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When an ionic liquid adsorbs onto a porous electrode, its ionic arrangementis deeply modified due to a screening of the Coulombic interactions by themetallic surface and by the confinement imposed upon it by the electrode'smorphology. In particular, ions of the same charge can approach at closecontact, leading to the formation of a superionic state. The impact of anelectrified surface placed between two liquid phases is much less understood.Here we simulate a full supercapacitor made of the 1-butyl-3-methylimidazoliumhexafluorophosphate and nanoporous graphene electrodes, with varying distancesbetween the graphene sheets. The electrodes are held at constant potential byallowing the carbon charges to fluctuate. Under strong confinement conditions,we show that ions of the same charge tend to adsorb in front of each otheracross the graphene plane. These correlations are allowed by the formation of ahighly localized image charge on the carbon atoms between the ions. They aresuppressed in larger pores, when the liquid adopts a bilayer structure betweenthe graphene sheets. These effects are qualitatively similar to the recenttemplating effects which have been reported during the growth of nanocrystalson a graphene substrate.

Ion-ion correlations across and between electrified graphene layers