Ambient crystallization; Photocatalysis; ZrO2 doping; Titania; Sol-gel process
Abstract :
[en] In this paper, several TiO2 materials doped with zirconia precursor (0.7, 1.4, 1.6 and 2.0 mol%) were synthesized by an easy aqueous sol-gel synthesis at ambient temperature. This method consisted in the peptization of the TiO2 colloid in presence of HNO3. The corresponding pure TiO2 material was also synthesized for comparison. The performances and the physico-chemical properties of these materials were compared to the well-known Evonik P25 photocatalyst.
The physico-chemical characterizations showed that nano-crystalline anatase-brookite particles were produced with the sol-gel process, with higher specific surface area than P25 (∼200 m2 g-1 vs. 47 m2 g-1). All samples presented a higher visible absorption than P25. The XPS spectra showed that all the samples were doped with nitrogen and that mixed TiO2–ZrO2 oxide materials were obtained when doping with zirconia precursor.
Photoactivity was evaluated through the degradation of p-nitrophenol in water. On the one hand, under UV/visible light, the ZrO2 doping increased the degradation efficiency of the pure TiO2 catalyst due to a better charge separation in the mixed TiO2–ZrO2 oxides. The activity of the sample with the highest dopant content was even higher than the one of P25. On the other hand, under visible light, all samples were much more efficient than P25. This activity shift towards visible range was due to the N-doping of the catalysts, with a slight improvement for the doped ones. Finally, the feasibility of producing films starting from an aqueous suspension of the photocatalyst was assessed on P25, pure TiO2 and the best doped material. The photoactivity of these films, evaluated on the degradation of methylene blue under UV-A light, showed that the sample with the highest dopant concentration had an efficiency 4 times higher than pure TiO2 and 20 times higher than P25.
Disciplines :
Materials science & engineering Chemical engineering
Author, co-author :
Mahy, Julien ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
Lambert, Stéphanie ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
Tilkin, Rémi ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
Wolfs, Cédric ; Université de Liège - ULiège > Department of Chemical Engineering > Génie chimique - Nanomatériaux et interfaces
Poelman, Dirk
Devred, François
Gaigneaux, Eric
Douven, Sigrid ; Université de Liège - ULiège > Department of Chemical Engineering > Nanomaterials, Catalysis, Electrochemistry
Language :
English
Title :
Ambient temperature ZrO2-doped TiO2 crystalline photocatalysts: Highly efficient powders and films for water depollution
Turolla, A., Fumagalli, M., Bestetti, M., Antonelli, M., Electrophotocatalytic decolorization of an azo dye on TiO2 self-organized nanotubes in a laboratory scale reactor. Desalination 285 (2012), 377–382, 10.1016/j.desal.2011.10.029.
Scholz, N., Setting Criteria on Endocrine Disruptors: Follow-Up to the General Court Judgment, Brief. From Eur. Parliam. 2016, 1–10 http://www.europarl.europa.eu/RegData/etudes/BRIE/2016/581986/EPRS_BRI(2016)581986_EN.pdf.
Oturan, M.A., Aaron, J.J., Advanced oxidation processes in water/wastewater treatment: principles and applications. A review. Crit. Rev. Environ. Sci. Technol. 44 (2014), 2577–2641, 10.1080/10643389.2013.829765.
Mahy, J.G., Lambert, S.D., Léonard, G.L.-M., Zubiaur, A., Olu, P.-Y., Mahmoud, A., Boschini, F., Lambert, S.D., 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. 329 (2016), 189–202, 10.1016/j.jphotochem.2016.06.029.
Fujishima, A., Hashimoto, K., Watanabe, T., TiO2 Photocatalysis: Fundamentals and Applications. first ed., 1999, BKC Inc., Tokyo, Japan.
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., Entezari, M.H., Dionysiou, D.D., A review on the visible light active titanium dioxide photocatalysts for environmental applications. Appl. Catal. B Environ. 125 (2012), 331–349, 10.1016/j.apcatb.2012.05.036.
