“…The broader peak at higher temperatures originates from the 'slower' decomposition of ethene/ethylidyne on the surface in the later process of carbon formation. Both temperature ranges are in very good accordance with the literature [110,109,5,332,115], describing the temperature dependent adsorption of ethene on Pt(111) presented in sec. 2.1.2.…”
Section: 12)supporting
confidence: 90%
“…2.1.1b, despite experimental [5,109,115,113,98,62,64,63,60] and theoretical [116,111,104,117] efforts, the elementary steps involved in the transformation from ethene to ethylidyne are still debated. Further, the influence of co-adsorbates (i.e.…”
Section: Ethene Hydrogenationmentioning
confidence: 99%
“…Further, the influence of co-adsorbates (i.e. oxygen, CO) on the reactivity (as a function of coverage) have been studied [118,119,100,115,113], however are not within scope of this thesis and are not discussed. Figure 2.1.1: Reaction scheme and energy diagram for the surface chemistry occurring during thermal conversion of ethene via hydrogenation on Pt(111) (a).…”
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.
“…The broader peak at higher temperatures originates from the 'slower' decomposition of ethene/ethylidyne on the surface in the later process of carbon formation. Both temperature ranges are in very good accordance with the literature [110,109,5,332,115], describing the temperature dependent adsorption of ethene on Pt(111) presented in sec. 2.1.2.…”
Section: 12)supporting
confidence: 90%
“…2.1.1b, despite experimental [5,109,115,113,98,62,64,63,60] and theoretical [116,111,104,117] efforts, the elementary steps involved in the transformation from ethene to ethylidyne are still debated. Further, the influence of co-adsorbates (i.e.…”
Section: Ethene Hydrogenationmentioning
confidence: 99%
“…Further, the influence of co-adsorbates (i.e. oxygen, CO) on the reactivity (as a function of coverage) have been studied [118,119,100,115,113], however are not within scope of this thesis and are not discussed. Figure 2.1.1: Reaction scheme and energy diagram for the surface chemistry occurring during thermal conversion of ethene via hydrogenation on Pt(111) (a).…”
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.
“…This result is not unexpected, considering the well-known CO poisoning effect on pure Pt surfaces. 73 Only at elevated temperatures may CO desorption occur, which leaves available surface sites for O 2 adsorption and helps CO oxidation.…”
Various well-defined Ni-Pt(111) model catalysts are constructed at atomiclevel precision under ultra-high-vacuum conditions and characterized by X-ray photoelectron spectroscopy and scanning tunneling microscopy. Subsequent studies of CO oxidation over the surfaces show that a sandwich surface (NiO 1-x /Pt/Ni/Pt(111)) consisting of both surface Ni oxide nanoislands and subsurface Ni atoms at a Pt(111) surface presents the highest reactivity. A similar sandwich structure has been obtained in supported Pt-Ni nanoparticles via activation in H 2 at an intermediate temperature and established by techniques including acid leaching, inductively coupled plasma, and X-ray adsorption nearedge structure. Among the supported Pt-Ni catalysts studied, the sandwich bimetallic catalysts demonstrate the highest activity to CO oxidation, where 100% CO conversion occurs near room temperature. Both surface science studies of model catalysts and catalytic reaction experiments on supported catalysts illustrate the synergetic effect of the surface and subsurface Ni species on the CO oxidation, in which the surface Ni oxide nanoislands activate O 2 , producing atomic O species, while the subsurface Ni atoms further enhance the elementary reaction of CO oxidation with O.
“…These surfaces may contain metal nanoparticles for catalytic purposes (Figure 1b). Nanoparticles are fabricated by lithography techniques or synthesized in colloidal solutions ( Figure 1c) [11][12][13] .…”
Model systems for studying molecular surface chemistry have evolved from single crystal surfaces at low pressure to colloidal nanoparticles at high pressure. Low pressure surface structure studies of platinum single crystals using molecular beam surface scattering and low energy electron diffraction techniques probe the unique activity of defects, steps and kinks at the surface for dissociation reactions (H-H, C-H, C-C, O=O bonds). High-pressure investigations of platinum single crystals using sum frequency generation vibrational spectroscopy have revealed the presence and the nature of reaction intermediates. High pressure scanning tunneling microscopy of platinum single crystal surfaces showed adsorbate mobility during a catalytic reaction. Nanoparticle systems are used to determine the role of metal-oxide interfaces, site blocking and the role of surface structures in reactive surface chemistry. The size, shape and composition of nanoparticles play important roles in determining reaction activity and selectivity.
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