Amine-Assisted Delaminated 2D Ti₃C₂T_x MXenes for High Specific Capacitance in Neutral Aqueous Electrolytes

Electrochemical capacitors using neutral aqueous electrolytes are safer and cheaper and allow diverse current collectors compared with the counterparts using organic or acidic/alkaline electrolytes. Two-dimensional (2D) MXenes have been demonstrated as the high-capacitive materials with high rate performance. However, MXene electrodes often exhibit a limited capacitance in neutral electrolytes, where the reversible electrochemical reactions rely greatly on the structural and surface properties of MXenes depending on their synthesis methods. Herein, a simple and highly efficient strategy, which combines HF etching of Ti3AlC2 powder and subsequent amine-assisted delamination at a low temperature, is developed to synthesize 2D Ti3C2Tx MXenes. The comprehensive results demonstrate that the enlarged interlayer spacing and the presence of more −O-containing functional groups synergistically contribute to the improvement of capacitive performance in neutral electrolytes. The 2D Ti3C2Tx MXenes show excellent electrochemical performance in various neutral electrolytes, and a high specific gravimetric capacitance of 149.8 F/g is achieved in 1.0 M Li2SO4. Furthermore, the flexible solid-state supercapacitors (SCs) with a neutral PVA/LiCl gel electrolyte possess a superior areal capacitance (163.1 mF/cm2) and high energy density (17.6 μWh/cm2 at 0.07 mW/cm2), together with high user safety. This work provides a promising guideline of synthesis strategy for high-capacitive MXenes used in neutral electrolytes, which may promote the development of safe and flexible power sources with a high energy density.