纳米薄层HZSM-5分子筛催化甲醇制丙烯

doi:10.3866/PKU.WHXB201401032

Abstract

Abstract:

Nanosheets of HZSM-5 zeolite with different SiO₂/Al₂O₃ molar ratios were synthesized, and their catalytic behavior in the methanol-to-propylene (MTP) reaction was evaluated in a fixed bed reactor. The effect of reaction conditions on catalytic performance was studied in detail. The catalytic performance of nanosheets of HZSM-5 zeolites in the MTP reaction was compared with that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had higher propylene selectivity, total three olefins' selectivity (ethylene, propylene, C₄ alkenes) , and a longer catalytic lifetime than the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite with a SiO₂/Al₂O₃ molar ratio of 213 yielded a propylene selectivity of 46.7%, total three olefins' selectivity of 78.7% at 470 ℃, and a methanol weight hourly space velocity (WHSV) of 3 h^-1. It also yielded a propylene/ethylene mass ratio of 6.5, which was double that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had a lower aromatic selectivity than the nanosized HZSM-5 zeolite. The good MTP catalytic performance of the nanosheets of HZSM-5 zeolite was attributed to their wide (010) surface, high external surface area, and large mesoporous volume.

Key words: Nanosheet, HZSM-5 zeolite, Methanol, Propylene

MSC2000:

O643

ZHANG Shao-Long, ZHANG Lan-Lan, WANG Wu-Gang, MIN Yuan-Yuan, MATong, SONG Yu, GONG Yan-Jun, DOU Tao. Methanol to Propylene over Nanosheets of HZSM-5 Zeolite[J].Acta Phys. -Chim. Sin., 2014, 30(3): 535-543.

