Brønsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by 1H and 27Al DQ-MAS NMR Spectroscopy

doi:10.1016/S1872-2067(10)60287-2

Abstract

Abstract: Brønsted/Lewis acid sites synergy in H-MCM-22 zeolite was studied by solid-state nuclear magnetic resonance (NMR). Two-dimensional ¹H double quantum-magic angle spinning (DQ-MAS) NMR revealed the details of the spatial relationship between the Lewis and the Brønsted acid sites in a dealuminated H-MCM-22 zeolite, which implied the existence of a Brønsted/Lewis acid sites synergy. Two-dimensional ²⁷Al DQ-MAS NMR was used to give the details of the spatial proximities of various aluminum species. The Brønsted/Lewis acid sites synergy occurred in the supercage of the H-MCM-22 zeolite between a T₆ site Al and extra-framework Al species. ¹³C CP/MAS NMR of adsorbed acetone demonstrated that the spatial proximities of the Brønsted and Lewis acid sites led to a synergy that enhanced the Brønsted acid strength of the dealuminated zeolites. ¹H MAS NMR of adsorbed deuterated pyridine confirmed that the Brønsted/Lewis acid sites synergy occurred in the supercage of H-MCM-22. This finding is important for understanding the mechanism of acid-catalyzed reactions on H-MCM-22 zeolites.

Key words: H-MCM-22 zeolite, dealumination, acidity, Brønsted/Lewis acid synergy, double quantum-magic angle spinning nuclear magnetic resonance

YU Zhi-Wu, WANG Qiang, CHEN Lei, DENG Feng. Brønsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by ¹H and ²⁷Al DQ-MAS NMR Spectroscopy[J]. Chinese Journal of Catalysis, 2012, 33(1): 129-139.

