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Catalysts based on pillared interlayered clays for the selective catalytic reduction of NO

Published online by Cambridge University Press:  09 July 2018

S. Perathoner
Affiliation:
Dipartimento di Chimica Industriale e dei Materiali, Università degli Studi di Bologna, Viale del Risorgimento 4, 40136 Bologna, Italy
A. Vaccari
Affiliation:
Dipartimento di Chimica Industriale e dei Materiali, Università degli Studi di Bologna, Viale del Risorgimento 4, 40136 Bologna, Italy

Abstract

The reactivity of an Al-pillared interlayered clay (PILC) (AZA) and a mixed Fe/Al-PILC (FAZA), used as references by the Concerted European Action-Pillared Layered Structure (CEA-PLS), was investigated in the selective catalytic reduction (SCR) of NO by NH3 or propane, as either catalysts or as supports of Cu ions. Both AZA and FAZA, either with or without Cu were found to be inactive in the reduction of NO with propane and oxygen. This is different from the behaviour with alumina with or without Cu, because of the different surface acidity properties. Good NO conversions were observed for both PILCs using NH3. The best catalytic performances were shown by FAZA, but the activity of AZA was also remarkable. The addition of Cu ions to both AZA and FAZA leads to an improvment in the activity in NO conversion and a reduction in the side formation of N2O. The catalytic behaviour was found to depend on the method of Cu addition, the Cu loading and the nature of the PILC. With AZA the best results were obtained for a Cu content up to 2 wt%, while further increases in the amount of Cu resulted in a considerable decrease in the conversion of NO. With FAZA, on the other hand, a high activity was observed at up to 3% of Cu introduced by ion exchange. By comparison with other Cu containing catalysts, Cu-FAZA allows operation in a wider range of reaction temperatures due to the reduced rate of side ammonia combustion. The surface acidity properties of AZA and FAZA were also characterized to interpret the above effects.

