Mössbauer Effect Methodology pp 1-29 | Cite as
Mössbauer Spectroscopy in Heterogeneous Catalysis
Abstract
A typical solid catalyst consists of 1–10 nm particles of the active components dispersed on a high-surface-area (~300 m2/g), relatively inert support. When one of the elements in the active component phase has a Mössbauer effect, a variety of catalytically important, and otherwise inaccessible, chemical properties of the catalyst can be measured. The detailed chemical information contained in the recoil free fraction, isomer shift, quadrupole splitting and magnetic dipole splitting derived from the Mössbauer spectrum can elucidate structure, bonding, composition and particle size of the active component phase. When particle size is small, a high fraction of the Mössbauer atoms are surface atoms, and their interactions with adsorbed gases make a strong contribution to the spectrum. The technique is illustrated by discussion of studies of supported iron, iron-exchanged zeolites, the ammonia synthesis catalyst and oxidation/ reduction catalysts. The emphasis is on the nature of catalytic problems susceptible to investigation by Mössbauer spectroscopy.
Keywords
MOSSBAUER Spectroscopy Isomer Shift Quadrupole Splitting Electric Field Gradient Heterogeneous CatalysisPreview
Unable to display preview. Download preview PDF.
References
- 1.P. A. Flinn, S. L. Ruby, and W. L. Kehl, Science 143, 1434 (1964).Google Scholar
- 2.H. M. Gager and M. C. Hobson, Jr., Catal. Rev-Sci. Eng. 11, 117 (1975).Google Scholar
- 3.J. A. Dumesic and H. Topsoe, Adv. in Catal. to be published.Google Scholar
- 4.M. Poltorok and V. S. Baronin, Intern. Chem. Engin. 7, 452 (1976).Google Scholar
- 5.J. Müller, Rev. Pure and Appl. Chem. 19, 151 (1969).Google Scholar
- 6.C. H. Bartholomew and M. Boudart, J. Catal. 29, 278 (1973).CrossRefGoogle Scholar
- 7.R. L. Garten and D. F. 011is, J. Catal. 35, 232 (1974).CrossRefGoogle Scholar
- 8.R. L. Garten and M. A. Vannice, J. Molecular Catal. in press.Google Scholar
- 9.R. L. Garten, J. Catal. in press.Google Scholar
- 10.J. M. Blakely and J. C. Shelton, in Surface Physics of Materials Vol. I, J. M. Blakely,Ed., Academic Press, New York, 1975, p. 189.CrossRefGoogle Scholar
- 11.R. Bauman, G. J. M. Lippits and W. M. H. Sachtler, J. Catal 25, 350 (1972).CrossRefGoogle Scholar
- 12.F. L. Williams and M. Boudart, J. Catal. 30, 438 (1973).CrossRefGoogle Scholar
- 13.L. D. Schmidt, Cat. Rev.-Sci. Eng. 9, 115 (1974).Google Scholar
- 14.E. K. Rideal, Concepts in Catalysis Academic Press, New York, 1968, p. 41.Google Scholar
- 15.R. Gomer, Solid State Physics 30, 93 (1975).CrossRefGoogle Scholar
- 16.J. W. Gadzuk, in Surface Physics of Materials Vol. II, J. M. Blakely, Ed., Academic Press, New York, 1975, p. 339.CrossRefGoogle Scholar
- 17.R. Van Hardeveld and F. Hartog, Surf. Sci. 15, 189 (1969).Google Scholar
- 18.M Boudart, Adv. in Catal. 20, 153 (1969).Google Scholar
- 19.R. C. Baetzold and R. E. Mack, J. Chem. Phys, 62, 1513 (1975).Google Scholar
- 20.K. Johnson and R. P. Messmer, J. Vac. Sci. Technol. 11, 236 (1974). J.G. Fripiat, K.T. Chow, M. Boudart, J.G. Diamond, K.H. Johnson, J. Molecular Catal. 1, 59 (1975).Google Scholar
- 21.G. A. Somorjai, Catal. Rev. 7, 87 (1972).Google Scholar
- 22.A. N. Karasev, Yu. A. Kolbanovskìi, L. S. Polak, and E. Sh. Shlikhter, Kirret. i Katal. 8, 232 (1967).Google Scholar
- 23.C. F. Cook, P. R. Gray and H. M. Barton, Jr., Proceedings of The Second Symposium on Low Energy X- and Gamma Sources and Applications ORNL-11C-10, p. 130 (1967).Google Scholar
- 24.I. P. Suzdalev, A. M. Afanas’ev, A. S. Plachinda, V. I. Gol’danskii, and E. F. Makarov, Soviet Phys. JETP 28, 923 (1969).Google Scholar
- 25.I. W. Burton, R. P. Godwin, and H. Frauenfelder, Applications of the Mössbauer Effect in Chemistry and Solid State Physics (Vienna 1966) IAEA Tech. Rep. Ser. 50, p. 73. and I. W. Burton and R. P. Godwin, Phys. Rev. 158, 218 (1967).Google Scholar
- 26.G. W. Simmons, E. Kellerman, and H. Leidheiser, Jr., Corrosion 29, 227 (1973).CrossRefGoogle Scholar
- 27.W. N. Delgass, L.-Y. Chen and G. Vogel, Rev. Sci. Instrum. 47, 136 (1976).Google Scholar
- 28.C. A. Clausen, III, and M. L. Good, J. Catal. 38, 92 (1975).Google Scholar
- 29.P. N. Ross, Jr., and W. N. Delgass, in Catalysis, Vol.1 J. W. Hightower, Ed., North Holland Publishing Co., Amsterdam, (1973) p. 597.Google Scholar
- 30.H. M. Gager, Ph.D. Thesis, Virginia Commonwealth University (1972).Google Scholar
- 31.L. V. Skalkina, I. P. Suzdalev, I. K. Kolchin and L. Ya. Margolis; Kinet. i Katal. 10, 456 (1969).Google Scholar
- 32.
