Comparative in situ XAS investigations during aerobic oxidation of alcohols over ruthenium, platinum and palladium catalysts in supercritical CO2

Caravati, Matteo; Grunwaldt, Jan‐Dierk; Baiker, A.

doi:10.1016/j.cattod.2006.10.005

Cited by 26 publications

(20 citation statements)

References 50 publications

(79 reference statements)

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“…Comparative in situ XAS of Ru, Pt and Pd/Al 2 O 3 catalysts under scCO 2 indicate that ruthenium is oxidised during reaction, 122 although the resulting RuO x may be less active than metallic species. The accumulation of carbonaceous residues, and slow removal of CO (a by-product of undesired decarbonylation) may play a role in differentiating the activity of Pd versus Pt systems.…”

Section: Mechanistic Studies Of Alcohol Seloxmentioning

confidence: 99%

“…X-ray based methods in particular can provide detailed insight into chemical composition and environment of active components and reacting adsorbates. 115 -117 Quick and dispersive X-ray absorption spectroscopies (XAS) have the capability to monitor dynamic changes in catalyst structure under reaction conditions (so-called operando spectroscopy) and have been applied to alcohol selox over Pd, 16,118 -121 Pt 66,122 and Ru 122 nanoparticles. An example of an operando reaction cell for such measurements is illustrated in Fig.…”

Section: Mechanistic Studies Of Alcohol Seloxmentioning

confidence: 99%

See 1 more Smart Citation

Recent advances in the heterogeneously catalysed aerobic selective oxidation of alcohols

Vinod

Wilson

Lee

2010

J. Chem. Technol. Biotechnol.

166

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The heterogeneously catalysed selective aerobic oxidation of alcohols is an important tool for the synthesis of valuable chemical intermediates and a hot topic within both academic and industrial arenas. In this mini-review, selected aspects of catalyst formulation, process operating conditions, and progress in identifying the active sites and surface reaction mechanisms notably through the application of synchrotron radiation, are highlighted.

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Section: Mechanistic Studies Of Alcohol Seloxmentioning

confidence: 99%

Section: Mechanistic Studies Of Alcohol Seloxmentioning

confidence: 99%

Recent advances in the heterogeneously catalysed aerobic selective oxidation of alcohols

Vinod

Wilson

Lee

2010

J. Chem. Technol. Biotechnol.

166

View full text Add to dashboard Cite

show abstract

“…X-ray-based methods in particular can provide detailed insight into chemical composition and environment of active components and reacting adsorbates [140][141][142]. Quick and dispersive XAS have the capability to monitor dynamic changes in catalyst structure under reaction conditions (so-called operando spectroscopy) and have been applied to alcohol selox over Pd [96,[143][144][145][146], Pt [67,147], and Ru [147] nanoparticles.…”

Section: X-ray Absorption Spectroscopymentioning

confidence: 99%

“…Comparative in situ XAS of Ru, Pt, and Pd/Al 2 O 3 catalysts under scCO 2 indicated that ruthenium is oxidized during reaction [147], although the resulting RuO x may be less active than the initial metal. The accumulation of carbonaceous residues and slow removal of CO (a by-product of undesired decarbonylation) may play a role in differentiating the activity of Pd versus Pt systems.…”

Section: In Situ and Operando X-ray Studies Of Selox Catalystsmentioning

confidence: 99%

Mechanistic Studies of Alcohol Selective Oxidation

Lee

2013

Heterogeneous Catalysts for Clean Technology

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IntroductionCatalytic selective oxidation (selox) is an important class of clean chemical transformations employed in the synthesis of valuable chemical intermediates, and a test bed for many fundamental concepts within heterogeneous catalysis and surface science. The selox of alcohols, carbohydrates, and aromatics is especially challenging in terms of understanding the dynamics of chemical reactions at the liquid-solid-gas interface, and requires new spectroscopic tools and analytical protocols to provide quantitative spatiotemporal information on structure-function relationships in order to optimize reaction conditions and design next-generation selox catalysts. Advances in inorganic methodologies to synthesize tunable nanostructures, and synchrotron science and the parallel development of multidimensional spectroscopies, afford new possibilities for understanding the operation of catalysts under working conditions (operando), and thereby nanoengineering the active site for improved activity, selective, and lifetime in selox chemistry. Applications of Selective OxidationThe oxidative dehydrogenation of alcohols represents key steps in the synthesis of aldehyde, ketone, ester, and acid intermediates employed within the fine chemical, pharmaceutical, and agrochemical sectors, with allylic aldehydes in particular high-value components used in the perfume and flavoring industries [1]. For example, crotonaldehyde is an important agrochemical and a valuable precursor for the food preservative sorbic acid, while citronellyl acetate and cinnamaldehyde confer rose/fruity and cinnamon flavors and aromas, respectively. There is also considerable interest in the exploitation of biomass-derived feedstocks such as glycerol (a by-product of biodiesel synthesis from plant or Heterogeneous Catalysts for Clean Technology: Spectroscopy, Design, and Monitoring, First Edition. Edited

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“…In this approach, the catalytic reaction condition and regeneration procedure are controlled by the aide of operando spectroscopic technique to achieve the high catalytic performance [4,5]. Many spectroscopic techniques such as Raman [4][5][6], infrared (IR) [7][8][9][10][11][12], ultraviolet-visible (UV-Vis) [13,14], X-ray absorption fine structure (XAFS) [11,12,[15][16][17][18], X-ray diffraction (XRD) [18], electron spin resonance (ESR) [19] and nuclear magnetic resonance (NMR) [20,21] have been applied in operando studies. Recently, two or more spectroscopic techniques were combined into one experimental setup in operando investigations [11,[22][23][24][25].…”

Section: Introductionmentioning

confidence: 99%

Operando X-ray Absorption Spectroscopy Study of Pt/γ-Al2O3 During the Total Oxidation of C3H6

et al. 2009

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Operando X-ray absorption fine structure (XAFS) investigations were performed on Pt/c-Al 2 O 3 during the total oxidation of C 3 H 6 in reducing and oxidizing atmospheres. Study of the Pt valance state and catalytic conversion behavior as a function of temperature revealed that both the creation of metallic Pt sites and the activation of adsorbed species on Pt are important for the functioning of the catalytic reaction at low temperature.

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Comparative in situ XAS investigations during aerobic oxidation of alcohols over ruthenium, platinum and palladium catalysts in supercritical CO2

Cited by 26 publications

References 50 publications

Recent advances in the heterogeneously catalysed aerobic selective oxidation of alcohols

Recent advances in the heterogeneously catalysed aerobic selective oxidation of alcohols

Mechanistic Studies of Alcohol Selective Oxidation

Operando X-ray Absorption Spectroscopy Study of Pt/γ-Al2O3 During the Total Oxidation of C3H6

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