Skip to main content Accessibility help
×
Home

Infra-red studies of ammoniation of pillared montmorillonites

  • S. Witkowski (a1), Z. Sojka (a1), K. Dyrek (a1) (a2), J. Fijał (a3), S. Olkiewicz (a3), P. Fink (a4) and H. Hobert (a4)...

Abstract

Ammoniation of montmorillonites pillared with polyhydroxo-complexes of Al was performed in flow conditions at 773–1073 K and monitored by IR spectroscopy. Interaction of the clay with ammonia revealed exchange of terminal and bridging -OH groups by NH2-, NH- and N- species depending on the reaction temperature. Amination begins at 773 K while formation of NH groups starts at 873 K. Transformation of NH- into N-species occurs at 973 K. A mechanism for the ammoniation reaction is proposed and the series of the relative reactivity of OH groups was established: Si–OH > Mg–OH–Mg > Al–OH–Mg > Al–OH–Al. This series was rationalized in terms of accessibility of the OH groups.

Copyright

Corresponding author

References

Hide All
Besson, G. & Drits, V.A. (1997a) Refined relationships between chemical composition of dioctahedral finegrained mica minerals and their infrared spectra within the OH stretching region. 1. Identification of the OH stretching bands. Clays Clay Miner. 45, 158–169.
Besson, G. & Drits, V.A. (1997b) Refined relationships between chemical composition of dioctahedral finegrained micaceous minerals and their infrared spectra within the OH stretching region. 2. The main factors affecting OH vibrations and quantitative analysis, Clays Clay Miner. 45, 170–183.
Brindley, G.W. & Sempels, R.E. (1977) Preparation and properties of some hydroxy-aluminium beidellites. Clay Miner. 12, 229–237.
Butruille, J.-R. & Pinnavaia TJ. (1993) Mesoporous clays and pillared clays as liquid phase alkylation catalysts. Pp. 359–372 in: Multifunctional Mesoporous Inorganic Solids (Sequeira, C.A.C. & Hudson, M.J., editors). NATO ASI Series, Ser. C.
Choudary, B.M., Shobha Rani, S. & Narender, N. (1993) Asymmetric oxidation of sulfides to sulfoxides by chiral titanium pillared montmorillonite catalyst. Catal. Lett. 19, 299–307.
Del Castillo, H.L. & Grange, P. (1993) Preparation and catalytic activity of titanium pillared montmorillonite. Appl. Catal., A General, 103, 23–24.
Dunken, H., Fink, P. & Piltz, E. (1966) Surface characterization of aluminium oxide by chemisorption of ammonia. Chem Tech. 18, 490–495.
Fijal, J. (1988) Physico-chemical studies of the structure of fluor-hydroxy- and hydroxy-aluminum polycations for cross-linking of smectites. Miner. Polon. 19, 41–62.
Fijal, J. (1991) Modification of surface properties of smectite with fluorine compounds and polymeric hydroxy-metal complexes. Zesz. Nauk. AGH, 50, 1–196.
Fink, P. & Datka, J. (1989) Infrared spectroscopic studies of amination of ZSM-5-zeolites. J. Chem. Soc. Faraday 1, 85, 3079–3086.
Fink, P., Hobert, H. & Rudakoff, G. (1987) Structural arrangement of hydroxyl groups on disperse silica and stoichiometry of adsorption complexes. Wiss. Z. FSU Jena, Naturwiss. R, 36, 581–588.
Fink, P., Plotzki, I. & Rudakoff, G. (1990) Die Aminierung vom SiO2-Oberf1achen und ihre Eigenshaften. 3. Zum Mechanismus der Reaktion von NH3 mit dispersem SiO2 (Aerosil); die Bildung von NH-Gruppen. Wiss. Z. FSU Jena, Naturwiss. R. 39, 217–226.
Fink, P., Miiller, B. & Rudakoff, G. (1992) Ammoniation and nitridation of highly disperse silica. J. Non- Cryst. Solids. 145, 99–104.
Guan, J., Yu, Z., Fu, Y., Lee, C. & Wang, X. (1994) Hydrogen transfer activity of the pillared rectorites. Prepr. Am. Chem. Soc. Div. Pet. Chem. 39, 384–387.
Guiu, G. & Grange, P. (1994) Synthesis and characterization of tantalum pillared montmorillonite. J. Chem. Soc. Chem. Commun. 14, 1729–1730.
Hallam, H.E. (1963) Hydrogen bonding and solvent effects. Pp. 405–440 in: Infra-red Spectroscopy and Molecular Structure (Davies, M., editor). Elsevier, Amsterdam.
Horio, M., Suzuki, K., Masuda, H. & Mori, T. (1991) Alkylation of toluene with methanol on aluminapillared montmorillonite. Suppression of deactivation by control of the lateral spacing of pillars. Appl. Catal. 72, 109–118.
Janek, M., Komadel, P. & Lagaly, G. (1997) Effect of autotransformation on the layer charge of smectites determined by the alkylammonium method. Clay Miner. 32, 623–632.
Kikuchi, E., Matsuda, T., Ueda, J. & Morita, Y. (1985) Conversion of trimethylbenzenes over montmorillonites pillared by aluminum and zirconium oxides. Appl. Catal. 16, 401-410.