Di Paola, A., Marcì, G., Palmisano, L., Schiavello, M., Uosaki, K., Ikeda, S., Ohtani, B., Preparation of polycrystalline TiO2 photocatalysts impregnated with various transition metal ions: characterization and photocatalytic activity for the degradation of 4-nitrophenol. J. Phys. Chem. B 106 (2002), 637–645, 10.1021/jp013074l.
Espino-Estévez, M.R., Fernández-Rodríguez, C., González-Díaz, O.M., Araña, J., Espinós, J.P., Ortega-Méndez, J.A., Doña-Rodríguez, J.M., Effect of TiO2–Pd and TiO2–Ag on the photocatalytic oxidation of diclofenac, isoproturon and phenol. Chem. Eng. J. 298 (2016), 82–95, 10.1016/j.cej.2016.04.016.
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. Comp. 682 (2016), 144–153, 10.1016/j.jallcom.2016.04.295.
Impellizzeri, G., Scuderi, V., Romano, L., Sberna, P.M., Arcadipane, E., Sanz, R., Scuderi, M., Nicotra, G., Bayle, M., Carles, R., Simone, F., Privitera, V., Fe ion-implanted TiO2 thin film for efficient visible-light photocatalysis. J. Appl. Phys., 116, 2016, 173507, 10.1063/1.4901208.
Wu, T., Lin, T., Zhao, J., Hidaka, H., Serpone, N., TiO2 -assisted photodegradation of dyes. 9. Photooxidation of a squarylium cyanine dye in aqueous dispersions under visible light irradiation. Environ. Sci. Technol. 33 (1999), 1379–1387, 10.1021/es980923i.
Min, K.S., Kumar, R.S., Lee, J.H., Kim, K.S., Lee, S.G., Son, Y.-A., Synthesis of new TiO2/porphyrin-based composites and photocatalytic studies on methylene blue degradation. Dyes Pigments 160 (2019), 37–47, 10.1016/j.dyepig.2018.07.045.
Mahy, J.G., Paez, C.A., Carcel, C., Bied, C., Tatton, A.S., Damblon, C., Heinrichs, B., Lambert, S.D., Porphyrin-based hybrid silica-titania as a visible-light photocatalyst. J. Photochem. Photobiol. A Chem. 373 (2019), 66–76, 10.1016/j.jphotochem.2019.01.001.
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. 350 (2018), 32–43, 10.1016/j.jphotochem.2017.09.036.
Tian, Q., Wei, W., Dai, J., Sun, Q., Zhuang, J., Zheng, Y., Liu, P., Fan, M., Chen, L., Porous core-shell TixSn1-xO2 solid solutions with broad-light response: one-pot synthesis and ultrahigh photooxidation performance. Appl. Catal. B Environ. 244 (2019), 45–55, 10.1016/j.apcatb.2018.11.045.
Wu, M., Leung, D.Y.C., Zhang, Y., Huang, H., Xie, R., Szeto, W., Li, F., Toluene degradation over Mn-TiO2/CeO2 composite catalyst under vacuum ultraviolet (VUV) irradiation. Chem. Eng. Sci. 195 (2019), 985–994, 10.1016/j.ces.2018.10.044.
Lang, J., Matějová, L., Troppová, I., Čapek, L., Endres, J., Daniš, S., Novel synthesis of ZrxTi1-xOn mixed oxides using titanyl sulphate and pressurized hot and supercritical fluids, and their photocatalytic comparison with sol-gel prepared equivalents. Mater. Res. Bull. 95 (2017), 95–103, 10.1016/j.materresbull.2017.07.023.
Maver, K., Štangar, U.L., Černigoj, U., Gross, S., Cerc Korošec, R., Low-temperature synthesis and characterization of TiO2 and TiO2-ZrO2 photocatalytically active thin films. Photochem. Photobiol. Sci. 8 (2009), 657–662, 10.1039/b817475j.
Ranjbar, S., Saberyan, K., Parsayan, F., A new process for preparation of Zr doped TiO2 nanopowders using APCVS method. Mater. Chem. Phys. 214 (2018), 337–344, 10.1016/j.matchemphys.2018.04.119.
