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Variable angle spectroscopic ellipsometry of very thin T2O5 layers on Si and the previously published appropriate algorithm for data interpretation have been successfully applied in terms of accurate characterization of very thin T2O5/Si systems. The simulation procedure following a simple three and four layered model was used assuming an existence of inhomogeneous interfacial layers. Quantitative determination of the thicknesses and composition identification were achieved, both for the top T2O5 layer and for an interfacial layer. The constituents in the interfacial layer and its depth profiles were recognized. 相似文献
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ABSTRACTHydrazones are popular building blocks in the development of functional materials because of their simple structure, straightforward synthesis, hydrolytic stability and tunable properties. Although a significant body of experimental information has been accumulated on the hydrazone-based rotary switches, mechanistic studies are still scarce. The effect of different stator units (phenyl-, naphthyl- and quinolinyl) on the on/off state distribution is studied in details at various computational levels in order to select a reliable computational level for a further computational study of the switching mechanism and rotary action of these systems. 相似文献
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Interactions between the seven-coordinate tweezerlike [Fe(dapsox)(H2O)2]ClO4 complex (H2dapsox = 2,6-diacetylpyridine-bis(semioxamazide)) with different lithium salts (LiOTf, LiClO4, LiBF4, and LiPF6) in CH3CN have been investigated by electrochemical, spectrophotometric, 7Li and 19F NMR, kinetic, and DFT methods. It has been demonstrated that this complex acts as ditopic receptor, showing spectral and electrochemical ion-pair-sensing capability for different lithium salts. In general, the apparent binding constants for lithium salts increase in the order LiOTf < LiClO4 < LiBF4. From the electrochemical measurements, the apparent lithium salt binding constants for the Fe(III) and Fe(II) forms of the complex have been obtained, suggesting a stronger host-guest interaction with the reduced form of the complex. In the presence of LiPF6, the solution chemistry is more complex because of the hydrolysis of PF6-. The kinetics of the complexation of [Fe(dapsox)(CH3CN)2]+ by thiocyanate at -15 degrees C in acetonitrile in the presence of 0.2 M NBu4OTf shows two steps with the following rate constants and activation parameters: k(1) = 411 +/- 14 M(-1) s(-1); DeltaH(1) not equal = 9 +/- 2 kJ mol(-1); DeltaS1 not equal = -159 +/- 6 J K(-1) mol(-1); k(2) = 52 +/- 1 M(-1) s(-1); DeltaH(2) not equal = 4 +/- 1 kJ mol(-1); DeltaS(2) not equal = -195 +/- 3 J K(-1) mol(-1). The very negative DeltaS not equal values are consistent with an associative (A) mechanism. Under the same conditions but with 0.2 M LiOTf, k1Li and k2Li are 1605 +/- 51 and 106 +/- 2 M(-1) s(-1), respectively. The increased rate constants for the {[Fe(dapsox)(CH3CN)2] x LiOTf}+ adduct are in agreement with an associative mechanism. Kinetic and spectrophotometric titration measurements show stronger interaction between the lithium salt and the anion-substituted forms, [Fe(dapsox)(CH3CN)(NCS)] and [Fe(dapsox)(NCS)2]-, of the complex. These experiments demonstrate that in nonaqueous media lithium salts cannot be simply used as supporting electrolytes, since they can affect the kinetic behavior of the studied complex. DFT calculations revealed that the negatively charged alpha-oxyazine oxygen atoms are responsible for cation binding (electrostatic interactions), whereas the two terminal amide groups bind the anion via hydrogen bonding. 相似文献
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Kroumova V Gobbato E Basso E Mucedola L Giani T Fortina G 《Rapid communications in mass spectrometry : RCM》2011,25(15):2247-2249
Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) has recently been demonstrated to be a powerful tool for the rapid identification of bacteria from growing colonies. In order to speed up the identification of bacteria, several authors have evaluated the usefulness of this MALDI-TOF MS technology for the direct and quick identification bacteria from positive blood cultures. The results obtained so far have been encouraging but have also shown some limitations, mainly related to the bacterial growth and to the presence of interference substances belonging to the blood cultures. In this paper, we present a new methodological approach that we have developed to overcome these limitations, based mainly on an enrichment of the sample into a growing medium before the extraction process, prior to mass spectrometric analysis. The proposed method shows important advantages for the identification of bacterial strains, yielding an increased identification score, which gives higher confidence in the results. 相似文献
