Fig. 1 Hydrogen Uptake on Metal Supported Active Carbon Fig. 2 Temperature Programmed Desorption Spectra of Hydrogen on Ni Supported Active Carbon
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2 Fig. 1 Hydrogen Uptake on Metal Supported Active Carbon Fig. 2 Temperature Programmed Desorption Spectra of Hydrogen on Ni Supported Active Carbon
3 X: active site on the carbon, M: supported metal particle. Fig. 5 Energy Diagram of Paraffin Dehydrogenation Promoted by Reverse Spillover Effect Fig. 3 Types of Catalyst Exhibiting Hydrogen Spillover, Where the Initiating Phase (I) Is Directly Supported on the Acceptor Phase (A) (a) or the Supported or Unsupported Phase from Simple Mixture (b) Table 1 Apparent Activation Energy, E and Activities of Isopentane Dehydrogenation Fig. 4 Dehydrogenation of Isopentane with Metal Supported Active Carbon Catalyst
4 Fig. 7 Model of Desulfurization by Hydrogen Transfer Fig. 6 Transfer Hydrogenolysis of Thiophene with Metal Supported Active Carbon Table 2 Hydrogen Charge and Recovery Fig. 8 Transfer Hydrocracking of Diphenylpropane Pyrolysis Fig. 9 Reaction Scheme of Diphenylpropane Pyrolysis
5
6 Fig. 10 Reverse Spillover Model of Aromatization of Lower Paraffin with ZSM-5 Zeolite Fig. 11 Aromatization of n-butane on Ni Containing Hybrid Catalyst Fig. 12 Hydrogen Adsorption on ZSM-5 Catalysts Fig. 13 Temperature Programmed Desorption Spectra of Hydrogen on ZSM-5 Hybrid Catalyst
7 Table 4 Isomerization of n-pentane on ZSM-5 Catalysts Table 5 Isomerization of n-pentane on a Two-stage Catalyst Bed
8 Fig. 14 Toluene Disproportionation with Hybrid Catalyst of USY and Co-Mo/Al2O3 References 1) Kuriacose, J. C., Indian J. Chem., 5, 646 (1961). 2) Taylor, H. S., Ann. Rev. Phys. Chem., 12, 147 (1961). 3) Khoobiar, S. J., J. Phys. Chem., 68, 411 (1964). 4) Robell, A. J., Ballou, E. V., Boudart, M., J. Phys. Chem., 68, 2748 (1964). 5) Delmon, B., Pouchot, Bull. Soc. Chim., 2677 (1966). 6) "Spillover of Adsorbed Species," eds. by Pajonk, G. M., Teichner, S. J., Germain, J. E., Elsevier, Amsterdam (1983). 7) Fujimoto, K., Stud. Surf. Sci. Catal., 77, 9 (1993). 8) Fujimoto, K., Nakamura, I., Yokota, K., Aimoto, K., Bull. Chem. Soc. Jpn., 64, 2275 (1991). 9) Hattori, H., Stud. Surf. Sci. Catal., 77, 69 (1993). 10) Nakamura, I., Iwamoto, R., I-ino, A., Stud. Surf. Sci. Catal., 77, 77 (1993). 11) Sermon, P. A., Bond, G. C., Catal. Rev., 8, 211 (1973). 12) Ono, Y., Baba, T., Kanae, K., Seo, S. G., Nippon Kagaku Kaishi, 985 (1988). 13) Carter, J. L., Lucchesi, P. J., Corneil, P., Yates, D. J. C., Sinfelt, J. H., J. Phys. Chem., 69, 3070 (1965). 14) Bianchi, D., Gardes, G. E. E., Pajonk, G. M., Teichner, S. J., J. Catal., 38, 135 (1975).
9 15) Ebitani, K., Konishi, J., Hattori, J. Catal., 130, 257 (1991). 16) Benson, J. E., Kohn, H. W., Boudart, M., J. Catal., 5, 307 (1966). 17) Levy, R. B., Boudart, M., J. Catal., 32, 304 (1974). 18) Fujimoto, K., Maeda, K., Aimoto, K., Appl. Catal., 91, 81 (1992). 19) Ohgoshi, S., Nakamura, I., Wakushima, Y., Stud. Surf. Sci. Catal., 77, 289 (1993). 20) Fujimoto, K., Toyoshi, S., Proceedings of 7th International Congress on Catalysis, (1980), p ) Asaoka, S., Masamizu, K., Fujimoto, K., Kunugi, T., Nippon Kagaku Kaishi, 1286 (1975). 22) Tokoro, Y., Misono, M., Uchijima, T., Yoneda, Y., Bull. Chem. Soc. Jpn., 51, 85 (1978). 23) Asaoka, S., Masamizu, K., Fujimoto, K., Kunugi, T., Nippon Kagaku Kaishi, 388 (1975). 24) Fujimoto, K., Ohno, A., Kunugi, T., Stud. Surf Sci. Catal., 17, 241 (1983). 25) Aimoto, K., Nakamura, I., Fujimoto, K., Energy & Fuels, 5, 739 (1991). 26) Mole, T., Anderson, J. R., Appl. Catal., 17, 141 (1985). 27) Sirokman, G., Sendoda, Y., Zeolite, 6, 299 (1986). 28) Inui, T., Makino, Y., Okazumi, F., Nagano, S., Miyamoto, Y., Ind. Eng. Chem. Res., 26, 647 (1987). 29) Ono, Y., Kitagawa, H., Sendoda, Y., Sekiyu Gakkaishi, 30, (2), 77 (1987). 30) Mills, G. A., Ind. Eng. Chem., 45, 130 (1953). 31) Fujimoto, K., Asami, K., Saima, H., Shikada, T., Tominaga, H., Ind. Eng. Chem. Res., 25, 262 (1986). Summary Catalyst Design Considering on Spillover and Reverse Spillover Phenomenon Ikusei NAKAMURA and Kaoru FUJIMOTO Dept. of Applied Chemistry, Faculty of Engineering, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113 Recently it has been pointed out that spillover and reverse spillover phenomenon contribute to various catalytic reactions including practical ones. The utilization of spillover phenomenon for elucidating the reaction mechanism and for developing new concepts of catalyst design are described with emphasis on the results of authors' work. The dehydrogenation of paraffins on active carbon catalyst was markedly promoted by added metals or metal sulfide. The added material should accelerate desorption of hydrogen from carbon surface through reverse spillover phenomena, because they have little activity for the dehydrogenation. An aromatization of lower paraffins on ZSM-5 zeolite was also promoted by reverse spillover effect of hydrogen from zeolite surface. Hybrid catalyst composed of physical mixture of Ga/Al2O3 and H-ZSM-5 showed comparable activities and aromatic selectivities to those of the Gasupported zeolite. Even hybridization of a Ni/SiO2 promoted the zeolite-catalyzed aromatization. Hydrogen in the spillover or reverse spillover system can react with organo-sulfur compounds, olefin or free radical. Hydrogen formed dehydrogenation of naphthene hydrocarbon transferred to these fragments in transfer hydrocracking of heavy oil with metal supported active carbon catalyst to give high quality distillates with small hydrogen consumption. Acid catalyzed reactions such as isomerization of n-paraffin, disproportionation of toluene or hydrocracking were promoted by hybridization of metal or supported metal catalyst to zeolites in hydrogen atmosphere. It can be concluded that acid sites generated on zeolites by hydrogen introduced from gas phase through spillover and that this acid site has the ability to act as catalyst for variety of acid catalyzed reactions. Keywords Hydrogen, Spillover, Supported catalyst, Aromatization, Dehydrogenation, Isomerization
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