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1.
《Solid State Ionics》2006,177(11-12):979-988
Electrode polarization and conductivity measurements were carried out at the Pd/YSZ interface and at conditions close to the Pd–PdO thermodynamic equilibrium. The steady-state current–overpotential characteristics were analyzed with a Butler–Volmer type of equation. Both, apparent exchange current density, Io, and anodic/cathodic charge transfer coefficients (αa/αc), were calculated. Based on the experimental results, it was concluded that the charge transfer at the electrode is rate-determining in the case of PdO during anodic operation and Pd during cathodic operation, while in the other case mass transport of adsorbed oxygen species along the electrode/solid electrolyte interface is in competition with the charge transfer process. 相似文献
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《Solid State Ionics》2006,177(9-10):915-921
Electrochemical cells formed by the interface between dense and porous lanthanum strontium manganate (LSM) and yttria stabilized zirconia (YSZ) were submitted to annealing temperatures varying from 1373 K to 1673 K for 200 h and studied by Impedance Spectroscopy (IS) in order to investigate how the high annealing temperature can modify the contact between LSM/YSZ and to which extension these changes influence the electrical behavior of dense and porous LSM electrodes before and after the formation of insulating phases. Up to 1473 K the annealing process did not lead to substantial electrical behavior modifications at the LSM/YSZ interfaces for both porous and dense electrodes. IS measurements show two capacitive semicircles, the best fitting of impedance data brings to an equivalent circuit constituted by a serial combination of the electrolyte resistance and two parallel combinations of a resistance and a constant phase element, CPE. The higher frequency semicircles, HF, were attributed to the diffusion of oxide ions from the interface LSM/YSZ to the oxide ion vacancies located at the electrolyte surface. The semicircle at lower frequency, LF, will be ascribed to the oxygen species adsorption and diffusion in the LSM. At 1473 K the only changes recorded are related with the sinterization process of the porous electrodes. Over of 1473 K, the resistance contributions increased largely, especially for porous electrodes, and one additional semicircle was observed. This semicircle was associated to the oxygen diffusion process at the new insulating phases formed from YSZ and LSM solid state reactions. Porous and dense electrodes exhibited different rates for the degradation process. The porous electrode degraded faster than the dense one, probably because of the morphological effects as grain growth and their coalescence during annealing at higher temperatures. 相似文献
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The effect of electric field assisted annealing on the microstructure, composition and ionic conductivity properties in CeO2/YSZ oxide heterostructures have been investigated using molecular dynamics simulations. Amorphization–recrystallization steps were performed with and without external electric field of strength 10?MV/cm along three different orientations: in-plane (YZ), normal (X) and 45° resultant (XY) with respect to the oxide heterointerfaces. The microstructural and compositional differences at the interfaces and in the interior of the oxide heterolayers were evaluated and were found to show a clear correlation with the orientations of the applied field. In particular, the XY configuration displayed a compressive lattice strain of ~9% along with a reduced oxygen vacancy concentration when compared to the others. Ionic density profiles suggest pronounced segregation (~60% higher compared to the average value in the interior) of yttrium ions closer to the YSZ/CeO2 interface for the XY configuration. Other configurations exhibit minimal to no such variations. These microstructural differences are found to affect the number of mobile charge carriers and the activation barriers associated with ionic migration through the oxide lattice and consequently, influence the ionic conductivity. 相似文献
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By means of ab initio simulations we here provide a comprehensive scenario for hydrogen oxidation reactions at the Ni/zirconia anode of solid oxide fuel cells. The simulations have also revealed that in the presence of water chemisorbed at the oxide surface, the active region for H oxidation actually extends beyond the metal/zirconia interface unraveling the role of water partial pressure in the decrease of the polarization resistance observed experimentally. 相似文献
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Long-chain alkanes exhibit surface freezing at the alkane-air but not the alkane-water interface. Ellipsometry and surface tensiometry are used to show that a simple cationic surfactant, hexadecyltrimethylammonium bromide (CTAB), can induce surface freezing at the tetradecane-water interface even when present in mole fractions as low as 0.1. The surface-freezing temperature T(s) is a linear function of the interfacial excess of CTAB. The excess surface entropy below T(s), S(sigma)=-0.76+/-0.02 mJ K-1 m(-2), is consistent with a rotator phase. Ellipsometry provides strong evidence for a frozen monolayer in which the chains are oriented near the surface normal. 相似文献
