[en] TiO2 thin films have been produced by a dip-coating process using a non-aqueous sol-gel method. This study investigated the influence of the operating variables such as nature of the substrate, sol concentration, withdrawing speed of the dip-coater and number of layers on the physico-chemical properties of the films using XRD, GIXRD, UV-Vis spectroscopy, profilometry, spectroscopic ellipsometry and SEM. Photocatalytic activity of the films was evaluated by following the degradation of methylene blue under artificial UV light at 25°C. The performances of the catalysts were compared through the reaction rate constants determined using an apparent first-order kinetic model adjusted on the experimental data. This study showed that the photocatalytic activity and the reaction rate constant depend on the film thickness through the synthesis and dipping variable, with an optimum thickness of 80 nm being observed. An optimized transparent film exhibiting a high adhesion, a well crystallized TiO2-anatase phase, a good photocatalytic activity and a reaction rate constant k equal to 0.126 h-1 was obtained using a simple process. The specific photocatalytic activity of this film was higher to the one measured for TiO2 powders in previous works.
Disciplines :
Chemistry Materials science & engineering Chemical engineering
Author, co-author :
Malengreaux, Charline ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Nanomatériaux et interfaces
Timmermans, Adrien
Pirard, Sophie ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Génie catalytique
Lambert, Stéphanie ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Génie catalytique
Pirard, Jean-Paul ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Génie catalytique
Poelman, Dirk; Universiteit Gent - Ugent
Heinrichs, Benoît ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Nanomatériaux et interfaces
Language :
English
Title :
Optimized deposition of TiO2 thin films produced by a non-aqueous sol-gel method and quantification of their photocatalytic activity
Publication date :
2012
Journal title :
Chemical Engineering Journal
ISSN :
1385-8947
eISSN :
1873-3212
Publisher :
Elsevier Science, Lausanne, Switzerland
Volume :
195-196
Pages :
347-358
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE] Interuniversity Attraction Pole (IAP-P6/17) MRW - Ministère de la Région wallonne [BE] FRFC - Fonds de la Recherche Fondamentale Collective [BE] FWO - Fonds Wetenschappelijk Onderzoek Vlaanderen [BE]
Fujishima A., Zhang X., Tryk D.A. Heterogeneous photocatalysis: from water photolysis to applications in environmental cleanup. Int. J. Hydrogen Energy 2007, 32:2664-2672.
Nakajima A., Nakamura A., Arimitsu N., Kameshima Y., Okada K. Processing and properties of transparent sulfated TiO 2 thin films using sol-gel method. Thin Solid Films 2008, 516:6392-6397.
Mills A., LeHunte S. An overview of semiconductor photocatalysis. J. Photochem. Photobiol. A - Chem. 1997, 108:1-35.
Tryk D.A., Fujishima A., Honda K. Recent topics in photoelectrochemistry: achievements and future prospects. Electrochim. Acta 2000, 45:2363-2376.
Fujishima A., Hashimoto K., Watanabe T. TiO 2 Photocatalysis: Fundamentals and Applications 1999, BKC, Inc., Tokyo.
Maira A.J., Yeung K.L., Soria J., Coronado J.M., Belver C., Lee C.Y. Gas-phase photo-oxidation of toluene using nanometer-size TiO 2 catalysts. Appl. Catal. B - Environ. 2001, 29:327-336.
Zhang B.L., Chen B.S., Shi K.Y., He S.J., Liu X.D., Du Z.J., Yang K.L. Preparation and characterization of nanocrystal grain TiO 2 porous microspheres. Appl. Catal. B - Environ. 2003, 40:253-258.
Bodson C.J., Lambert S.D., Alié C., Cattoen X., Pirard J.P., Bied C., Wong Chi Man M., Heinrichs B. Effects of additives and solvents on the gel formation rate and on the texture of P- and Si-doped TiO 2 materials. Micropor. Mesopor. Mater. 2010, 134:157-164.
