Citation: SHAO Xin-Chao, DUAN Lin-Hai, WU Yu-Ye, QIN Yu-Cai, YU Wen-Guang, WANG Yuan, LI Huai-Lei, SUN Zhao-Lin, SONG Li-Juan. Effect of Surface Acidity of CuO-SBA-15 on Adsorptive Desulfurization of Fuel Oils[J]. Acta Physico-Chimica Sinica, ;2012, 28(06): 1467-1473. doi: 10.3866/PKU.WHXB201203312 shu

Effect of Surface Acidity of CuO-SBA-15 on Adsorptive Desulfurization of Fuel Oils

1.
1. Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning ShiHua University, Fushun 113001, Liaoning Province, P. R. China;
2. College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 257061, Shandong Province, P. R. China

Received Date: 27 February 2012
Available Online: 31 March 2012
Fund Project: 国家自然科学基金(20976077, 21076100) (20976077, 21076100) 国家重点基础研究发展规划项目(973) (2007CB216403) (973) (2007CB216403)

Solid-state grinding is a simple and effective technique to incorporate active species into the channels of mesoporous materials with different degrees of filling. Using this method, different concentrations of CuO were loaded into the mesochannels of as-prepared mesoporous silica (APS) and calcined SBA-15 (CS). The samples were prepared and characterized using X-ray diffraction (XRD), N₂ physisorption, and Fourier transform infrared (FTIR) spectroscopy. The relative number of hydroxyl groups was studied by in situ FTIR spectroscopy, and the total surface acidity of the adsorbents was monitored by FTIR spectroscopy at 423 K using pyridine as a probe. Desulfurization of fluid catalytic cracking (FCC) fuel oils using these materials was investigated. The results suggest that CuO interacts directly with support hydroxyl groups to form [Si-O-Cu-O-Si] linkages in the mixtures, which can effectively constrain the condensation of hydroxyl groups in SBA-15 to improve the mesostructure of the adsorbents during calcination. Saturated coverage of the surface of APS is reached using 3 mmol·g^-1 CuO. However, using CS, aggregation of CuO is observed in the material containing 3 mmol·g^-1 of CuO. Both the surface acidity and desulfurization performance significantly increase upon modification of SBA-15 with CuO, and then decrease slowly as the concentration of CuO is increased. The sample containing 3 mmol·g^-1 CuO shows the highest Lewis acidity and desulfurization performance. The Lewis acidity of the adsorbents matches the adsorptive desulfurization performance. It is also demonstrated that reduction of charge density around copper atoms helps to form Lewis acid sites.
- SBA-15 mesoporous material,
- Surface acidity,
- Hydroxyl group,
- Adsorptive desulfurization,
- Lewis acid
1. [1]
  (1) Wang, Y. H.; Yang, R. T. Ind. Eng. Chem. Res. 2009, 48, 142. doi: 10.1021/ie800208g
2. [2]
  (2) Wang, H. G.; Jiang, H.; Xu, J.; Sun, Z. L.; Zhang, X. T.; Zhu, H. L.; Song, L. J. Acta Phys. -Chim. Sin. 2008, 24, 1714. [王洪国, 姜恒, 徐静, 孙兆林, 张晓彤, 朱赫礼, 宋丽娟. 物理化学学报, 2008, 24, 1714.]
3. [3]
  (3) Wang, W. Y.; Pan, M. X.; Qin, Y. C.;Wang, L. T.; Song, L. J. Acta Phys. -Chim. Sin. 2011, 27, 1176. [王旺银, 潘明雪, 秦玉才, 王凌涛, 宋丽娟. 物理化学学报, 2011, 27, 1176.] doi: 10.3866/PKU.WHXB20110442
4. [4]
  (4) Ma, X. L.; Velu, S.; Kim, J. H.; Song, C. S. Appl. Catal. B-Enviro. 2005, 56, 137. doi: 10.1016/j.apcatb.2004.08.013
5. [5]
  (5) Shan, J. H.; Chen, L.; Sun, L. B.; Liu, X. Q. Energy Fuels 2011, 25, 2993.
6. [6]
  (6) Wu, W. Z.; Ren, S. H.; Hou, Y. C.; Jin, M. J. Ind. Eng. Chem. Res. 2011, 50, 998. doi: 10.1021/ie101126a
7. [7]
