Submonolayer sensitive adsorption study of trichloroethene on single crystal surfaces by means of MIES, UPS and TPD

Schweinberger, Florian F.; Crampton, Andrew S.; Zimmermann, Teresa K.; Kwon, Gihan; Ridge, Claron J.; Günther, Sebastian; Heiz, Ulrich

doi:10.1016/j.susc.2012.09.005

Cited by 11 publications

(16 citation statements)

References 46 publications

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“…The Mo(100) (MaTeck, Germany, 0.785 cm 2 ) single crystal was cleaned by heating to 2,000 K and subsequent oxidation at 900 K in a 5 × 10 −7 mbar O 2 background (5.5 purity, Air Liquide Germany). The purity of the crystal was checked with Auger electron spectroscopy (AES) and ultraviolet photoelectron spectroscopy (UPS) 48 . The MgO(100) film was then grown at 600 K on the Mo(100) single crystal by evaporating a magnesium (≥99.95%, Merck Germany) ribbon in front of the crystal in a 5 × 10 −7 mbar background of O 2 .…”

Section: Methodsmentioning

confidence: 99%

Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters

et al. 2016

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The sensitivity, or insensitivity, of catalysed reactions to catalyst structure is a commonly employed fundamental concept. Here we report on the nature of nano-catalysed ethylene hydrogenation, investigated through experiments on size-selected Ptn (n=8–15) clusters soft-landed on magnesia and first-principles simulations, yielding benchmark information about the validity of structure sensitivity/insensitivity at the bottom of the catalyst size range. Both ethylene-hydrogenation-to-ethane and the parallel hydrogenation–dehydrogenation ethylidyne-producing route are considered, uncovering that at the <1 nm size-scale the reaction exhibits characteristics consistent with structure sensitivity, in contrast to structure insensitivity found for larger particles. The onset of catalysed hydrogenation occurs for Ptn (n≥10) clusters at T>150 K, with maximum room temperature reactivity observed for Pt13. Structure insensitivity, inherent for specific cluster sizes, is induced in the more active Pt13 by a temperature increase up to 400 K leading to ethylidyne formation. Control of sub-nanometre particle size may be used for tuning catalysed hydrogenation activity and selectivity.

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Section: Methodsmentioning

confidence: 99%

Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters

et al. 2016

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“…The MgO(100) thin film as support material was grown on a Mo(100) single crystal, and characterized, using techniques that have been previously described [21]. The Ni (99.98 % purity, Goodfellow, England), Pd (99.95 %, ESG Edelmetalle, Germany) and Pt (99.95 %, Alfa-Aesar, Germany) nanoparticles are generated by a laser evaporation source, coupled with a mass spectrometer.…”

Section: Methodsmentioning

confidence: 99%

Ethylene hydrogenation on supported Ni, Pd and Pt nanoparticles: Catalyst activity, deactivation and the d-band model

Crampton

Rötzer

Schweinberger

et al. 2016

Journal of Catalysis

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Ethylene hydrogenation catalyzed at 300 K by 1-1.5 nm nanoparticles of Ni, Pd and Pt supported on MgO(100) with a narrow size-distribution, as well as the deactivation under reaction conditions at 400 K, were investigated with pulsed molecular beam experiments. Ni nanoparticles deactivate readily at 300 K, whereas Pd particles deactivate only after pulsing at 400 K, and Pt particles were found to retain hydrogenation activity even after the 400 K heating step. The hydrogenation turnover frequency normalized to the number of particles exhibited the trend, Pt>Pd>Ni. The activity/deactivation was found to scale with the location of the particles' d-band centroid, ε c , with respect to the Fermi energy of the respective metals calculated with density-functional theory. An ε c closer to the Fermi level is indicative of a facile deactivation/low activity and an ε c farther from the Fermi level is characteristic of higher activity/impeded deactivation. CO adsorption, probed with infrared reflection absorption spectroscopy was used to investigate the clusters before and after the reaction, and the spectral features correlated with the observed catalytic behavior.

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“…Unfortunately, these electrons also suppress features from the adsorbed molecule in the spectra. In order to reveal features obscured by these secondaries, it is a common approach to subtract a fit function [171]; for the spectra in this work a polynomial function is fitted to the spectra and subtracted from the original spectrum [172]. A more detailed description of this approach, along with the used peak fitting procedure and details on the parameters, is stated in the appendix in sec.…”

Section: Photoemission Of Adsorbates -Data Treatmentmentioning

confidence: 99%

“…In particular, the adsorption behavior of TCE is studied on the surfaces MgO(100), Mo(100), Pt (111) and Mo(112) [172] and on MgO supported Pt x clusters of different sizes. Ethene adsorption is probed on MgO(100), Pt(111) as well as supported Pt x clusters.…”

Section: And A15)mentioning

confidence: 99%

Catalysis with Supported Size-selected Pt Clusters

Schweinberger¹

2014

Springer Theses

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Under ultra high vacuum conditions the electronic structure, adsorption properties and reactivity of two olefins on surfaces and Pt clusters were probed in the submonolayer range. With adsorbed trichloroethene a possible cluster-adsorbate induced change in the electronic structure and for ethene a low temperature, size dependent self-/hydrogenation was observed.In a collaborative approach, the Pt clusters were investigated under ambient pressure conditions. The clusters were characterized on local and integral level and tested towards temperature stability. Experiments in gas phase μ-reactors and in liquid, as part of a hybrid photo catalytic system, revealed size dependent reactivity.

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Submonolayer sensitive adsorption study of trichloroethene on single crystal surfaces by means of MIES, UPS and TPD

Cited by 11 publications

References 46 publications

Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters

Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters

Ethylene hydrogenation on supported Ni, Pd and Pt nanoparticles: Catalyst activity, deactivation and the d-band model

Catalysis with Supported Size-selected Pt Clusters

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