Abstract
A composite zeolite HY/SBA-15 has been synthesized by an overgrowth approach, and then doped with Ce by a liquid phase ion exchange process to form the Ce modified HY/SBA-15 catalyst. The synthesized materials were examined by X-ray diffraction (XRD), nitrogen adsorption–desorption, transmission electron microscopy (TEM), BJH analysis and pyridine adsorption Fourier-transform infrared spectroscopy (Py-FTIR). The results showed the existence of two different pores sizes of 1.8 and 6 nm. Thus, the HY/SBA-15 composite includes both microporous and mesoporous structures. Desulfurization activity of the composite materials was evaluated using as simulated oil gas. The results showed that the SOx adsorption capacity of Ce-HY/SBA-15 was enhanced by 1.97 mg/g compared to HY/SBA-15, which suggested that the Ce plays an important role in the desulfurization of simulated oil over composite zeolite. Furthermore, the Py-FTIR results revealed the relationship between the surface acids and the desulfurization performance. It was found that the weak Lewis acids were important for the improved desulfurization performance, while the Brönsted acids inhibited the desulfurization performance.
Similar content being viewed by others
References
I.V. Babich, J.A. Moulijn, Science and technology of novel processes for deep desulfurization of oil refinery streams: a review. Fuel 82, 607–631 (2003)
F. Subhan, B.S. Liu, Y. Zhang, High desulfurization characteristic of lanthanum loaded mesoporous MCM-41 sorbents for diesel fuel. Fuel Process. Technol. 97, 71–78 (2012)
W.Y. Wang, M.X. Pan, Y.C. Qin, L.T. Wang, L.J. Song, Effects of surface acidity on the adsorption desulfurization of Cu(I)Y zeolites. Acta Phys.-Chim. Sin. 27, 1176–1180 (2011)
C. Song, An overview of new approaches to deep desulfurization for ultra-clean gasoline, diesel fuel and jet fuel. Catal. Today 86(1), 211–263 (2003)
X.L. Ma, S. Velu, J.H. Kim, C.S. Song, Deep desulfurization of gasoline by selective adsorption over solid adsorbents and impact of analytical methods on ppm-level sulfur quantification for fuel cell applications. Appl. Catal. B Environ. 56, 137–147 (2005)
A.Z. He, H.G. Liu, K. Wang, Y. Zhao, L. Wang, Research progress of light fuel oil desulfurization technology. Ind. Catal. 18, 8–12 (2010)
T.W. Kim, M.J. Kim, F. Kleitz, M.M. Nair, R. Guillet-Nicolas, K.E. Jeong, H.J. Chae, C.U. Kim, S.Y. Jeong, Tailor-made mesoporous Ti-SBA-15 catalysts for oxidative desulfurization of refractory aromatic sulfur compounds in transport fuel. Chem. Cat. Chem. 4, 687–697 (2012)
F.P. Tian, W. Wu, Z.X. Jiang, C.H. Liang, Y.X. Yang, P.L. Ying, X.P. Sun, T.X. Cai, C. Li, The study of thiophene adsorption onto La (III)-exchanged zeolite NaY by FT-IR spectroscopy. J. Colloid Interface Sci. 301, 395–401 (2006)
Y.H. Chang, B.Q. Dai, D.Q. Wang, F.M. Sun, R. Tian, Synthesis and application of MCM-41-HY composite with mesoporous and microporous structure. Acta Petrol. Sin. 25, 835–840 (2009)
X.J. Zhang, G. Wang, F.M. Sun, Z.S. Yuan, Z.X. Wang, Novel miroporous mesoporous composite hydrocracking catalysts. J. Daqing Petrol. Inst. 32, 75–78 (2008)
B.Q. Wu, J. Shen, Q.R. Zhang, Characterization and catalytic application of HY-SBA-15 composite molecular sieves. J. Fuel Chem. Technol. 40, 732–736 (2012)
C. Han, H.P. Li, T.F. Cai, H. Zhao, H.J. Dong, X.Q. Qi, Preparation and characterization of ZSM-5/SBA-15 catalytic oxidation desulfurization catalyst and its desulfurization performance. Appl. Chem. Ind. 11, 2068–2071 (2015)
S.H. Yin, S.W. Li, B. Zhang, J.H. Peng, L.B. Zhang, Mass transfer kinetics of lanthanum (III) extraction in the presence of two complexing agents by D2EHPA using a constant interfacial area cell with laminar flow. Chem. Eng. Res. Des. 104, 92–97 (2015)
