Solvent-free selective oxidation of benzyl alcohol by molecular oxygen over uranium oxide supported nano-gold catalyst for the production of chlorine-free benzaldehyde
“…Following the discoveries by Haruta and Hutchings in the use of gold nanoparticles as catalysts for the oxidation of CO and ethyne hydrochlorination respectively in the 1980 s, interest in catalysis by supported gold and gold-palladium nanoparticles has expanded dramatically. [1] This has led to the discoveries of gold and gold palladium based catalysts for the direct synthesis of H 2 O 2 from H 2 and O 2 , [2] epoxidation of alkenes [3] and oxidation of alcohols [4] and polyols. [5] Oxidation is a fundamental functional-group transformation in general organic synthesis.…”
Section: Introductionmentioning
confidence: 99%
“…[9] For the stoichiometric oxidant, the obvious green candidate is molecular oxygen (air) or derived hydrogen peroxide, [10] while both supported gold and palladium nanoparticles show considerable promise as recyclable heterogeneous catalysts in this area, a combination which offers tremendous potential in terms of general environmental friendliness. [2][3][4][5] Selectivity and mechanism are features of this new science which must be understood to assist catalyst design and fine tuning. To achieve very high selectivity in a particular reaction, it is important to understand all the parallel and consecutive reactions that are active in the overall transformation, which can lead to side-products and thus a lower selectivity for the product of interest.…”
In the solvent-free oxidation of benzyl alcohol to benzaldehyde using supported gold-palladium nanoparticles as catalysts, two pathways have been identified as the sources of the principal product, benzaldehyde. One is the direct catalytic oxidation of benzyl alcohol to benzaldehyde by O(2), whereas the second is the disproportionation of two molecules of benzyl alcohol to give equal amounts of benzaldehyde and toluene. Herein we report that by changing the metal oxide used to support the metal-nanoparticles catalyst from titania or niobium oxide to magnesium oxide or zinc oxide, it is possible to switch off the disproportionation reaction and thereby completely stop the toluene formation. It has been observed that the presence of O(2) increases the turnover number of this disproportionation reaction as compared to reactions in a helium atmosphere, implying that there are two catalytic pathways leading to toluene.
“…Following the discoveries by Haruta and Hutchings in the use of gold nanoparticles as catalysts for the oxidation of CO and ethyne hydrochlorination respectively in the 1980 s, interest in catalysis by supported gold and gold-palladium nanoparticles has expanded dramatically. [1] This has led to the discoveries of gold and gold palladium based catalysts for the direct synthesis of H 2 O 2 from H 2 and O 2 , [2] epoxidation of alkenes [3] and oxidation of alcohols [4] and polyols. [5] Oxidation is a fundamental functional-group transformation in general organic synthesis.…”
Section: Introductionmentioning
confidence: 99%
“…[9] For the stoichiometric oxidant, the obvious green candidate is molecular oxygen (air) or derived hydrogen peroxide, [10] while both supported gold and palladium nanoparticles show considerable promise as recyclable heterogeneous catalysts in this area, a combination which offers tremendous potential in terms of general environmental friendliness. [2][3][4][5] Selectivity and mechanism are features of this new science which must be understood to assist catalyst design and fine tuning. To achieve very high selectivity in a particular reaction, it is important to understand all the parallel and consecutive reactions that are active in the overall transformation, which can lead to side-products and thus a lower selectivity for the product of interest.…”
In the solvent-free oxidation of benzyl alcohol to benzaldehyde using supported gold-palladium nanoparticles as catalysts, two pathways have been identified as the sources of the principal product, benzaldehyde. One is the direct catalytic oxidation of benzyl alcohol to benzaldehyde by O(2), whereas the second is the disproportionation of two molecules of benzyl alcohol to give equal amounts of benzaldehyde and toluene. Herein we report that by changing the metal oxide used to support the metal-nanoparticles catalyst from titania or niobium oxide to magnesium oxide or zinc oxide, it is possible to switch off the disproportionation reaction and thereby completely stop the toluene formation. It has been observed that the presence of O(2) increases the turnover number of this disproportionation reaction as compared to reactions in a helium atmosphere, implying that there are two catalytic pathways leading to toluene.
“…Uranium dioxide (urania) shows a hydrogen evolution electrocatalytic activity when combined with graphene [10]. Nevertheless, uranium oxides were seldom tested as the promoter in catalytic reaction, comparing to the conventional metal oxides [11,12]. However, the unique redox property may endow uranium oxides special advantage in serving as a catalyst promoter.…”
Urania-palladium-graphene nanohybrids were synthesized via a solvothermal process in ethylene glycol. With the solvothermal treatment, the Pd nanocrystals surrounded by well-crystallized urania supported on graphene oxide was obtained. This ternary hybrid showed considerably higher catalytic activity than palladium-graphene hybrids toward the reduction of 4-nitrophenol by NaBH4. Besides the smaller sizes of palladium nanoparticles in the ternary hybrids, in which the aggregation of Pd nanoparticles was prevented by urania, the charge transfer between the nano-structured Pd and urania may also contribute to the enhancement of catalytic activity by offering more active sites for adsorption and reaction.
“…[1][2][3][4] These carbonyl compounds are normally produced by selective catalytic oxidation, which has been widely used in clean production of chemicals. [5][6][7][8][9] One of the major concerns for oxidation reaction is product selectivity, a challenge arising from the fact that most products are thermodynamically unstable.…”
A series of metal oxide supported tungstophosphoric acid catalysts were prepared by impregnation. The physicochemical and acidic properties of these materials were characterized by a variety of different analytical and spectroscopic techniques, namely Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) method, and nuclear magnetic resonance (NMR), and exploited as heterogeneous catalysts for selective oxidation of benzyl alcohol (BzOH)
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