The effects of wet impregnation and sol-gel methods and presence of competitive hydrocarbons on oxidation of dibenzothiophene over titanium-silica nanocatalyst

Document Type : Research Article

Authors

1 Department of Chemical, Petroleum, and Gas Engineering, Iran University of Science and Technology, Tehran, Iran

2 Energy and Environment Research Center, Niroo Research Institute

Abstract

Oxidative desulfurization process using heterogeneous catalysts is considered as a complementary and promising method for hydrodesulfurization of liquid hydrocarbon fuels to remove their sulfur-resistant compounds. In this research, a titania-silica catalyst with a 10 wt.% loading of titania as the active phase was synthesized using two methods, i.e., sol-gel and wet impregnation, and the performance in the oxidative desulfurization of dibenzothiophene was investigated and compared. Oxidative desulfurization was carried out at a low temperature of 50°C, atmospheric pressure, an O/S molar ratio of 5, and a catalyst loading of 0.3 g per 3 g of fuel. To better identify the physico-chemical characteristics of the catalysts and find the structure-performance relationship, analytical techniques such as nitrogen adsorption-desorption, Fourier-transform infrared spectroscopy, X-ray fluorescence, and X-ray diffraction were employed. By comparing the performance of the catalyst samples, it was found that the conversion of dibenzothiophene in the presence of the catalyst prepared by the sol-gel method was higher, achieving 100% conversion within a short reaction time of 30 minutes. Furthermore, the effect of the presence of competitive nitrogen-containing compounds (indole and quinoline) and olefin (cyclohexene) on the oxidative desulfurization of dibenzothiophene with the optimized catalyst was evaluated. The highest and lowest negative effects were observed for cyclohexene and quinoline, respectively.