  (7) Rath, D.; Parida, K. M. Ind. Eng. Chem. Res. 2011, 50, 2839. doi: 10.1021/ie101314f
8. [8]
  (8) Cedeno-Caero, L.; Fabian-Mijan s, L. Ind. Eng. Chem. Res. 2011, 50, 2659. doi: 10.1021/ie100680p
9. [9]
  (9) Song, X. M.; Zhang, W.; Xu, K.; Zhang, Q. A.; Liu, D. L.; Wu, S. Y.; Verpoort, F. Ind. Eng. Chem. Res. 2010, 49, 11760. doi: 10.1021/ie100957k
10. [10]
  (10) Li, W. L.; Xing, J. M.; Xiong, X. C.; Huang, J. X.; Liu, H. Z. Ind. Eng. Chem. Res. 2006, 45, 2845. doi: 10.1021/ie051125l
11. [11]
  (11) Wang, Y. H.; Yang, R. T.; Heinzel, J. M. Chem. Eng. Sci. 2008, 63, 356
12. [12]
  (12) Ju, X. F.; Jin, L. L.; Ma, T.; Chen, X. L.; Song, L. J. Acta Phys. -Chim. Sin. 2009, 25, 2256. [鞠秀芳, 靳玲玲, 马涛, 陈晓陆, 宋丽娟. 物理化学学报, 2009, 25, 2256.] doi: 10.3866/PKU.WHXB20091024
13. [13]
  (13) Hernandez-Maldonado, A. J.; Yang, R. T. Ind. Eng. Chem. Res. 2003, 42, 123. doi: 10.1021/ie020728j
14. [14]
  (14) Zhao, D. Y.; Huo, Q. S.; Feng, J. L.; Chmelka, B. F.; Stucky, G. D. J. Am. Chem. Soc. 1997, 120, 6025.
15. [15]
  (15) Wan, Y.; Zhao, D. Y. Chem. Rev. 2006, 107, 2721.
16. [16]
  (16) Vinu, A.; Kumar, G. S.; Ariga, K.; Murugesan, V. J. Mol. Catal. A-Chem. 2005, 234, 57.
17. [17]
  (17) Zhao, D. Y.; Feng, J. L.; Huo, Q. S.; Melosh, N.; Fredrickson, G. H.; Chmelka, B. F.; Stucky, G. D. Science 1998, 279, 548. doi: 10.1126/science.279.5350.548
18. [18]
  (18) Szegedi, A.; Popova, M.; Minchev, C. J. Mater. Sci. 2008, 44, 6710.
19. [19]
  (19) Yang, J. S.; Jung, W. Y.; Lee, G. D.; Park, S. S.; Hong, S. S. Top. Catal. 2010, 53, 543. doi: 10.1007/s11244-010-9484-x
20. [20]
  (20) Wang, Y. H.; Yang, F. H.; Yang, R. T. Ind. Eng. Chem. Res. 2006, 45, 7649. doi: 10.1021/ie060922w
21. [21]
  (21) Guo, X. Y.; Yin, A. Y.; Dai, W. L.; Fan, K. N. Catal. Lett. 2009, 131, 22.
22. [22]
  (22) Wang, Y. M.; Wu, Z. Y.; Wei, Y. L.; Zhu, J. H. Microporous Mesoporous Mat. 2005, 84, 128.
23. [23]
  (23) Basaldella, E. I.; Tara, J. C.; Armenta, G. A.; Patino-Iglesias, M. E.; Castellon, E. R. J Sol-Gel Sci. Technol. 2006, 37, 141. doi: 10.1007/s10971-006-6434-y
24. [24]
  (24) Wang, Y. M.; Wu, Z. Y.; Shi, L. Y.; Zhu, J. H. Adv. Mater. 2005, 17, 323. doi: 10.1002/adma.200400860
25. [25]
  (25) Sun, Y.; Walspurger, S.; Tessonnier, J. P.; Louis, B.; Sommer, J. Appl. Catal. A -Gen. 2006, 300, 91. doi: 10.1016/j.apcata.2005.09.038
26. [26]
  (26) Mohamed, A. B.; Synthesis, Characterization and Activity of Al-MCM-41 Catalyst for Hydroxyalkylation of Epoxides. Ph. D. Dissertation, University of Teknologi Malaysia, Johor, 2005.
27. [27]
  (27) Wang, X. G.; Lin, K. S. K.; Chan, J. C. C.; Cheng, S. J. Phys. Chem. B 2005, 109, 1763. doi: 10.1021/jp045798d
28. [28]
  (28) Tian, B. Z.; Liu, X. Y.; Yang, H. F.; Xie, S. H.; Yu, C. Z.; Tu, B.; Zhao, D. Y. Adv. Mater. 2003, 15, 1370. doi: 10.1002/adma.200305211
29. [29]
  (29) Zhou, C. F.; Wang, Y. M.; Cao, Y.; Zhuang, T. T.; Huang, W.; Chun, Y.; Zhu, J. H. J. Mater. Chem. 2006, 16, 1520. doi: 10.1039/b514317a
30. [30]
  (30) Wang, Y. M.; Wu, Z. Y.; Zhu, J. H. J. Solid State Chem. 2004, 177, 3815. doi: 10.1016/j.jssc.2004.07.013
31. [31]
  (31) Lopez, N.; Illas, F. J. Phys. Chem. B 1999, 103, 1712. doi: 10.1021/jp9840174
32. [32]
  (32) Lercher, J. A.; Grundling, C.; Eder-Mirth, G. Catal. Today 1996, 27, 343.
33. [33]
  (33) Tanabe K.; Sumiyoshi, T.; Shibata, K.; Kiyoura, T.; Kitagawa, J. Bull. Chem. Soc. Jpn. 1974, 47, 1065.
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