journal article·2014-01

Synthesis and characterization of SiO2–CrO3, SiO2–MoO3, and SiO2–WO3 mixed oxides produced using the non-hydrolytic sol–gel process

Arthur A. Bernardes, Claudio Radtke, Maria do Carmo M. Alves, Ione M. Baibich, Márcia Lucchese, João Henrique Z. dos Santos

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Abstract

Silica-based mixed oxide xerogels, namely SiO2–CrO3, SiO2–MoO3, and SiO2–WO3, were prepared using the non-hydrolytic sol–gel process. The materials were synthesized using metal chloride:tetraethoxysilane (TEOS) molar ratios of 0.1:2; 0.2:2 and 0.4:2 for each metal chloride and 1:2 SiCl4:TEOS molar ratio. All of the xerogels containing Cr, Mo or W had considerably greater surface areas than that of SiO2. The small angle X-ray scattering experiments suggest that the surface roughness of the aggregates in SiO2–CrO3 is less than that of SiO2–MoO3 and SiO2–WO3. The morphological characteristics of the silica-based mixed oxide xerogels were not affected by the nature and amount of metal chloride employed in the synthesis. An irregular morphology was observed for SiO2–CrO3, SiO2–MoO3 and SiO2–WO3, but a lamellar structure was observed for SiO2. X-ray photoelectron spectroscopy analysis suggests that tungsten species were preferentially distributed on the outmost part of the grain. The resulting particle diameter was shown to be lower for the mixed oxides compared to that of bare silica. Furthermore, the presence of metals (Cr, Mo and W) on silica caused a decrease in the size of the particles as the atomic radii of these metals increased. According to the Fourier transform infrared spectroscopy and Raman, Cr, Mo and W were incorporated within the silica framework.
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OpenAlex topics: Catalysis and Oxidation Reactions · Catalytic Processes in Materials Science · Transition Metal Oxide Nanomaterials

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References (44)

