Two-dimensional (2D) layered transition metal carbides/nitrides, called MXenes, are attractive alternative electrode materials for electrochemical energy storage. Owing to their metallic electrical conductivity and low ion diffusion barrier, MXenes are promising anode materials for sodium-ion batteries (SIBs). Herein, we report on a new 2D carbonitride MXene, viz., Ti2C0.5N0.5Tx (Tx stands for surface terminations), and the only second carbonitride after Ti3CNTx so far. A new type of in situ HF (HCl/KF) etching condition was employed to synthesize multilayer Ti2C0.5N0.5Tx powders from Ti2AlC0.5N0.5. Spontaneous intercalation of tetramethylammonium followed by sonication in water allowed for large-scale delamination of this new titanium carbonitride into 2D sheets. Multilayer Ti2C0.5N0.5Tx powders showed higher specific capacities and larger electroactive surface area than those of Ti2CTx powders. Multilayer Ti2C0.5N0.5Tx powders show a specific capacity of 182 mAh g−1 at 20 mA g−1, the highest among all reported MXene electrodes as SIBs with excellent cycling stability. (Figure presented.).

MXene is investigated as an electrode material for different energy storage systems due to layered structures and metal-like electrical conductivity. Experimental results show MXenes possess excellent cycling performance as anode materials, especially at large current densities. However, the reversible capacity is relatively low, which is a significant barrier to meeting the demands of industrial applications. This work synthesizes N-doped graphene-like carbon (NGC) intercalated Ti₃C₂T_x (NGC-Ti₃C₂T_x) van der Waals heterostructure by an in situ method. The as-prepared NGC-Ti₃C₂T_x van der Waals heterostructure is employed as sodium-ion and lithium-ion battery electrodes. For sodium-ion batteries, a reversible specific capacity of 305 mAh g^-1 is achieved at a specific current of 20 mA g^-1, 2.3 times higher than that of Ti₃C₂T_x. For lithium-ion batteries, a reversible capacity of 400 mAh g^-1 at a specific current of 20 mA g^-1 is 1.5 times higher than that of Ti₃C₂T_x. Both sodium-ion and lithium-ion batteries made from NGC-Ti₃C₂T_x shows high cycling stability. The theoretical calculations also verify the remarkable improvement in battery capacity within the NGC-Ti₃C₂O₂ system, attributed to the additional adsorption of working ions at the edge states of NGC. This work offers an innovative way to synthesize a new van der Waals heterostructure and provides a new route to improve the electrochemical performance significantly.

Two-dimensional transition-metal carbides and nitrides "MXenes" have demonstrated great potential as electrode materials for electrochemical energy storage systems. This is especially true for delaminated Ti3C2Tx, which already shows outstanding gravimetric and volumetric capacitance, with areal capacitance limited by thickness (only a few microns). However, the performance of multilayer Ti3C2Txhas been more modest. Here, we report on using metal cation (viz., Na+, K+, and Mg2+) pre-intercalated multilayer Ti3C2Txas electrodes for aqueous supercapacitors. These electrodes are scalable and amenable to roll-to-roll manufacturing, with adjustable areal loadings of 5.2 to 20.1 mg/cm2. K-Ti3C2Txexhibited the highest capacitances at different scan rates. A gravimetric capacitance comparable to that of delaminated MXene of up to 300 F/g was achieved for multilayer K-Ti3C2Txbut with an outstanding ultra-high areal capacitance of up to 5.7 F/cm2, which is 10-fold higher than the 0.5 F/cm2of delaminated MXene and exceeds the 4.0 F/cm2of microengineered MXene electrodes.