[en] The objective of this work is to improve the efficiency of TiO2 photocatalysts by activation treatments and by modification with palladium nanoparticles and doping with SiO2. The influence of the additive loading was explored, and two activation treatments were performed: UV exposition and H2 reduction. TiO2/SiO2/Pd photocatalysts were synthesized by an original cogelation method: a modified silicon alkoxide, i.e., [3-(2-aminoethyl)aminopropyl]trimethoxysilane (EDAS), was used to complex the palladium ions, thanks to the ethylenediamine group, while the alkoxide groups reacted with TiO2 precursors. Pure TiO2 was also synthesized by the sol–gel process for comparison. X-ray diffraction evidenced that the crystallographic structure of TiO2 was anatase and that Pd was present, either in its oxidized form after calcination, or in its reduced form after reduction. The specific surface area of the samples varied from 5 to 145 m2 g-1. Transmission electron microscopy allowed us to observe the homogeneous dispersion and nanometric size of Pd particles in the reduced samples. The width of the band gap for pure TiO2 sample, measured by UV/Visible diffuse reflectance spectroscopy at approximately 3.2 eV, corresponded to that of anatase. The band gap for the TiO2/SiO2/Pd composite samples could not be calculated, due to their high absorption in visible range. The photocatalytic activity of the various catalysts was evaluated by the degradation of a methylene blue solution under UV radiation. The results showed that the photocatalytic activity of the catalysts was inversely proportional to the content of silica present in the matrix. A small amount of silica improved the photocatalytic activity, as compared to the pure TiO2 sample. By contrast, a high amount of silica delayed the crystallization of TiO2 in its anatase form. The activation treatment under UV had little influence on photocatalytic efficiency. The introduction of Pd species increased the photocatalytic activity of the samples because it allowed for a decrease in the rate of electron–hole recombinations in TiO2. The reduction treatment improved the activity of photocatalysts, whatever the palladium content, thanks to the reduction of Ti4+ into Ti3+, and the formation of defects in the crystallographic structure of anatase.
Disciplines :
Chemical engineering Materials science & engineering
Author, co-author :
Mahy, Julien ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
Sotrez, Valériane ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
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Bibliography
Pignatello, J.J.; Oliveros, E.; MacKay, A. Advanced oxidation processes for organic contaminant destruction based on the fenton reaction and related chemistry. Crit. Rev. Environ. Sci. Technol. 2006, 36, 1-84.
Kuyukina, M.S.; Ivshina, I.B. Application of Rhodococcus in Bioremediation of Contaminated Environments. In Biology of Rhodococcus; Alvarez, H., Ed.; Springer: Berlin/Heidelberg, Germany, 2010; pp. 231-262, ISBN 9783642129377.
Linsebigler, A.L.; Lu, G.; Yates, J.T. Photocatalysis on TiO2 Surfaces: Principles, Mechanisms, and Selected Results. Chem. Rev. 1995, 95, 735-758.
Pelaez, M.; Nolan, N.T.; Pillai, S.C.; Seery, M.K.; Falaras, P.; Kontos, A.G.; Dunlop, P.S.M.; Hamilton, J.W.J.; Byrne, J.A.; O’Shea, K.; et al. A review on the visible light active titanium dioxide photocatalysts for environmental applications. Appl. Catal. B: Environ. 2012, 125, 331-349.
Oseghe, E.O.; Ofomaja, A.E. Study on light emission diode/carbon modified TiO2 system for tetracycline hydrochloride degradation. J. Photochem. Photobiol. A: Chem. 2018, 360, 242-248.
Mahy, J.G.; Paez, C.A.; Carcel, C.; Bied, C.; Tatton, A.S.; Damblon, C.; Heinrichs, B.; Wong Chi Man, M.; Lambert, S.D. Porphyrin-based hybrid silica-titania as a visible-light photocatalyst. J. Photochem. Photobiol. A: Chem. 2019, 373, 66-76.
Banerjee, S.; Dionysiou, D.D.; Pillai, S.C. Self-cleaning applications of TiO2 by photo-induced hydrophilicity and photocatalysis. Appl. Catal. B: Environ. 2015, 176, 396-428.
Espino-Estévez, M.R.; Fernández-Rodríguez, C.; González-Díaz, O.M. Effect of TiO2-Pd and TiO2-Ag on the photocatalytic oxidation of diclofenac, isoproturon and phenol. Chem. Eng. J. 2016, 298, 82-95.
Léonard, G.L.-M.; Malengreaux, C.M.; Mélotte, Q.; Lambert, S.D.; Bruneel, E.; Van Driessche, I.; Heinrichs, B. Doped sol-gel films vs. powders TiO2: On the positive effect induced by the presence of a substrate. J. Environ. Chem. Eng. 2016, 4, 449-459.