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I. Abbati L. Braicovich B. De Michelis O. Bisi R. Rovetta 《Solid State Communications》1981,37(2):119-122
The electronic structure of Platinum silicides produced by thin film reaction is studied using ultraviolet photoemission and Auger spectroscopy. Spectra have been taken during the various stages of Si-Pt intermixing, in order to monitor the changes in the valence band, which take place during the reaction. The experimental data are compared with semi-empirical LCAO calculations. The importance of the coupling between Silicon p and Platinum d-states in determining the basic features of the chemical bond is discussed. 相似文献
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The model of an edge misfit dislocation at the interface of the hollow nanopore and the infinite substrate with surface/interface stress is investigated. Using the complex variable method, analytical solutions for complex potentials of a film due to an edge misfit dislocation located in the film with surface/interface effect are derived, and the stress fields of the film and the edge misfit dislocation formation energy can be obtained. The critical conditions for edge misfit dislocation formation are given at which the generation of an edge misfit dislocation is energetically favourable. The influence of the ratio of the shear modulus between the film and the infinite substrate, the misfit strain, the radius of the nanopore and the surface/interface stress on the critical thickness of the film is discussed. 相似文献
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The generation of structural and electrical defects in Si/SiO2 structures upon high temperature annealing by the oxide decomposition reaction Si+SiO2→2SiO ↑ has been studied using scanning electron microscopy (SEM) and ramped current-voltage measurements. The SiO decomposition is nucleated at crystalline defects in the substrate and results in the formation of voids in the oxide. The voids grow laterally with annealing time, independent of the nature of the defect. Prior to the formation of physical voids in the oxide, defects become electrically active, leading to low field dielectric breakdown. The breakdown degradation is prevented when the O2 pressure in the annealing ambient is sufficient to reverse the decomposition reaction by reoxidizing the SiO product at the interface. 相似文献
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《Solid State Ionics》2004,166(1-2):183-189
The Pt/yttria-stabilized cubic zirconia (YSZ) interface exposed to a reactive gas was characterised by solid electrolyte potentiometry and cyclic voltammetry. The catalytic reactions included total combustion of C3H8 and C3H6 to CO2 and H2O as well as NO reduction by C3H6 in the presence of O2 under oxygen-rich and stoichiometric conditions. The solid electrolyte potentiometry as a function of the temperature in C3Hx/O2 (with x=6 or 8) reflected the catalytic properties of Pt for C3Hx oxidation. In C3H6/NO/O2, the reduction of NO was evidenced below 300 °C. The cyclic voltammetry evidenced the formation of an oxygen chemisorbed layer on the Pt surface under anodic potential. Propane had no effect on this chemisorbed layer, whereas propene weakened significantly the strength of this Pt–O bond. Addition of NO to C3H6/O2 led to the disappearing of this chemisorbed layer. The use of solid electrolyte potentiometry in conjunction with cyclic voltammetry allowed us to determine the surface oxidation state of Pt during the catalytic reactions. 相似文献
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New phase formation at the La0.9Sr0.1MnO3/YSZ interface and its effects on the cathodic performances were studied at 900 °C in air. The resistance caused by the interfacial product layer kept increasing with time to reach up to 40% of the total resistance after 500 h. The interfacial product was identified as La2Zr2O7 by XRD measurement. The electrical conductivity of La2Zr2O7 (2.4 × 10−5 S cm−1 at 1000 °C), measured by AC impedance and current interruption methods, was 4 to 7 orders of magnitude smaller than those of La0.9Sr0.1MnO3 electrode or YSZ electrolyte. Either the electronic conductivity or the electrochemical O2 reduction activity of La2Zr2O7 was negligible. Combining these results, a conclusion was made that the cathodic degradation comes mainly from the growth of interfacial product layer and its contribution to the cell resistance increment is ohmic in nature. 相似文献
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《Composite Interfaces》2013,20(3-4):291-306
Intermolecular interactions determine the reinforcement of polydimethylsiloxane (PDMS) elastomers by fumed silica, and a water interlayer on the fumed silica/PDMS interface may act as a lubricant, decreasing the interaction energy and promoting the PDMS molecule motion over the filler surface. A quantum-chemical (QCh) modelling has been performed to study a microscopic aspect of water impact on the intermolecular interactions in the system. The results obtained for a series of superclusters simulating fragments of the real silica filler surface, both hydroxylated and silylated, interacting with five-member PDMS oligomer in presence of individual water molecules and of a 'water drop', of several H-bonded water molecules, are in good agreement with results from IGC adsorption experiments. 相似文献
14.
