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1

2 Fig. 1 Activity Changes with Time on Stream Fig. 2 Selectivity Changes with Time on Stream

3 Fig. 3 PSD Change in Four Catalysts Fig. 4 XRD Patterns of Catalysts

4 Fig. 5 Changes of Specific CO Uptake and Specific BET Surface Area with Time on Stream Data before reduction and spent (100h) one are similar to those in Fig. 3. Fig. 6 PSD Change in Catalyst B Measured by Hg Penetration Method Table 1 Catalyst Composition before Reduction

5 Table 2 Ni Crystallite Size of the Catalysts by XRD

6 Fig. 7 Relation between CO Uptake of Spent Catalysts (100h) and CH4 Conversion Fig. 8 Changes in Amounts of Carbon on Catalysts with Time on Stream

7 The vertical axis is scaled to the maximum peak in each spectrum. The value in the each figure expresses the desorbed-nh3 amount observed above 600K. Fig. 9 TPD Patterns of Reduced Catalysts Fig. 10 Relation between the Amount of Acid of Reduced Catalyst and the Rate of Average Carbon Deposition on the Catalyst References 1) Ihara, S., Kagaku Keizaishi, 1, 86 (1994). 2) Twigg, M. V., "Catalyst Handbook," Wolfe Publishing Ltd., London (1989), p ) Rostrup-Nielsen, J. R., "Catalysis Science and Technology," vol 5., Springer-Verlag, Berlin (1984), p ) Kikuchi, E., Sekiyu Gakkaishi, 20, (2), 109 (1977). 5) Rhodes, A. K., OGJ Special, Oct. 14, 43 (1991). 6) Arnold, M. A., Atwood, K., Baugh, M. H., Smyser, H. D., Ind. Eng. Chem., 44, (5), 999 (1952).

8 210 7) Numaguchi, T., Kikuchi, K., Ind. Eng. Chem. Res., 30, 447 (1991). 8) Niiyama, H., Shokubai, 34, (5), 264 (1992). 9) Twigg, M. V., "Catalyst Handbook," Wolfe Publishing Ltd., London (1989), p ) In, S., Sekiyu Gakkaishi, 15, (8); 657 (1972). 11) Kiriyama, R., Koizumi, M., Yamada, K., Kitagaki, R., Kobutsushi, 2, 359 (1956). 12) Kiriyama, R., Koizumi, M., Yamada, K., Kitagaki, R., Kobutsushi, 3, 107 (1957). 13) Hashimoto, K., Hamano, K., "Ceramics no Kiso," Kyoritsu Shuppan, Tokyo (1975), p ) Catalysis Society of Japan, Sansho Shokubai Iinkai, Shokubai, 26, (5), 280 (1984). 15) Bartholomew, C. H., Pannell, R. B., J. Catal., 65, 390 (1980). 16) Matsumoto, H., "Shokubai Koza," eds. by Onoda, T., Tamura, T., Misono, M., Morooka, Y., vol. 8, Kodansha, Tokyo (1985), p ) Hisazumi, Y., Okada, O., Fujiwara, H., 5th Int. Iron & Steel Congr., 45, 295 (1986). 18) Rostrup-Nielsen, J. R., Ammonia Plant Safety, 15, 82 (1973). 19) Andrew, S. P. S., Ind. Eng. Chem., Prod. Res. Dev., 8, 321 (1961). 20) Bhatta, K. S. M., Ind. Eng. Chem., Prod. Res. Dev., 8, 324 (1969). 21) Saito, M., Tokuno, M., Amano, I., Morita, Y., Kogyo Kagakushi, 73, 2405 (1970). 22) Matsumoto, H., Shokubai, 13, (3), 71 (1976). 23) Catalysis Society of Japan, Sansho Shokubai Iinkai, Shokubai, 33, (3), 249 (1991). 24) Storgaard, L., Kagaku Keizaishi, 3, 83 (1983). Summary Evaluation of Activity and Carbon Deposition of Steam Methane Reforming Catalysts Four different nickel catalysts for steam methane reforming were evaluated using an integral fixed bed reactor in continuous flow under such operating conditions: 1.0MPa, 873K, S/C (steam-carbon molar ratio)=3, W/F=33sec, for 285h (the longest operation). The catalyst composition in wt% was: Ni ; CaO ; K2O ; Al2O The nickel crystallite size (after reduction) was nm. The following results were obtained. (1) The most active catalyst was 1.4 times that of the lowest at the beginning of the operation, but the difference decreased with time, especially after 100h of operation. (2) Fresh catalysts had a large difference in pore size distribution (PSD); however, all catalysts with alkaline components sintered in the 100h operation, and then PSD changed similarly to that of a catalyst without alkaline component whose version showed no relation to CO uptake per catalyst bed corresponding to the total nickel surface area, suggesting that the reaction was controlled by intra-particle diffusion. (4) There was a large difference in carbon deposition among the catalysts. The amount of acid measured by the NH3-TPD method showed some relation to the carbon deposition; however, the amount of alkaline component showed no relation to the carbon deposition. The catalyst with the smallest BET surface area of 3.6m2/g, having no alkaline component, but having a trace amount of acid, yielded the corresponding amount of carbon deposition. It was observed that the alkaline component is not always necessary to suppress the carbon deposition. Keywords Steam reforming, Natural gas, Activity, Catalyst stability

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