Type
Research Article
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 1997

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References

Adams, J.M., Martin, K., McCabe, R.W. & Murray, S. (1986) Methyl t-buthyl ether (MTBE) production: a comparison of montmorillonite-derived catalysts with an ion-exchange resin. Clays Clay Miner. 34, 597603.CrossRefGoogle Scholar
Armor, J.N. (1992) Environmental catalysis. Appl. Catal. B1, 221256.Google Scholar
Barrault, J., Gatineau, L., Hassoun, N. & Bergaya, F. (1992) Selective syngas conversion over mixed A1- Fe pillared Laponite clay. Energy Fuels, 6, 760763.CrossRefGoogle Scholar
Bergaya, F. (1990) Argiles á piliers. Pp. 513-537 in: Matdriaux Argileaux: Structure, Propriétés et Applications (Decarreau, A., editor). Soc. Franç. de Minalogie et de Cristalographie, Paris.Google Scholar
Bergaoui, L., Lambert, J.-F., Suquet, H. & Che, M. (1995) CuII and Al13-pillared saponites: macroscopic adsorption measurements and EPR spectra. J. Phys. Chem. 99, 21552161.Google Scholar
Bodoardo, S., Figueras, F. & Garrone, E. (1994) IR study of BrCnsted acidity of Al-pillared montmorillonite. J. Catal. 147, 223230.Google Scholar
Bosch, H. & Janssen, F. (1987) Catalytic reduction of nitrogen oxides. Catal. Today, 2, 369521.Google Scholar
Bradley, S.M. & Kydd, R.A. (1993) Ga13, Al13, GaAl12, and chromium-pillared montmorillonites: acidity and reactivity for cumene conversion. J. Catal. 141, 239249.Google Scholar
Burch, R. (Editor) (1987) Pillared clays. Catal. Today, 2, 185366.CrossRefGoogle Scholar
Butruille, J.R. & Pinnavaia, T.J. (1992) Propene alkylation of biphenyl catalyzed by alumina pillared clays and related acidic oxides. Catal. Letters, 12, 187192.Google Scholar
Centi, G. & Perathoner, S. (1995) Chemistry, reaction mechanism and use of Cu-based catalysts for the conversion of nitrogen oxides. Appl. Catal., A132, 179259.Google Scholar
Centi, G., Cristiani, C., Forzatti, P. & Perathoner, S. (Editors) (1995b) Pp. 1-85 in: Environmental Catalysis – Proc. 1st World Congr. Environmental Catalysis – For a Better Worm and Life. Societ∼ Chimica Italiana, Roma.Google Scholar
Centi, G., Nigro, C., Perathoner, S. & Stella, G. (1993) Role of the support and of adsorbed species on the behaviour of Cu-based catalysts for NO conversion. Catal. Today, 17, 103111.Google Scholar
Centi, G., Perathoner, S., Biglino, D. & Giamello, E. (1995a) Adsorption and reactivity of NO on copperon-alumina catalysts. I. Formation of nitrate species and their influence on reactivity in NO and NH3 conversion. J. Catal. 152, 75–92.Google Scholar
De Stefanis, A., Perez, G. & Tomlinson, A.A.G. (1994) Pillared layered structures vs. zeolites as sorbents and catalysts. Part 1. Hydrocarbon separations on two alumina-pillared clays and an α-tin phosphate analogue. J. Mater. Chem. 4, 959964.Google Scholar
Del Castillo, H.L. & Grange, P. (1993) Preparation and catalytic activity of titanium pillared montmorillonite. Appl. Catal. A103, 2334.CrossRefGoogle Scholar
Doblin, C., Mathews, J.F. & Turney, T.W. (1994) Shape selective cracking of n-octane and 2,2,4-trimethylpentane over an alumina-pillared clay. Catal. Letters, 23, 151160.Google Scholar
Figueras, F. (1988) Pillared clays as catalysts. Catal. Rev.-Sci. Eng. 30, 457499.Google Scholar
Gangas, N. & Papayannokos, N.G. (1995) Composition of AZA and FAZA and their starting clays. Abstracts–CEA-PLS Meeting on Reference Pillared Layered Clays, Athens (GK), November 18-19, 1995. Google Scholar
Guan, J. & Pinnavaia, T. (1994) A pillared rectorite clay with highly stable supergalleries. Mater. Sci. Forum, 152-153, 109114.Google Scholar
Iwamoto, M. (1994) Zeolites in environmental catalysis. Pp. 1395-1410 in: Zeolites and Related Microporous Materials: State of the Art 1994. (Weitkamp, T., Karge, H.G., Pfeifer, H. & Helderich, W., editors). Elsevier, Amsterdam.Google Scholar
Knözinger, H. (1993) Infrared spectroscopy as a probe of surface acidity. Pp. 267–285 in: Elementary Reaction Steps in Heterogeneous Catalysis (Joyner, R.W. & van Santen, R.A., editors). Kluwer, The Netherlands.Google Scholar
Komarneni, S. (1992) Nanocomposites. J. Mater. Chem. 2, 12191230.Google Scholar
Kukkadapu, R.K. & Kevan, L. (1988) Synthesis and electron spin resonance studies of copper-doped alumina-pillared montmorillonite clay. J. Phys. Chem. 92, 60736078.Google Scholar
Lavados, A.K., Trikalitis, P.N. & Pomonis, P.J. (1996) Surface characteristics and catalytic activity of A1- pillared (AZA) and Fe-Al-pillared (FAZA) clays for isopropanol decomposition. J. MoL Catal. 106, 241254.Google Scholar
Maes, N., Zhu, H.Y. & Vansant, E.F. (1994) Determination of the micropore-size distribution of AZA and FAZA based on the logarithmic adsorption isotherms. Abstracts–CEA-PLS Meeting on Reference Pillared Layered Clays, Athens (GK), November 18-19, 1995. Google Scholar
Martin, C., Martin, I. & Rives, V. (1992) An FF-IR study of the adsorption of pyridine, formic acid and acetic acid on magnesia and molybdena-magnesia. J. Mol. Catal. 73, 5163.Google Scholar
Molina, R., Schutz, A. & Poncelet, G. (1994) Transformation of m-xylene over Al-pillared clays and ultrastable zeolite Y. J. Catal. 145, 7985.Google Scholar
Pinnavaia, T. J. (1983) Intercalated clay catalysts. Science, 220, 365371.Google Scholar
Pinnavaia, T.J. (1985) Pillared clays: synthesis and structural features. Pp. 151 – 164 in: Chemical Reactions in Organic and Inorganic Constrained Systems. NATO ASI Series, Set. C 165.Google Scholar
Suib, L.S. (1993) Zeolitic and layered materials. Chem. Rev. 93, 803826.Google Scholar
Taylor, K.C. (1993) Nitric oxide catalysis in automotive exhaust systems. CataL Rev. Sci. Eng. 35, 457481.Google Scholar
Yang, R.T., Chen, J.P., Kikkinides, E.S., Cheng, L.S. & Cichanowicz, J.E. (1992) Pillared clays as superior catalysts for selective catalytic reduction of NO with NH3 . Ind. Eng. Chem. Res. 31, 14401445.CrossRefGoogle Scholar