References

(1) Lin, B. M.; Zhang, Q. H.;Wang, Y. Ind. Eng. Chem. Res. 2009, 48 (24), 10788. doi: 10.1021/ie901227p
(2) Rothaemel, M.; Holtmann, H. D. Erdöl Erdgas Kohle 2002, 118, 234.
(3) Teketel, S.; Skistad,W.; Benard, S.; Olsbye, U.; Lillerud, K. P.; Beato, P.; Svelle, S. ACS Catal. 2012, 2 (1), 26. doi: 10.1021/cs200517u
(4) Lacarriere, A.; Luck, F.; wierczy ski, D.; Fajula, F.; Hulea, V. Appl. Catal. A 2011, 402 (1-2), 208. doi: 10.1016/j.apcata.2011.06.003
(5) Li, J. Z.;Wei, Y. X.; Liu, G. Y.; Qi, Y.; Tian, P.; Li, B.; He, Y. L.; Liu, Z. M. Catal. Today 2011, 171 (1), 221. doi: 10.1016/j.cattod.2011.02.027
(6) Hu, S.; Gong, Y. J.; Xu, Q. H.; Liu, X. L.; Zhang, Q.; Zhang, L. L.; Dou, T. Catal. Commun. 2012, 28, 95. doi: 10.1016/j.catcom.2012.08.011
(7) Masih, D.; Imai, H.; Yokoi, T.; Kondo, J. N.; Tatsumi, T. Catal. Commun. 2013, 37, 1. doi: 10.1016/j.catcom.2013.03.023
(8) Wei, R. C.; Li, C. Y.; Yang, C. H.; Shan, H. H. J. Nat. Gas Chem. 2011, 20, 261. doi: 10.1016/S1003-9953(10)60198-3
(9) Wang, Z. Y.; Li, J. L. Chem. React. Eng. Technol. 2008, 24 (5), 440. [王志彦, 李金来. 化学反应工程与工艺, 2008, 24 (5),440.]
(10) Firoozi, M.; Baghalha, M.; Asadi, M. Catal. Commun. 2009, 10, 1582. doi: 10.1016/j.catcom.2009.04.021
(11) Zhang,W.; Ren, L. J.; Guang, C.; Qi, J. Guangzhou Chem. Ind. 2012, 40 (2), 20. [张伟, 任立军, 关翀, 齐静. 广州化工, 2012, 40 (2), 20.]
(12) Mei, C. S.;Wen, P. Y.; Liu, Z. C.; Liu, H. X.;Wang, Y. D.; Yang, W. M.; Xie, Z. K.; Hua,W. M.; Gao, Z. J. Catal. 2008, 258, 243. doi: 10.1016/j.jcat.2008.06.019
(13) Kim, J.; Choi, M.; Ryoo, R. J. Catal. 2010, 269, 219. doi: 10.1016/j.jcat.2009.11.009
(14) Schmidt, F.; Hoffmann, C.; Giordanino, F.; Bordiga, S.; Simon, P.; Carrillo-Cabrera,W.; Kaskel, S. J. Catal. 2013, 307, 238.doi: 10.1016/j.jcat.2013.07.020
(15) Choi, M.; Na, K.; Kim, J.; Sakamoto, Y.; Terasaki, O.; Ryoo, R. Nature 2009, 461, 246. doi: 10.1038/nature08288
(16) Kim, J.; Park,W.; Ryoo, R. ACS Catal. 2011, 1 (4), 337. doi: 10.1021/cs100160g
(17) Seo, Y.; Cho, K.; Jung, Y.; Ryoo, R. ACS Catal. 2013, 3 (4), 713. doi: 10.1021/cs300824e
(18) Kim, J.; Kim,W.; Seo, Y.; Kim, J. C.; Ryoo, R. J. Catal. 2013, 301, 187. doi: 10.1016/j.jcat.2013.02.015
(19) Hu, S.; Shan, J.; Zhang, Q.;Wang, Y.; Liu, Y. S.; Gong, Y. J.; Wu, Z. J.; Dou, T. Appl. Catal. A 2012, 445 -446, 215.
(20) Wang,W. G.; Zhang, S. L.; Zhang, L. L.;Wang, Y.; Liu, X. L.; Gong, Y. J.; Dou, T. Acta Phys. -Chim. Sin. 2013, 29 (9), 2035. [王务刚, 张少龙, 张兰兰, 王艳, 刘晓玲, 巩雁军, 窦涛. 物理化学学报, 2013, 29 (9), 2035.] doi: 10.3866/PKU.WHXB201306183
(21) Stöcker, M. Microporous Mesoporous Mat. 1999, 29, 3. doi: 10.1016/S1387-1811(98)00319-9
(22) Zhao, T. S.; Takemoto, T.; Tsubaki, N. Catal. Commun. 2006, 7, 647. doi: 10.1016/j.catcom.2005.11.009
(23) Askari, S.; Halladj, R.; Sohrabi, M. Microporous Mesoporous Mat. 2012, 163, 334. doi: 10.1016/j.micromeso.2012.07.041
(24) Olsbye, U.; Svelle, S.; Bjørgen, M.; Beato, P.; Janssens, T. V. W.; Joensen, F.; Bordiga, S.; Lillerud, K. P. Angew. Chem. Int. Edit. 2012, 51, 5810. doi: 10.1002/anie.v51.24
(25) Yang, Y. S.; Sun, C.; Du, J. M.; Yue, Y. H.; Hua,W. M.; Zhang, C. L.; Shen,W.; Xu, H. L. Catal. Commun. 2012, 24, 44. doi: 10.1016/j.catcom.2012.03.013
(26) Bjørgen, M.; Svelle, S.; Joensen, F.; Nerlov, J.; Kolboe, S.; Bonino, F.; Palumbo, L.; Bordiga, S.; Olsbye, U. J. Catal. 2007, 249, 195. doi: 10.1016/j.jcat.2007.04.006
(27) Mao, D. S.; Guo, S. Q.; Meng, T.; Lu, G. Z. Acta Phys. -Chim. Sin. 2010, 26 (2), 338. [毛东森, 郭强胜, 孟涛, 卢冠忠. 物理化学学报, 2010, 26 (2), 338.] doi: 10.3866/PKU.WHXB20100208
(28) Fougerit, J. M.; Gnep, N. S.; Guisnet, M. Microporous Mesoporous Mat. 1999, 29, 79. doi: 10.1016/S1387-1811(98)00322-9
(29) Kaarsholm, M.; Joensen, F.; Nerlov, J.; Cenni, R.; Chaouki, J.; Patience, G. S. Chem. Eng. Sci. 2007, 62, 5527. doi: 10.1016/j.ces.2006.12.076
(30) Schulz, H. Catal. Today 2010, 154, 183. doi: 10.1016/j.cattod.2010.05.012
(31) Obrzut, D.; Adekkanattu, P.; Thundimadathil, J.; Liu, J.; Dubois, D.; Guin, J. React. Kinet. Catal. Lett. 2003, 80 (1), 113. doi: 10.1023/A:1026088327000
(32) Bjørgen, M.; Akyalcin, S.; Olsbye, U.; Benard, S.; Kolboe, S.; Svelle, S. J. Catal. 2010, 275 (1), 170. doi: 10.1016/j.jcat.2010.08.001
(33) Zhu, X. X.; Liu, S. L.; Niu, X. L.; Sun, X. D.; Bai, J.; Xu, L. Y. Petrochem. Technol. 2004, 33 (4), 320. [朱向学, 刘盛林, 牛雄雷, 孙新德, 白杰, 徐龙伢. 石油化工, 2004, 33 (4), 320.]
(34) Huang, Z. Y.; Ke, L.; Feng, J.; Liu, X.W.; Zhang, M. S. J. Mol. (China) 2008, 22 (1), 22. [黄志永, 柯丽, 冯静, 刘学武, 张明森. 分子催化, 2008, 22 (1), 22.]
(35) Guo, Q. S.; Mao, D. S.; Lao, Y. P.; Lu, G. Z. Chin. J. Catal. 2009, 30 (12), 1248. [郭强胜, 毛东森, 劳嫣萍, 卢冠忠. 催化学报, 2009, 30 (12), 1248.]
(36) Caro, J.; Noack, M.; Richter-Mendau, J.; Marlow, F.; Petersohn, D.; Griepentrog, M.; Kornatowski, J. J. Phys. Chem. 1993, 97, 13685. doi: 10.1021/j100153a043
(37) Bibby, D. M.; Milestone, N. B.; Patterson, J. E.; Aldridge, L. P. J. Catal. 1986, 97, 493. doi: 10.1016/0021-9517(86)90020-5
(38) Bibby, D. M.; Howe, R. F.; McLellan, G. D. Appl. Catal. A 1992, 93, 1. doi: 10.1016/0926-860X(92)80291-J

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Methanol to Propylene over Nanosheets of HZSM-5 Zeolite

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