Design and Formulation of Engineered 2D Nb2CTx MXene for Ultra-Stable NH4+ Aqueous Hybrid Supercapacitors

Two-dimensional (2D) transition metal carbides/nitrides (MXenes), which possess layered structures with excellent electrical conductivity, are auspicious materials for energy storage applications. The presence of van der Waals interactions between Nb2CTx MXene nanosheets tends to induce self-stacking, which reduces the accessible surface area and the number of electrochemically active sites. This structural limitation adversely affects cycling stability and specific capacitance when employed in supercapacitor applications. Herein, nitrogen (N)-functionalized Nb2CTx MXene (N-Nb2CTx) materials were optimized by annealing Nb2CTx in an ammonia (NH3) atmosphere at different temperatures (denoted as N-Nb2CTx-300 °C, N-Nb2CTx-400 °C, and N-Nb2CTx-500 °C). Based on the experimental results in the three-electrode system, it was found that N-Nb2CTx-400 °C exhibited the most favorable electrochemical performance, attributed to effective nitrogen doping and enhanced structural stability. Annealing at 400 °C helps nitrogen atoms to be more evenly doped into the lattice of Nb2CTx, thereby increasing the material’s surface area and porosity while minimizing significant structural agglomeration and partial decomposition or oxidation. N-Nb2CTx-400 °C shows a specific capacitance of 382 F/g at 1 A/g, retaining 140 F/g at a current density of 20 A/g in ammonium sulfate ((NH4)2SO4) electrolyte. Assembled NH4+ ion hybrid supercapacitors (AHSCs) exhibit a specific energy density of 23.36 Wh/kg at a power density of 900 W/kg. Through density functional theory (DFT) calculations, it is revealed that N-Nb2CTx MXene exhibits superior thermodynamic and diffusion properties toward SO42– and NH4+ ions, providing theoretical guidance for the design and development of high-performance electrode materials for energy storage devices.