- 33.I. P. Suzdalev and E. F. Makarov, Proceedings of the Conference on the Application of the Mössbauer Effect (Tihany, 1969) Akademiai Kiado, Budapest, 1971, p. 201.Google Scholar
- 34.I. P. Suzdalev, A. S. Plachinda, and E. F. Makarov, Soviet Phys. JETP 26, 897 (1968).Google Scholar
- 35.H. Tops0e and M. Boudart, J. Catal. 31, 346 (1973).CrossRefGoogle Scholar
- 36.E. A. Samuel and W. N. Delgass, J. Chem. Phys. 62, 1590 (1975).Google Scholar
- 37.P. N. Ross, Jr. and W. N. Delgass, J. Catal. 33, 219 (1974).Google Scholar
- 38.G. A. Somorjai, Principles of Surface Chemistry Prentice Hall, Englewood Cliffs, N.J., 1972, p. 99.Google Scholar
- 39.K. S. Singwi and S. A. Sjölander, Phys. Rev., 120 1093 (1960).Google Scholar
- 40.V. I. Gol’danskii and I. P. Suzdalev, Russian Chem. Rev. 39, 609 (1970).Google Scholar
- 41.W. Kundig, H. Bömmel, G. Constabaris, and R. H. Lindquist, Phys. Rev. 142, 327 (1966).Google Scholar
- 42.I. P. Suzdalev, Proceedings of the Conference on the Application of the Mössbauer Effect (Tihany, 1969) Akademiai Kiado, Budapest, 1971, p. 193.Google Scholar
- 43.H. Hobert and D. Arnold, ibid p. 325.Google Scholar
- 44.A. M. Rubashov, P. B. Fabrichnyi, B. V. Shakhov and A. M. Babeshkin, Zh. Fiz. Khim. 46, 1327 (1972).Google Scholar
- 45.Y.-Y. Huang and J. R. Anderson, J. Catal. 40, 143 (1975).CrossRefGoogle Scholar
- 46.F. A. Fortunato and W. N. Delgass, unpublished results.Google Scholar
- 47.J. A. Dumesic, H. Topshe, S. Khammouma, and M. Boudart, J. Catal. 37, 503 (1975).CrossRefGoogle Scholar
- 48.R. L. Garten, W. N. Delgass, and M. Boudart, J. Catal. 18, 90 (1970).Google Scholar
- 49.M. Boudart, R. L. Garten and W. N. Delgass, Memoires de la Soc. Roy. Sc. Liège, 6e Serie, I (4), 135 (1971).Google Scholar
- 50.Y. Y. Huang, J. E. Benson, and M. Boudart, Ind. Eng. Chem. Fundam. 8, 346 (1969).Google Scholar
- 51.R. L. Garten, J7 Gallard-Nechtschein and M. Boudart, Ind. Eng. Chem. Fundam. 12, 299 (1973).Google Scholar
- 52.E. A. Samuel, Ph.D. Thesis, Yale University (1973).Google Scholar
- 53.H. Topshe, J. A. Dumesic and M. Boudart, J. Catal. 28, 477 (1973).CrossRefGoogle Scholar
- 54.P. H. Emmett and S. J. Brunauer, J. Amer. Chem. Soc. 59, 1553 (1937) and 62, 1732 (1940).Google Scholar
- 55.R. Hosemann, A. Preisinger, and W. Vogel, Ber. der Bunseng 70, 796 (1966).Google Scholar
- 56.R. Hosemann, K. Lemur, A. Schonfeld, and W. Wilke, Kolloid-Z. Z. Polym. 216–217, 103 (1967).Google Scholar
- 57.R. Hosemann, Chem. Inq. Tech. 42, 1252 and 1325 (1970).Google Scholar
- 58.A. A. Firsova, N. N. Khovanskaya, A. D. Tsyganov, I. P. Suzdalev, and L. Ya. Margolis, Kinet. i Katal. 12, 792 (1971).Google Scholar
- 59.L. Ya. Margolis, J. Catal. 21, 93 (1971).CrossRefGoogle Scholar
- 60.I. P. Suzdalev, A. A. Firsova, A. U. Aleksandrov, L. Ya. Margolis, and D. A. Baltrunas, Dok. Akad. Nauk. SSSR. 204, 408 (1972).Google Scholar
- 61.Yu. V. Maksimov, I. P. Suzdalev, V. I. Gol’danskii, 0. V. Krylov, L. Ya. Margolis, and A. E. Nechitailo, Chem. Phys. Letters 34, 172 (1975).Google Scholar
- 62.G. K. Boreskov, Kinet. i Katal. 11, 374 (1970).Google Scholar
- 63.D. S. Shihabi and W. N. Delgass, unpublished results.Google Scholar
- 64.L.-Y. Chen, Ph.D. Thesis, Purdue University (1975).Google Scholar
- 65.K. Tamaru, Adv. in Catal., 15, 65 (1964).Google Scholar
- 66.R. J. Kokes, Cat. Rev. 6, 1 (1972).CrossRefGoogle Scholar