Tunc, I. The effect of the presence of Ag nanoparticles on the photocatalytic degradation of oxalic acid adsorbed on TiO2 nanoparticles monitored by ATR-FTIR. Mater. Chem. Phys. 2014, 144, 444-450.
Bodson, C.J.; Heinrichs, B.; Tasseroul, L.; Bied, C.; Mahy, J.G.; Wong Chi Man, M.; Lambert, S.D. Efficient P-and Ag-doped titania for the photocatalytic degradation of waste water organic pollutants. J. Alloy. Compd. 2016, 682, 144-153.
Vaiano, V.; Iervolino, G.; Sannino, D.; Murcia, J.J.; Hidalgo, M.C.; Ciambelli, P.; Navío, J.A. Photocatalytic removal of patent blue V dye on Au-TiO2 and Pt-TiO2 catalysts. Appl. Catal. B: Environ. 2016, 188, 134-146.
Borzyszkowska, A.F.; Stepnowski, P.; Ofiarska, A.; Pieczynska, A.; Siedlecka, E.M. Pt-TiO2-assisted photocatalytic degradation of the cytostatic drugs ifosfamide and cyclophosphamide under artificial sunlight. Chem. Eng. J. 2016, 285, 417-427.
Abdelaal, M.Y.; Mohamed, R.M. Novel Pd/TiO2 nanocomposite prepared by modified sol-gel method for photocatalytic degradation of methylene blue dye under visible light irradiation. J. Alloy. Compd. 2013, 576, 201-207.
Léonard, G.L.-M.; Pàez, C.A.; Ramírez, A.E.; Mahy, J.G.; Heinrichs, B. Interactions between Zn2+ or ZnO with TiO2 to produce an efficient photocatalytic, superhydrophilic and aesthetic glass. J. Photochem. Photobiol. A: Chem. 2018, 350, 32-43.
Mahy, J.G.; Lambert, S.D.; Tilkin, R.G.; Poelman, D.; Wolfs, C.; Devred, F.; Gaigneaux, E.M.; Douven, S. Ambient temperature ZrO2-doped TiO2 crystalline photocatalysts: Highly efficient powders and films for water depollution. Mater. Today Energy 2019, 13, 312-322.
Pirard, S.L.; Mahy, J.G.; Pirard, J.-P.; Heinrichs, B.; Raskinet, L.; Lambert, S.D. Development by the sol-gel process of highly dispersed Ni-Cu/SiO2 xerogel catalysts for selective 1, 2-dichloroethane hydrodechlorination into ethylene. Microporous Mesoporous Mater. 2015, 209, 197-207.
Belet, A.; Wolfs, C.; Mahy, J.G.; Poelman, D.; Vreuls, C. Sol-Gel Syntheses of Photocatalysts for the Removal of Pharmaceutical Products in Water. Nanomaterials 2019, 9(1), 126.
Yang, J.; Xu, X.; Liu, Y.; Gao, Y.; Chen, H.; Li, H. Preparation of SiO2@TiO2 composite nanosheets and their application in photocatalytic degradation of malachite green at emulsion interface. Colloids Surf. A: Physicochem. Eng. Asp. 2019, 582, 123858.
Bodson, C.J.; Lambert, S.D.; Alié, C.; Cattoën, X.; Pirard, J.; 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 TiO2 materials. Microporous Mesoporous Mater. 2010, 134, 157-164.
Lecloux, A.J. Texture of Catalysts. In Catalysis: Science and Technology; Anderson, J.R., Boudart, M., Eds.; Springer: Berlin/Heidelberg, Germany, 1981; Volume 2, pp. 171-230.
Mahy, J.G.; Claude, V.; Sacco, L.; Lambert, S.D. Ethylene polymerization and hydrodechlorination of 1, 2-dichloroethane mediated by nickel(II) covalently anchored to silica xerogels. J. Sol-Gel Sci. Technol. 2017, 81, 59-68.
Lambert, S.; Cellier, C.; Grange, P.; Pirard, J.P.; Heinrichs, B. Synthesis of Pd/SiO2, Ag/SiO2, and Cu/SiO2 cogelled xerogel catalysts: Study of metal dispersion and catalytic activity. J. Catal. 2004, 221, 335-346.
Khaki, M.R.D.; Shafeeyan, M.S.; Raman, A.A.A.; Daud, W.M.A.W. Application of doped photocatalysts for organic pollutant degradation-A review. J. Environ. Manag. 2017, 198, 78-94.
