Synthesis of mesoporous chromium aluminophosphate (CrAlPO) via solid state reaction at low temperature

Abstract

Mesoporous chromium aluminophosphate (CrAlPO) was successfully synthesized via solid state reaction (SSR) route at low temperature in the presence of a cationic surfactant cetyltrimethyl ammonium bromide (CTAB) and inorganic sources such as AlCl₃·6H₂O, CrCl₃·6H₂O and NaH₂PO₄·2H₂O. Characterizations by means of powder X-ray diffraction (XRD), N₂ adsorption-desorption, high resolution transmission electron microscopy (HR-TEM), scanning electron micrography (SEM), energy dispersion spectroscopy (EDS), thermo-gravimetry (TG), Fourier transform infrared spectroscopy (FT-IR), and ultraviolet visible light spectroscopy (UV-Vis) were carried out to understand both the pore characteristics and electron transition route of these obtained materials. The experimental results show that the meso-CrAlPO materials with various Cr/Al molar ratios possess a mesostructure and a specifi c surface area of 193 to 310 m²/g corresponding to an average pore size of 5.5 to 2.2 nm, respectively. The maxium content of Cr in meso-CrAlPO materials synthesized via SSR route can achieve 16.7wt%, being significantly higher than that of the meso-CrAlPO prepared via a conventional sol-gel route. Meanwhile, the formation mechanism of the meso-CrAlPO was also proposed.

Keywords

mesoporous / chromium aluminophosphate / solid state reaction / low temperature

References

[1] Alberti G., Costantino U., Casciola M., . Preparation, Characterization and Proton Conductivity of Titanium Phosphate Sulfophenylphosphonate [J]. Solid State Ionics, 2001, 145: 249-255.

[2] Kevin B., Annette B., John T. Highly Selective Chromium Based Ethylene Trimerization Catalysts with Bulky Diphosphinoamine Ligands[J]. Chem.Commun., 2005, 5: 620-621.

[3] Julbe A., Farrusseng D., Guizard C. Synthesis and Characterisation of a Vanadium-Based ‘Chemical Valve’ Membrane [J]. Sep. Purif. Technol., 2001, 25: 11-24.

[4] Schüth F., Schmidt W. Microporous and Meso-porous Materials [J]. Adv. Mater., 2002, 14: 629-638.

[5] Ying J. Y., Mehnert C. P., Wong M. S. Synthesis and Applications of Supramolecular-Templated Mesoporous Materials [J]. Angew. Chem. Int. Ed., 1999, 38: 56-77.

[6] Corma A. From Microporous to Mesoporous Molecular Sieve Materials and Their Use in Catalysis [J]. Chem. Rev., 1997, 97: 2 373-2 419.

[7] Davis M. E. Ordered Porous Materials for Emerging Applications [J]. Nature, 2002, 417: 813-821.

[8] Bagshaw S. A., Pouzet E., Pinnavaia T. J. Templating of Mesoporous Molecular Sieves by Nonionic Polyethylene Oxide Surfactants[J]. Science, 1995, 269: 1 242-1 244.

[9] Perez O. J. O., Borade R. B., Clearfield A. Synthesis of a Mesoporous Aluminophosphate[J]. J. Mol. Struct., 1998, 470: 221-228.

[10] Akolekar D. B. Acidity and Catalytic Properties of AlPOd-11, SAPO-11, MAPO-11, NiAPO-11, MnAPO-11 and MnAPSO-1 1 Molecular Sieves [J]. J. Mol. Catal. A: Chem., 1995, 104: 95-102.

[11] Kimura T. Surfactant-Templated Mesoporous Aluminophosphate — Based Materials and the Recent Progress [J]. Micropor. Mesopor. Mater., 2005, 77: 97-107.

[12] Tian P., Liu Z. G., Wu Z. H., . Characterization of Metal-Containing Molecular Sieves and Their Catalytic Properties in the Selective Oxidation of Cyclohexane [J]. Catal. Today, 2004, 93/95: 735-742.

[13] Selvam P., Mohapatra S. K. Synthesis and Characterization of Divalent Cobalt-Substituted Mesoporous Aluminophosphate Molecular Sieves and Their Applicationas as Novel Heterogeneous Catalysts for the Oxidation of Cycloalkanes [J]. J. Catal., 2005, 233: 276-287.

[14] Selvam P., Mohapatra S. K. Thermally Stable Trivalent Iron-Substituted Hexagonal Mesoporous Aluminophosphate (FeHMA) Molecular Sieves: Synthesis, Characterization, and Catalytic Properties [J]. J. Catal., 2006, 238: 88-99.

