Characterization and Photocatalytic Activity of N/TiO₂ Prepared by a Mechanochemica1 Method Using Various Nitrogenous Compounds

Abstract:

Nitrogen doped TiO₂ (N/TiO₂) photocatalysts were prepared using a mechanochemica1 method with raw amorphous TiO₂ as precursors and various nitrogenous compounds doses (NH₄F, NH₄HCO₃, NH₃·H₂O, NH₄COOCH₃, and CH₄N₂O). The photocatalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV-Vis diffuse reflection spectra (UV-Vis-DRS). Their photocatalytical activities were evaluated with the degradation of p-nitrophenol and methyl orange under UV or sunlight irradiation. The catalysts had a strong visible light absorption which corresponding to doped nitrogen and consequent oxygen deficient. Concentration of the nitrogen substances also affected the visible light adsorption of the TiO₂. The XPS results indicated the doped nitrogen in the TiO₂ may exist in the formation of O₂Ti−N−H and/or O₂Ti−N, nitrogen was in form of interstitial atom. The results of photocatalytic activity showed the visible light adsorption mechanisms, as the doped nitrogen species gave rise to a mid-gap level slightly above the top of the (O-2p) valence band, but not from the mixed band gap of the N-2p and O-2p electronic levels.

• Periodical: Applied Mechanics and Materials (Volumes 71-78)
• Pages: 748-754
• DOI: https://doi.org/10.4028/www.scientific.net/AMM.71-78.748
• Online since: July 2011
• Authors: Yu Chao Tang, Xian Huai Huang, Chang Nian Wu, Li Hua Tang, Li Ping Xue, Fa Kang Pan
• Keywords: Mechanochemica1, Nitrogen-Doped, Nitrogenous Compound, Photocatalyst, TiO₂

References

[1] T Lindgren, J M Mwabora, E Avendano, et al. Photoelectrochemical and optical properties of nitrogen doped titanium dioxide films prepared by reactive DC magnetron sputtering[J]. J. Phys. Chem. B, 2003, 107: 5709-5716.

DOI: 10.1021/jp027345j

[2] M Anpo. and M Takeuchi. The design and development of highly reactive titanium oxidephotocatalysts operating under visible light irradiation[J]. J. Catal., 2003, 216: 505-516.

DOI: 10.1016/s0021-9517(02)00104-5

[3] R Asahi, T Morikawa, T Ohwaki, et al. Visible-light photocatalysis in nitrogen-doped titanium oxides[J]. Science, 2001, 293: 269-271.

DOI: 10.1126/science.1061051

[4] B Kosowska, S Mozia, A W Morawski, et al. The preparation of TiO2-nitrogen doped by calcination of TiO2∙xH2O under ammonia atmosphere for visible light photocatalysis[J]. Solar Energy Materials & Solar Cells , 2005, 88: 269-280.

DOI: 10.1016/j.solmat.2004.11.001

[5] S Mozia, M Tomaszewska, B Kosowska, et al. Morawski, Kazimierz Kalucki. Decomposition of nonionic surfactant on a nitrogen-doped photocatalyst under visible-light irradiation[J]. Appl. Catal. B: Environ., 55 (2005) 195–200.

DOI: 10.1016/j.apcatb.2004.09.019

[6] T Ihara, M Miyoshi, Y Iriyama, et al. Visible light active titanium oxide photocatalyst realized by an oxygen deficient structure and by nitrogen doping[J]. Appl. Catal. B: Environ., 2003, 42: 403-409.

DOI: 10.1016/s0926-3373(02)00269-2

[7] Y Nosaka, M Matsushita, J Nishino, A Y Nosaka. Nitrogen-doped titanium dioxide photocatalysts for visible response prepared by using organic compounds[J]. Sci. Technol. Adv. Materials, 2005, 6: 143-148.

DOI: 10.1016/j.stam.2004.11.006

[8] Y Suda, H Kawasaki, T Ueda, T Ohshima. Preparation of high quality nitrogen doped TiO2 thin film as a photocatalyst using a pulsed laser deposition method[J]. Thin Solid Films, 2004, (453/454): 162-166.

DOI: 10.1016/j.tsf.2003.11.185

[9] S Yin, H Yamaki, Q W Zhang, M Komatsu, et al. Mechanochemical synthesis of nitrogen-doped titania and its visible light induced NOx destruction ability[J]. Solid State Ionics, 2004, 172: 205–209.

DOI: 10.1016/j.ssi.2004.05.018

[10] S F Chen, L Chen, S Gao, G Y Cao. The preparation of nitrogen-doped photocatalyst TiO2-xNx by ball milling[J]. Chem. Phys. Lett., 2005, 413: 404-409.

DOI: 10.1016/j.cplett.2005.08.038

[11] H X Li, J X Li, Y N Huo. Highly active TiO2N photocatalysts prepared by treating TiO2 precursors in NH3/ethanol fluid under supercritical conditions[J]. J. Phys. Chem. B, 2006, 110, 1559-1565.

DOI: 10.1021/jp055830j

[12] O Diwald, T L Thompson, E G Goralski., et al. The effect of nitrogen ion implantation on the photoactivity of TiO2 rutile single crystals[J]. J. Phys. Chem. B, 2004, 108: 52-57.

DOI: 10.1021/jp030529t

[13] M M Julius, L Torbjorn, A Esteban, F J Thomas, L Jun, L Sten-Eric, G Claes-Goran. Structure, composition, and morphology of photoelectron chemically active TiO2-xNx thin films deposited by reactive DC magnetron sputtering[J]. J. Phys. Chem. B, 2004, 108, 20193-20198.

DOI: 10.1021/jp0368987

[14] C D Valentin, G Pacchioni, A Selloni, et al. Characterization of paramagnetic species in N-doped TiO2 powders by EPR spectroscopy and DFT calculations[J]. J. Phys. Chem. B, 2005, 109: 11414-11419.

DOI: 10.1021/jp051756t

[15] O Diwald, T L Thompson, T Zubkov, et al. Photochemical activity of nitrogen-doped rutile TiO2(110) in visible light[J]. J. Phys. Chem. B, 2004, 108: 6004-6008.

DOI: 10.1021/jp031267y

[16] G R Torres, T Lindgren, J Lu, et al. Photoelectrochemical study of nitrogen-doped titanium dioxide for water oxidation[J]. J. Phys. Chem. B, 2004, 108: 5995-6003.

DOI: 10.1021/jp037477s