Interaction of ethylene with the hydrogen-preadsorbed palladium (110) surface: hydrogenation and hydrogen-deuterium-exchange reactions

Sekitani, T.; Takaoka, Tsuyoshi; Fujisawa, Masashi; Nishijima, Michiharu

doi:10.1021/j100200a048

Cited by 37 publications

(25 citation statements)

References 5 publications

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“…[19] This observation implies that the di-s-bonded alkenes rapidly exchange H atoms with D atoms present on the surface via half-hydrogenated ethyl and pentyl species from which alkenes desorb, thus resulting in the HT peak in the TPD spectra. This finding is in line with results previously reported by Vasquez Jr. and Madix [20] for 1-hexene on Pd(111) and by Sekitani et al [21] for ethene on Pd(110), and can explain the H-D exchange reaction observed. Stacchiola et al [13] have recently proposed the formation of an h 1 -allyl species for propene on Pd(111), based on infrared spectroscopic measurements.…”

supporting

confidence: 94%

Surface‐Bonded Precursor Determines Particle Size Effects for Alkene Hydrogenation on Palladium

2005

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Reactions of linear alkenes with metal surfaces have been previously studied on model catalyst systems with varying degrees of complexity, from single crystals to metal particles deposited on well-ordered oxide films. [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15] Based on these studies, the majority of which were conducted with ethene, it has been suggested that alkene hydrogenation is structure insensitive. This means that the reaction only depends on the number of metal atoms on the surface and is independent of the crystallographic orientation of the particle facets and particle size. These size effects are difficult to study in real catalytic systems because the mean particle size and distribution cannot be controlled accurately. Herein, we report the particle size effects on alkene reactivity (ethene and trans-2-pentene) using well-defined Pd/Al 2 O 3 model catalysts, where the particle size can be varied in a controllable manner. Temperature-programmed desorption (TPD) indicated that alkene adsorption exhibits site-specific behavior, which is assigned to the reactions occurring separately on facets and on low-coordination-number atoms such as edge and corner atoms. A strong particle size effect (within the 1-5-nm range) is observed for the hydrogenation of pentene over a hydrogen-precovered surface, whereas the reaction for ethene is independent of size. These effects are explained by the reactions proceeding via di-s-bonded pentene, which is favored on the terrace sites of large particles, and p-bonded ethene.The morphology of the Pd model system has been studied intensively in our laboratory by scanning tunneling microscopy. [9,16] Thin alumina films were grown on a clean NiAl(110) single crystal, and subsequently Pd was vapordeposited onto the films (see the Experimental Section for details). An average particle size was determined from the amount of Pd deposited and could be varied within the range 1-5 nm with a narrow particle-size distribution (20 %); [16] the corresponding relationship is presented in reference [9]. To exclude any effects of morphology changes on Pd particles during TPD measurements, the samples were preannealed at 500 K before the adsorption experiments.

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supporting

confidence: 94%

Surface‐Bonded Precursor Determines Particle Size Effects for Alkene Hydrogenation on Palladium

2005

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“…3b. For the largest Pd particles studied (>30Å), the TPD spectrum is similar to those observed for the Pd single-crystal surfaces with a dominant desorption peak at around 300 K (16,28,29).…”

Section: Fragmentation (C 2 H +supporting

confidence: 65%

“…Based on IRAS and vibrational spectroscopy studies, it is concluded that rough metal surfaces, and particularly highly dispersed palladium, preferentially adsorb ethene via a πcomplex at low temperature (7,12,13,29). Therefore, we attribute the low temperature (T < 230 K) TPD signals to the desorption of π -bonded ethene.…”

Section: Fragmentation (C 2 H +mentioning

confidence: 89%

Structure–Reactivity Relationships on Supported Metal Model Catalysts: Adsorption and Reaction of Ethene and Hydrogen on Pd/Al2O3/NiAl(110)

Shaikhutdinov

Heemeier

Bäumer

et al. 2001

Journal of Catalysis

138

109

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“…Sekitani et al also presented experimental evidence that this reaction occurred on the Pd(110)-H(2 × 1) surface via ethyl species [33].…”

Section: Alkene Adsorption On Pd(111) and D/pd(111): General Trendsmentioning

confidence: 94%

Alkene chemistry on the palladium surface: nanoparticles vs single crystals

Doyle

Shaikhutdinov

Freund

2004

Journal of Catalysis

136

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Interaction of ethylene with the hydrogen-preadsorbed palladium (110) surface: hydrogenation and hydrogen-deuterium-exchange reactions

Cited by 37 publications

References 5 publications

Surface‐Bonded Precursor Determines Particle Size Effects for Alkene Hydrogenation on Palladium

Surface‐Bonded Precursor Determines Particle Size Effects for Alkene Hydrogenation on Palladium

Structure–Reactivity Relationships on Supported Metal Model Catalysts: Adsorption and Reaction of Ethene and Hydrogen on Pd/Al2O3/NiAl(110)

Alkene chemistry on the palladium surface: nanoparticles vs single crystals

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