Synthesis and Characterization of Iron Oxide Nanoparticles Supported on Ziconia and Its Application in the Gas-Phase Oxidation of Cyclohexanol to Cyclohexanone

Abstract

Iron oxide nanoparticles supported on zirconia were prepared by precipitation-deposition method and characterized by XRD, SEM, FT-IR, TGA/DTA, surface area and particle size analysis. Catalytic activities of the catalysts were tested in the gas-phase conversion of cyclohexanol in a fixed-bed flow type, Pyrex glass reactor, at 433 - 463 K. Major detected products were cyclohexanone, cyclohexene and benzene, depending on the used catalyst. The rate of reaction was significantly raised by the introduction of molecular oxygen in the feed gas, thereby suggesting the oxidation of cyclohexanol to cyclohexanone. Furthermore, the catalytic activity of iron oxide nanoparticles supported on zirconia treated with hydrogen at 553 K for 2 hours, was more selective and better than the unreduced iron oxide nanoparticles supported on zirconia, in the gas-phase oxidation of cyclohexanol to cyclohexanone. Experimental results showed that there was no leaching of metal, and that the catalyst was thus truly heterogeneous.

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M. Sadiq, G. Zamin, R.   and M. Ilyas, "Synthesis and Characterization of Iron Oxide Nanoparticles Supported on Ziconia and Its Application in the Gas-Phase Oxidation of Cyclohexanol to Cyclohexanone," Modern Research in Catalysis, Vol. 3 No. 1, 2014, pp. 12-17. doi: 10.4236/mrc.2014.31003.

