Journal
NEW JOURNAL OF CHEMISTRY
Volume 32, Issue 6, Pages 1038-1047Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/b719498f
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N-doped TiO2 (anatase) with high visible light photoactivity was obtained by the thermal treatment of nanotube titanic acid (denoted as NTA) in an NH3 flow and investigated by means of X-ray diffraction (XRD), transmission electronic microscopy (TEM), diffuse reflectance spectra (DRS), X-ray photoelectron spectroscopy (XPS), electron spin resonance (ESR), and photoluminescence (PL). With increasing NH3 treatment temperature at T = 400 to 600 degrees C, the anatase crystallinity of the N-NTA(400-600) samples was gradually enhanced, while at 700 degrees C a new phase, TiN, appeared in the N-NTA(700) sample. XPS results show that the doped N atoms incorporated into anatase TiO2 exist in the form of NO. A revised explanation for the triplet ESR signals obtained from the N-NTA(500-700) samples was put forward, i.e. the g = 2.004 main peak is contributed by single-electron-trapped oxygen vacancies (denoted as V-o(center dot)), while two weak peaks (g = 2.023, 1.987) are contributed by chemisorbed NO in well-crystallized anatase TiO2. The visible light photoactivity is proportional to the height of the g = 2.004 main peak, which suggests that the photoactive centers are V-o(center dot)-NO-Ti. The adsorbed NO molecule can effectively suppress the photoluminescence of V-o(center dot) defects, which facilitates photogenerated charge transfer to the surface reactive centers to conduct redox reactions. The higher the V-o(center dot)-NO-Ti concentration, the better the visible light photoactivity. The highest photoactivity was obtained for the catalyst, NH3-treated at 600 degrees C. But the formation of TiN at T = 700 degrees C can readily destruct V-o(center dot)-NO-Ti photoactive centers, and thus readily decreases photoactivity effciency.
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