Pd/Si3N4 catalysts: preparation, characterization and catalytic activity for the methane oxidation

Méthivier, C.; Massardier, J.; Bertolini, J.C.

doi:10.1016/s0926-860x(99)00026-5

Cited by 44 publications

(32 citation statements)

References 19 publications

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“…The total conversion of methane under the experimental conditions was achieved already at 400°C (Fig. 3a) and the temperature at which 50% conversion occurs (320°C) is close to that of the Pd/a-Si 3 N 4 sample prepared with Pdbis-acetylacetonate in toluene [14]. The catalyst remains active and stable after 3 h of time on stream at 650°C (Fig.…”

Section: Methane Total Oxidationsupporting

confidence: 59%

“…It is mainly constituted the low temperature hexagonal a-phase; although the presence of the high temperature b-phase was also observed by XRD [14].…”

Section: Catalyst Preparationmentioning

confidence: 77%

“…It was shown that it can be used as support for metallic particles, giving rise to highly efficient catalysts in comparison with metals supported on oxides for oxidation reactions working at high temperatures [14][15][16]. For example, Pd/a-Si 3 N 4 catalysts prepared by decomposition of Pd-acetyl-acetonate dissolved in toluene are very efficient for methane combustion [14]. Moreover, they present similar properties to that of Pd supported on more classical (silica, alumina) oxide supports for the gas phase 1,3-butadiene hydrogenation reaction, both with respect to their activity and selectivity to butenes [17].…”

Section: Introductionmentioning

confidence: 99%

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Surface Modification of Pd/α-Si3N4 Catalysts Through the Solvent Used During Synthesis. Implications on the CO Chemisorption Properties and Catalytic Performances

2009

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Palladium catalysts supported on a-Si 3 N 4 were prepared by impregnation with Pd(II)-acetate dissolved either in toluene or in water. The mean metal particle size of *0.5 wt% Pd catalysts was similar (*5 nm) and independent of the way of preparation. Nevertheless, the two catalysts present very different chemisorption behaviour chemisorptive and catalytic properties. Fourier transformed infrared (FTIR) spectra of adsorbed CO at different temperatures (ranging from room temperature to 300°C) show a very different behaviour for both catalysts. While the CO adsorption states on the Pd/a-Si 3 N 4 prepared in toluene are very similar to those generally measured for silica and/or alumina supported palladium catalysts, CO chemisorbs less strongly on Pd/a-Si 3 N 4 prepared in water and on different adsorption sites. The Pd/a-Si 3 N 4 catalyst obtained by aqueous impregnation is much less efficient for the methane total oxidation. It is less active and less stable: it deactivates strongly after 3 h on stream at 650°C. The two catalysts present about the same activity for the 1,3-butadiene hydrogenation after stabilisation at 20°C. But, the catalyst prepared in water shows a much better selectivity to butenes. The results are discussed in terms of the possible migration of silicon atoms from the silicon nitride support to the surface of the palladium particles, when the catalyst is prepared in water. This is not the case when prepared in an organic solvent.

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Section: Methane Total Oxidationsupporting

confidence: 59%

“…It is mainly constituted the low temperature hexagonal a-phase; although the presence of the high temperature b-phase was also observed by XRD [14].…”

Section: Catalyst Preparationmentioning

confidence: 77%

Section: Introductionmentioning

confidence: 99%

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Surface Modification of Pd/α-Si3N4 Catalysts Through the Solvent Used During Synthesis. Implications on the CO Chemisorption Properties and Catalytic Performances

2009

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“…Therefore, studies of the performance of metal catalysts deposited on pure silicon nitride, compared to more widely used oxides, are necessary to elucidate its potential development as a catalyst support material. Studies by Lednor [5] and Méthivier et al [6,7] are pioneering in this respect. Development of these kinds of support materials and the synthesis of high area forms which can efficiently replace the more classical oxide supports, may provide new opportunities in catalysis.…”

Section: Introductionmentioning

confidence: 99%

On the Use of Silicon Nitride in Catalysis

Aires¹,

Bertolini²

2009

Top Catal

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Aires, F. J. Cadete Santos Bertolini, J. C.Silicon nitride has very good thermal and chemical stability, as well as high thermal conductivity compared to oxide materials, which are commonly used as catalyst supports. In exothermic reactions working at high temperature, this facilitates heat transfer and thus limits the formation of local hot spots, which are often responsible for structural modification of the support in addition to sintering of active phases. However, it is only recently that this material has been considered for application as a catalyst support for high temperature reactions. It is now established that silicon nitride can be a good support for catalytically active phases. Its range of application is continually expanding (e.g., partial/total oxidation of methane, hydrogenation and dehydrogenation reactions, photocatalysis, base catalysis, etc.)

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“…Zirconia exhibits three different crystalline forms: monoclinic (M), stable to temperatures below 1373° K; tetragonal (T), stable between 1373 OK and 2173 OK and cubic(C), stable above 2173°K. However, the monoclinic and tetragonal forms can be generated as structures at lower temperatures than those before mentioned (2). At ambient temperature the tetragonal form is usually referred to as "stable", and also from the thermodynamic point of view it is a very stable phase.…”

Section: -Introductionmentioning

confidence: 99%

Sol-Gel Zirconia: Phosphate Addition Effect

Collado-Pérez

Ramos-Ramírez

López

et al. 2003

Emerging Fields in Sol-Gel Science and Technology

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Abstract.Zirconia (Zr02) and phosphate zirconia gels were obtained by the sol-gel process. It was used as a precursor to the zirconium n-butoxide in ethanol. The process took place instantly when different solutions containing the ion phosphate, like phosphoric acid and sodium acidic phosphate were added to the initial solution; a hydrolysis catalyst was not used. The samples were characterized by means of X-Ray powder diffraction, Infrared Spectroscopy (FTIR) and Textural Analysis BET. The addition of the phosphate ion produces an increase in the specific area of the samples. The X-Ray diffraction, shows that the tetragonal phase has been stabilized to low annealed temperatures and how the phosphate ion contributes to obtain a second phase, the monoclinic one.

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Pd/Si3N4 catalysts: preparation, characterization and catalytic activity for the methane oxidation

Cited by 44 publications

References 19 publications

Surface Modification of Pd/α-Si3N4 Catalysts Through the Solvent Used During Synthesis. Implications on the CO Chemisorption Properties and Catalytic Performances

Surface Modification of Pd/α-Si3N4 Catalysts Through the Solvent Used During Synthesis. Implications on the CO Chemisorption Properties and Catalytic Performances

On the Use of Silicon Nitride in Catalysis

Sol-Gel Zirconia: Phosphate Addition Effect

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