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1] [1] R. M. Cornell and U. Schwertmann, “The Iron Oxides: Structure, Properties, Reactions, Occurrences and Uses,” 2nd Edition, Wiley-VCH, Weinheim, 2003.
http://dx.doi.org/10.1002/3527602097
[2] M. Azharuddin, H. Tsuda, S. Wu and E. Sasaoka, “Catalytic Decomposition of Biomass Tars with Iron Oxide Catalysts,” Fuel, Vol. 87, No. 4-5, 2008, pp. 451-459.
http://dx.doi.org/10.1016/j.fuel.2007.06.021
[3] C. Li, Y. Shen, M. Jia, S. Sheng, M. O. Adebajo and H. Zhu, “Catalytic Combustion of Formaldehyde on Gold/ Iron-Oxide Catalysts,” Catalysis Communications, Vol. 9, No. 3, 2008, pp. 355-361.
http://dx.doi.org/10.1016/j.catcom.2007.06.020
[4] K. Choavarit, K. Tossapol, P. Phairat, C. Sumateand S. Ekasith, “Synergistic Activities of Magnetic Iron-Oxide Nanoparticles and Stabilizing Ligands Containing Ferrocene Moieties in Selective Oxidation of Benzyl Alcohol,” Catalysis Communications, Vol. 26, 2012, pp. 1-5.
http://dx.doi.org/10.1016/j.catcom.2012.04.016
[5] R. J. Zhang, J. J. Huang, H. T. Zhao, Z. Q. Sun and Y. Wang, “Sol-Gel Auto-Combustion Synthesis of Zinc Ferrite for Moderate Temperature Desulfurization,” Energy & Fuels, Vol. 21, 2007, pp. 2682-2687.
[6] C. T. Wang and R. J. Willey, “Oxidation of Methanol over Iron Oxide Based Aerogels in Supercritical CO2,” Journal of Non-Crystalline Solids, Vol. 225, 1998, pp. 173-177.
http://dx.doi.org/10.1016/S0022-3093(98)00040-4
[7] S. Al-Sayari, A. F. Carley, S. H. Taylor and G. J. Hutchings, “Au/ZnO and Au/Fe2O3 Catalysts for CO Oxidation at Ambient Temperature: Comments on the Effect of Synthesis Conditions on the Preparation of High Activity Catalysts Prepared by Coprecipitation,” Topics in Catalysis, Vol. 44, No. 1-2, 2007, pp. 123-128.
http://dx.doi.org/10.1007/s11244-007-0285-9
[8] Y. Wang and B. H. Davis, “Fischer-Tropsch Synthesis. Conversion of Alcohols over Iron Oxide and Iron Carbide Catalysts,” Applied Catalysis A: General, Vol. 180, No. 1-2, 1999, pp. 277-285.
http://dx.doi.org/10.1016/j.apcatb.2005.10.039
[9] F. M. Bautista, J. M. Campelo, D. Luna, J. M. Marinas, R. A. Quiros and A. A. Romero, “Screening of Amorphous Metal-Phosphate Catalysts for the Oxidative Dehydrogenation of Ethylbenzene to Styrene,” Applied Catalysis B: Environmental, Vol. 70, No. 1-4, 2007, pp. 611-620.
http://dx.doi.org/10.1016/j.apcatb.2005.10.039
[10] V. R. Pradhan, D. E. Herrick, J. W. Tierney and I. Wender, “Finely Dispersed Iron, Iron-Molybdenum, and Sulfated Iron Oxides as Catalysts for Coprocessing Reactions,” Energy & Fuels, Vol. 5, No. 5, 1991, pp. 712-720.
http://dx.doi.org/10.1021/ef00029a015
[11] V R. Pradhan, J. Hu, J. W. Tierney and I. Wender, “Activity and Characterization of Anion-Modified Iron(III) Oxides as Catalysts for Direct Liquefaction of Low Pyrite Coals,” Energy & Fuel, Vol. 7, No. 4, 1993, pp. 446-454.
http://dx.doi.org/10.1021/ef00040a002
[12] G. T. Hager, E. N. Givens and F. J. Derbyshire, “The Activity of Nanoscale Iron Oxide for Model Compounds Reactions,” ACS-Division of Fuel Chemistry Preprints, Vol. 38, 1993, pp. 1087-1096.
[13] Z. Zhong, J. Ho, J. Teo, S. Shen and A. Gedanken, “Synthesis of Porous Alpha-Fe2O3 Nanorods and Deposition of Very Small Gold Particles in the Pores for Catalytic Oxidation of CO,” Chemistry of Materials, Vol. 19, No. 19, 2007, pp. 4776-4780.
http://dx.doi.org/10.1021/cm071165a
[14] A. K. Kandalam, B. Chatterjee, S N. Khanna, B. K. Rao, P. Jena and B. V. Reddy, “Oxidation of CO on Fe2O3 Model Surfaces,” Surface Science, Vol. 601, No. 21, 2007, pp. 4873-4880.
http://dx.doi.org/10.1016/j.susc.2007.08.015
[15] H. Martin, H. Pavla and P. Jiri, “Quasi-Isothermal Decomposition: A Way to Nanocrystallinemesoporous Like Fe2O3 Catalyst for Rapid Heterogeneous Decomposition of Hydrogen Peroxide,” Journal of Materials Chemistry, Vol. 20, 2010, pp. 3709-3715.