Neppolian, B., Wang, Q., Yamashita, H., Choi, H., Synthesis and characterization of ZrO2-TiO2 binary oxide semiconductor nanoparticles: application and interparticle electron transfer process. Appl. Catal. Gen. 333 (2007), 264–271, 10.1016/j.apcata.2007.09.026.
Mohammadi, M.R., Fray, D.J., Synthesis and characterisation of nanosized TiO2-ZrO2 binary system prepared by an aqueous sol-gel process: physical and sensing properties. Sensor. Actuator. B Chem. 155 (2011), 568–576, 10.1016/j.snb.2011.01.009.
Thejaswini, T.V.L., Prabhakaran, D., Maheswari, M.A., Synthesis of mesoporous worm-like ZrO2–TiO2 monoliths and their photocatalytic applications towards organic dye degradation. J. Photochem. Photobiol. A Chem. 344 (2017), 212–222, 10.1016/j.jphotochem.2017.05.015.
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. 71 (2014), 557–570, 10.1007/s10971-014-3405-6.
Romeiro, A., Azenha, M.E., Canle, M., Rodrigues, V.H.N., Da Silva, J.P., Burrows, H.D., Titanium dioxide nanoparticle photocatalysed degradation of ibuprofen and naproxen in water: competing hydroxyl radical attack and oxidative decarboxylation by semiconductor holes. Chemistry 3 (2018), 10915–10924, 10.1002/slct.201801953.
Mbouopda, A.P., Acayanka, E., Nzali, S., Kamgang, G.Y., Njoyim Tamungang, E.B., Laminsi, S., Richard, D., Comparative study of plasma-synthesized and commercial-P25 TiO2 for photocatalytic discoloration of Reactive Red 120 dye in aqueous solution. Desalin. Water Treat. 136 (2018), 413–421, 10.5004/dwt.2018.23118.
Ohno, T., Sarukawa, K., Tokieda, K., Matsumura, M., Morphology of a TiO2 photocatalyst (Degussa, P-25) consisting of anatase and rutile crystalline phases. J. Catal. 203 (2001), 82–86, 10.1006/jcat.2001.3316.
Ohtani, B., Prieto-Mahaney, O.O., Li, D., Abe, R., What is Degussa (Evonic) P25? Crystalline composition analysis, reconstruction from isolated pure particles and photocatalytic activity test. J. Photochem. Photobiol. A Chem. 216 (2010), 179–182, 10.1016/j.jphotochem.2010.07.024.
Janus, M., Morawski, A.W., New method of improving photocatalytic activity of commercial Degussa P25 for azo dyes decomposition. Appl. Catal. B Environ. 75 (2007), 118–123, 10.1016/j.apcatb.2007.04.003.
McNeill, A., Wells, N., Xu, Y., Li, X., Bell, S.E.J., Mills, A., Production and testing of novel photocatalytic TiO2 surface-exposed nanoparticle (TiO2-SEN) thin plastic films. J. Photochem. Photobiol. A Chem. 369 (2019), 142–149, 10.1016/j.jphotochem.2018.10.025.
Tasseroul, L., Páez, C.A., Lambert, S.D., Eskenazi, D., Heinrichs, B., Photocatalytic decomposition of hydrogen peroxide over nanoparticles of TiO2 and Ni(II)-porphyrin-doped TiO2: a relationship between activity and porphyrin anchoring mode. Appl. Catal. B Environ. 182 (2016), 405–413, 10.1016/j.apcatb.2015.09.042.
Mahy, J.G., Tasseroul, L., Zubiaur, A., Geens, J., Brisbois, M., Herlitschke, M., Heinrichs, B., Lambert, S.D., Highly dispersed iron xerogel catalysts for p-nitrophenol degradation by photo-Fenton effects. Microporous Mesoporous Mater. 197 (2014), 164–173, 10.1016/j.micromeso.2014.06.009.
Doebelin, N., Kleeberg, R., Profex: a graphical user interface for the Rietveld refinement program BGMN. J. Appl. Crystallogr. 48 (2015), 1573–1580, 10.1107/S1600576715014685.
