Thickness-Independent Capacitive Performance of Holey Ti3C2Tx Film Prepared through a Mild Oxidation Strategy

The Ti3C2Tx film with metallic conductivity and high pseudo-capacitance holds profound promise in flexible high-rate supercapacitors. However, the restacking of Ti3C2Tx sheets hinders ion access to thick film electrodes. Herein, a mild yet green route has been developed to partially oxidize Ti3C2Tx to TiO2/Ti3C2Tx by introducing O-2 molecules during refluxing the Ti3C2Tx suspension. The subsequent etching away of these TiO2 nanoparticles by HF leaves behind numerous in-plane nanopores on the Ti3C2Tx sheets. Electrochemical impedance spectroscopy shows that longer oxidation time of 40 min yields holey Ti3C2Tx (H-Ti3C2Tx) with a much shorter relax time constant of 0.85 s at electrode thickness of 25 mu m, which is 89 times smaller than that of the pristineTi(3)C(2)T(x) film (75.58 s). Meanwhile, H-Ti3C2Tx film with 25 min oxidation exhibits less-dependent capacitive performance in film thickness range of 10-84 mu m (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 Ti3C2Tx film. The method reported herein would pave way for fabricating porous MXene materials toward high-rate flexible supercapacitor applications.

Automated summary

A mild and green method has been developed to partially oxidize Ti3C2Tx, resulting in holey Ti3C2Tx (H-Ti3C2Tx) films with shorter relax time and less thickness dependence. The in-plane nanopores in the film not only provide more electrochemically active sites but also allow for rapid ion impregnation.