酸催化及竞争吸附对CeY分子筛吸附脱硫性能的影响

doi:10.3866/PKU.WHXB201401021

Abstract

Abstract:

The effects of olefin and aromatic hydrocarbons, as well as the acidic catalytic reactions on the adsorption desulfurization performance of CeY zeolites prepared by liquid phase ion exchange (LPIE) technique were systemically investigated. The capacities of sulfur removal were measured by fixed-bed breakthrough experiments. It is shown that the desulfurization performance of the adsorbents is reduced by olefin and aromatic hydrocarbons in model gasoline with olefin having a more significant effect. In-situ Fourier transform infrared (FTIR) spectroscopy was used to study the adsorption of thiophene, cyclohexene, and benzene on the zeolites. The effects of the olefin and aromatic hydrocarbons differed. For the olefins, the desulfurization capacity of the CeY adsorbents depends on the surface acidity of the zeolites, particularly on the Brönsted acidity. Protonation of olefin and thiophene compounds can be found at Brönsted acidic sites. It is the oligomerization of the protonated species that decrease the adsorption of other thiophenes. It is, therefore, the acidic catalytic reactions caused by the strong Brönsted acidity on the adsorbent surface that could be the dominant factor for olefin hydrocarbons. While for the aromatic hydrocarbons, the decreased desulfurization capacity can be ascribed to the competitive adsorption on the active sites by π-complexation between the organic sulfur compounds and arenes.

Key words: Adsorption desulfurization, Brö, nsted acidity, π-complexation, Protonization, Oligomerization

MSC2000:

O643

QIN Yu-Cai, GAO Xiong-Hou, DUAN Lin-Hai, FAN Yue-Chao, YU Wen-Guang, ZHANG Hai-Tao, SONG Li-Juan. Effects on Adsorption Desulfurization of CeY Zeolites：Acid Catalysis and Competitive Adsorption[J].Acta Phys. -Chim. Sin., 2014, 30(3): 544-550.

