Optimization of Oxidative Desulfurization Reaction with Fe2O3 Catalyst Supported on Graphene Using Box-Behnken Experimental Method

*Hameed Hussein Alwan  -  Chemical Engineering Department, College of engineering, University of Babylon, Iraq
Ammar Ali Ali  -  Water Resources Engineering Department, Al-Qasim Green University, Iraq
Hasan F. Makki  -  Chemical Engineering Department, College of engineering, University of Baghdad, Iraq
Received: 7 Dec 2019; Revised: 23 Dec 2019; Accepted: 27 Dec 2019; Published: 1 Apr 2020; Available online: 28 Feb 2020.
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Abstract

In this study, the catalyst activity of Fe2O3 supported on Graphene for Iraqi gas oil oxidation desulfurization (ODS) by hydrogen peroxide (H2O2) was investigated. The prepared catalyst was synthesized by wet impregnation for ferric nitrate as a Fe2O3 precursor while Graphene represented as catalyst support. The synthesized catalyst was characterized by XRD, FTIR, and EDS analysis. The experiments were designed according to three-level for three variables by Box-Behnken experimental design; Stirring time, catalyst dosage and temperature while the sulfur removal efficiency acts as experiment response. Catalyst activity was studied by ODS reaction for Iraqi gas oil (sulfur content 9400 ppm) at temperature range (40-60 ºC), stirring time (160-240 minutes) and catalyst dosage (0.5-2.5 g), the results show maximum sulfur removal efficiency 90% at stirring time, catalyst dosage and temperature 240 min, 1.5 g, and 60 ºC, respectively. ANOVA analysis shows the important effect of each independent variable on sulfur removal efficiency (response) as following influential order; stirring time, reaction temperature and catalyst dosage. Kinetics calculation showed that the ODS reaction obeys pseudo first-order reaction with reaction rate constant equal 1.0837, 1.5893, and 2.5053 at temperature 40, 50, and 60 ºC, respectively, while activation energy equal 36.26 kJ/mol. Copyright © 2020 BCREC Group. All rights reserved

 

Keywords
Oxidative desulfurization; ODS; Graphene; Design experiment; Box-Behnken; ANOVA

Article Metrics:

  1. Liu, S., Wang, B., Cui, B., Sun, L. (2008). Deep desulfurization of diesel oil oxidized by Fe(VI) systems. Fuel, 87(3), 422–428. doi: 10.1016/j.fuel.2007.05.029.
  2. Mérida-Robles, J., Rodríguez-Castellón, E., Jiménez-López, A. (1999). Characterization of Ni, Mo, and Ni–Mo catalysts supported on alumina-pillared α-zirconium phosphate and reactivity for the thiophene HDS reaction. Journal of Molecular Catalysis A: Chemical, 145(1-2), 169–181. doi:10.1016/s1381-1169(99)00048-5.
  3. Prabhu, N., Dalai, A.K., Adjaye, J. (2011). Hydrodesulphurization and hydrodenitrogenation of light gas oil using NiMo catalyst supported on functionalized mesoporous carbon. Applied Catalysis A: General, 401(1-2), 1–11. doi: 10.1016/j.apcata.2011.04.019.
  4. Babich, I. (2003). Science and technology of novel processes for deep desulfurization of oil refinery streams: a review. Fuel, 82(6), 607–631. doi: 10.1016/s0016-2361(02)00324-1.
  5. Ding, Y., Zhu, W., Li, H., Jiang, W., Zhang, M., Duan, Y., Chang, Y. (2011). Catalytic oxidative desulfurization with a hexatungstate/aqueous H2O2/ionic liquid emulsion system. Green Chemistry, 13(5), 1210-1216. doi: 10.1039/c0gc00787k.
  6. Hao, L., Hurlock, M.J., Li, X., Ding, G., Kriegsman, K.W., Guo, X., Zhang, Q. (2019). Efficient Oxidative Desulfurization Using a Mesoporous Zr-based MOF. Catalysis Today, (Article In Press). doi: 10.1016/j.cattod.2019.04.012.
  7. Caero, L.C., Hernández, E., Pedraza, F., Murrieta, F. (2005). Oxidative desulfurization of synthetic diesel using supported catalysts. Catalysis Today, 107-108, 564–569. doi: 10.1016/j.cattod.2005.07.017.
  8. Bagiyan, G.A., Koroleva, I.K., Soroka, N.V., Ufimtsev, A.V. (2004). Kinetics of the Catalytic Oxidation Reactions of Thiol Compounds in Aqueous Solutions in the Presence of Copper Ions. Kinetics and Catalysis, 45(3), 372-380. doi:10.1023/b: kica.0000032171.81652.91.
  9. Cedeño-Caero, L., Gomez-Bernal, H., Fraustro-Cuevas, A., Guerra-Gomez, H.D., Cuevas-Garcia, R. (2008). Oxidative desulfurization of synthetic diesel using supported catalysts. Catalysis Today, 133-135, 244–254. doi: 10.1016/j.cattod.2007.12.017.
  10. Murata, S., Murata, K., Kidena, K., Nomura, M. (2004). A Novel Oxidative Desulfurization System for Diesel Fuels with Molecular Oxygen in the Presence of Cobalt Catalysts and Aldehydes. Energy & Fuels, 18(1), 116–121. doi: 10.1021/ef034001z.
  11. Makki, H.H., Alwan, H.H. (2019). Synthesis and characterization of Graphene produced from Iraqi date syrup. Association of Arab Universities Journal of Engineering Sciences, 26(1), 49–54.
  12. Ugal, J.R., Jima’a, R.B., Al-Jubori, W.M.K., Abbas, B.F., Al-Jubori, N.M. (2018). Oxidative Desulfurization of Hydrotreated Gas Oil using Fe2O3 and Pd Loaded over Activated Carbon as Catalysts. Oriental Journal of Chemistry, 34(2), 1091–1097. doi:10.13005/ojc/340261.
  13. Mourabet, M., El Rhilassi, A., El Boujaady, H., Bennani-Ziatni, M., Taitai, A. (2017). Use of response surface methodology for optimization of fluoride adsorption in an aqueous solution by Brushite. Arabian Journal of Chemistry, 10, S3292–S3302. doi: 10.1016/j.arabjc.2013.12.028.
  14. Ferreira, S.L.C., Bruns, R.E., Ferreira, H.S., Matos, G.D., David, J.M., Brandão, G.C., da Silva, E.G.P., Portugal, L.A., dos Reis, P.S., Souza, A.S., dos Santos, W.N.L. (2007). Box-Behnken design: An alternative for the optimization of analytical methods. Analytica Chimica Acta, 597(2), 179–186. doi: 10.1016/j.aca.2007.07.011.
  15. Mazaheri, H., Lee, K.T., Bhatia, S., Mohamed, A.R. (2010). Subcritical water liquefaction of oil palm fruit press fiber in the presence of sodium hydroxide: An optimisation study using response surface methodology. Bioresource Technology, 101(23), 9335–9341. doi: 10.1016/j.biortech.2010.07.004.
  16. Lima, S.B., Borges, S.M.S., Rangel, M.d.C., Marchetti, S.G. (2013). Effect of Iron Content on the Catalytic Properties of Activated Carbon-Supported Magnetite Derived from Biomass. Journal of the Brazilian Chemical Society, 24(2), 344–354. doi: 10.5935/0103-5053.20130044.
  17. Al-Saadi, T.M., Jihad, M.A.K. (2015). Preparation and characterization of Graphene / PMMA composite. International Journal of Advanced Research in Science, Engineering and Technology, 2(10), 902-909.
  18. Choi, W., Lahiri, I., Seelaboyina, R., Kang, Y.S. (2010). Synthesis of Graphene and its applications: A review. Critical Reviews in Solid State and Materials Sciences, 35, 52-71.
  19. Mamaghani, A.H., Fatemi, S., Asgari, M. (2013). Investigation of Influential Parameters in Deep Oxidative Desulfurization of Dibenzothiophene with Hydrogen Peroxide and Formic Acid. International Journal of Chemical Engineering, 2013, 1–10. doi: 10.1155/2013/951045.
  20. Fogler, H.S. (2005). Elements of chemical reaction engineering, 4th edition, Prentice Hall, New York, pp. 91.
  21. Choi, A.E., Roces, S., Dugos, N., Wan, M.-W. (2016), Mixing-assisted oxidative desulfurization of model sulfur compounds using plyoxometalate/H2O2 catalytic system. Sustainable Environment Research, 26(4), 184-190. doi: 10.1016/j.serj.2015.11.005.
  22. Huang, P., Luo, G., Kang, L., Zhu, M., Dai, B. (2017). Preparation characterization and catalytic performance of HPW/aEVM catalyst on oxidative desulfurization. RSC Advances, 7, 4681-4687.