Paez C.A., Poelman D., Pirard J.P., Heinrichs B. Unpredictable photocatalytic ability of H- 2-reduced rutile-TiO 2 xerogel in the degradation of dye-pollutants under UV and visible light irradiation. Appl. Catal. B - Environ. 2010, 94:263-271.
Chen Y.J., Stathatos E., Dionysiou D.D. Microstructure characterization and photocatalytic activity of mesoporous TiO 2 films with ultrafine anatase nanocrystallites. Surf. Coat. Technol. 2008, 202:1944-1950.
Novotna P., Zita J., Krysa J., Kalousek V., Rathousky J. Two-component transparent TiO 2/SiO 2 and TiO 2/PDMS films as efficient photocatalysts for environmental cleaning. Appl. Catal. B - Environ. 2008, 79:179-185.
Maira A.J., Lau W.N., Lee C.Y., Yue P.L., Chan C.K., Yeung K.L. Performance of a membrane-catalyst for photocatalytic oxidation of volatile organic compounds. Chem. Eng. Sci. 2003, 58:959-962.
Brinker S.G.W., Jeffrey C. Sol-Gel Science: The Physics and Chemistry of Sol-Gel Processing 1990, Academic Press, Boston.
Yu J.G., Zhao X.J. Effect of surface treatment on the photocatalytic activity and hydrophilic property of the sol-gel derived TiO 2 thin films. Mater. Res. Bull. 2001, 36:97-107.
Legrand-Buscema C., Malibert C., Bach S. Elaboration and characterization of thin films of TiO 2 prepared by sol-gel process. Thin Solid Films 2002, 418:79-84.
Arrachart G., Cassidy D.J., Karatchevtseva I., Triani G. Nanostructural evolution of titania-based materials using modified titanium precursors. J. Am. Ceram. Soc. 2009, 92:2109-2115.
Choi H., Stathatos E., Dionysiou D.D. Synthesis of nanocrystalline photocatalytic TiO 2 thin films and particles using sol-gel method modified with nonionic surfactants. Thin Solid Films 2006, 510:107-114.
Schubert U. Chemical modification of titanium alkoxides for sol-gel processing. J. Mater. Chem. 2005, 15:3701-3715.
Karatchevtseva I., Heinemann A., Hartley V., Knott R. Structure of organic-inorganic nanohybrids incorporating titanium(IV) oxoalkoxyacylate nanoclusters: a SANS study. J. Phys. Chem. B 2008, 112:16478-16484.
Rozes L., Steunou N., Fornasieri G., Sanchez C. Titanium-oxo clusters, versatile nanobuilding blocks for the design of advanced hybrid materials. Mon. Chem. 2006, 137:501-528.
Maira A.J., Yeung K.L., Lee C.Y., Yue P.L., Chan C.K. Size effects in gas-phase photo-oxidation of trichloroethylene using nanometer-sized TiO 2 catalysts. J. Catal. 2000, 192:185-196.
Avci N., Smet P.F., Poelman H., Van de Velde N., De Buysser K., Van Driessche I., Poelman D. Characterization of TiO 2 powders and thin films prepared by non-aqueous sol-gel techniques. J. Sol-Gel Sci. Technol. 2009, 52:424-431.
Euvananont C., Junin C., Inpor K., Limthongkul P., Thanachayanont C. TiO 2 optical coating layers for self-cleaning applications. Ceram. Int. 2008, 34:1067-1071.
Rauf M.A., Ashraf S.S. Fundamental principles and application of heterogeneous photocatalytic degradation of dyes in solution. Chem. Eng. J. 2009, 151:10-18.
Houas A., Lachheb H., Ksibi M., Elaloui E., Guillard C., Herrmann J.-M. Photocatalytic degradation pathway of methylene blue in water. Appl. Catal. B - Environ. 2001, 31:145-157.
Huang J., Cao Y., Liu Z., Deng Z., Wang W. Application of titanate nanoflowers for dye removal: a comparative study with titanate nanotubes and nanowires. Chem. Eng. J. 2012, 191:38-44.
