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1.
Langmuir ; 26(21): 16568-77, 2010 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-20462255

RESUMO

We report the preparation of Au-Pd nanocrystalline catalysts supported on activated carbon prepared via a sol-immobilization technique and explore their use for the direct synthesis of hydrogen peroxide and the oxidation of benzyl alcohol. In particular, we examine the synthesis of a systematic set of Au-Pd colloidal nanoparticles having a range of Au/Pd ratios. The catalysts have been structurally characterized using a combination of UV-visible spectroscopy, transmission electron microscopy, STEM HAADF/XEDS, and X-ray photoelectron spectroscopy. The Au-Pd nanoparticles are found in the majority of cases to be homogeneous alloys, although some variation is observed in the AuPd composition at high Pd/Au ratios. The optimum performance for the synthesis of hydrogen peroxide is observed for a catalyst having a Au/Pd 1:2 molar ratio. However, the competing hydrogenation reaction of hydrogen peroxide increases with increasing Pd content, although Pd alone is less effective than when Au is also present. Investigation of the oxidation of benzyl alcohol using these materials also shows that the optimum selective oxidation to the aldehyde occurs for the Au/Pd 1:2 molar ratio catalyst. These measured activity trends are discussed in terms of the structure and composition of the supported Au-Pd nanoparticles.


Assuntos
Álcool Benzílico/síntese química , Ouro/química , Peróxido de Hidrogênio/síntese química , Paládio/química , Ligas/síntese química , Ligas/química , Álcool Benzílico/química , Catálise , Peróxido de Hidrogênio/química , Nanopartículas Metálicas/química , Oxirredução , Tamanho da Partícula , Propriedades de Superfície
2.
ChemSusChem ; 8(24): 4189-94, 2015 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-26611807

RESUMO

Pt nanoparticles were prepared by a sol immobilization route, deposited on supports with different acid/base properties (MgO, activated carbon, TiO2 , Al2O3, H-Mordenite), and tested in the selective oxidation of sorbose to 2-keto-gulonic acid (2-KGUA), an important precursor for vitamin C. In general, as the basicity of the support increased, a higher catalytic activity occurred. However, in most cases, a strong deactivation was observed. The best selectivity to 2-KGUA was observed with acidic supports (TiO2 and H-Mordenite) that were able to minimize the formation of C1/C2 products. We also demonstrated that, by alloying Pt to Au, it is possible to enhance significantly the selectivity of Pt-based catalysts. Moreover, the AuPt catalyst, unlike monometallic Pt, showed good stability in recycling because of the prevention of metal leaching during the reaction.


Assuntos
Ligas/química , Ouro/química , Platina/química , Sorbose/química , Açúcares Ácidos/química , Titânio/química , Catálise , Oxirredução
3.
Chem Commun (Camb) ; 50(84): 12612-4, 2014 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-25032752

RESUMO

The selectivity of photocatalytic phenol production from the direct oxidation of benzene can be enhanced by fine adjustment of the morphology and composition of Au-Pd metal nanoparticles supported on titanium dioxide thereby suppressing the decomposition of benzene and evolution of phenolic compounds.


Assuntos
Ligas/química , Benzeno/química , Nanopartículas Metálicas/química , Fenol/síntese química , Titânio/química , Catálise , Ouro/química , Radical Hidroxila/química , Oxirredução , Paládio/química , Fenol/química , Raios Ultravioleta
4.
Phys Chem Chem Phys ; 11(25): 4952-61, 2009 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-19562125

RESUMO

The use of bio-renewable resources for the generation of materials and chemicals continues to attract significant research attention. Glycerol, a by-product from biodiesel manufacture, is a highly functionalised renewable raw material, and in this paper the oxidation of glycerol in the presence of base using supported gold, palladium and gold-palladium alloys is described and discussed. Two supports, TiO(2) and carbon, and two preparation methods, wet impregnation and sol-immobilisation, are compared and contrasted. For the monometallic catalysts prepared by impregnation similar activities are observed for Au and Pd, but the carbon-supported monometallic catalysts are more active than those on TiO(2). Glycerate is the major product and lesser amounts of tartronate, glycolate, oxalate and formate are observed, suggesting a sequential oxidation pathway. Combining the gold and palladium as supported alloy nanocrystals leads to a significant enhancement in catalyst activity and the TiO(2)-supported catalysts are significantly more active for the impregnated catalysts. The use of a sol-immobilisation preparation method as compared to impregnation leads to the highest activity alloy catalysts and the origins of these activity trends are discussed.


Assuntos
Ligas/química , Glicerol/química , Ouro/química , Nanopartículas/química , Paládio/química , Catálise , Oxirredução
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