Removing Fluoride-Terminations from Multilayered V₂C<i>T</i>_<i>x</i> MXene by Gas Hydrolyzation

Abstract

Two-dimensional MXenes have shown great promise for many different applications, but in order to fully utilize their potential, control of their termination groups is essential. Here we demonstrate hydrolyzation with a continuous gas flow as a method to remove F-terminations from multilayered V₂C<i>T</i> _<i>x</i> particles, in order to prepare nearly F-free and partly bare vanadium carbide MXene. Density functional theory calculations demonstrate that the substitution of F-terminations is thermodynamically feasible and presents partly nonterminated V₂CO as the dominating hydrolyzation product. Hydrolyzation at elevated temperatures reduced the F content but only subtly changed the O content, as inferred from spectroscopic data. The ideal hydrolyzation temperature was found to be 300 °C, as a degradation of the V₂C<i>T</i> _<i>x</i> phase and a transition to vanadium oxycarbides and V₂O₃ were observed at higher temperature. When tested as electrodes in Li-ion batteries, the hydrolyzed MXene demonstrated a reduced polarization compared with the pristine MXene, but no change in intercalation voltage was observed. Annealing in dry Ar did not result in the same F reduction, and the importance of water vapor was concluded, demonstrating hydrolyzation as a new and efficient method to control the surface terminations of multilayered V₂C<i>T</i> _<i>x</i> post etching. These results also provide new insights on the thermal stability of V₂C<i>T</i> _<i>x</i> MXene in hydrated atmospheres.