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Synthesis of Ionic Liquid Based Electrolytes, Assembly of Li-ion Batteries, and Measurements of Performance at High Temperature

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Published on: December 20, 2016

Structural transitions at electrodes, immersed in simple ionic liquid models.

Hongduo Lu¹, Samuel Stenberg, Clifford E Woodward

¹Theoretical Chemistry, Chemical Centre, P.O. Box 124, S-221 00 Lund, Sweden. jan.forsman@teokem.lu.se.

|March 4, 2021

Summary

This summary is machine-generated.

Density Functional Theory (DFT) reveals ionic fluid phase transitions near electrodes. Cation-anion competition at charged surfaces leads to demixing, impacting electrochemical behavior and capacitance.

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Area of Science:

Physical Chemistry
Computational Chemistry
Materials Science

Background:

Ionic fluids near charged interfaces exhibit complex behaviors.
Surface polarization effects significantly influence ion distribution.
Understanding these interactions is crucial for electrochemical applications.

Purpose of the Study:

To investigate the structures, phase transitions, and electrochemical properties of coarse-grained ionic fluid models.
To analyze the role of surface polarization and ion correlations in interfacial phenomena.
To explore the impact of different Density Functional Theory (DFT) approximations.

Main Methods:

Utilized a classical Density Functional Theory (DFT) method.
Studied two coarse-grained ionic fluid models with a model electrode.
Incorporated screened image interactions to model surface polarization.

Main Results:

Observed cation-anion competition at positively charged electrodes, leading to demixing into distinct phases.
Demonstrated that phases exhibit different structures and surface charge densities at the same potential.
Found that neglecting ion correlations in mean-field DFT eliminates phase transitions but shows capacitance drops.

Conclusions:

DFT provides insights into ionic fluid interfacial behavior, including phase transitions and demixing.
Surface polarization plays a key role in attracting cations and driving demixing.
Findings are relevant for understanding ionic liquids with asymmetric ions and charge distributions.