[15] Chou B., Tsai J. L., Cheng S. Cu-substituted Molecular Sieves as Liquid Phase Oxidation Catalysts[J]. Micropor. Mesopor. Mater., 2001, 48: 309-318.

[16] Dongare M. K., Sabde D. P., Shaikh R. A., . Synthesis, Characterization and Catalytic Properties of ZrAPO-5 [J]. Catal. Today, 1999, 49: 267-276.

[17] Selvam P., Mohapatra S. K. Synthesis, Characterization and Catalytic Properties of Mesoporous TiHMA Molecular Sieves: Selective Oxidation of Cycloalkanes[J]. Micropor. Mesopor. Mater., 2004, 73: 137-149.

[18] Hartmann K., Kevan L. Transition-Metal Ions in Aluminophosphate and Silicoaluminophosphate Molecular Sieves: Location, Interaction with Adsorbates and Catalytic Properties [J]. Chem. Rev., 1999, 99: 635-663.

[19] Demuth D., Unger K. K., Schuth F., . Photoluminescence of Chromium (III)-doped Silico-aluminophosphate with AFI Structure [J]. Adv. Mater., 1994, 6: 931-934.

[20] Shylesh S., Srilakshmi C., Singh A. P., . One Step Synthesis of Chromium-Containing Periodic Mesoporous Organosilicas and Their Catalytic Activity in the Oxidation of Cyclohexane [J]. Micropor. Mesopor. Mater., 2007, 99: 334-344.

[21] Laha S. C., Glaser R. Characterization and Catalytic Performance of [Cr]MCM-41 and [Cr]MCM-48 Prepared by Either Classical or Microwave Heating [J]. Micropor. Mesopor. Mater., 2007, 99: 159-166.

[22] JhaR K., Shylesh S., Singh A. P. Oxidation of Ethyl Benzene and Diphenyl Methane over Ordered Mesoporous M-MCM-41 (M = Ti, V, Cr): Synthesis, Characterization and Structure Activity Correlations [J]. Micropor. Mesopor. Mater., 2006, 95: 154-163.

[23] Toda F. Solid State Organic Chemistry: Effi cient Reaction, Remarkable Yield, and Stereo-selectivity [J]. Acc. Chem. Res., 1995, 28: 480-486.

[24] Luan Z. H., Zhao D. Y., He H. Y., . Characterization of Aluminophosphate-Based Tubular Mesoporous Molecular Sieves [J]. J. Phys. Chem. B, 1998, 102: 1 250-1 259.

[25] Tanev P. T., Pinnavaia T. A Neutral Templating Route to Mesoporous Molecular Sieves [J]. Science, 1995, 267: 865-867.

[26] Polarz S., Smarsly B., Bronstein L., . From Cyclodextrin Assemblies to Porous Materials by Silica Templating [J]. Angew. Chem. Int. Ed., 2001, 40: 4 417-4 421.

[27] Li W., Zhang M., Zhang J. L. Self-assembly of Cetyltrimethylammonium Bromide in Ethanol-Water Mixture [J]. Front. Chem. China, 2006, 1: 438-442.

[28] Subrahmanyam C., Louis B., Rainone F., . Partial Oxidation of Toluene by O2 over Mesoporous Cr-AlPO [J]. Catal. Commum., 2002, 3: 45-50.

[29] Laha S. C., Kamalakar G., Glaser R. Microwave-assisted Synthesis of [Cr] APO-5 [J]. Micropor. Mesopor. Mater., 2006, 90: 45-52.

[30] Subrahmanyam C., Louis B., Rainone F., . Catalytic Oxidation of Toluene with Molecular Oxygen over Cr-substituted Mesoporous Materials [J]. Appl. Catal. A: General, 2003, 241: 205-215.

[31] Fan H. J., Knez M., Scholz R., . Monocrystal-line Spinel Nanotube Fabrication Based on the Kirkendall Effect [J]. Nature Mater., 2006, 5: 627-631.

[32] Rokita M., Handke M., Mozgawa W. The AIPO₄ Polymorphs Structure in the Light of Raman and IR Spectroscopy Studies [J]. J. Mol. Struct., 2000, 555: 351-356.

[33] Frunza L., Pelgrims J., Leeman H., . Incorpora tion of Transition Metal Ions in Luminophosphate Molecular Sieves with AST Structure [J]. J. Phys. Chem. B, 2001, 105: 2 677-2 686.

