A Collaborative Effect between Gold and a Support Induces the Selective Oxidation of Alcohols

Abad, Alberto; Concepción, Patricia; Corma, Avelino; Garcı́a, Hermenegildo

doi:10.1002/anie.200500382

Cited by 1,032 publications

(653 citation statements)

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“…The TOF values became roughly constant in the range of 0.1-1 MPa O 2 , revealing that oxygen pressure does not affect the reaction rates, in some degree (Entries 2, 3, Table 3). Under the same conditions with previous reports 17,26,50 , the TOF of 1-phenylethanol oxidation (160°C, O 2 0.1 Mpa) reached B210,000 h À 1 , which could be comparable with the result (B269,000 h À 1 ) using the Au-Pd/TiO 2 catalyst reported by Hutchings et al 26 (Entry 4, Table 3). …”

Section: Fabrication Of Nanostructured Nitrogen-doped Carbonsupporting

confidence: 88%

Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

et al. 2013

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The development of efficient systems for selective aerobic oxidation of hydrocarbons and alcohols to produce more functional compounds (aldehydes, ketones, acids or esters) with atmospheric air or molecular oxygen is a grand challenge for the chemical industry. Here we report the synthesis of palladium nanoparticles supported on novel nanoporous nitrogendoped carbon, and their impressive performance in the controlled oxidation of hydrocarbons and alcohols with air. In terms of catalytic activity, these catalysts afford much higher turnover frequencies (up to 863 turnovers per hour for hydrocarbon oxidation and up to B210,000 turnovers per hour for alcohol oxidation) than most reported palladium catalysts under the same reaction conditions. This work provides great potential for the application of ambient air and recyclable palladium catalysts in fine-chemical production with high activity.

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Section: Fabrication Of Nanostructured Nitrogen-doped Carbonsupporting

confidence: 88%

Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

et al. 2013

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“…In line with the importance of the interactions between gold and the support, it has been found that nanoscale forms of ceria contribute to the high activity of small gold particles [18][19][20][21][22][23][24]. Several authors [25][26][27][28] have used nanostructured ceria that expose certain planes to investigate the influence of the nature of the ceria surface on the nature and activity of gold species.…”

Section: Introductionmentioning

confidence: 99%

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

et al. 2011

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The interaction of gold atoms with CeO 2 nanocrystals having rod and cube shapes has been examined by cyanide leaching, TEM, TPR, CO IR and X-ray absorption spectroscopy. After deposition-precipitation and calcination of gold, these surfaces contain gold nanoparticles in the range 2-6 nm. For the ceria nanorods, a substantial amount of gold is present as cations that replace Ce ions in the surface as follows from their first and second coordination shells of oxygen and cerium by EXAFS analysis. These cations are stable against cyanide leaching in contrast to gold nanoparticles. Upon reduction the isolated Au atoms form finely dispersed metal clusters with a high activity in CO oxidation, the WGS reaction and 1,3-butadiene hydrogenation. By analogy with the very low activity of reduced gold nanoparticles on ceria nanocubes exposing the {100} surface plane, it is inferred that the gold nanoparticles on the ceria nanorod surface also have a low activity in such reactions. Although the finely dispersed Au clusters are thermally stable up to quite high temperature in line with earlier findings (Y. Guan and E. J. M. Hensen, Phys Chem Chem Phys 11:9578, 2009), the presence of gold nanoparticles results in their more facile agglomeration, especially in the presence of water (e.g., WGS conditions). For liquid phase alcohol oxidation, metallic gold nanoparticles are the active sites. In the absence of a base, the O-H bond cleavage appears to be rate limiting, while this shifts to C-H bond activation after addition of NaOH. In the latter case, the gold nanoparticles on the surface of ceria nanocubes are much more active than those on the surface of nanorod ceria.

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“…During the past two decades, numerous efforts have been devoted to developing the catalytic activity of gold for different purposes, for instance, the use of fuel cells [2], synthesis of esters, olefin epoxidation [3][4][5][6][7][8], and selective oxidation of alcohols [9][10][11][12][13][14][15][16][17][18][19][20]. Among them, alcohol oxidation is of particular interest since it is not only one of the most important reactions in industry and organic synthesis, but also one that Au-based catalysts carry out most efficiently.…”

Section: Introductionmentioning

confidence: 99%

Reaction mechanism for methanol oxidation on Au(111): A density functional theory study

Liu¹,

Jin²,

Zhang³

et al. 2013

Applied Surface Science

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A Collaborative Effect between Gold and a Support Induces the Selective Oxidation of Alcohols

Cited by 1,032 publications

References 36 publications

Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

Reaction mechanism for methanol oxidation on Au(111): A density functional theory study

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