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1.
J Phys Condens Matter ; 25(9): 095009, 2013 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-23376839

RESUMO

We have studied the adsorption of copper on the clean Re(101[overline]0) surface between 300 and 900 K by means of low- and medium-energy electron diffraction (LEED and MEED) and temperature-programmed thermal desorption (TPD). The persistence of a (1 × 1) LEED pattern during Cu deposition suggests the formation of pseudomorphic Cu islands. Accordingly, the intensity-voltage behaviour of the (1 × 1) LEED beams can be quantitatively superimposed by the coverage-weighed fractions of the I(V)-curves of uncovered Re areas and of Cu-covered (1 × 1) islands. At a coverage of 1.625 × 10(19) Cu atoms m(-2) dynamical LEED I(V) calculations suggest a full hcp-oriented Cu bilayer (BL). Within this first BL, Cu wets the Re surface completely, while all following layers exhibit remnant roughness due to small Cu nuclei, as confirmed by in situ grazing-incidence MEED experiments. The completion of the first BL coincides with the saturation of a single ß TPD state at 1180 K, whilst higher coverages produce an additional zero-order α state, which peaks at 1080 K at 2.6 BL. The energy of desorption rises from 320 kJ mol(-1) at small coverages to ~360 kJ mol(-1) for a bilayer Cu film, pointing to attractive lateral Cu-Cu interactions. An analysis of the leading edge of the multilayer α state yields a desorption energy of ~305 kJ mol(-1), somewhat lower than the sublimation enthalpy of bulk Cu. Our data are discussed and compared with previous results on related systems.


Assuntos
Cobre/química , Rênio/química , Adsorção , Elétrons , Gases/química , Cinética , Propriedades de Superfície , Temperatura , Termodinâmica
2.
Chemphyschem ; 11(7): 1344-63, 2010 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-20183844

RESUMO

The peculiar catalytic activity of Au-supported titanium dioxide surfaces in the CO oxidation reaction has been a focus of interest for more than twenty years. Herein, recent data concerning preparation and structural characterisation of planar catalyst model systems consisting of single-crystalline titania and/or gold nanoparticles deposited thereon is presented and reviewed. We first expand on the deposition and growth of TiO(2) films on selected metal host surfaces and then consider the deposition of Au nanoparticles on these surfaces, including information on their geometric and electronic structures. The second issue is the interaction of these materials with carbon monoxide (one of the essential ingredients of the CO oxidation reaction) which serves as a probe molecule and monitor of the chemical activity of the model catalyst samples. Concerted efforts relating the structural and chemical properties of the respective binary materials (titania support plus deposited gold) can help to tackle and finally resolve the still open problems concerning the high activity of Au-TiO(2) catalysts in the CO oxidation reaction.


Assuntos
Monóxido de Carbono/química , Ouro/química , Nanopartículas Metálicas/química , Modelos Químicos , Titânio/química , Catálise , Oxirredução , Tamanho da Partícula
3.
Langmuir ; 23(10): 5386-93, 2007 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-17402751

RESUMO

Thin, crystallographically oriented single-crystalline Al2O3 films can be grown epitaxially on Cr2O3(0001) by codeposition of Al vapor and O2 at a substrate temperature of 825 K. The properties and growth of these films were monitored by Auger electron spectroscopy (AES), low-energy electron diffraction (LEED), low-energy ion scattering (LEIS), and X-ray photoelectron spectroscopy (XPS). Two routes of preparation were investigated: (i) stepwise growth by alternating deposition of Al at room temperature and subsequent exposure to O2 at elevated temperatures; (ii) codeposition of Al and O2 at T > 800 K. The first route was consistently found to result in the growth of a complex interfacial oxide followed by the growth of polycrystalline Al2O3. The second mode of preparation provided homogeneous and ordered, probably (0001)-oriented, films of Al2O3 that maintained a LEED pattern up to a thickness around 10 A. The surface sensitive Cr MVV Auger transition at 34 eV was completely attenuated once the Al2O3 layer had reached a thickness of 6 A, pointing to film homogeneity at an early stage. This was confirmed by the absence of a significant Cr signal in LEIS spectra.

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