Electrochemical Performance of Ti3C2Tx MXenes During Structural Evolution

MXenes, with a high surface area, abundant active sites, and excellent ion transport properties, have demonstrated excellent electrochemical performance. However, systematic comparisons of the structural evolution process and electrochemical performance for MXene are lacking. In this study, multilayer MXene (M-Ti3C2Tx) was successfully fabricated by in situ etching. During the subsequent centrifugation process, the thicker and heavier multilayer sheets settled due to their faster sedimentation rate, while the lighter, surface-functionalized monolayer sheets remained colloidally stable in the supernatant due to solvation and electrostatic repulsion, thereby achieving separation and obtaining delaminated MXene (D-Ti3C2Tx). Structural analysis indicates that the removal of the aluminum layer synergizes with the exfoliation of the nanosheets, significantly increasing the interlayer spacing and making the sheet structure more pronounced, and the pore structure is more abundant. Especially, in three-electrode and two-electrode systems at an identical mass loading of 5 mg on carbon paper, D-Ti3C2Tx delivered a higher specific capacitance, more pronounced pseudocapacitive behavior, and a superior rate capability compared to Ti3AlC2 and M-Ti3C2Tx. Such excellent electrochemical performance of D-Ti3C2Tx is due to the shortened ion diffusion path in the delaminated structure, which enables rapid ion migration, an extremely large specific surface area, and a mesoporous structure that provides abundant active sites. This study underscores the significant potential of D-Ti3C2Tx in emerging energy storage systems and offers insights into guiding MAX phase synthesis during its preparation.