López A., Acosta D., Martínez A.I., Santiago J. Nanostructured low crystallized titanium dioxide thin films with good photocatalytic activity. Powder Technol. 2010, 202:111-117.
A. Mills, An overview of the methylene blue ISO test for assessing the activities of photocatalytic films, Appl. Catal. B - Environ, 2012, in press, doi:10.1016/j.apcatb.2012.01.019.
Di Paola A., García-López E., Marcì G., Palmisano L. A survey of photocatalytic materials for environmental remediation. J. Hazard. Mater. 2012, 211-212:3-29.
Yu J.G., Zhao X.J., Zhao Q.N. Photocatalytic activity of nanometer TiO 2 thin films prepared by the sol-gel method. Mater. Chem. Phys. 2001, 69:25-29.
Patterson A.L. Phys. Rev. 1939, 978.
Kubelka P. Ein Beitrag zur Optik der Farbanstriche. Z. Tech. Phys. 1931, 12:593-601.
Kubelka P. New contributions to the optics of intensely light-scattering materials. J. Opt. Am. 1948, 38:448-457.
Braconnier B., Paez C.A., Lambert S., Alié C., Henrist C., Poelman D., Pirard J.P., Cloots R., Heinrichs B. Ag- and SiO 2-doped porous TiO 2 with enhanced thermal stability. Micropor. Mesopor. Mater. 2009, 122:247-254.
Morales A.E.M., Sanchez E., Pal U. Use of diffuse reflectance spectroscopy for optical characterization of un-supported nanostructures. Rev. Mex. Fis. S 2007, 53:18-22.
Alié C., Tcherkassova N., Ferauche F., Lambert S., Heinrichs B., Pirard R., Pirard J.P. Multigram scale synthesis and characterization of low-density silica xerogels. J. Non-Cryst. Solids 2006, 352:2763-2771.
Lecloux A.J. Catalysis: Science and Technology 1981, Springer, Berlin.
Eufinger K., Poelman D., Poelman H., De Gryse R., Marin G.B. TiO 2 thin films for photocatalytic applications. Thin Solid Films: Process and Applications Transworld Research Network 2008, Kerala, India, pp. 189-227. S. Nam (Ed.).
Tomaszewski H., Eufinger K., Poelman H., Poelman D., De Gryse R., Smet P.F., Marin G.B. Effect of substrate sodium content on crystallization and photocatalytic activity of TiO 2 films prepared by DC magnetron sputtering. Int. J. Photoenergy 2007, 5. (Art. No. 95213).
Paz Y., Heller A. Photo-oxidatively self-cleaning transparent titanium dioxide films on soda lime glass: the deleterious effect of sodium contamination and its prevention. J. Mater. Res. 1997, 12:2759-2766.
Zita J., Krysa J., Mills A. Correlation of oxidative and reductive dye bleaching on TiO 2 photocatalyst films. J. Photochem. Photobiol. A - Chem. 2009, 203:119-124.
Addamo M., Augugliaro V., Di Paola A., Garcia-Lopez E., Loddo V., Marci G., Palmisano L. Photocatalytic thin films of TiO 2 formed by a sol-gel process using titanium tetraisopropoxide as the precursor. Thin Solid Films 2008, 516:3802-3807.
Oh S.H., Kim J.S., Chung J.S., Kim E.J., Hahn S.H. Crystallization and photoactivity of TiO 2 films formed on soda lime glass by a sol-gel dip-coating process. Chem. Eng. Commun. 2005, 192:327-335.
Yu J.G., Zhao X.J., Zhao Q.N. Effect of film thickness on the grain size and photocatalytic activity of the sol-gel derived nanometer TiO 2 thin films. J. Mater. Sci. Lett. 2000, 19:1015-1017.
Zare-Hossein-abadi D., Ershad-Langroudi A., Rahimi A., Afsar S. Photo-generated activities of nanocrystalline TiO 2 thin films. J. Inorg. Organomet. Polym. Mater. 2010, 20:250-257.