[34] Shan F. K., Liu G. X., Lee W. J., . Stokes Shift, Blue Shift and Red Shift of ZnO-Based Thin Films Deposited by Pulsed-Laser Deposition[J]. J. Cryst. Growth, 2006, 291: 328-333.

[35] Wells A. F. Structural Inorganic Chemistry [M], 1984 Oxford Clarendon Press 112

[36] Ballhausen C. J. Introduction to Ligand Field Theory [M], 1962 New York Mc Graw-Hill Book Co. 24

[37] Lever P., A. B. Inorganic Electronic Spectroscopy [M], 1984 Amsterdam Elsevier Pub. Co. 148

[38] Beale A. M., Grandjean D., Kornatowski J., . Unusual Coordination Behavior of Cr³⁺ in Micro-porous Aluminophosphates[J]. J. Phys. Chem. B, 2006, 110: 716-722.

[39] Miyake M., Uehara H., Suzuki H., . Syntheses of Chromium (III) -doped Aluminophosphate-5 Molecular Sieves from Various Gels [J]. Micropor. Mesopor. Mater., 1999, 32: 45-53.

[40] Beale A. M., Grandjean D., Kornatowski J., . Unusual Coordination Behavior of Cr³⁺ in Microporous Aluminophosphates [J]. J. Phys. Chem. B, 2006, 110: 716-722.

[41] Subrahmanyam C., Louis B., Rainone F., . Catalytic Oxidation of Toluene with Molecular Oxygen over Cr-substituted Mesoporous Materials[J]. Appl. Catal. A: General, 2003, 241: 205-215.

[42] Miyake M., Uehara H., Suzuki H., . Syntheses of chromium (III) -doped Aluminophosphate-5 Molecular Sieves from Various Gels[J]. Micropor. Mesopor. Mater., 1999, 32: 45-53.

[43] Liu L., Li H., Zhang Y. Effect of Synthesis Parameters on the Chromium Content and Catalytic Activities of Mesoporous Cr-MSU-x Prepared under Acidic Conditions[J]. J. Phys. Chem. B, 2006, 110: 1 5478-1 5485.

[44] Gontier S., Tuel A. Novel Zirconium Containing Mesoporous Silicas for Oxidation Reactions in the Liquid Phase [J]. Appl. Catal. A: General, 1996, 143: 125-135.

[45] Tarafdar A., Biswas S., Pramanik N. K., . Synthesis of Mesoporous Chromium Phosphate Through an Unconventional Sol-gel Route [J]. Micropor. Mesopor. Mater., 2006, 89: 204-208.

[46] Szostack R., Thomas T. L. Reassessment of Zeolite and Molecular Sieve Framework Infrared Vibrations [J]. J. Catal., 1986, 101: 549-552.

[47] Trowski P. K., Chmielarz L., Dziembaj R., . Dehydrogenation of Ethylbenzene with Nitrous Oxide in the Presence of Mesoporous Silica Materials Modifi ed with Transition Metal Oxides [J]. J. Phys. Chem. A., 2005, 109: 330-336.

[48] Mohapatra S. K., Hussain F., Selvam P. Synthesis, Characterization, and Catalytic Properties of Chromium-containing Hexagonal Mesoporous Aluminophosphate Molecular Sieves [J]. Catal. Lett., 2003, 85: 217-222.

[49] Tarafdar A., Biswas S., Pramanik N. K., . Synthesis of Mesoporous Chromium Phosphate Through an Unconventional Sol-gel Route[J]. Micropor. Mesopor. Mater., 2006, 89: 204-208.

[50] Chen J. D., Sheldon R. A. Selective Oxidation of Hydrocarbons with O₂ over Chromium Alumino-phosphate-5 Molecular Sieve [J]. J. Catal., 1995, 153: 1-8.

[51] Rokita M., Handke M., Mozgawa W. Spectro-scopic Studies of Polymorphs of AlPO₄ and SiO₂[J]. J. Mol. Struct., 1998, 450: 213-217.

[52] Oliver S., Kuperman A., Coombs N., . Lamellar Aluminophosphates that Mimic Radiolaria and Diatom Skeletons [J]. Nature, 1995, 378: 47-50.

[53] Bu X., Feng P., Stucky G. D. Large Cage Zeolite Structures with Multidimensional 12-Ring Channels [J]. Science, 1997, 278: 2 080-2 085.

[54] Zhang K. L., Sun J. T., Yuan L. J., Feng C. Q. Synthetic Inorganic Chemistry[M], 2008 Wuhan Wuhan University Press 284