S.H. Yin, S.W. Li, F. Xie, L.B. Zhang, J.H. Peng, Study on the aqueous solution behavior and extraction mechanism of Nd(III) in the presence of a complexing agent lactic acid with di-(2-ethylhexyl) phosphoric acid. RSC Adv. 5, 64550–64556 (2015)
S.H. Yin, L.B. Zhang, J.H. Peng, S.W. Li, S.H. Ju, L.H. Zhang, Microfluidic solvent extraction of La(III) with 2-ethylhexyl phosphoric acid-2-ethylhexyl ester (P507) by a microreactor. Chem. Eng. Process. 91C, 1–6 (2015)
Z.Q. Cai, W.Y. Ma, X. Hou, S.J. Li, Improved synthesis of dabigatran etexilate. Fine Chem. 32, 308–311 (2015)
W.Y. Yu, Y.J. Ruan, Y.C. Qin, F. Yin, Y.C. Fan, L.J. Song, Preparation of HY/MCM-41 composite and application in adsorption desulfurization. J. Petrol. Univ. 27, 41–47 (2014)
C.M. Song, Z.F. Yan, H.P. Wang, J. Jiang, K. Qiao, Synthesis of MCM-41-type composite materials using alkali-treated ZSM-5 zeolite. J. Petrol. Univ. 30, 113–117 (2006)
Y. Zhang, D. Wu, Y.H. Sun, S.Y. Peng, Synthesis of micropore-mesopore composite silica-alumina molecular sieves. J. Fuel Chem. Technol. 28, 28–29 (2001)
Z.M. Tian, Q.G. Deng, D.F. Zhao, Synthesis and catalytic performance of Cerium Modified SBA-15 mesoporous molecular sieves. J Petrochem. Univ. 32, 18–21 (2008)
C.W. Shi, W.Y. Wu, X. Bian, X. Wang, J.H. Li, S.L. Zhao, P. Chen, Y.T. Bai, W.Y. Yang, Study on hydrothermal synthesis and characterization of Ce-Y/SBA-15 composite materials. Asian J. Chem. 27, 1857–1860 (2015)
J. Wang, Y.S. Jin, Y.H. Zhou, J.B. Mo, Catalytic activity of double-metal-modified HZSM-5 catalyst for methanol to olefins. Appl. Chem. Ind. 5, 20–24 (2012)
G.S. Lin, H. Dai, S.Y. Chang, Y.K. Zhao, Y.M. Wang, D.X. Yang, The influence of the modification with Ce on the performance of molecular sieve precious metals. Precious Met. 34, 30–34 (2013)
C.W. Shi, Microwave synthesis, characterization and catalytic properties of Ce doped on Y/SBA-15 microporous and mesoporous composite molecular sieves. Northeast. Univ. 88–90 (2015)
D. Solís, A.L. Agudo, J. Ramírez, Hydrodesulfurization of hindered dibenzothiophenes on bifunctional NiMo catalysts supported on zeolite-alumina composites. Catal. Today 116, 469–477 (2006)
S. Kowalak, E. Szymkowiak, M. Łaniecki, Catalytic properties of zeolite CeY modified with NH4F. J. Fluor. Chem. 93, 175–180 (1999)
M. Jiang, Y.L. Fu, Characterization of Cu(I)Y zeolites prepared by solid-state ion exchange. Acta Phys. Chim. Sin. 13, 822–826 (1997)
C.Z. Lin, X.H. Cai, Y.C. Xie, Study of dispersion state of CuCl2 onto the surface of NaY zeolite. Acta Phys. Chim. Sin. 12, 523–528 (1996)
Acknowledgments
We thank the Research Fund for the Doctoral Program of Higher Universities (20100042110008), Found for Research Project of Education and Teaching Reform of Liaoning Shihua University (20165230080023), Found for Liaoning Shihua University Students Innovation and Entrepreneurship (2016008) and Supported by talent scientific research fund of LSHU.
Authors’ contribution
Chun-Wei Shi, Wen-Yuan Wu and Xue Bian conceived and designed the experiments. Chun-Wei Shi, Yongfu Wu and Wen-Yi Chen performed the experiments and analyzed the data. Chun-Wei Shi, Yongfu Wu, Wen-Yi Chen, Wen-Yuan Wu, Xue Bian, Shan-Lin Zhao and Mingyuan Pei wrote the paper.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The author stated that there was no conflict of interest.
Rights and permissions
About this article
Cite this article
Shi, CW., Wu, Y., Chen, WY. et al. Synthesis and characteristics of Ce modified HY/SBA-15 and its desulfurization performance for simulated oil. J Porous Mater 24, 381–388 (2017). https://doi.org/10.1007/s10934-016-0271-3
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10934-016-0271-3