An experimental and theoretical investigation of the structure and reactivity of bilayered VO /TiO /SiO2 catalysts for methanol oxidation

Vining, William C.; Goodrow, Anthony; Strunk, Jennifer; Bell, Alexis T.

doi:10.1016/j.jcat.2009.12.017

Cited by 38 publications

(49 citation statements)

References 41 publications

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“…For example, Au particles have been shown to be much more stable on TiO x /SiO 2 than on SiO 2 25 and isolated vanadate species dispersed on TiO x /SiO 2 exhibit turnover frequencies that are up to 60-fold higher than when dispersed on SiO 2 . 7 CeO 2 is a highly reducible oxide exhibiting oxygen storage and release properties that are important for the operation of threeway, automotive exhaust catalysts. 26 It can also stabilize the dispersion of noble metal particles, 27 and CeO 2 -supported vanadia is much more active for methanol synthesis than vanadia dispersed on other supports.…”

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confidence: 99%

Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties

2011

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An investigation was performed to establish the effects of precursor composition on the structure of ceria deposited onto mesoporous silicas, MCM-41 and SBA-15. The structure of the deposited ceria was characterized by XRD, TEM, Raman and UV-visible spectroscopy, XANES, and EXAFS. Using Ce(acac) 3 as the precursor resulted in formation of 3 nm diameter ceria particles located predominantly in the mouths of the support pores. Amorphous agglomerates, but with domains of comparable size to those obtained using Ce(acac) 3 , were obtained using Ce(O i Pr) 4 . Much smaller domains and a high degree of dispersion were obtained using Ce(O t Bu) 4 as the precursor. The structure of the deposited ceria affects its reduction-reoxidation properties. Reduction and reoxidation are almost fully reversible for the nanoparticles. Only surface reduction is observed up to 723 K, whereas partial bulk reduction takes place at higher reduction temperatures. In case of the well-dispersed, layerlike Ce species on the silica surface, an extent of reduction similar to that of the nanoparticles is achievable, but upon heating the samples in 10% H 2 /He to 923 K the reduction becomes partially irreversible. The latter effect might be explained by a formation of cerium silicates that prevent the complete reoxidation of the cerium species. ' INTRODUCTIONDispersion of a transition metal oxide on a high surface area support such as Al 2 O 3 or SiO 2 makes it possible to combine the catalytic properties of the transition metal oxide with the high surface area and thermal and mechanical stability of the support. 1 Good illustrations of the manner in which the transition metal oxide is introduced onto the support and the physical properties of the deposited oxide are given for the cases of TiO x , 1-9 VO x , 5,[9][10][11][12][13][14] or MoO x 10,11,15-21 dispersed on high surface area supports. A notable consequence of this approach is the formation of catalytically active sites which are not present on either the support or the bulk transition metal oxide. For example, neither TiO 2 nor SiO 2 is active for the liquid-phase epoxidation of alkenes, but TiO 2 /SiO 2 exhibits high activity and selectivity for this reaction. 6,[22][23][24] The appearance of such novel catalytically active sites has been attributed to the formation of a twodimensional oxide overlayer whose physical properties differ from those of the corresponding bulk oxide. Dispersed transition metal oxides have also been shown to stabilize the dispersion of small metal particles and to enhance the activity of supported metal oxo species. For example, Au particles have been shown to be much more stable on TiO x /SiO 2 than on SiO 2 25 and isolated vanadate species dispersed on TiO x /SiO 2 exhibit turnover frequencies that are up to 60-fold higher than when dispersed on SiO 2 . 7 CeO 2 is a highly reducible oxide exhibiting oxygen storage and release properties that are important for the operation of threeway, automotive exhaust catalysts. 26 It can also stabilize the dispersion of n...

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Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties

2011

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“…Each unit of the (2 × 2) superstructure contains two V atoms and four Pt atoms. Same structure was identified in the s-V 2 O 3 /Pd(1 1 1) and VO x /Rh(1 1 1) system [10,14,34,35]. The density of the surface atom of Pt(1 1 1) is 8.3 Pt atoms per nm 2 .…”

Section: Kinetic Study Of Oxidation Of Propane On Vo X /Smo X /Pt(1 1mentioning

confidence: 59%

“…The 69 meV peak reaches its maximum intensity along with a sharp (2 × 2) LEED pattern at 1 ML, above which there appears a new HREELS peak at 62 meV and it dominates at 2 ML. Altogether, also with the detailed structural information on similar systems of VO x /Pd and VO x /Rh in the literature [10,14,34,35], we proposed a possible structural model for the 1 ML V 2 O 3 /Pt(1 1 1) as shown in Fig. 4C.…”

Section: Resultsmentioning

confidence: 83%

“…Partial oxidation of C 3 H 8 to C 3 H 6 is an attractive route to bridge the propene supply-demand gap, but the selectivity of C 3 H 6 is low because of the further oxidation to CO x . VO x -based catalysts, being studied extensively for decades [6][7][8][9][10][11][12], show considerable high reaction activity and C 3 H 6 selectivity at a relatively low temperature. However, in most cases, selectivity of C 3 H 6 decreased when the conversion of C 3 H 8 increased at an elevated temperature.…”

Section: Introductionmentioning

confidence: 99%

“…Modifications of the VO x -based catalysts have been shown to enhance the selectivity of C 3 H 6 at higher reaction temperatures, which include varying the oxide supports, adding alkali metals and/or alkali earth metals, mixing with other catalytically active components, etc. [6,[3][4][5][6][7][8][9][10][11][12][13][14][15][16].…”

Section: Introductionmentioning

confidence: 99%

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An experimental and theoretical investigation of the structure and reactivity of bilayered VO /TiO /SiO2 catalysts for methanol oxidation

Cited by 38 publications

References 41 publications

Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties

Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties

Model catalysis studies of the oxidation of propane over VO -based catalysts

Photocatalysis – The Heterogeneous Catalysis Perspective

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An experimental and theoretical investigation of the structure and reactivity of bilayered VO /TiO /SiO2 catalysts for methanol oxidation

Cited by 38 publications

References 41 publications

Synthesis of Different CeO2 Structures on Mesoporous Silica and Characterization of Their Reduction Properties

Synthesis of Different CeO2 Structures on Mesoporous Silica and Characterization of Their Reduction Properties

Model catalysis studies of the oxidation of propane over VO -based catalysts

Photocatalysis – The Heterogeneous Catalysis Perspective

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Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties

Synthesis of Different CeO₂ Structures on Mesoporous Silica and Characterization of Their Reduction Properties