TY - JOUR
T1 - A computational chemistry approach to modelling conducting polymers in ionic liquids for next generation batteries
AU - Craig, Ben
AU - Skylaris, Chris Kriton
AU - Schoetz, Theresa
AU - de León, Carlos Ponce
N1 - Publisher Copyright:
© 2020
PY - 2020/5
Y1 - 2020/5
N2 - 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.
AB - 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.
KW - Aluminium
KW - Computational chemistry
KW - Density Functional Theory
KW - DFT
KW - PEDOT
UR - http://www.scopus.com/inward/record.url?scp=85084943225&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85084943225&partnerID=8YFLogxK
U2 - 10.1016/j.egyr.2020.03.025
DO - 10.1016/j.egyr.2020.03.025
M3 - Article
AN - SCOPUS:85084943225
SN - 2352-4847
VL - 6
SP - 198
EP - 208
JO - Energy Reports
JF - Energy Reports
ER -