Hydrogenation over gold catalysts: The interaction of gold with hydrogen

Kartusch, Christiane; Bokhoven, Jeroen A. van

doi:10.1007/bf03214957

Cited by 65 publications

(59 citation statements)

References 65 publications

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“…During transition to uncharged Au 12 0 (3D) structures that contain flat elements (planes) and structural defects (corners and edges), the Q(H 2 ) increases up to 78 kJ/mol. The obtained results confirmed the existing hypotheses on the positive impact of cluster defects to the activation of H 2 [13,30,[32][33][34][35] and are in agreement with explanation of NiO/ Au synergy (II).…”

Section: The Nature Of Au Activation In Nio/au Clusterssupporting

confidence: 90%

“…Our recent research on the TOF of Au particles of different sizes (2-30 nm) in hydrogenation of ethynylbenzene [13] and studies by Bus [30,31], Serna [32], Boronat [33], and Jia [28] have proved the positive influence of small gold clusters on hydrogenation rate. It was concluded that H 2 is dissociatively adsorbed only at the corners and edges of the supported gold particles [34,35]. Gold atoms at the corner and edge sites have a low coordination number compared with face atoms and thus have a more reactive d-band, resulting in these atoms to be able to interact more easily with H 2 [30] and facilitate the H 2 dissociation.…”

Section: Resultsmentioning

confidence: 99%

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Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

2012

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Au, NiO, and NiO/Au clusters of 2.5-16 nm, supported on Al 2 O 3 , ZrO 2 , TiO 2 , and ZnO, were studied in the purification of ethene feedstock from ethyne by hydrogenation at 357 K. The Au, NiO, and NiO/Au catalysts possessed 100 % selectivity to ethene. As the size of NiO clusters decreased from 7 to 3 nm, the turnover frequency (TOF) decreased from 812-1,023 to 276 h −1 . In contrast with NiO, Au activity increased with decreasing particle size. NiO/Au catalysts possessed higher stability and activity in comparison with Au and NiO catalysts. The synergistic gain on NiO/Au clusters (SG) calculated as TOF NiO/Au -TOF Au -TOF NiO was 1,466; 1,147; 563; and 569 h −1 for NiO/Au/Al 2 O 3, NiO/Au/TiO 2 , NiO/Au/ZnO, and NiO/Au/ ZrO 2 , respectively. The reasons of the observed catalytic trends and the origin of the most active and selective sites are discussed.

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Section: The Nature Of Au Activation In Nio/au Clusterssupporting

confidence: 90%

Section: Resultsmentioning

confidence: 99%

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

2012

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“…Typically, calcination of the gold hydroxide precursor phase results in gold metal nanoparticles with some residual surface oxygen [49]. As a large fraction of gold is already reduced, hydrogen atoms from H 2 dissociation by gold spill over to the ceria support and reduce its surface [50][51][52]. The hydrogen uptake for the cyanideleached Au/CeO 2 (rod) takes place in a much smaller temperature range.…”

Section: Resultsmentioning

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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“…4 Another important application is in catalysis, especially for hydrogenation reactions. [5][6][7][8][9][10][11] Although well studied, the magnetic properties of gold nanoparticles are very controversial. While bulk gold is diamagnetic, theories predict and recent studies report ordered magnetism in GNPs.…”

mentioning

confidence: 99%

Communication: Chemisorption of muonium on gold nanoparticles: A sensitive new probe of surface magnetism and reactivity

Dehn

Arseneau

Böni

et al. 2016

The Journal of Chemical Physics

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Chemisorption of muonium onto the surface of gold nanoparticles has been observed. Muonium (μ+e−), a light hydrogen-like atom, reacts chemically with uncapped 7 nm gold nanoparticles embedded in mesoporous silica (SBA-15) with a strong temperature-dependent rate. The addition rate is fast enough to allow coherent spin transfer into a diamagnetic muon state on the nanoparticle surface. The muon is well established as a sensitive probe of static or slowly fluctuating magnetic fields in bulk matter. These results represent the first muon spin rotation signal on a nanoparticle surface or any metallic surface. Only weak magnetic effects are seen on the surface of these Au nanoparticles consistent with Pauli paramagnetism.

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Hydrogenation over gold catalysts: The interaction of gold with hydrogen

Cited by 65 publications

References 65 publications

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

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

Communication: Chemisorption of muonium on gold nanoparticles: A sensitive new probe of surface magnetism and reactivity

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