Metallic porous nitride single crystals at two-centimeter scale delivering enhanced pseudocapacitance

Pseudocapacitors that originate from chemisorption contain redox active sites mainly composed of transition metal ions with unsaturated coordination in lattice on the electrode surface. The capacitance is generally dictated by the synergy of the porous microstructure, electronic conduction and active sites in the porous electrode. Here we grow metallic porous nitride single crystals at 2-cm scale to enhance pseudocapacitance through the combination of large surface area with porous microstructure, high conductivity with metallic states and ordered active sites with unsaturated coordination at twisted surfaces. We show the enhanced gravimetric and areal pseudocapacitance and excellent cycling stability both in acidic and alkaline electrolyte with porous MoN, Ta₅N₆ and TiN single crystals. The long-range ordering of active metal-nitrogen sites account for the fast redox reactions in chemisorption while the high conductivity together with porous microstructure facilitate the charge transfer and species diffusion in electrodes.