Hostname: page-component-78c5997874-94fs2 Total loading time: 0 Render date: 2024-11-17T19:08:26.519Z Has data issue: false hasContentIssue false
  • English
  • Français

Structure-Property Relationships of BaCeO Perovskites for the Oxidative Dehydrogenation of Alkanes

Published online by Cambridge University Press:  10 February 2011

T. M. Nenoff ,
N. B. Jackson ,
J. E. Miller ,
A. G. Sault  and
D. Trudeil
T. M. Nenoff
Affiliation:
Sandia National Laboratories, Catalysis and Chemical Technologies Department, PO Box 5800, Albuquerque, NM 87185–0710
N. B. Jackson
Affiliation:
Sandia National Laboratories, Catalysis and Chemical Technologies Department, PO Box 5800, Albuquerque, NM 87185–0710
J. E. Miller
Affiliation:
Sandia National Laboratories, Catalysis and Chemical Technologies Department, PO Box 5800, Albuquerque, NM 87185–0710
A. G. Sault
Affiliation:
Sandia National Laboratories, Catalysis and Chemical Technologies Department, PO Box 5800, Albuquerque, NM 87185–0710
D. Trudeil
Affiliation:
Sandia National Laboratories, Catalysis and Chemical Technologies Department, PO Box 5800, Albuquerque, NM 87185–0710
Get access

Abstract

The oxidative dehydrogenation (ODH) reactions for the formation of two important organic feedstocks ethylene and propylene are of great interest because of the potential in capital and energy savings associated with these reactions. Theoretically, ODH can achieve high conversions of the starting materials (ethane and propane) at lower temperatures than conventional dehydrogenation reactions. The important focus in our study of ODH catalysts is the development of a structure-property relationship for catalyst with respect to selectivity, so as to avoid the more thermodynamically favorable combustion reaction. Catalysts for the ODH reaction generally consist of mixed metal oxides. Since for the most selective catalyst lattice oxygen is known to participate in the reaction, catalysts are sought with surface oxygen atoms that are labile enough to perform dehydrogenation, but not so plentiful or weakly bound as to promote complete combustion. Also, catalysts must be able to replenish surface oxygen by transport from the bulk.

Perovskite materials are candidates to fulfill these requirements. We are studying BaCeO3 perovskites doped with elements such as Ca, Mg, and Sr. During the ODH of the alkanes at high temperatures, the perovskite structure is not retained and a mixture of carbonates and oxides is formed, as revealed by XRD. While the Ca doped materials showed enhanced total combustion activity below 600°C, they only showed enhanced alkene production at 700°C. Bulk structural and surface changes, as monitored by powder X-ray diffraction, and X-ray photoelectron spectroscopy are being correlated with activity in order to understand the factors affecting catalyst performance, and to modify catalyst formulations to improve conversion and selectivity.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 497: Symposium Z – Recent Advances in Catalytic Materials , 1997 , 21
Copyright
Copyright © Materials Research Society 1998

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Linpinsky, E. S., Ingham, J. D., Brief Characterization of the Top 50 US Commodity Chemicals, USDOE, ILA 207376-A-Hl, Sept. 1994. Also see: Chemical & Engineering News, April 8, 1996, p. 17.Google Scholar
2. Labinger, J. A., Ott, K. C., Metha, S., Rockstad, H. K, Zoumalan, S.. J. Chem. Soc., Chem. Comm, p. 543 (1987).Google Scholar
3. Vatcha, S.R., Catalytica, Studies Division: Oxidative Dehyrogenation and Alternative Dehydrogenation Processes, Study Number 4192 OD, 1993.Google Scholar
4. Thorsteinson, E. M., Wilson, T. P., Young, F. G., Kasai, P. H., J. Catal. 52, p. 116 (1978).Google Scholar
5. Bayerlein, R. A., Jacobson, A. J., Poeppelmeyer, K. R., US 4,482,644, 1984.Google Scholar
6. Bayerlein, R. A., Jacobson, A. J., Poeppelmeyer, K. R., US 4,503,166, 1985.Google Scholar
7. Bayerlein, R. A., Jacobson, A. J., Poeppelmeyer, K. R., J. Chem. Soc., Chem. Commun., p. 225 (1988).10.1039/C39880000225Google Scholar
8. Verhoeve, R. J. H., Advanced Materials in Catalysis; Burton, J. J.; Garten, R. L., Eds.; Academic: New York, 1977, p. 129.Google Scholar
9. Iwahara, H., Esaka, T., Uchida, H., Maeda, N., Solid State Ionics, 3/4, p. 359 (1981).10.1016/0167-2738(81)90113-2Google Scholar
10. Yajima, T., Iwahara, H., Solid State Ionics, 50, p. 281 (1992).Google Scholar
11. Iwahara, H.H., Uchida, H., Ono, K., Ogaki, K., J. Electrochem. Soc. 135(2), p. 529 (1988).Google Scholar
12. Paria, M. K., Maiti, H. S., Solid State Ionics. 13, p. 285 (1984).Google Scholar
13. Mastromonaco, D., Barbariol, I., Cocco, A., Ann. Chim. (Rome). 59, p. 465 (1969).Google Scholar
14. Velie, O. J., Andersen, A., Jens, K.-J., Catalysis Today. 6, p. 567 (1990).Google Scholar
15. Yi, G., Hayakawa, T., Andersen, A. G., Suzuki, K., Hamakawa, S., York, A. P. E., Shimizu, M., Takehira, K., Catalysis Letters. 38, p. 189 (1996).10.1007/BF00806567Google Scholar
16. Sault, A. G., Boespflug, E. P., Peden, C. H. F., J. Phys. Chem. 98, 1652 (1994).Google Scholar
17. Sault, A. G., J. Catal. 156, 154 (1995).Google Scholar
18. Wagner, C. D., Six, H. A, Jansen, W. T., Taylor, J. A., Appl. Surface Sci. 9, 203 (1981).10.1016/0378-5963(81)90037-4Google Scholar
19. Wagner, C. D., Riggs, W. M., Davis, L. E., Moulder, J. F., Muilenberg, G. E., Handbook of X-ray Photoelectron Spectroscopy. Perkin-Elmer Corp., Eden Prairie, MN, 1979.Google Scholar
20. Longo, V., Ricciardiello, F., Minichelli, D., J. Materials Chem. 16, 3503 (1981).Google Scholar
21. Wagner, C. D., Davis, L. E., Zeller, M. V., Taylor, J. A., Raymond, R. H., Gale, L. H., Surface Int. Anal. 3, 211 (1981).Google Scholar