Nanopatterning of Electrode Surfaces as a Potential Route to Improve the Energy Density of Electric Double-Layer Capacitors: Insight from Molecular Simulations

Electrostatic double-layer capacitors (EDLCs) with room-temperature ionic liquids (RTILs) as electrolytes are among the most promising energy storage technologies. Utilizing atomistic molecular dynamics simulations, we demonstrate that the capacitance and energy density stored within the electric double layers (EDLs) formed at the electrode-RTIL electrolyte interface can be significantly improved by tuning the nanopatterning of the electrode surface. Significantly increased values and complex dependence of differential capacitance on applied potential were observed for surface patterns having dimensions similar to the ions' dimensions. Electrode surfaces patterned with rough edges promote ion separation in the EDL at lower potentials and therefore result in increased capacitance. The observed trends, which are not accounted for by the current basic EDL theories, provide a potentially new route for optimizing electrode structure for specific electrolytes.