electrolytes and their interaction with the electrodes for high energy density lithium ion batteries; 3) electrolytes for zinc metal batteries.Accurate molecular dynamics (MD) simulations of these electrolytes using many-body polarizable force field will be used to establish a correlation between the ion transport mechanisms, electrolyte structure and transference number. Reactive modeling will focus on the competitive solvent and salt reduction at the passivated electrochemical interfaces using Born Oppenheimer Molecular Dynamics (BOMD) simulations using DFT functionals. These BOMD simulations included critical factors needed to realistically represent electrolyte reactivity at electrodes such as explicit description of the substrate – electrolyte interactions; accurate representation of electrolyte structure, ion pairing and aggregation near an electrode; and collection of sufficient statistics from multiple unique simulations that were initiated with differing initial configurations. Electrolyte reduction at the passivated interfaces from these simulations will be contrasted with other solvents ranging from ethers with mixed salts or carbonates and results from the representative quantum chemistry (QC) calculations performed on the small model electrolyte clusters to estimate oxidation and reduction.