http://dx.doi.org/10.1039/c000632g
[16] T. L. Jorgensen, H. Livbjerg and P. Glarborg, “Homogeneous and Heterogeneously Catalyzed Oxidation of SO2,” Chemical Engineering Science, Vol. 62, No. 16, 2007, pp. 4496-4499. http://dx.doi.org/10.1016/j.ces.2007.05.016
[17] M. L. Peterson, J. G. E. Brown, G. A. Parks and C. L. Stein, “Differential Redox and Sorption of Cr(III/VI) on Natural Silicate and Oxide Minerals: EXAFS and XANES Results,” Geochimica et Cosmochimica Acta, Vol. 61, No. 16, 1997, pp. 3399-3412.
http://dx.doi.org/10.1016/S0016-7037(97)00165-8
[18] S. Zhou, M. Johnson and J. G. C. Veinot, “Iron/Iron Oxide Nanoparticles: A Versatile Support for Catalytic Metals and Their Application in Suzuki-Miyaura Cross-Coupling Reactions,” Chemical Communications, Vol. 46, No. 14, 2010, pp. 2411-2413.
http://dx.doi.org/10.1039/b922462a
[19] M. Ilyas and M. Sadiq, “Liquid Phase Aerobic Oxidation of Benzyl Alcohol Catalyzed by Pt/ZrO2,” Chemical Communications, Vol. 30, No. 10, 2007, pp. 1391-1397.
http://dx.doi.org/10.1002/ceat.200700072
[20] Y. P. Ji, G. O. Seong and H. H. Baik, “Characterization of Imn01I) Oxide Nanoparticles Prepared Ammonium Acetate as Precipitating Agent,” Korean Journal of Chemical Engineering, Vol. 18, 2001, pp. 215-219.
[21] W. Damien, D. Olivier, P. Fabrice and A. Denis, “Alaboratory Study of the Reduction of Iron Oxides,” In: F. Kongoli and R. G. Reddy, Eds., Proceedings of Hydrogensohn International Symposium, San Diego, 27-31 August 2006, p. 111.
[22] H. E. Ghandoor, H. M. Zidan, M. M. H. Khalil and M. I. M. Ismail, “Synthesis and Some Physical Properties of Magnetite (Fe3O4) Nanoparticles,” International Journal of Electrochemical Science, Vol. 7, 2012, pp. 5734-5745.
[23] D. M. Sherman and T. D. Waite, “Electronic Spectra of Fe3+ Oxides and Oxide Hydroxides in the near IR to near UV,” American Mineralogist, Vol. 70, 1985, pp. 1262-1269.
[24] H. Jung, H. Park, J. Kim, J. H. Lee, H. G. Hur, N. V. Myung and H. Choi, “Preparation of Biotic and Abiotic Iron Oxide Nanoparticles (IOnPs) and Their Properties and Applications in Heterogeneous Catalytic Oxidation,” Environmental Science & Technology, Vol. 41, No. 13, 2007, pp. 4741-4747.
http://dx.doi.org/10.1021/es0702768
[25] S. T. Amyn and K. Pei-Yoong, “Synthesis, Properties, and Application of Magnetic Iron Oxide Nanoparticles,” Progress in Crystal Growth and Characterization of Materials, Vol. 55, No. 1-2, 2009, pp. 22-45.
http://dx.doi.org/10.1016/j.pcrysgrow.2008.08.003
[26] S. M. Chaudhari, A. S. Waghulde, V. Samuel, M. L. Bari and V. R. Chumbhale, “Characterization of ZnO and Mo-dified ZnO Catalysts for Anaerobic Oxidation of Cyclohexanol,” Research Journal of Chemical Sciences, Vol. 3, 2013, pp. 38-44.
[27] H. I. Rekkab, B. A. Choukchou, R. L. Pirault and C. Kappenstein, “Catalytic Oxidation of Cyclohexane to Cyclohexanone and Cyclohexanol by Tert-Butyl Hydroperoxide over Pt/Oxide Catalysts,” Bulletin of Materials Science, Vol. 34, No. 5, 2011, pp. 1127-1135.
http://dx.doi.org/10.1007/s12034-011-0157-6
[28] M. Dominique and D. Daniel, “Evaluation of the AcidBase Surface Properties of Several Oxides and Supported Metal Catalysts by Means of Model Reactions,” Journal of Molecular Catalysis A: Chemical, Vol. 118, No. 1, 1997, pp. 113-128.
http://dx.doi.org/10.1016/S1381-1169(96)00371-8
[29] F. M. Bautista, J. M. Campelo, A. Garcia, D. Luna, J. M. Marinas, R. A. Quiros and A. A. Romero, “Influence of Acid-Base Properties of Catalysts in the Gas-Phase Dehydration-Dehydrogenation of Cyclohexanol on Amorphous AlPO4 and Several Inorganic Solids,” Applied Catalysis A: General, Vol. 243, No. 1, 2003, pp. 93-107.
http://dx.doi.org/10.1016/S0926-860X(02)00540-9

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