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Novel Microfabricated Pd-Au/SiO2 Model Catalysts for the Hydrogenation of 1,3-Butadiene

Published online by Cambridge University Press:  15 February 2011

Anthony C. Krauth  and
Eduardo E. Wolf
Anthony C. Krauth
Affiliation:
University of Notre Dame, Department of Chemical Engineering, Notre Dame, Indiana 46556
Eduardo E. Wolf
Affiliation:
University of Notre Dame, Department of Chemical Engineering, Notre Dame, Indiana 46556
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Abstract

Model Pd-Au/SiO2 catalysts were prepared via a microfabrication methodology and their catalytic activity was evaluated using the hydrogenation of 1,3-butadiene as a probe reaction. The catalytic particles of the microfabricated catalyst were Pd-Au squares, ranging in composition, each approximately 4 µm in size and separated by 4 µm on a silica/silicon support. The reaction was carried out at atmospheric pressure with a hydrogen to hydrocarbon ratio of 125. The bimetallic catalysts exhibited lower apparent activation energies than the pure Pd catalyst with a minimum occurring at ˜65 at% Pd. Corresponding to the decrease in activation energy, there is an increase in the turnover frequency over the monometallic catalyst at low temperatures, i.e. room temperature. At high temperatures (above 200°C) the pure Pd catalyst has the highest conversion (0.61) and the largest pre-exponential factor (4.71×1016 cc/g Pd/s), while the 73 at% Pd catalyst has the lowest conversion (0.45) and the smallest pre-exponential factor (5.59 × 10 6 cc/g Pd/s). The bimetallic catalysts also showed a higher selectivity towards 1-butene than the monometallic catalyst; however, at lower conversions (less than 25%) the pure Pd catalyst was more selectivity towards 1-butene. AFM was used to characterize the surface morphology of each of the samples.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 368: Symposium T – Synthesis and Properties of Advanced Catalytic Materials , 1994 , 157
Copyright
Copyright © Materials Research Society 1995

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References

1. Eley, D. D., J. Res. Inst. Catal., Hokkaido Univ., 16 (1), 101 (1968).Google Scholar
2. Allison, E. G. and Bond, G. C., Catal. Rev., 7 (2), 233 (1972).Google Scholar
3. Moss, R. L. and Whalley, L., Adv. Catal., 22, 115 (1972).Google Scholar
4. Schwank, J., Gold Bull., 18 (1), 2 (1985).Google Scholar
5. Okamoto, H. and Massalski, T. B., Binary Alloy Phase Diagrams, Vol.1. 2nd ed., editor-inMassalski, chief T. B. (ASM International, 1990), p. 409.Google Scholar
6. Wood, B. J. and Wise, H., Surf. Sci., 52, 151–160 (1975).Google Scholar
7. Lam, Y. L. and Boudart, M., J. Catal., 50, 530–540 (1977).Google Scholar
8. Ollis, D. F., J. Catal., 59, 430–433 (1979).Google Scholar
9. Maire, G., Hilaire, L., Gault, F. G. and O'Cinneide, A., J. Catal., 44, 293–299 (1976).Google Scholar
10. Jablonski, A., Overbury, S. H. and Somorjai, G. A., Surf. Sci., 65, 578–592 (1977).Google Scholar
11. Eley, D. D. and Moore, P. B., J. C. S. Faraday 1, 76, 1388–1390 (1980).Google Scholar
12. Krauth, A. C., Lee, K. H., Bernstein, G. H. and Wolf, E. E., Catal. Lett., 27, 43–51 (1994).Google Scholar
13. Joice, B.J., Rooney, J.J., Wells, P.B. and Wilson, G.R., Disc. Faraday Soc., 41, 223 (1966).Google Scholar
14. Miura, H., Terasaka, M., Oki, K. and Matsuda, T., New Frontiers in Catalysis: Proceedings of the 10th International Congress on Catalysis, edited by Guczi, L. et al., (Elsevier Science Publishers, New York, 1993), p. 2379.Google Scholar
15. Vuillemin, J. J. and Priestley, M. G., Phys. Rev. Lett., 14, 307 (1965).Google Scholar
16. Meuller, F. M. and Priestley, M. G., Phys. Rev., 148, 638 (1966).Google Scholar
17. Kimura, H., Katsuki, A. and Shimizu, M., J. Phys. Soc. Japan, 21 307 (1966).Google Scholar
18. Phillipson, J. J., Wells, P. B. and Wilson, G. R., J. Chem. Soc., 1351 (1969).Google Scholar
19. Pradier, C. M., Margot, E., Berthier, Y. and Oudar, J., Appl. Catal., 31, 243 (1987).Google Scholar