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References

1Sastre G, Fornes V, Corma A. J Phys Chem B, 2000, 104: 4349
2Asensi M A, Corma A, Martínez A. J Catal, 1996, 158: 561
3Corma A, Mart?nez-Triguero J. J Catal, 1997, 165: 102
4Wu P, Komatsu T, Yashima T. Microporous Mesoporous Mater, 1998, 22: 343
5Park S H, Rhee H K. Appl Catal A, 2001, 219: 99
6Okumura K, Hashimoto M, Mimura T, Niwa M. J Catal, 2002, 206: 23
7Fu J Q, Ding C H. Catal Commun, 2005, 6: 770
8Ren X Q, Liang J H, Wang J. J Porous Mater, 2006, 13: 353
9Corma A, Fornes V, Rey F. Appl Catal, 1990, 59: 267
10Lonyi F, Lunsford J H. J Catal, 1992, 136: 566
11Batamack P, Dorémieux-Morin C, Vincent R, Fraissard J. Microporous Mater, 1994, 2: 525
12Viswanadham N, Gupta J K, Dhar G M, Garg M O. Energy Fuels, 2006, 20: 1806
13Kanellopoulos J, Unger A, Schwieger W, Freude D. J Catal, 2006, 237: 416
14Mirodatos C, Barthomeuf D. J Chem Soc, Chem Commun, 1981, 2: 39
15Hunger M. Catal Rev Sci Eng, 1997, 39: 345
16Hunger M. Solid State Nucl Magn Reson, 1996, 6: 1
17Fyfe C A, Bretherton J L, Lam L Y. J Am Chem Soc, 2001, 123: 5285
18Jiao J, Kanellopoulos J, Wang W, Ray S S, Foerster H, Freude D, Hunger M. Phys Chem Chem Phys, 2005, 7: 3221
19van Bokhoven J A, Koningsberger D C, Kunkeler P, van Bek-kum H, Kentgens A P M. J Am Chem Soc, 2000, 122: 12842
20Haw J F, Nicholas J B, Xu T, Beck L W, Ferguson D B. Acc Chem Res, 1996, 29: 259
21Fang H J, Zheng A M, Chu Y Y, Deng F. J Phys Chem C, 2010, 114: 12711
22Lunsford J H, Rothwell W P, Shen W. J Am Chem Soc, 1985, 107: 1540
23Kao H M, Grey C P. Chem Phys Lett, 1996, 259: 459
24Hung J, Jiang Y J, Marthala V R R, Thomas B J, Romanova E, Hunger M. J Phys Chem C, 2008, 112: 3811
25Freude D, Hunger M, Pfeifer H, Schwieger W. Chem Phys Lett, 1986, 128: 62
26Brown S P, Spiess H W. Chem Rev, 2001, 101: 4125
27Li S H, Zheng A M, Su Y C, Zhang H L, Chen L, Yang J, Ye C H, Deng F. J Am Chem Soc, 2007, 129: 11161
28Li S H, Huang S J, Shen W L, Zhang H L, Fang H J, Zheng A M, Liu S B, Deng F. J Phys Chem C, 2008, 112: 14486
29Mota C J A, Bhering D L, Rosenbach N. Angew Chem, Int Ed, 2004, 43: 3050
30Carvajal R, Chu P, Lunsford J H. J Catal, 1990, 125:123
31Sokol A A, Catlow C R A, Garces J M, Kuperman A. Adv Mater, 2000, 12: 1801
32van Bokhoven J A, van der Eerden A M J, Koningsberger D C. J Am Chem Soc, 2003, 125: 7435
33Yu Z W, Zheng A M, Wang Q, Chen L, Xu J, Amoureux J P, Deng F. Angew Chem, Int Ed, 2010, 49: 8657
34Leonowicz M E, Lawton J A, Lawton S L, Rubin M K. Science, 1994, 264: 1910
35Grey C P, Vega A J. J Am Chem Soc, 1995, 117: 8232
36Hohwy M, Jakobsen H J, Eden M, Levitt M H, Nielsen N C. J Chem Phys, 1998, 108: 2686
37Wang Q, Hu B W, Lafon O, Trébosc J, Deng F, Amoureux J P. J Magn Reson, 2009, 200: 251
38Madhu P K, Goldbourt A, Frydman L, Vega S. Chem Phys Lett, 1999, 307: 41
39Mastikhin V M, Mudrakovsky I L, Nosov A V. Prog Nucl Magn Reson Spectrosc, 1991, 23: 259
40Ma D, Han X W, Xie S J, Bao X H, Hu B, Au-Yeung S C F. Chem Eur J, 2002, 8: 162
41Ma D, Deng F, Fu R Q, Han X W, Bao X H. J Phys Chem B, 2001, 105: 1770
42陈雷, 邓风, 叶朝辉. 物理化学学报 (Chen L, Deng F, Ye Ch H. Acta Phys-Chim Sin), 2003, 19: 805
43Xu T, Kob N, Drago R S, Nicholas J B, Haw J F. J Am Chem Soc, 1997, 119: 12231
44Xu T, Haw J F. J Am Chem Soc, 1994, 116: 10188
45Biaglow A I, Sepa J, Gorte R J, White D. J Catal, 1995, 151: 373
46Zheng A M, Zhang H L, Chen L, Yue Y, Ye Ch H, Deng F. J Phys Chem B, 2007, 111: 3085
47Yu H G, Fang H J, Zhang H L, Li B J, Deng F. Catal Commun, 2009, 10: 920
48Xu J, Zheng A M, Yang J, Su Y C, Wang J Q, Zeng D L, Zhang M J, Ye Ch H, Deng F. J Phys Chem B, 2006, 110: 10662
49胡伟, 罗晴, 李申慧, 申万岭, 岳勇, 邓风. 物理化学学报 (Hu W, Luo Q, Li Sh H, Shen W L, Yue Y, Deng F. Acta Phys-Chim Sin), 2006, 22: 1233
50Freude D. Chem Phys Lett, 1995, 235: 69

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Brønsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by ¹H and ²⁷Al DQ-MAS NMR Spectroscopy

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