Biomedical subjects

Alessandro Baraldi

Publications and source records attributed to Alessandro Baraldi.

4 recordsLinked to original sources

PubMed2005

Unexpected behavior of the surface composition of PtRh alloys during chemical reaction.

The changes in the surface composition of a Pt(50)Rh(50)(100) alloy due to an ongoing 2H(2) + O(2)-->2H(2)O chemical reaction have been studied in situ. Exploiting the high-energy resolution and surface sensitivity of synchrotron radiation core-level spectroscopy it was possible to monitor the population of the two transitions metals atoms at the gas-surface interface. Sequences of fast high-resolution core-level spectra of the Rh3d(5/2), Pt4f(7/2), and O1s core levels showed a continuous exchange of atoms between the first and subsurface layers. An unexpected Pt surface enrichement was found under slightly oxidizing conditions, opposite to what found in a highly oxidizing atmosphere.

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PubMed2004

Ethanol decomposition: C--C cleavage selectivity on Rh(111).

Ethanol adsorption, desorption and decomposition on Rh(111) have been studied by X-ray photoelectron spectroscopy and tem-perature-programmed desorption experiments. The evolution of the C is and O is core level spectra was monitored as a function of ethanol exposure and surface temperature. Ethanol adsorption at 90 K results in two nonequivalent ethanol-adsorbed species at low surface coverage, while a third species--related to multilayer formation--appears after longer exposures. Upon surface annealing, ethanol undergoes both desorption and dissociation, thus creating intermediate surface species which further decompose to hydrogen, carbon monoxide and atomic carbon. Our results clearly show that C--C bond cleavage is the preferential dissociation channel, while C--O bond scission is not observed. Calculations performed within the framework of the unity bond index-quadratic exponent potential model, have been used to test and compare different competing dissociation channels, providing an estimate of adsorption energies and dissociation barriers.

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PubMed2003

Adsorption of CO2 and coadsorption of H and CO2 on potassium-promoted Cu(115).

The influence of potassium, in the submonolayer regime, on the adsorption and coadsorption of CO2 and H on a stepped copper surface, Cu(115), has been studied by photoelectron spectroscopy, temperature-programmed desorption, and work-function measurements. Based on the fast recording of C 1s and O 1s core-level spectra, the uptake of CO2 on K/Cu(115) surfaces at 120 K has been followed in real time, and the different reaction products have been identified. The K 2p3/2 peak exhibits a chemical shift of -0.4 eV with CO2 saturation, the C 1s peaks of the CO3 and the CO species show shifts of -0.8 and -0.5 eV, respectively, and the C 1s peak of the physisorbed CO2 exhibits no shift. The effects of gradually heating the CO2/K/Cu(115) surface include the desorption of physisorbed CO2 at 143 K; the desorption of CO at 193 K; the ordering of the CO3 species, and subsequently the dissociation of the carbonate with desorption at 520-700 K. Formate, HCOO-, was synthesized by the coadsorption of H and CO2 on the K/Cu(115) surface at 125 K. Formate formed exclusively for potassium coverages of less than 0.4 monolayer, whereas both formate and carbonate were formed at higher coverages. The desorption of formate-derived CO2 took place in the temperature range 410-425 K and carbonate-derived CO2 desorbed at 645-660 K, depending on the potassium coverage.

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PubMed2002

Impact of defects on the surface chemistry of ZnO(0001 macro)-O.

Scanning tunneling microscopy and core level photoelectron spectroscopy measurements have been used to investigate the morphology of ZnO(0001 macro)-O, and its reactivity with carbon monoxide and carbon dioxide, as a function of surface preparation. Real space images of the surface indicate that increasing the substrate anneal temperature during preparation significantly reduces the surface step density. Surface defect concentration is also monitored by employing formic acid as a chemical probe, which is shown to adsorb dissociatively (HCOOH --> [HCOO](-) + H(+)) only on zinc cations at step edges. Carbon 1s X-ray photoelectron spectra show that carbon monoxide and carbon dioxide both react to form surface carbonate species. Spectra, recorded both as a function of surface preparation and following coadsorption, demonstrate that the carbonate formed from either reactant molecule is located at oxygen vacancies at step edges, evidencing the significant role that defects can play in the surface chemistry of ZnO(0001 macro)-O.

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