Tajana Preo?anin Ati?a Selmani Darko Mazur Nikola Kallay 《Applied Surface Science》2010,256(17):5412-15
The method for evaluation of surface potential from the electrode potential of single crystal electrodes is refined. The effect of NaCl and LiCl concentrations on the dependency of the surface potential of TiO2 on pH was examined. The point of zero potential was shifted to lower pH values in the presence of NaCl and to higher pH values in the presence of LiCl. The interpretation of the data based on the Surface Complexation Model suggested that at 0 0 1 crystal plane of rutile, sodium ions as counterions have more pronounced affinity for association with negatively charged surface groups with respect to the lithium ions. 相似文献
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Yamanaka T 《Physical review letters》2008,101(13):136101
Active sites for a thermally induced bimolecular two-step catalytic reaction (O2-->2O, O + CO-->CO2) that occurs on a Pt(113)(1 x 2) structure at around 160 K were studied by angular distribution measurements of desorbing product CO2. It was found that the intrinsic activity level of two-atom-wide (001) facets is significantly higher than that of two-atom-wide (111) facets, while the activity of (111) facets was also significant when this reaction was induced by irradiation of 193 nm photons. Possible mechanisms for the difference in activities of the two facets are discussed. 相似文献
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Two distinct humic acids, one extracted from Brazilian peat soil, HAPS, and another one obtained from commercial source, HAFL, were attachment onto silica gel modified with aminopropyltrimethoxysilane, producing two material named SiHAPS and SiHAFL, respectively. The ability of these materials in removing indigo carmine dye from aqueous solution was followed through series of adsorption isotherms adjusted to modified Langmuir equation. The maximum number of moles adsorbed gave 6.82 ± 0.12 × 10−4 and 2.15 ± 0.17 × 10−4 mol g−1 for SiHAPS and SiHAFL, respectively. Same interactions were calorimetrically followed and the thermodynamic data showed endothermic enthalpic values: 12.31 ± 0.55 and 24.69 ± 1.05 kJ mol−1 for SiHAPS and SiHAFL surfaces, respectively. Gibbs free energies for two adsorption processes of indigo carmine dye presented negative values, reflecting dye/surface interactions must be accompanied by an increased in entropy values, which are 65 ± 3 and 98 ± 5 J mol−1 K−1 for SiHAPS and SiHAFL materials, respectively. The adsorption processes for both materials were spontaneous in nature although they presented an endothermic enthalpy for the interaction, resulting in an entropically favored process. 相似文献
18.
Clive A. Croxton 《Physics letters. A》1979,74(5):325-328
Preliminary results are reported on the molecular orientation and surface potential of liquid water at 4°C. 相似文献
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FePt films were rf sputtered at room temperature and 550?C on MgO monocrystalline substrates. Room temperature films were post-annealed at 550?C. The high temperature growth induces a tetragonal distortion of the structure with the formation of L10-FePt phase. Soft iron layers, with different thickness, were e-beam deposited on these hard films. The phenomena occurring at the interface have been analysed and connected with the final magnetic behaviour of the system. It has been found that a strong exchange coupling between soft and hard layers has been established through the formation of an interfacial layer constituted by FePt small particles. 相似文献