Show source-provided references
1. Wachs IE, Roberts CA (2010) Monitoring surface metal oxide catalytic active sites with Raman spectroscopy. Chem Soc Rev 39:5002–501710.1039/c0cs00145g ↗
2. Arzoumanian H, Castellanos NJ, Martinez FO, Páez-Mozo EA, Ziarelli F (2010) Silicon-assisted direct covalent grafting on metal oxide surfaces: synthesis and characterization of carboxylate N, N′-ligands on TiO2. Eur J Inorg Chem 11:1633–164110.1002/ejic.200901092 ↗
3. Irurzun VM, Tan Y, Resasco DE (2009) Sol–gel synthesis and characterization of Co–Mo/Silica catalysts for single-walled carbon nanotube production. Chem Mater 21(11):2238–224610.1021/cm900250k ↗
4. Gao G, Feng W, Wu G, Shen J, Zhang Z, Jin X, Zhang Z, Du A (2012) An investigation on the assembling of WO3 particles on the matrix of silica solution. J Sol–Gel Sci Technol 64:427–43510.1007/s10971-012-2873-9 ↗
5. Wachs IE (2005) Recent conceptual advances in the catalysis science of mixed metal oxide catalytic materials. Catal Today 100:79–9410.1016/j.cattod.2004.12.019 ↗
6. De Boer M, Van Dillen AJ, Koningsberger DC, Geus JW, Vuurman MA, Wachs IE (1991) Remarkable spreading behavior of molybdena on silica catalysts. An in situ EXAFS-Raman study. Catal Lett 11:227–24010.1007/BF00764089 ↗
7. Van Schalkwyk C, Spamer A, Moodley DJ, Dube T, Reynhardt J, Botha JM (2003) Application of a WO3/SiO2 catalyst in an industrial environment: part I. Appl Catal A 255:121–13110.1016/S0926-860X(03)00534-9 ↗
8. Choi KY, Tang S (2004) Polymerization rate modeling of ethylene polymerization with supported chromium oxide catalysts. J Appl Polym Sci 91:2923–292710.1002/app.13490 ↗
9. Li W, Meitzner GD, Borry RW III, Iglesia E (2000) Raman and X-ray absorption studies of Mo species in Mo/H-ZSM5 catalysts for non-oxidative CH4 reactions. J Catal 191:373–38310.1006/jcat.1999.2795 ↗
10. Thielemann JP, Ressler T, Walter A, Tzolova-Müller G, Hess C (2011) Structure of molybdenum oxide supported on silica SBA-15 studied by Raman, UV–Vis and X-ray absorption spectroscopy. Appl Catal A 399:28–3410.1016/j.apcata.2011.03.032 ↗
11. Vioux A (1997) Nonhydrolytic sol–gel routes to oxides. Chem Mater 9:2292–229910.1021/cm970322a ↗
12. Mutin PH, Vioux A (2009) Nonhydrolytic processing of oxide-based materials: simple routes to control homogeneity, morphology, and nanostructure. Chem Mater 21:582–59610.1021/cm802348c ↗
13. Niederberger M, Garnweitner G (2006) Organic reaction pathways in the nonaqueous synthesis of metal oxide nanoparticles. Chem Eur J 12:7282730210.1002/chem.200600313 ↗
14. Debecker DP, Mutin PH (2012) Non-hydrolytic sol–gel routes to heterogeneous catalysts. Chem Soc Rev 41:3624–365010.1039/c2cs15330k ↗
15. Fisch AG, Cardozo NSM, Secchi AR, Stedile FC, Radtke C, de Sá DS, da Rocha ZN, dos Santos JHZ (2009) Immobilization of zirconocene within silica-tungsten by entrapment: Tuning electronic effects of the support on the supported complex. Appl Catal A 370:114–12210.1016/j.apcata.2009.09.032 ↗
16. Fisch AG, Petry CF, Pozebon D, Stedile FC, Cardozo NSM, Secchi AR, dos Santos JHZ (2006) Immobilization of zirconocene into silica prepared by non-hydrolytic sol–gel method. Macromol Symp 245–246:77–8610.1002/masy.200651311 ↗
17. Fisch AG, Cardozo NSM, Secchi AR, Stedile FC, Livotto PR, de As DS, da Rocha ZN, dos Santos JHZ (2009) Immobilization of metallocene within silica-titania by a non-hydrolytic sol–gel method. Appl Catal A 354:88–10110.1016/j.apcata.2008.11.013 ↗
18. Fisch AG, Cardozo NSM, Secchi AR, Stedile FC, da Silveira NP, dos Santos JHZ (2008) Investigation of silica particle structure containing metallocene immobilized by a sol–gel method. J Non Cryst Solids 354:3973–397910.1016/j.jnoncrysol.2008.05.018 ↗
19. Hay JN, Haval HM (1998) Preparation of inorganic oxides via a non-hydrolytic sol–gel route. J Sol–Gel Sci Technol 13:109–11210.1023/A:1008615708489 ↗
20. Bourget L, Corriu RJP, Leclereq D, Mutin PH, Vioux A (1998) Non-hydrolytic sol–gel routes to silica. J Non Cryst Solids 242:81–9110.1016/S0022-3093(98)00789-3 ↗
21. Ilavsky J, Jemian PR (2009) Irena: tool suite for modeling and analysis of small-angle scattering. J Appl Crystallogr 42:347–35310.1107/S0021889809002222 ↗
22. Beaucage G (1995) Approximations leading to a unified exponential/power-law approach to small-angle scattering. Appl Crystallogr 28:717–72810.1107/S0021889895005292 ↗
