Ion Transport in Organic Electrolyte Solutions for Lithium-ion Batteries and Beyond

Abstract

The performance of metal-ion batteries at low temperatures and their fast charge/discharge rates are determined mainly by the electrolyte (ion) transport. Accurate transport properties must be evaluated for designing and/or optimization of lithium-ion and other metal-ion batteries. In this review, we report and discuss experimental and atomistic computational studies on ion transport, in particular, ion diffusion/dynamics, transference number, and ionic conductivity. Although a large number of studies focusing on lithium-ion transport in organic liquids have been performed, only a few experimental studies have been conducted in the organic liquid electrolyte phase for other alkali metals that are used in batteries (such as sodium, potassium, magnesium, etc.). Atomistic computer simulations can play a primary role and predict ion transport in organic liquids. However, to date, atomistic force fields and models have not been explored and developed exhaustively to simulate such organic liquids in quantitative agreement to experimental measurements.

Data-Driven Analysis of High-Throughput Experiments on Liquid Battery Electrolyte Formulations: Unraveling the Impact of Composition on Conductivity

“…Organic solvent-based electrolyte formulations are of central relevance and still considered as state-of-the-art. 14,15 Common electrolyte formulations consist of lithium conducting salt such as lithium hexafluorophosphate (LiPF6) and solvent mixtures comprising cyclic carbonates like ethylene carbonate (EC) and propylene carbonate (PC) with linear organic carbonates like dimethyl carbonate (DMC), ethyl methyl carbonate (EMC) and diethyl carbonate (DEC) and provide desirable electrochemical properties for Li-ion batteries. [16][17][18][19][20][21] Here we perform HT impedance spectroscopic experiments on LiPF6-based electrolyte formulations containing EC and EMC as solvent mixture and vinylene carbonate (VC) as functional additive/co-solvent to determine ionic conductivities of resulting electrolyte formulations and develop a data driven model to predict ionic conductivities for variable electrolyte compositions.…”

Data‐Driven Analysis of High‐Throughput Experiments on Liquid Battery Electrolyte Formulations: Unraveling the Impact of Composition on Conductivity**

“…Organic solvent-based electrolyte formulations are of central relevance and still considered as state-of-the-art. [26,27] Common electrolyte formulations consist of lithium conducting salt such as lithium hexafluorophosphate (LiPF 6 ) and solvent mixtures comprising cyclic carbonates like ethylene carbonate (EC) and propylene carbonate (PC) with linear organic carbonates like dimethyl carbonate (DMC), ethyl methyl carbonate (EMC) and diethyl carbonate (DEC) and provide desirable electrochemical properties for Li-ion batteries. [28][29][30][31][32][33]…”

Extension of the TraPPE Force Field for Battery Electrolyte Solvents

“…Commonly used methods to investigate the structure of the electrolyte and interactions of dissolved salt ions with solvent molecules include neutron diffraction measurements, , nuclear magnetic resonance (NMR), − and vibrational spectroscopies (infrared (IR) spectroscopy and Raman scattering) ,,,,, as well as computational methods: quantum chemical calculations , and molecular dynamics (MD) simulations. − …”