Theoretical Insights into the Structures and Capacitive Performances of Confined Ionic Liquids

Room-temperature ionic liquids (RTILs) together with nano-porous electrodes are the most promising materials for supercapacitors and batteries. Many theoretical works have addressed the structures and performances of RTILs inside nanopores. However, only limited attention has been given to how the dispersion forces of RTILs influence the behavior of ions inside the slit pores. Toward this aim, we investigate the effects of various dispersion forces between ions on the macroscopic structures in nanoconfinement and the capacitance performance of supercapacitors by the classical density functional theory (CDFT). The results show that the dispersion force can significantly change the mechanism of the charging process and even the shape of differential capacitance curves. In addition, the voltage-dependent structures of RTILs with appropriate dispersion force appears in a given silt pore, which leads to extremely high capacitance and enhances the energy storage density. We hope that this work could further offer guidance for the optimizing of electrolytes for electrical double layer capacitors, like tuning the dispersion force between ions by adding/removing certain chemical groups on the cations and anions of RTILs.