Applying Hydrogenation to Stabilize N-TiO2 and Enhance Its Visible Light Photocatalytic Activity

Abstract

Up to now, the explanation for the origin of enhanced photocatalytic activity of N doped TiO2 (N-TiO2) with H incorporation, which is observed in experiment, is still lacking. In our work, the effects of hydrogenation on the stability and electronic properties of N-TiO2 have been systematically investigated by first-principles calculations. Our results of the study on stability demonstrate that, both full and part hydrogenation could stabilize N-TiO2 by largely reducing the formation energy of N doping under Ti-rich conditions. Moreover, the calculated results on the electronic structure show that, for the completely hydrogenated N-TiO2, band gap becomes slightly larger, which is caused by the full passivation for unpaired electron from N atom. However, for the partially hydrogenated N-TiO2, due to the interaction between hydrogenated and unhydrogenated N atoms, its valence band maximum shifts to higher energy by 0.32 eV and the valence band states mix with the wide band-gap states, which results in a higher light absorption capacity and carrier separation. Our results not only explain the enhancement of visible light photocatalytic activity experimentally found in N-TiO2 specimen with H incorporation, but also indicate that, tuning the hydrogenation degree is a hopeful routine to improve the photocatalytic performance of N-TiO2.