Search results for "Chemisorption"
showing 10 items of 53 documents
Metal Cluster — Surface Interaction: Simple Models and Ab Initio Calculations
1999
We review recent ab initio atomistic calculations on interactions between metal clusters and electronically inert (insulating) substrates. The model system is sodium clusters on the sodium-chloride (001) surface. This system provides an example of weak cluster-support interaction (physisorption) which can however be easily modified by introducing color centers at the surface, resulting in chemisorption of sodium adatom or cluster. The results obtained from atomistic calculations can be used for constructing simple jellium-type models for the adsorbed cluster. These models allow for systematic investigations in a large size-range of clusters on the shell structure, dimensionality, and stabil…
Surface functionalization and surface recognition: Plasmon optical detection of molecular recognition at self assembled monolayers
1991
The synthesis of biotin- functionalized organic mercaptans and their chemisorption on gold surfaces is described. Biotin bound covalently to self assembled monolayers is recognized by streptavidin from aqueous buffer solutions. Spacer length and packing density of the biotin labels on the organic surface determine the docking kinetics. With a flexible and hydrophilic spacer very fast -diffusion controlled-docking is observed. As an alternative method of self assembly the spreading of organic mercaptans on water surfaces is established. Pressure-area diagrams of different functionalized mercaptans and disulfides are shown and their monolayer properties are discussed.
A First-Principles Study of the Ag/a-Al2O3(0001) Interface
2001
Ab initio simulations of the Ag/a-Al2O3(0001) interface have been performed for periodic slab models. We have considered Al- and O-terminated corundum surfaces, low and high substrate coverages by silver, as well as the two preferred Ag adsorption sites. The two different terminations give rise to qualitatively different results: silver physisorption on the Al-terminated substrate and chemisorption on O-terminated one. The latter could be treated as a possible model for the defective Al-terminated substrate, where the outermost aluminium ions are removed (completely or partly). This makes O-terminated surface highly reactive towards a deposited metal, in order to restore initial corundum st…
Evaluating Thermal Corrections for Adsorption Processes at the Metal/Gas Interface
2019
International audience; Adsorption and desorption steps are key for active catalysts and rely on a subtle balance between enthalpic and entropic terms. While the enthalpic term is becoming ever more accurate through density functional development, the entropic term remains underrated and its precise determination a great challenge. In this work, we have performed extensive first principles thermodynamic integration (TI) simulations for the 1 adsorption of small (e.g., CO) to larger (e.g., phenol) molecules at metallic surfaces and compared their adsorption free energies to the values obtained by vertical, static statistical mechanics approximations to thermal corrections invoking three diff…
Investigation of the porosity of silica and alumina with chemically bonded polystyrene
1996
The effect of modification of porous silica and alumina with a copolymer of styrene and vinylsilane on the porosity of oxides have been investigated by means of low temperature nitrogen sorption. Only small changes of the specific surface area and of the specific pore volume were observed on modification of oxides with non-cross-linked copolymer. The specific surface area significantly increased after the cross-linking of the deposited polymeric layer while the specific pore volume remains almost unaffected. A broad hysteresis loop appears in the nitrogen sorption isotherm for the alumina modified with the cross-linked polymer. The porosity of oxides modified by chemisorption method differe…
Formation and Characterization of Self-Assembled Films of Thiol-Derivatized Poly(Dimethylsiloxane) on Gold
1997
Poly(dimethylsiloxane) (PDMS) copolymers containing propanethiol side chain “stickers” for forming self-assembled films on gold surfaces have been studied by various experimental techniques including ellipsometry, contact angle measurements, FT-IR, angle-dependent XPS, and ToF−SIMS. The results show that the thiol-containing side chains do not all chemisorb to the gold surfaces. In addition, the concentration of these sticker units was found to have a dominant effect on the polymer film thickness, the surface wetting properties, and the orientation of the PDMS backbone. Ab initio calculations reveal that the IR-active PDMS Si−O stretching bands can be used as indications of chain orientatio…
On the mechanism of the interaction between oxygen and close-packed single-crystal aluminum surfaces
2003
Abstract Using periodic first principles simulations we investigate the interaction of oxygen molecules with both regular Al(111) and Al(001) surfaces as well as a stepped Al(111) substrate. The limitation of this approach is the use of thin metallic slabs with a limited range for their coverage by adsorbed oxygen. The advantage is the detailed modeling that is possible at an atomic level. On the regular Al(111) surface, we have been able to follow the oxidation process from the approach of O 2 molecules to the surface, through the chemisorption and absorption of O atoms, up to the formation of first Al 2 O 3 formula units. An energetically feasible mechanism for the formation of these Al 2…
Fabrication of Single Cylindrical Au-Coated Nanopores with Non-Homogeneous Fixed Charge Distribution Exhibiting High Current Rectifications
2014
We have designed and characterized a cylindrical nanopore that exhibits high electrochemical current rectification ratios at low and intermediate electrolyte concentrations. For this purpose, the track-etched single cylindrical nanopore in polymer membrane is coated with a gold (Au) layer via electroless plating technique. Then, a non-homogeneous fixed charge distribution inside the Au-coated nanopore is obtained by incorporating thiol-terminated uncharged poly(N-isopropylacrylamide) (PNIPAM) chains in series to poly(4-vinyl pyridine) (PVP) chains, which are positively charged at acidic pH values. The functionalization reaction is checked by measuring the current–voltage (I–V) curves prior …
Oxygen on Fe(110): magnetic properties of the adsorbate system
1999
Abstract Investigations concerning the electronic and magnetic properties of oxygen adsorbed on magnetized iron films were carried out by means of angle and spin resolving photoelectron spectroscopy. Iron(1 1 0), epitaxially grown on a W(1 1 0) crystal, served as the ferromagnetic substrate. Exchange splittings of the O 2p x derived level were detected demonstrating a magnetic coupling between the chemisorbate and the iron layer. This observation indicates the presence of an induced magnetic moment within the adsorbate overlayer. Variations of the exchange splitting occurred as a function of the oxygen coverage, energy of the exciting radiation, and detection angle of the emitted photoelect…
Phase analysis and oxygen strorage capacity of ceria-lanthana-based TWC promoters prepared by sol-gel routes
2002
Ceria–lanthana-based promoters of three-way catalysts are synthesized by two different sol–gel routes, involving nitrate precursors. The oxygen uptake ability of these compounds is measured by O2 chemisorption. The specific surface area is determined by N2 adsorption (BET). X-ray diffraction data are analyzed by Rietveld refinement, demonstrating that lanthanum forms solid solution with CeO2; its total amount in ceria depends on the competitive formation of La–Al mixed oxides and on the synthetic method. The O2 uptake ability is essentially determined by the La content in the ceria–lanthana solid solution, while it is independent on the surface area and on the CeO2 particle size. The O2 upt…