In Situ 1H MAS NMR Spectroscopic Observation of Proton Species on a Mo-Modified HZSM-5 Zeolite Catalyst for the Dehydroaromatization of Methane
Ding Ma
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorYuying Shu Yuying
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorWeiping Zhang Weiping
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorXiuwen Han, Prof.
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorYide Xu
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorXinhe Bao Prof. Dr.
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorDing Ma
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorYuying Shu Yuying
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorWeiping Zhang Weiping
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorXiuwen Han, Prof.
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorYide Xu
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorXinhe Bao Prof. Dr.
State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Dalian 116023 (P. R. China) Fax: (+86) 411-4694447
Search for more papers by this authorWe are grateful for the support of the National Natural Science Foundation of China and the Ministry of Science and Technology of China.
Abstract
The NMR analysis of high-temperature reactions, even at temperatures over 800 K, has been carried out with the aid of a specially designed apparatus. The reaction studied was the catalytic methane aromatization on a molybdenum-modified ZSM-5 catalyst. The experiments could be performed under conditions identical to those used in the real catalytic process.
References
- 1a Y. Ono, Catal. Rev. Sci. Eng. 1992, 34, 179;
- 1b P. Meriaudeau, C. Naccache, Catal. Rev. Sci. Eng. 1997, 39, 5.
- 2 G. Buckles, G. J. Hutchings, C. D. Williams, Catal. Lett. 1991, 11, 89.
- 3 L. Wang, L. Tan, M. Xie, G. Xu, J. Huang, Y. Xu, Catal. Lett. 1993, 21, 35.
- 4a Y. Xu, S. Liu, L. Wang, M. Xie, X. Guo, Catal. Lett. 1995, 30, 135; W. Liu, Y. Xu, J. Catal. 1999, 185, 386;
- 4b Y. Shu, Y. Xu, S.-T. Wong, L. Wang, X. Guo, J. Catal. 1997, 170, 11;
- 4c D. Wang, J. H. Lunsford, M. P. Rosynek, J. Catal. 1997, 169, 347;
- 4d
B. M. Weckhuygsen, D. Wang, M. P. Rosynek, J. H. Lunsford, Angew. Chem. 1997, 109, 2471; Angew. Chem. Int. Ed. Engl. 1997, 36, 2374;
10.1002/ange.19971092131 Google Scholar
- 4e S. Liu, L. Wang, R. Ohnishi, M. Ichikawa, J. Catal. 1999, 181, 175;
- 4f F. Solymosi, J. Cserenyi, A. Szoke, T. Bansagi, A.Oszko, J. Catal. 1997, 165, 150;
- 4g F. Solymosi, L. Bugyi, A. Oszko, Catal. Lett. 1999, 57, 103.
- 5 H. Ernst, D. Freude, T. Mildner, I. Wolf, Stud. Surf. Sci. Catal. 1995, 94, 413; T. Mildner, D. Freude, J. Catal. 1998, 178, 309.
- 6 M. Hunger, T. Horvath, J. Chem. Soc. Chem. Commum. 1995, 1423; M. Hunger, M. Seiler, T. Horvath, Catal. Lett. 1999, 57, 199; P. K. Isbester, A. Zalusky, D. H. Lewis, M. C. Douskey, M. J. Pomije, K. R. Mann, J. Munson, Catal. Today 1999, 49, 363.
- 7 E. MacNamara, D. Raftery, J. Catal. 1998, 175, 135.
- 8
J. F. Haw, B. R. Richardson, I. S. Oshiro, N. D. Lazo, J. S. Speed, J. Am. Chem. Soc. 1989, 111, 2052;
J. Munson, J. F. Haw, J. Am. Chem. Soc. 1991, 113, 6303;
J. Munson, D. Murray, J. F. Haw, J. Catal. 1993, 141, 733;
J. F. Haw, T. Xu, J. B. Nicholas, P. W. Goguen, Nature 1997, 389, 23;
J. F. Haw, P. W. Goguen, T. Xu, T. W. Skloss, W. Song, Z. Wang, Angew. Chem. 1998, 110, 1001–1005; Angew. Chem. Int. Ed. 1998, 37, 948.
10.1002/(SICI)1521-3757(19980403)110:7<993::AID-ANGE993>3.0.CO;2-L Google Scholar
- 9 M. Hunger, Catal. Rev. Sci. Eng. 1997, 39, 345.
- 10 M. Hunger, D. Freude, H. Pfeifer, J. Chem. Soc. Faraday Trans. 1991, 87, 657.
- 11 V. R. Choudhary, A. K. Kinage, T. V. Choudhary, Science 1997, 275, 1286.
- 12 In the TPSR (temperature program surface reaction) profile of this reaction (detected by the on-line mass spectrometer) water was shown to be produced when the temperature reached 973 K, with a maximum at about 13 min after the reaction began. Two minutes later (15 min after the start of the reaction) the start of benzene formation is observed. The formation of water stopped about 1 h later at the same temperature, but that of benzene increases slowly in the first hour, and then appears to be constant. This indicates that the water formation is a stoichiometric (not catalytic) reaction [see Eq. (1)], where as benzene formation is a catalytic reaction.
- 13 C. C. Liu, G. E. Maciel, Anal. Chem. 1996, 68, 1401.
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