Yukselen, Y.; Kaya, A. Suitability of the methylene blue test for surface area, cation exchange capacity and swell potential determination of clayey soils. Eng. Geol. 2008, 102, 38-45.
Calleja, G.; Serrano, D.P.; Sanz, R.; Pizarro, P. Mesostructured SiO2-doped TiO2 with enhanced thermal stability prepared by a soft-templating sol-gel route. Microporous Mesoporous Mater. 2008, 111, 429-440.
Zhang, Z.; Long, J.; Xie, X.; Zhuang, H.; Zhou, Y.; Lin, H.; Yuan, R.; Dai, W.; Ding, Z.; Wang, X.; et al. Controlling the synergistic effect of oxygen vacancies and N dopants to enhance photocatalytic activity of N-doped TiO2 by H2 reduction. Appl. Catal. A: Gen. 2012, 425-426, 117-124.
Páez, C.A.; Lambert, S.D.; Poelman, D.; Pirard, J.P.; Heinrichs, B. Improvement in the methylene blue adsorption capacity and photocatalytic activity of H2-reduced rutile-TiO2caused by Ni(II)porphyrin preadsorption. Appl. Catal. B: Environ. 2011, 106, 220-227.
Liu, H.; Ma, H.T.; Li, X.Z.; Li, W.Z.; Wu, M.; Bao, X.H. The enhancement of TiO2 photocatalytic activity by hydrogen thermal treatment. Chemosphere 2003, 50, 39-46.
Tong, H.-x.; Chen, Q.-y.; Yin, Z.-l.; Hu, H.-p.; Wu, D.-x; Yang, Y.-h. Preparation, characterization and photo-catalytic behavior of WO3-TiO2 catalysts with oxygen vacancies. Trans. Nonferrous Met. Soc. China 2009, 19, 1483-1488.
Pirard, S.L.; Malengreaux, C.M.; Toye, D.; Heinrichs, B. How to correctly determine the kinetics of a photocatalytic degradation reaction? Chem. Eng. J. 2014, 249, 1-5.
Arabatzis, I.M.; Stergiopoulos, T.; Andreeva, D.; Kitova, S.; Neophytides, S.G.; Falaras, P. Characterization and photocatalytic activity of Au/TiO2 thin films for azo-dye degradation. J. Catal. 2003, 220, 127-135.
Fisher, M.B.; Keane, D.A.; Fernández-Ibáñez, P.; Colreavy, J.; Hinder, S.J.; McGuigan, K.G.; Pillai, S.C. Nitrogen and copper doped solar light active TiO2 photocatalysts for water decontamination. Appl. Catal. B: Environ. 2013, 130-131, 8-13.
Patterson, A.L. The Scherrer Formula for X-Ray Particle Size Determination. Phys. Rev. 1939, 56, 978-982.
Malengreaux, C.M.; Douven, S.; Poelman, D.; Heinrichs, B.; Bartlett, J.R. An ambient temperature aqueous sol-gel processing of efficient nanocrystalline doped TiO2-based photocatalysts for the degradation of organic pollutants. J. Sol-Gel Sci. Technol. 2014, 71, 557-570.
Kubelka, P. Ein Beitrag zur Optik der Farban striche. Z Tech. Phys. 1931, 12, 593-601.
Kubelka, P. New contributions to the optics of intensely light-scattering materials. J. Opt. Soc. Am. 1948, 38, 448-457.
Mahy, J.G.; Lambert, S.D.; Léonard, G.L.-M.; Zubiaur, A.; Olu, P.-Y.; Mahmoud, A.; Boschini, F.; Heinrichs, B. Towards a large scale aqueous sol-gel synthesis of doped TiO2: Study of various metallic dopings for the photocatalytic degradation of p-nitrophenol. J. Photochem. Photobiol. A: Chem. 2016, 329, 189-202.
Malengreaux, C.M.; Pirard, S.L.; Léonard, G.; Mahy, J.G.; Herlitschke, M.; Klobes, B.; Hermann, R.; Heinrichs, B.; Bartlett, J.R. Study of the photocatalytic activity of Fe3+, Cr3+, La3+ and Eu3+ single-doped and co-doped TiO2 catalysts produced by aqueous sol-gel processing. J. Alloy. Compd. 2017, 691, 726-738.
Tasseroul, L.; Pirard, S.L.; Lambert, S.D.; Páez, C.A.; Poelman, D.; Pirard, J.P.; Heinrichs, B. Kinetic study of p-nitrophenol photodegradation with modified TiO2 xerogels. Chem. Eng. J. 2012, 191, 441-450.
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