where is the distance from the electrode surface to the bulk electrolyte. This method has been proven to be applicable on solid/liquid interfaces . The simulations allow also for the introduced during the transfer process. Both phenomena have been found to strongly influence the electrowetting response . Furthermore, the electronic interactions between the graphene overlayer and the substrate are expected to affect the wetting response. Such phenomena have not been considered in our calculations and therefore a direct comparison would be rather ambiguous . On this basis, though we recognize that the wetting behavior of the two pristine surfaces (i.e., defect-free, uncontaminated, free-standing graphene and highly oriented graphite) can differ, we believe that our approach can effectively provide significant insights into the wetting behavior of carbon surfaces under external potential bias by linking theory and experiments. In this respect, we envisage that the reported data and approaches assist the development of models that encompass the complete physics of the carbon/aqueous electrolytes interface. Finally, we further note that in order to minimize the experimental uncertainties often appear in electrowetting experiments when using the traditional liquid/air configuration (related mainly to the environmental effects, i.e., airborne contaminations, electrolyte evaporation and the necessary use of a micropipette to establish an electrolytic contact between the drop and the substrate ), we adopted the pioneering liquid/liquid configuration introduced by Frumkin , where an electrolytically inactive solvent is used in combination with the electrolyte of interest (refer to the next section for a detailed description of the mechanism of the process).