Highly Enhanced Photoactivity of Anatase TiO2 Nanocrystals by Controlled Hydrogenation-Induced Surface Defects

Anatase TiO2 nanocrystals (aTiO(2)) of a uniform size have been synthesized and were subject to a successive hydrogenation under a H-2 gas flow at elevated temperatures (500-700 degrees C). We found that the concentration of Ti3+ defects, such as Ti3+ interstitials and oxygen vacancies, and their distribution between surface and bulk varied significantly, depending on the hydrogenation temperature and time. Such changes in defects were found to be critical in enhancing the photoactivity of the hydrogenated TiO2 (H-aTiO(2)) by an order of magnitude. In our case, H-aTiO(2) nanocrystals hydrogenated at 600 degrees C for longer than 10 h showed 10 times higher photoactivity than aTiO(2), which was explained from a high surface-to-bulk defect ratio and a nonuniform distribution of defects between bulk and surface due to a preferential diffusion of bulk defects to the surface. Our study showed that a kinetically controlled hydrogenation condition could be used not only to control the surface/bulk defects but also to enhance the photoactivity of oxide nanocrystals.