Keywords

Main Subjects

References

[1] Gupta N., Roychoudhury P.K., Deb J.K., Biotechnology of Desulfurization of Diesel: Prospects and Challenges, Appl. Microbiol. Biotechnol. 66: 356–366 (2005).
[2] Song C., Ma X., New Design Approaches to Ultra-Clean Diesel Fuels by Deep Desulfurization and Deep Dearomatization, Appl. Catal. B Environ. 41: 207–238 (2003).
[3] Zhang L., Wang J., Sun Y., Jiang B., Yang H., Deep Oxidative Desulfurization of Fuels by Superbase-Derived Lewis Acidic Ionic Liquids, Chem. Eng. J. 328: 445–453 (2017).
[4] Palomeque J., Clacens J.-M., Figueras F., Oxidation of Dibenzothiophene by Hydrogen Peroxide Catalyzed by Solid Bases, J. Catal. 211: 103–108 (2002).
[5] Subhan S., Rahman A.U., Yaseen M., Rashid H.U., Ishaq M., Sahibzada M., Tong Z., Ultra-Fast and Highly e ffi Cient Catalytic Oxidative Desulfurization of Dibenzothiophene at Ambient Temperature Over Low Mn Loaded Co-Mo/Al2O3 and Ni-Mo/Al2O3 Catalysts Using NaClO as Oxidant, Fuel. 237: 793–805 (2019).
[6] Bazyari A., Khodadadi A.A., Mamaghani A.H., Beheshtian J., Thompson L.T., Mortazavi Y., Microporous Titania–Silica Nanocomposite Catalyst-Adsorbent for Ultra-Deep Oxidative Desulfurization, Appl. Catal. B Environ. 180: 65–77 (2016).
[7] Wei S., He H., Cheng Y., Yang C., Zeng G., Kang L., Qian H., Zhu C., Preparation, Characterization, and Catalytic Performances of Cobalt Catalysts Supported on KIT-6 Silicas in Oxidative Desulfurization of Dibenzothiophene, Fuel. 200: 11–21 (2017).
[8] Caero L.C., Hernández E., Pedraza F., Murrieta F., Oxidative Desulfurization of Synthetic Diesel Using Supported Catalysts: Part I. Study of the Operation Conditions With a Vanadium Oxide Based Catalyst, Catal. Today. 107: 564–569 (2005).
[9] Moghaddam M.S., Towfighi J., Synthesis of Vanadium Catalysts Supported on Cerium Containing TiO2 Nanotubes for the Oxidative Dehydrogenation of Propane 1, 58: 659–665 (2018).
[10] Wang H., Shi C., Chen S., Chen R., Sun P., Chen T., Accepted, J., Hierarchically Mesoporous Titanosilicate Single- Crystalline Nanospheres for Room-Temperature Oxidative-Adsorptive Desulfurization, (2019). doi:10.1021/acsanm.9b01496.
[11] Rivoira L.P., Valles V.A., Ledesma B.C., V Ponte M., Martínez M.L., Anunziata O.A. Beltramone, A.R., Sulfur Elimination by Oxidative Desulfurization with Titanium-Modified SBA-16, Catal. Today. 271: 102–113 (2016).
[12] Hilonga A., Kim J.-K., Sarawade P.B., Kim H.T., Mesoporous Titania–Silica Composite from Sodium Silicate and Titanium Oxychloride. Part II: One-Pot Co-Condensation Method, J. Mater. Sci. 45: 1264–1271 (2010).
[13] Zhang X., Zhang F., Chan K.-Y., Synthesis of Titania–Silica Mixed Oxide Mesoporous Materials, Characterization and Photocatalytic Properties, Appl. Catal. A Gen. 284: 193–198 (2005).
[14] Torres-García E., Galano A., Rodriguez-Gattorno G., Oxidative Desulfurization (ODS) of Organosulfur Compounds Catalyzed by Peroxo-Metallate Complexes of WOx–ZrO2: Thermochemical, Structural, and Reactivity Indexes Analyses, J. Catal. 282: 201–208 (2011).
[15] Bu J., Loh G., Gwie C.G., Dewiyanti S., Tasrif M., Borgna A., Desulfurization of Diesel Fuels by Selective Adsorption on Activated Carbons: Competitive Adsorption of Polycyclic Aromatic Sulfur Heterocycles and Polycyclic Aromatic Hydrocarbons, Chem. Eng. J. 166: 207–217 (2011).
[16] Koivikko N., Laitinen T., Mouammine A., Ojala S., Keiski R.L., Catalytic Activity Studies of Vanadia / Silica – Titania Catalysts in SVOC Partial Oxidation to Formaldehyde : Focus on the Catalyst Composition, (2018). doi:10.3390/catal8020056.
[17] Qiu L., Cheng Y., Yang C., Zeng G., Long Z., Wei S., Zhao K., Luo L., Oxidative Desulfurization of Dibenzothiophene Using a Catalyst of Molybdenum Supported on Modified Medicinal Stone, Rsc Adv. 6: 17036–17045 (2016).
[18] Zhang X., Zhu Y., Huang P. Zhu M., Phosphotungstic Acid on Zirconia-Modified Silica as Catalyst for Oxidative Desulfurization, RSC Adv. 6: 69357–69364 (2016).
[19] Kumar S., Srivastava V.C., Badoni R.P., Oxidative Desulfurization of Dibenzothiophene by Zirconia-Based Catalysts, Int. J. Chem. React. Eng. 12: 295–302 (2014).
[20] Xiao J., Wu L., Wu Y., Liu B., Dai L., Li Z., Xia Q., Xi H., Effect of Gasoline Composition on Oxidative Desulfurization Using a Phosphotungstic Acid/Activated Carbon Catalyst with Hydrogen Peroxide, Appl. Energy. 113: 78–85 (2014).
[21] Liu W., Liu X., Yang Y., Zhang Y., Xu B., Selective Removal of Benzothiophene and Dibenzothiophene from Gasoline Using Double-Template Molecularly Imprinted Polymers on the Surface of Carbon Microspheres, Fuel. 117: 184–190 (2014).
[22] Caero L.C., Jorge F., Navarro A., Gutiérrez-Alejandre A., Oxidative Desulfurization of Synthetic Diesel Using Supported Catalysts: Part II. Effect of Oxidant and Nitrogen-Compounds on Extraction–Oxidation Process, Catal. Today. 116: 562–568 (2006).
[23] Rafiee E., Rahpeyma N., Selective Oxidation of Sulfurs and Oxidation Desulfurization of Model Oil by 12-Tungstophosphoric Acid on Cobalt-Ferrite Nanoparticles as Magnetically Recoverable catalyst, Chinese J. Catal. 36: 1342–1349 (2015).
[24] Bhadra B.N., Song J.Y., Uddin N., Khan N.A., Kim S., Choi C.H., Jhung S.H., Oxidative Denitrogenation with TiO2@ Porous Carbon Catalyst for Purification of Fuel: Chemical Aspects, Appl. Catal. B Environ. 240: 215–224 (2019).
[25] Sugi Y., Shape‐Selective Alkylation of Naphthalene Over Zeolites: Steric Interaction of Reagents With Zeolites, J. Chinese Chem. Soc. 57: 1–13 (2010).
[26] Khademian F., Bazyari A., Haghighi P., Thompson L.T., Enhanced oxidative desulfurization of dibenzothiophene in the presence of cyclohexene, indole, quinoline, and p-xylene using surface-silylated titania-silica catalyst, Fuel 344: 128022–128036 (2023).

Files

Share

How to cite

Statistics