Iron and copper immobilised on mesoporous MCM-41 molecular sieves as catalysts for the oxidation of cyclohexane

Carvalho, Wagner A.; Wallau, Martin; Schuchardt, Ulf

doi:10.1016/s1381-1169(99)00031-x

Cited by 118 publications

(60 citation statements)

References 35 publications

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“…Details of the catalyst preparation were described elsewhere [33]. Briefly, the functionalization of SBA-15 was achieved by stirring 2.5 g SBA-15 in 100 ml of toluene at 65 °C [37]. To this suspension, 6.5 g 3-aminopropyltrimethoxysilane (APTMS) was added while stirring.…”

Section: Materials Preparationmentioning

confidence: 99%

The mechanism for the controlled synthesis of highly dispersed vanadia supported on silica SBA-15

Heß

Wild

Schlögl

2006

Microporous and Mesoporous Materials

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The mechanism for the controlled synthesis of highly dispersed vanadia supported on mesoporous silica SBA-15 (VO x /SBA-15) is elucidated using X-ray photoelectron spectroscopy (XPS), Raman and diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS). The synthesis consists of functionalization of SBA-15 using 3-aminopropyltrimethoxysilane (APTMS) followed by HCl treatment, anion exchange of decavanadate (V 10 O 28 6-) and calcination to yield the final material. Spectroscopic analysis yields that APTMS is grafted onto the surface via hydroxyl groups. Under ambient conditions, protonated APTMS on SBA-15 is largely hydrolyzed and present in its bidentate and tridentate form. Detailed XPS analysis reveals a strong influence of surface water on the resulting structure of APTMS on SBA-15. Under dry conditions, the protonated APTMS molecules on SBA-15 adopt the monodentate and bidentate form. During the anion exchange reaction, decavanadate is incorporated intactly into the pores, without any changes in the structure of the organic framework. In the calcination step, decavanadate is decomposed and vanadia is anchored onto the surface of SBA-15 via silanol groups resulting in highly dispersed surface vanadia species, while the organic resiues are fully removed from the pores of the silica matrix. d

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Section: Materials Preparationmentioning

confidence: 99%

The mechanism for the controlled synthesis of highly dispersed vanadia supported on silica SBA-15

Heß

Wild

Schlögl

2006

Microporous and Mesoporous Materials

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“…Functionalization of SBA-15 was achieved by stirring 2.5 g SBA-15 in 100 mL of toluene at 65°C as described in [17]. To this suspension, 6.5 g 3-APTMS was added while stirring.…”

Section: Catalyst Preparationmentioning

confidence: 99%

“…In a previous study, 3-aminopropyltrimethoxy-silane (APTMS) has been used as a linker to attach iron and copper species to the surface of MCM-41 [17]. Recently, by using molecular designed dispersion (MDD) of VO(acac) 2 , highly dispersed VO x species have been grafted on MCM-48 [13,18].…”

Section: Introductionmentioning

confidence: 99%

Partial Oxidation of Methanol Over Highly Dispersed Vanadia Supported on Silica SBA-15

et al. 2005

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The partial oxidation of methanol to formaldehyde (FA) was studied over highly dispersed vanadia supported on mesoporous silica SBA-15 (VO x /SBA-15). VO x /SBA-15 catalysts were prepared by a novel grafting/ion-exchange method and characterized using UV-VIS-and Raman spectroscopy. The resulting surface vanadium oxide species (0-2.3 V/nm 2 ), grafted on the inner pores of the SBA-15 silica matrix, consist of tetrahedrally coordinated monomeric and polymeric vanadia. The VO x /SBA-15 catalysts are active and highly selective for the production of FA between 300 and 400°C. Comparison of the reactivity results with literature data reveals that a better catalytic performance can be obtained over vanadia supported on mesoporous silica in comparison with conventional silica samples with the same vanadium loading. Raman characterization of the catalyst after reaction at high conversion indicates that dispersed vanadia partly agglomerates into vanadia crystallites during methanol oxidation.

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“…[9][10][11][12][13] Immobilization of complexes in solid supports has been shown to be a promising alternative means to provide heterogeneous catalysts for industry. 9,[14][15][16][17] In this regard, zeolites can provide a good support due to their particular characteristics, including mechanical resistance, porosity, appropriate shape, high adsorption power and selectivity, which favor an increase in the catalytic power of the supported complex. 15,16,18 The encapsulation method named ship-in-a-bottle consists of the synthesis of the complex inside the zeolite cavity through the reaction of a flexible ligand with the metal-exchanged zeolite.…”

Section: Introductionmentioning

confidence: 99%

“…9,[14][15][16][17] In this regard, zeolites can provide a good support due to their particular characteristics, including mechanical resistance, porosity, appropriate shape, high adsorption power and selectivity, which favor an increase in the catalytic power of the supported complex. 15,16,18 The encapsulation method named ship-in-a-bottle consists of the synthesis of the complex inside the zeolite cavity through the reaction of a flexible ligand with the metal-exchanged zeolite. The resulting complex is large enough to remain within the zeolite cavity, and thus the catalytic reaction is carried out inside the zeolite 'supercage'.…”

Section: Introductionmentioning

confidence: 99%

Synthesis and characterization of Fe(III)-piperazine-derived complexes encapsulated in zeolite Y

Berezuk

Paesano²,

Carvalho³

et al. 2012

Quím. Nova

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Recebido em 6/4/11; aceito em 22/11/11; publicado na web em 31/1/12Zeolite-encapsulated complexes have been widely applied in hydrocarbon oxidation catalysis. The "ship-in-a-bottle" encapsulation of iron(III) complexes containing piperazine and piperazine-derivative ligands in zeolite-Y is described. The flexible ligand methodology was employed and the efficiency and reproducibility of the procedure was investigated. The catalysts were characterized employing several techniques and the results indicate the presence of coordinated and uncoordinated iron(III) ions inside and outside the zeolitic cage.

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Iron and copper immobilised on mesoporous MCM-41 molecular sieves as catalysts for the oxidation of cyclohexane

Cited by 118 publications

References 35 publications

The mechanism for the controlled synthesis of highly dispersed vanadia supported on silica SBA-15

The mechanism for the controlled synthesis of highly dispersed vanadia supported on silica SBA-15

Partial Oxidation of Methanol Over Highly Dispersed Vanadia Supported on Silica SBA-15

Synthesis and characterization of Fe(III)-piperazine-derived complexes encapsulated in zeolite Y

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