Madsen, I.C., Finney, R.J., Flann, R.C.A., Frost, M.T., Wilson, B.W., Quantitative analysis of high-alumina refractories using X-ray powder diffraction data and the Rietveld method. J. Am. Ceram. Soc. 74 (1991), 619–624, 10.1111/j.1151-2916.1991.tb04069.x.
Lecloux, A., Exploitation des isothermes d'adsorption et de désorption d'azote pour l’étude de la texture des solides poreux. Mémoires Société R. Des Sci. Liège., 1971, 169–209.
Mahy, J.G., Léonard, G.L.-M., Pirard, S., Wicky, D., Daniel, A., Archambeau, C., Heinrichs, B., Aqueous sol-gel synthesis and film deposition methods for the large-scale manufacture of coated steel with self-cleaning properties. J. Sol. Gel Sci. Technol. 81 (2017), 27–35, 10.1007/s10971-016-4020-5.
Kubelka, P., Munk, F., Ein Beitrag zur Optik der Farban striche. Z. Tech. Phys. 12 (1931), 593–601.
Kubelka, P., New contributions to the optics of intensely light-scattering materials. J. Opt. Soc. Am. 38 (1948), 448–457, 10.1364/JOSA.38.000448.
Malengreaux, C.M., Pirard, S.L., Léonard, G., Mahy, J.G., Herlitschke, M., Klobes, B., 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. Comp. 691 (2017), 726–738, 10.1016/j.jallcom.2016.08.211.
Bryson, C.E., Surface potential control in XPS. Surf. Sci. 189/190 (1987), 50–58, 10.1016/S0039-6028(87)80414-4.
Shirley, D.A., High-resolution X-ray photoemission spectrum of the valence bands of gold. Phys. Rev. B 5 (1972), 4709–4714, 10.1103/PhysRevB.5.4709.
Páez, C.A., Liquet, D.Y., Calberg, C., Lambert, S.D., Willems, I., Germeau, A., Pirard, J.P., Heinrichs, B., Study of photocatalytic decomposition of hydrogen peroxide over ramsdellite-MnO2 by O2-pressure monitoring. Catal. Commun. 15 (2011), 132–136, 10.1016/j.catcom.2011.08.025.
Mahy, J.G., Deschamps, F., Collard, V., Jérôme, C., Bartlett, J., Lambert, S.D., Heinrichs, B., Acid acting as redispersing agent to form stable colloids from photoactive crystalline aqueous sol–gel TiO2 powder. J. Sol. Gel Sci. Technol. 87 (2018), 568–583, 10.1007/s10971-018-4751-6.
Bischoff, B.L., Anderson, M.A., Peptization process in the sol-gel preparation of porous anatase (TiO2). Chem. Mater. 7 (1995), 1772–1778, 10.1021/cm00058a004.
Mahshid, S., Askari, M., Ghamsari, M.S., Synthesis of TiO2 nanoparticles by hydrolysis and peptization of titanium isopropoxide solution. J. Mater. Process. Technol. 189 (2007), 296–300, 10.1016/j.jmatprotec.2007.01.040.
Mahy, J.G., Lambert, S.D., Geens, J., Daniel, A., Wicky, D., Archambeau, C., Heinrichs, B., Large scale production of photocatalytic TiO2 coating for volatile organic compound (VOC) air remediation. AIMS Mater. Sci. 5 (2018), 945–956, 10.3934/matersci.2018.5.945.
Azouani, R., Tieng, S., Chhor, K., Bocquet, J.F., Eloy, P., Gaigneaux, E.M., Klementiev, K., Kanaev, A.V., TiO2 doping by hydroxyurea at the nucleation stage: towards a new photocatalyst in the visible spectral range. Phys. Chem. Chem. Phys. 12 (2010), 11325–11334, 10.1039/B923548E.
Bittencourt, C., Rutar, M., Umek, P., Mrzel, A., Vozel, K., Arcon, D., Henzler, K., Krüger, P., Guttmann, P., Molecular nitrogen in N-doped TiO2 nanoribbons. RSC Adv. 5 (2015), 23350–23356, 10.1039/C4RA14410D.
