On the thickness of the double layer in ionic liquids†
In this study, we examined the thickness of the electrical double layer (EDL) in ionic liquids using density functional theory (DFT) calculations and molecular dynamics (MD) simulations. We focused on BF4− anion adsorption from the 1-ethyl-3-methylimidazolium tetrafluoroborate (EMImBF4) ionic liquid on the Au(111) surface. At both DFT and MD levels, we evaluated the capacitance–potential dependence for the Helmholtz model of the interface. Using MD simulations, we also explored a more realistic, multilayer EDL model accounting for the ion layering. Concurrent analysis of the DFT and MD results provides a ground for thinking whether the electrical double layer in ionic liquids is one- or multi-ionic-layer thick.