Kikuchi, E., Seki, H. & Matsuda, T. (1991) Preparation of pillared montmorillonite with enriched pillars. Stud. Surf. Sci. Catal. 63, 311–318.
Kloprogge, J.T., Booy, E., Jansen, J.B.H. & Geus, J.W. (1994) Synthesis of Al-pillared beidellite and its catalytic activity in the hydroconversion of N-heptane. Catal. Lett. 29, 293–297.
Kooli, F., Bovey, J. & Jones, W. (1997) Dependence of the properties of titanium-pillared clays on the host matrix: a comparison of montmorillonite, saponite, and rectorite pillared materials. J. Mater. Chem. 7, 153–158.
Kubelkova, L., Beran, S., Matecka, A. & Mastikhin, V.M. (1989) Acidity of modified Y zeolites: effect of nonskeletal aluminum, formed by hydrothermal treatment, dealumination with silicon tetrachloride and cationic exchange with aluminum. Zeolites, 9, 283–291.
Lahav, N., Shani, U. & Shabtai, J. (1978) Cross-linked smectites. I. Synthesis and properties of hydroxyaluminium- montmorillonite. Clays Clay Miner. 26, 107–115.
Matsuda, T., Matsukata, M., Kikuchi, E. & Morita, Y. (1986) Reaction of 1,2,4-trimethylbenzene and methanol on montmorillonite catalysts pillared by aluminum hydroxyl complexes. Appl. Catal. 21, 297–306.
Mishra, T. & Parida, K. (1997) Transition-metal oxide pillared clays. Part 2. A comparative study of textural and acid properties of manganese (III) pillared montmorilonite and pillared acid-activated montmorillonite. J. Mater. Chem. 7, 147–152.
Mishra, T., Parida, K. & Rao, S.B. (1997) Transitionmetal oxide pillared clays. Part 1. A comparative study of textural and acid properties of Fe (III) pillared montmorilonite and pillared acid-activated montmorillonite. J. Mater. Chem. 7, 138–146.
Monnier, J., Charland, J.P., Brown, J.R. & Wilson, M.F. (1993) Hydrocracking gas oil from synthetic crude with mixed pillared clay-alumina supported catalysts. Stud. Surf. Sci. Catal. (New Frontiers in Catalysis, Pt. C), 75, 1943–1946.
Perathoner, S. & Vaccari, A. (1997) Catalysts based on pillared interlayered clays for the selective catalytic reduction of NO. Clay Miner. 32, 123–134.
Petit, S., Robert, J.-L., Decarreau, A., Besson, G., Grauby, O. & Martin, F. (1995) Contribution of spectroscopic methods to 2:1 clay characterization. Bull. Centres Reck Explor. -Prod. Elf Aquitaine, 19, 119–147.
Pinnavaia, T.J. (1983) Intercalated clay catalysts. Science, 220, 365–371.
Radoslovich, E.W. (1961) Surface symmetry and cell dimensions of layer silicates. Nature, 191, 67–68.
Rosa-Brussin D., M.F. (1995) The use of clays for the hydrotreatment of heavy crude oils. Catal. Rev.-Sci. Eng. 37, 1–100.
Shabtai, J. (1979) Zeolites and crosslinked silicates as media for selective oxidation. Chim. Ind. (Milan), 61, 734–741.
Vaccari, A. (1996) Advanced applications of clay catalysts. Adas del XV Simposio Iberoamericano de Catalisis, Cordoba, Argentina, Unica Edicion, PL37-PL58.
Vaughan, D.E.W. & Lussier, R.J. (1980) Preparation of molecular sieves based on pillared intercalated clays. Proc. 5th Int. Conf. Zeolites, London, pp. 94–101.
Vaughan, D.E.W., Lussier, R.J. & Magee, I.S. Jr. (1981) Stabilized pillared intercalated clays. U.S. Patent 4,271,043.
Wiberg, N. & Uhlenbrock, W. (1971) Silicon compounds. 13. Trimethylsilylamine. Chem. Ber. 904, 2643–2645.
Yamagishi, A. & Aramata, A. (1985) Asymmetric electrooxidation of phenyl alkyl sulfide on an SnO2 electrode coated with a film of λ-Ru(Phen)2+ 3- montmorillonite. J. Electroanal. Chem. 191, 449–452.
Yang, R.T., Chen, J.P., Kikkinides, E.S., Chen, L.S. & Ciechanowicz, J.E. (1992) Pillared clays as superior catalysts for selective catalytic reduction of nitric oxide with ammonia. Ind. Eng. Chem. Res. 31, 1440–1445.
Zecchina, Z., Collucia, S. & Morterra, C. (1985) Infrared spectra of molecules adsorbed on oxide surfaces. Appl. Spec. Rev. 12, 259–310.

Keywords

Infra-red studies of ammoniation of pillared montmorillonites

  • S. Witkowski (a1), Z. Sojka (a1), K. Dyrek (a1) (a2), J. Fijał (a3), S. Olkiewicz (a3), P. Fink (a4) and H. Hobert (a4)...

Metrics

Full text views

Total number of HTML views: 0
Total number of PDF views: 0 *
Loading metrics...

Abstract views

Total abstract views: 0 *
Loading metrics...

* Views captured on Cambridge Core between <date>. This data will be updated every 24 hours.

Usage data cannot currently be displayed