The influence of real structure of gold catalysts in the partial hydrogenation of acrolein

Mohr, Christian; Hofmeister, H.; Claus, Peter

doi:10.1016/s0021-9517(02)00043-x

Cited by 209 publications

(148 citation statements)

References 19 publications

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“…These facts indicate that the selectivity of acrolein hydrogenation has close relationship with cluster size, which is consistent with the experiments observation that the activity and selectivity to the desired unsaturated alcohol depends on particle size and increases with increasing particle size [17,[23][24].…”

Section: Comparison Of Acrolein Hydrogenation On Au3 and Au5supporting

confidence: 90%

Theoretical Studies of Acrolein Hydrogenation to Propenol and Propanal on Au3 and Au5

Kang

Ren

2016

Preprint

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Abstract:The stepwise hydrogenation of the C=C bond and C=O group of acrolein on Au3 and Au5 model systems is investigated using the density functional theory(DFT) PW91 functional. Our results show that the C=C hydrogenation is more favorable than that of C=O bond on Au3 with the barriers of the rate-determining step being 0.35 and 0.62 eV respectively. On the other hand, the C=O reduction is preferred over the hydrogenation of the C=C bond on Au5. The corresponding barriers of the rate-determining steps are 0.45 and 0.54 eV, respectively. This demonstrated that the second hydrogenation step controls the reaction on both Au3 and Au5 for C=O and C=C hydrogenation and the C=O hydrogenation on Au5 is preferred over the hydrogenation of the C=C bond, which is helpful to address the reactivity of small size-selected supported gold clusters.

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Section: Comparison Of Acrolein Hydrogenation On Au3 and Au5supporting

confidence: 90%

Theoretical Studies of Acrolein Hydrogenation to Propenol and Propanal on Au3 and Au5

Kang

Ren

2016

Preprint

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“…Selectivity can be altered by eliminating certain types of sites from the surface of nanoparticles. A convincing demonstration of the role of specific surface sites controlling selectivity in a catalytic reaction was demonstrated recently for the chemoselective hydrogenation of acrolein over supported gold nanoparticle catalysts [15,16]. For Au nanoparticle catalyzed acrolein hydrogenation, the edges of single-crystalline gold particles have been identified as the active sites for the preferred C=O hydrogenation suggesting that the size (and/or shape) of the nanoparticle can influence reaction selectivity [16].…”

Section: Introductionmentioning

confidence: 93%

Influence of Particle Size on Reaction Selectivity in Cyclohexene Hydrogenation and Dehydrogenation over Silica-Supported Monodisperse Pt Particles

et al. 2008

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The role of particle size during the hydrogenation/dehydrogenation of cyclohexene (10 Torr C 6 H 10 , 200-600 Torr H 2 , and 273 -650 K) was studied over a series of monodisperse Pt/SBA-15 catalysts. The conversion of cyclohexene in the presence of excess H 2 (H 2 :C 6 H 10 ratio = 20-60) is characterized by three regimes: hydrogenation of cyclohexene to cyclohexane at low temperature (< 423 K), an intermediate temperature range in which both hydrogenation and dehydrogenation occur; and a high temperature regime in which the dehydrogenation of cyclohexene dominates (> 573 K). The rate of both reactions demonstrated maxima with temperature, regardless of Pt particle size. For the hydrogenation of cyclohexene, a nonArrhenius temperature dependence (apparent negative activation energy) was observed.Hydrogenation is structure insensitive at low temperatures, and apparently structure sensitive in the non-Arrhenius regime; the origin of the particle-size dependent reactivity with temperature is attributed to a change in the coverage of reactive hydrogen. Small particles were more active for dehydrogenation and had lower apparent activation energies than large particles. The selectivity can be controlled by changing the particle size, which is attributed to the structure sensitivity of both reactions in the temperature regime where hydrogenation and dehydrogenation are catalyzed simultaneously.

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“…The exposure of specific surfaces and the presence of particular grain boundaries facilitates interesting mechanical and chemical behaviors and alters the surface properties. 1,3,4 The argument has been made that these crystal structures are adopted by clusters because the energy cost of the internal strain is offset by a favorable rearrangement of surface atoms. 5 The question then arises, what happens to the internal strain and the atomic structure if one puts an external stress, such as pressure, onto these types of structures?…”

Section: Introductionmentioning

confidence: 99%

Structural distortions in 5–10 nm silver nanoparticles under high pressure

et al. 2008

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We present experimental evidence that silver nanoparticles in the size range of 5 -10 nm undergo a reversible structural transformation under hydrostatic pressures up to 10 GPa. We have used xray diffraction with a synchrotron light source to investigate pressure-dependent and size-dependent trends in the crystal structure of silver nanoparticles in a hydrostatic medium compressed in a diamond-anvil cell. Results suggest a reversible linear pressure-dependent rhombohedral distortion which has not been previously observed in bulk silver. We propose a mechanism for this transition that considers the bond-length distribution in idealized multiply twinned icosahedral particles. To further support this hypothesis, we also show that similar measurements of single-crystal platinum nanoparticles reveal no such distortions.

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The influence of real structure of gold catalysts in the partial hydrogenation of acrolein

Cited by 209 publications

References 19 publications

Theoretical Studies of Acrolein Hydrogenation to Propenol and Propanal on Au<sub>3</sub> and Au<sub>5</sub>

Theoretical Studies of Acrolein Hydrogenation to Propenol and Propanal on Au<sub>3</sub> and Au<sub>5</sub>

Influence of Particle Size on Reaction Selectivity in Cyclohexene Hydrogenation and Dehydrogenation over Silica-Supported Monodisperse Pt Particles

Structural distortions in 5–10 nm silver nanoparticles under high pressure

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