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A computational chemistry approach to modelling conducting polymers in ionic liquids for next generation batteries

A computational chemistry approach to modelling conducting polymers in ionic liquids for next generation batteries
A computational chemistry approach to modelling conducting polymers in ionic liquids for next generation batteries
An overview of modern quantum chemical methods is presented followed by a discussion of their application in the field of conducting organic polymers (COPs), with a view towards modelling the cathodic half-cell of a poly(3,4-ethylenedioxythiophene) (PEDOT) cathode in an AlCl3-1-ethyl-3-methylimidazolium chloride (EMImCl) ionic liquid electrolyte. The most popular combination of hybrid DFT functional and polarized moderate basis set has been broadly and successfully applied to COPs in the literature. However, in the presence of anions and intermolecular interactions, diffuse functions and dispersion corrections must also be included. A comprehensive specification of these elements appears well suited to the determination of many relevant parameters including molecular geometry, bandgap of oligomers and energies for systems including multiple chains and chloroaluminate anions. However, range-separated hybrid functionals may be more suitable for determining electron transport properties of very long chains. The clearest benefit of DFT to this system is the ability to visualize charge distribution and the interaction between charged PEDOT and the active species, which will help to explain the specific capacity, voltage and charge/discharge characteristics — insights that may help identify further improvements.
DFT, PEDOT, aluminium, computational chemistry, density functional theory
2352-4847
198-208
Craig, Benjamin
d616e0d5-d164-46e5-9f2d-ee768a2c7674
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Schoetz, Theresa
cf930a0a-087e-4be0-ac2b-614abcc3f424
Ponce De Leon Albarran, Carlos
508a312e-75ff-4bcb-9151-dacc424d755c
Craig, Benjamin
d616e0d5-d164-46e5-9f2d-ee768a2c7674
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Schoetz, Theresa
cf930a0a-087e-4be0-ac2b-614abcc3f424
Ponce De Leon Albarran, Carlos
508a312e-75ff-4bcb-9151-dacc424d755c

Craig, Benjamin, Skylaris, Chris-Kriton, Schoetz, Theresa and Ponce De Leon Albarran, Carlos (2020) A computational chemistry approach to modelling conducting polymers in ionic liquids for next generation batteries. Energy Reports, 6 (5), 198-208. (doi:10.1016/j.egyr.2020.03.025).

Record type: Article

Abstract

An overview of modern quantum chemical methods is presented followed by a discussion of their application in the field of conducting organic polymers (COPs), with a view towards modelling the cathodic half-cell of a poly(3,4-ethylenedioxythiophene) (PEDOT) cathode in an AlCl3-1-ethyl-3-methylimidazolium chloride (EMImCl) ionic liquid electrolyte. The most popular combination of hybrid DFT functional and polarized moderate basis set has been broadly and successfully applied to COPs in the literature. However, in the presence of anions and intermolecular interactions, diffuse functions and dispersion corrections must also be included. A comprehensive specification of these elements appears well suited to the determination of many relevant parameters including molecular geometry, bandgap of oligomers and energies for systems including multiple chains and chloroaluminate anions. However, range-separated hybrid functionals may be more suitable for determining electron transport properties of very long chains. The clearest benefit of DFT to this system is the ability to visualize charge distribution and the interaction between charged PEDOT and the active species, which will help to explain the specific capacity, voltage and charge/discharge characteristics — insights that may help identify further improvements.

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Accepted/In Press date: 22 March 2020
e-pub ahead of print date: 21 May 2020
Published date: May 2020
Additional Information: 4th Annual CDT Conference in Energy Storage and Its Applications, Professor Andrew Cruden, 2019, 07-19, University of Southampton, U.K.
Keywords: DFT, PEDOT, aluminium, computational chemistry, density functional theory

Identifiers

Local EPrints ID: 443463
URI: http://eprints.soton.ac.uk/id/eprint/443463
ISSN: 2352-4847
PURE UUID: 4225642a-a801-4fa5-88a6-2bc27a2d4612
ORCID for Chris-Kriton Skylaris: ORCID iD orcid.org/0000-0003-0258-3433
ORCID for Carlos Ponce De Leon Albarran: ORCID iD orcid.org/0000-0002-1907-5913

Catalogue record

Date deposited: 26 Aug 2020 16:35
Last modified: 18 Feb 2021 17:07

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