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We theoretically study electrostatic properties of electric double layerusing a generalized Poisson-Boltzmann approach taking into account theorientational ordering of water dipoles and the excluded volume effect of watermolecules as well as those of positive and negative ions with different sizesin electrolyte solution. Our approach enables one to predict that the numberdensities of water molecules, counterions and coions and the permittivity ofelectrolyte solution close to a charged surface, asymmetrically vary dependingon both of sign and magnitude of the surface charge density and the volume ofcounterion. We treat several phenomena in more detail. Firstly, an increase inthe volume of counterions and an increase in the surface charge density cancause the position of the minimum number density of water molecules to befarther from the charged surface. Secondly, width of the range of voltage inwhich the properties at the charged surface symmetrically vary decreases withincreasing bulk salt concentration. In addition, we show that the excludedvolume effect of water molecules and the orientational ordering of waterdipoles can lead to early onset and lowering of the maximum of electriccapacitance according to surface voltage. Our approach and results can beapplied to describing electrostatic properties of biological membranes andelectric double layer capacitor for which excluded volume effects of watermolecules and ions with different sizes may be important.

electrochimica acta

Asymmetric electrostatic properties of an electric double layer: a  generalized Poisson-Boltzmann approach taking into account non-uniform size  effects and water polarization