Thickness-Independent Capacitive Performance of Holey Ti₃C₂T_x Film Prepared through a Mild Oxidation Strategy

Abstract

The Ti₃C₂T_x film with metallic conductivity and high pseudo-capacitance holds profound promise in flexible high-rate supercapacitors. However, the restacking of Ti₃C₂T_x sheets hinders ion access to thick film electrodes. Herein, a mild yet green route has been developed to partially oxidize Ti₃C₂T_x to TiO₂/Ti₃C₂T_x by introducing O₂ molecules during refluxing the Ti₃C₂T_x suspension. The subsequent etching away of these TiO₂ nanoparticles by HF leaves behind numerous in-plane nanopores on the Ti₃C₂T_x sheets. Electrochemical impedance spectroscopy shows that longer oxidation time of 40 min yields holey Ti₃C₂T_x (H-Ti₃C₂T_x) with a much shorter relax time constant of 0.85 s at electrode thickness of 25 µm, which is 89 times smaller than that of the pristineTi₃C₂T_x film (75.58 s). Meanwhile, H-Ti₃C₂T_x film with 25 min oxidation exhibits less-dependent capacitive performance in film thickness range of 10–84 µm (1.63–6.41 mg cm⁻²) and maintains around 60% capacitance as the current density increases from 1 to 50 A g⁻¹. The findings clearly demonstrate that in-plane nanopores not only provide more electrochemically active sites, but also offer numerous pathways for rapid ion impregnation across the thick Ti₃C₂T_x film. The method reported herein would pave way for fabricating porous MXene materials toward high-rate flexible supercapacitor applications.