23. Beaucage G (1996) Small-angle scattering from polymeric mass fractals of arbitrary mass-fractal dimension. Appl Crystallogr 29:134–14610.1107/S0021889895011605 ↗
24. Cullity BD (1978) Elements of X-ray diffraction, 2nd edn. Addison-Wesley Publishing Company Inc., Indiana, pp 1–509
25. Fidalgo A, Ilharco LM (2004) Chemical tailoring of porous silica xerogels: local structure by vibrational spectroscopy. Chem Eur J 10(2):392–39810.1002/chem.200305079 ↗
26. Cappeletti LB, Moncada E, Poisson J, Butler I, dos Santos JHZ (2013) Determination of the network structure of sensor materials prepared by three different sol–gel routes using Fourier transform infrared spectroscopy (FT-IR). Appl Spectrosc 67(4):44110.1366/12-06748 ↗
27. Ressler T (1998) High-pressure EXAFS and EDXRD K investigation of unit cell parameters of SnO. J Synch Rad 5:11810.1107/S0909049597019298 ↗
28. Newville M (2001) IFEFFIT: interactive EXAFS analysis and FEFF fitting. J Synch Rad 8:322–32410.1107/S0909049500016964 ↗
29. Mustre de Leon J, Rehr JJ, Zabinsky SI, Albers RC (1991) Ab initio curved-wave X-ray-absorption fine structure. Phys Rev B 44:4146–415610.1103/PhysRevB.44.4146 ↗
30. Silveira F, Brambilla R, da Silveira NP, do Alves MCM, Stedile FC, Pergher SBC, dos Santos JHZ (2010) Effect of textural characteristics of supported metallocenes on ethylene polymerization. J Mater Sci 45:1760–176810.1007/s10853-009-4153-9 ↗
31. Fisch AG, Da Silveira N Jr, Cardozo NSM, Secchi AR, dos Santos JHZ, Soares JBP (2013) Direct production of ultra-high molecular weight polyethylene with oriented crystalline microstructures. J Mol Catal A: Chem 366:74–8310.1016/j.molcata.2012.08.028 ↗
32. Wooster NZ (1930) International center for diffraction data. Kristall 74:363
33. Almeida RM (2004) Handbook of sol–gel science and technology: processing, characterization and applications. Volume II: characterization of sol–gel materials and products. Kluwer Academic Press, New York
34. Almeida RM, Guiton TA, Pantano CG (1990) Detection of LO Mode in ν-SiO2 by infrared diffuse reflectance spectroscopy. J Non Cryst Solids 119(2):238–24110.1016/0022-3093(90)90847-F ↗
35. Fidalgo A, Ciriminna R, Ilharco LM, Pagliaro M (2005) Role of the alkyl–alkoxide precursor on the structure and catalytic properties of hybrid sol–gel catalysts. Chem Mater 17(26):6686–669410.1021/cm051954x ↗
36. Morais EC, Correa GG, Brambilla R, Radtke C, Baibich IM, dos Santos JHZ (2013) The interaction of encapsulated pharmaceutical drugs with a silica matrix. Colloids Surf B Biointerfaces 103:422–42910.1016/j.colsurfb.2012.10.059 ↗
37. Lana SLB, Seldon AB (1998) X-ray diffraction studies of sol–gel derived ORMOSILs based on combinations of tetramethoxysilane and trimethoxysilane. J Sol–Gel Sci Technol 13(1–3):461–46610.1023/A:1008685614559 ↗
38. Lee EL, Wachs IE (2007) In situ spectroscopic investigation of the molecular and electronic structures of SiO2 supported surface metal oxides. J Phys Chem C 111:14410–1442510.1021/jp0735482 ↗
39. Borghesi A, Guizzetti G, Marabelli F, Nosenzo L, Reguzzoni E (1984) Far-infrared optical properties of CrC13 and CrBr 3. Solid State Commun 52(4):463–46510.1016/0038-1098(84)90036-X ↗
40. Zhang Q, Wang Y, Ohishi Y, Shihido T, Takehira K (2001) Vanadium-containing MCM-41 for partial oxidation of lower alkanes. J Catal 202:308–31810.1006/jcat.2001.3276 ↗
41. Takehira K, Ohishi Y, Shishido T, Kawabata T, Takaki K, Zhang QH, Wang Y (2004) Behavior of active sites on Cr-MCM-41 catalysts during the dehydrogenation of propane with CO2. J Catal 224:404–41610.1016/j.jcat.2004.03.014 ↗
42. Groppo E, Lamberti C, Bordiga S, Spoto G, Zecchina A (2005) The structure of active centers and the ethylene polymerization mechanism on the Cr/SiO2 catalyst: a frontier for the characterization methods. Chem Rev 105:115–18410.1021/cr040083s ↗
43. Naydenov V, Tosheva L, Sterte J (2002) Spherical silica macrostructures containing vanadium and tungsten oxides assembled by the resin templating method. Microp Mosop Mat 55:253–26310.1016/S1387-1811(02)00427-4 ↗
44. Tromp M, Moulin J, Reid G, Evans J (2007) Cr K-Edge XANES spectroscopy: ligand and oxidation state dependence—what is oxidation state? AIP Conf Proc 882:699–70110.1063/1.2644637 ↗