Mbiri, A., Taffa, D.H., Gatebe, E., Wark, M., Zirconium doped mesoporous TiO2 multilayer thin films : influence of the zirconium content on the photodegradation of organic pollutants. Catal. Today 328 (2019), 71–78, 10.1016/j.cattod.2019.01.043.
Qian, J., Hu, Q., Hou, X., Qian, F., Dong, L., Li, B., Study of different Ti/Zr ratios on the physicochemical properties and catalytic activities for CuO/Ti−Zr−O composites. Ind. Eng. Chem. Res. 57 (2018), 12792–12800, 10.1021/acs.iecr.8b02674.
Tian, J., Shao, Q., Zhao, J., Pan, D., Dong, M., Jia, C., Ding, T., Microwave solvothermal carboxymethyl chitosan templated synthesis of TiO2/ZrO2 composites toward enhanced photocatalytic degradation of Rhodamine B. J. Colloid Interface Sci. 541 (2019), 18–29, 10.1016/j.jcis.2019.01.069.
Renuka, L., Anantharaju, K.S., Vidya, Y.S., Nagaswarupa, H.P., Prashantha, S.C., Sharma, S.C., Nagabhushana, H., Darshan, G.P., A simple combustion method for the synthesis of multi-functional ZrO2/CuO nanocomposites : excellent performance as Sunlight photocatalysts and enhanced latent fingerprint detection. Appl. Catal. B Environ. 210 (2017), 97–115, 10.1016/j.apcatb.2017.03.055.
Xu, Y., Schoonen, M.A.A., The absolute energy positions of conduction and valence bands of selected semiconducting minerals. Am. Mineral. 85 (2000), 543–556, 10.2138/am-2000-0416.
Jiang, H., Gomez-abal, R.I., Rinke, P., Scheffler, M., Electronic band structure of zirconia and hafnia polymorphs from the GW perspective. Phys. Rev. B 81 (2010), 1–9, 10.1103/PhysRevB.81.085119.
Gole, J.L., Stout, J.D., Burda, C., Lou, Y., Chen, X., Highly efficient formation of visible light tunable TiO2-xNx photocatalysts and their transformation at the nanoscale. J. Phys. Chem. B 108 (2004), 1230–1240, 10.1021/jp030843n.
Kohut, A., Ranjan, S., Voronov, A., Peukert, W., Tokarev, V., Bednarska, O., Gevus, O., Voronov, S., Design of a new invertible polymer coating on a solid surface and its effect on dispersion colloidal stability. Langmuir 22 (2006), 6498–6506, 10.1021/la060162u.
Zhitomirsky, I., Petric, A., Electrophoretic deposition of electrolyte materials for solid oxide fuel cells. J. Mater. Sci. 39 (2004), 825–831, 10.1023/B:JMSC.0000012910.70526.61.
Ferrari, B., González, S., Moreno, R., Baudín, C., Multilayer coatings with improved reliability produced by aqueous electrophoretic deposition. J. Eur. Ceram. Soc. 26 (2006), 27–36, 10.1016/j.jeurceramsoc.2004.10.018.
Feng, M., Gu, C., Bao, C., Chen, X., Yan, H., Shi, Z., Liu, X., Lin, Q., Synthesis of a benzyl-grafted alginate derivative and its effect on the colloidal stability of nanosized titanium dioxide aqueous suspensions for Pickering emulsions. RSC Adv. 8 (2018), 34397–34407, 10.1039/C8RA04300K.
Gebauer, J.S., Mackert, V., Ognjanović, S., Winterer, M., Tailoring metal oxide nanoparticle dispersions for inkjet printing. J. Colloid Interface Sci. 526 (2018), 400–409, 10.1016/j.jcis.2018.05.006.
Van der Biest, O.O., Vandeperre, L.J., Electrophoretic deposition of materials. Annu. Rev. Mater. Sci. 29 (1999), 327–352, 10.1146/annurev.matsci.29.1.327.