References

(1) Yang, R. T.; Hernández-Maldonado, A. J.; Yang, F. H. Science 2003, 301 (5629), 79. doi: 10.1126/science.1085088
(2) Velu, S.; Ma, X. L.; Song, C. S.; Namazian, M.; Sethuraman, S.; Venkataraman, G. Energy Fuels 2005, 19 (3), 1116. doi: 10.1021/ef049800b
(3) Jeevanandam, P.; Klabunde, K. J.; Tetzler, S. H. Microporous Mesoporous Mat. 2005, 79 (1), 101.
(4) Nair, S.; Tatarchuk, B. J. Fuel 2010, 89 (11), 3218. doi: 10.1016/j.fuel.2010.05.006
(5) Santos, A. L.; Reis, R. A.; Rossa, V.; Reis, M. M.; Costa, A. L. H.; Veloso, C. O.; Henriques, C. A.; Zotin, F. M. Z.; Paredes, M. L. L.; Silveira, E. B.; Chiaro, S. S. X. Mater. Lett. 2012, 83, 158. doi: 10.1016/j.matlet.2012.06.011
(6) Marín-Rosas, C.; Ramírez-Verduzco, L. F.; Murrieta-Guevara, F. R.; Hernández-Tapia, G.; Rodríguez-Otal, L. M. Ind. Eng. Chem. Res. 2010, 49 (9), 4372. doi: 10.1021/ie901756b
(7) Seredych, M.; Bandosz, T. J. Fuel Process. Technol. 2010, 91 (6), 693. doi: 10.1016/j.fuproc.2010.01.019
(8) Fallah, R. N.; Azizian, S. Fuel Process. Technol. 2012, 93 (1), 45. doi: 10.1016/j.fuproc.2011.09.012
(9) Park, J. G.; Ko, C. H.; Yi, K. B.; Park, J.; Han, S.; Cho, S.; Kim, J. Appl. Catal. B: Environ. 2008, 81 (3), 244.
(10) Subhan, F.; Liu, B.; Zhang, Y.; Li, X. Fuel Process. Technol. 2012, 97, 71. doi: 10.1016/j.fuproc.2012.01.016
(11) Shao, X. C.; Duan, L. H.;Wu, Y. Y.; Qin, Y. C.; Yu,W. G.; Wang, Y.; Li, H. L.; Sun, Z. L.; Song, L. J. Acta Phys. -Chim. Sin. 2012, 28, 1467. [邵新超, 段林海, 武玉叶, 秦玉才, 于文广, 王源, 李怀雷, 孙兆林, 宋丽娟. 物理化学学报, 2012, 28,1467.] doi: 10.3866/PKU.WHXB201203312
(12) Shao, X. C.; Zhang, X. T.; Yu,W. G.;Wu, Y. Y.; Qin, Y. C.; Sun, Z. L.; Song, L. J. Appl. Surf. Sci. 2012, 263, 1. doi: 10.1016/j.apsusc.2012.07.142
(13) Yang, R. T.; Takahashi, A.; Yang, F. H. Ind. Eng. Chem. Res 2001, 40 (26), 6236. doi: 10.1021/ie010729w
(14) Velu, S.; Ma, X. L.; Song, C. S. Ind. Eng. Chem. Res. 2003, 42 (21), 5293. doi: 10.1021/ie020995p
(15) Hernández-Maldonado, A. J.; Yang, R. T. Ind. Eng. Chem. Res. 2003, 42 (1), 123. doi: 10.1021/ie020728j
(16) Hernández-Maldonado, A. J.; Yang, R. T. J. Am. Chem. Soc. 2004, 126 (4), 992.
(17) Hernández-Maldonado, A. J.; Yang, R. T. Ind. Eng. Chem. Res. 2004, 43 (4), 1081. doi: 10.1021/ie034206v
(18) Yang, R. T.; Hernández-Maldonado, A. J. Catal. Rev. -Sci. Eng. 2004, 46 (2), 111. doi: 10.1081/CR-200032697
(19) Hernández-Maldonado, A. J.; Yang, F. H.; Qi, G.; Yang, R. T. Appl. Catal. B: Environ. 2005, 56 (1), 111.
(20) Tang, K.; Song, L. J.; Duan, L. H.; Li, X. Q.; Gui, J. Z.; Sun, Z. L. Fuel Process. Technol. 2008, 89 (1), 1. doi: 10.1016/j.fuproc.2007.06.002
(21) 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.] doi: 10.3866/PKU.WHXB20080933
(22) 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
(23) 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
(24) Lin, L.; Zhang, Y.; Zhang, H.; Lu, F. J. Colloid Interface Sci. 2011, 360, 753. doi: 10.1016/j.jcis.2011.04.075
(25) Wang, H. G.; Song, L. J.; Jiang, H.; Xu, J.; Jin, L. L.; Zhang, X. T.; Sun, Z. L. Fuel Process. Technol. 2009, 90 (6), 835. doi: 10.1016/j.fuproc.2009.03.004
(26) Duan, L. H.; Gao, X. H.; Meng, X. H.; Zhang, H. T.;Wang, Q.; Qin, Y. C.; Zhang, X. T.; Song, L. J. J. Phys. Chem. C 2012, 116 (49), 25748. doi: 10.1021/jp303040m
(27) Shi, Y. C.; Yang, X. J.; Tian, F. P.; Jia, C. Y.; Chen, Y. Y. J. Nat. Gas Chem. 2012, 21 (4), 421. doi: 10.1016/S1003-9953(11)60385-X
(28) Chen, N. Y.; Mitchell, T. O.; Olson, D. H.; Pelrine, B. P. Ind. Eng. Chem. Prod. Res. Dev. 1977, 16 (3), 247. doi: 10.1021/i360063a012
(29) Garcia, C.; Lercher, J. J. Phys. Chem. 1992, 96 (6), 2669. doi: 10.1021/j100185a050
(30) Chica, A.; Strohmaier, K.; Iglesia, E. Langmuir 2004, 20 (25), 10982. doi: 10.1021/la048320+
(31) Richardeau, D.; Joly, G.; Canaff, C.; Magnoux, P.; Guisnet, M.; Thomas, M.; Nicolaos, A. Appl. Catal. A: Gen. 2004, 263 (1), 49. doi: 10.1016/j.apcata.2003.11.039
(32) Deangelis, B. A.; Appierto, G. J. Colloid Interface Sci. 1975, 53(1), 14. doi: 10.1016/0021-9797(75)90029-6
(33) Datka, J.; Sulikowski, B.; Gil, B. J. Phys. Chem. 1996, 100 (27), 11242. doi: 10.1021/jp951523+
(34) Gil, B.; MierzyDska, K.; SzczerbiDska, M.; Datka, J. Microporous Mesoporous Mat. 2007, 99 (3), 328. doi: 10.1016/j.micromeso.2006.09.025
(35) Rabo, J. A.; Angell, C. L.; Kasai, P. H.; Schoemaker, V. Discuss. Faraday Soc. 1966, 41, 328. doi: 10.1039/df9664100328
(36) Ward, J.W. J. Phys. Chem. 1968, 72 (12), 4211. doi: 10.1021/j100858a046
(37) Layman, K. A.; Bussell, M. E. J. Phys. Chem. B 2004, 108 (40), 15791. doi: 10.1021/jp047882z
(38) Garcia, C. L.; Lercher, J. A. J. Phys. Chem. 1992, 96 (6), 2669. doi: 10.1021/j100185a050
(39) Zhang, X. T.; Yu,W. G.; Qin, Y. C.; Dong, S.W.; Pei, T. T.; Wang, L.; Song, L. J. Acta Phys. -Chim. Sin. 2013, 29, 1273. [张晓彤, 于文广, 秦玉才, 董世伟, 裴婷婷, 王琳, 宋丽娟.物理化学学报, 2013, 29, 1273.] doi: 10.3866/PKU.WHXB201303183
(40) Qin, Y. C.; Mo, Z. S.; Yu,W. G.; Dong, S.W.; Duan, L. H.; Gao, X. H.; Song, L. J. Appl. Surf. Sci. 2014, 292, 5. doi: 10.1016/j.apsusc.2013.11.036
(41) Yang, S.; Kondo, J. N.; Domen, K. Catal. Today 2002, 73 (1), 113.
(42) Kukulska-Zajac, E.; Kozyra, P.; Datka, J. Appl. Catal. A: Gen. 2006, 307 (1), 46. doi: 10.1016/j.apcata.2006.03.005

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Effects on Adsorption Desulfurization of CeY Zeolites：Acid Catalysis and Competitive Adsorption

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