Tunable energy storage capacity of two-dimensional Ti3C2Tx modified by a facile two-step pillaring strategy for high performance supercapacitor electrodes

Abstract

This paper proposed to tailor the layer microstructures of two-dimensional Ti₃C₂T_xvia a facile Li⁺ pre-pillaring and successive pillaring strategy by various cations. By ion exchange with pre-intercalated Li⁺, as well as “coulombic attraction” to electronegative Ti₃C₂T_x, various inexpensive and column-like K⁺, Ca²⁺, Mg²⁺, Al³⁺ and NH₄⁺ cations were migrated into the Ti₃C₂T_x interlayers. By expanding the interlayer about 17.02%, as well as enhancing the electron density of Ti atoms and C atoms, the Al³⁺ intercalated MXene Ti₃C₂T_x sheets delivered the highest specific capacity of 175 F g⁻¹ at 0.3 A g⁻¹. Coupling the Ti₃C₂T_x-Al³⁺ working electrode with a platinum counter electrode and a Hg/HgO reference electrode, the single electrode (calculated from a three-electrode system) exhibited a high energy density of 87.5 W h kg⁻¹ and a high power density (2100 W kg⁻¹) with an ultra-long and stable cycling performance. The binding energies of the intercalated ions with hydroxyl groups, the Bader charge distribution and degree of electron localization were evaluated by density functional theory calculations to further validate the ultra-high energy storage capacity of Al³⁺ pillared-Ti₃C₂T_x in the present study.