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The Ti-doped Ta2O5 thin films (<10 nm) obtained by rf sputtering are studied with respect to their composition, dielectric and electrical properties. The incorporation of Ti is performed by two methods - a surface doping, where a thin Ti layer is deposited on the top of Ta2O5 and a bulk doping where the Ti layer is sandwiched between two layers of Ta2O5. The effect of the process parameters (the method and level of doping) on the elemental distribution in-depth of the films is investigated by the time of flight secondary ion mass spectroscopy (ToF-SIMS). The Ti and Ta2O5 are intermixed throughout the whole thickness but the layers are very inhomogeneous. Two sub-layers exist in all the samples — a near interfacial region which is a mixture of Ta-, Ti-, Si-oxides as well as TaSiO, and an upper Ti-doped Ta2O5 sub-layer. For both methods of doping, Ti tends to pile-up at the Si interface. The electrical characterisation is performed on capacitors with Al- and Ru-gate electrodes. The two types of MIS structures exhibit distinctly different electrical behavior: the Ru gate provides higher dielectric permittivity while the stacks with Al electrode are better in terms of leakage currents. The specific metal-dielectric reactions and metal-induced electrically active defects for each metal electrode/high-k dielectric stack define its particular electrical behavior. It is demonstrated that the Ti doping of Ta2O5 is a way of remarkable improvement of leakage characteristics (the current reduction with more than four orders of magnitude as compared with undoped Ta2O5) of Ru-gated capacitors which originates from Ti induced suppression of the oxygen vacancy related defects. 相似文献
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Reactive ion etching (RIE) damage effects on thin (13 nm) thermal SiO2 on Si have been studied using X-ray photoelectron spectroscopy. It is found that 5 min exposure of the oxide to N2 plasma operating in RIE-mode causes structural modifications which manifest only as a deterioration of the oxide quality but without actual nitridation of the oxide. The presence of a small (<10%) constant amount of SiO species through the oxide and a broadening of Si---SiO2 interface transition region are detected as consequences from the RIE process. 相似文献
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R. Magdolna Mihályi Hermann K. Beyer Yanka Neinska Vesselina Mayrodinova Christo Minchev 《Reaction Kinetics and Catalysis Letters》1999,68(2):355-362
In+ cations introduced by reductive solid-state ion exchange into zeolites (Y, ZSM-5, mordenite) and cationic InO+ species created by oxidation of the incorporated univalent cations were found to be detectable and distinguishable by IR
spectroscopy using pyridine as probe molecule. Relatively weak interactions of In+ lattice cations with pyridine give rise, after degassing at temperatures not higher than 370 K, to typical bands at 1446
and 1599 cm−1. After oxidation to InO+, these bands are shifted to 1452 and 1610 cm−1, being significantly more resistant towards degassing. Because of restrictions in the accessibility of InO+ to pyridine, the respective bands are absent in the spectra of mordenite. 相似文献
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Valtchev V Balanzat E Mavrodinova V Diaz I El Fallah J Goupil JM 《Journal of the American Chemical Society》2011,133(46):18950-18956
The present study demonstrated the possibility to form a secondary system of parallel macropores in zeolite crystals. The secondary pore formation was predetermined by the creation of defect zones in ZSM-5 crystals. A high energy (238)U ion beam was employed to form latent tracks in zeolite crystals, which were further subjected to attack with diluted HF solution and thus developed to uniformally sized macropores. The selective extraction of material from latent tracks was due to the higher etching velocity of highly agitated zones created by heavy ion bombardment. The combination of complementary methods unambiguously demonstrated the formation of hierarchical zeolite material comprising parallel macropores that extended through the entire crystal. The catalytic tests revealed improved activity at retained selectivity in the reaction of m-xylene conversion. The possibility to control the number of macropores per unit of crystal surface and thus the catalytic performance of the material was demonstrated. This model material is expected to bring better understanding to the effect of a secondary pore system in the catalytic performance of hierarchical zeolites obtained by the top-down or bottom-up approach. 相似文献
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Vesselina Mavrodinova Margarita Popova Magdolna R. Mihályi Gabriella Pál-Borbély Christo Minchev 《Reaction Kinetics and Catalysis Letters》2004,83(2):345-352
The catalytic performance of MCM-22 modified with Cs to different extents by Solid-State Ion Exchange has been investigated
in toluene disproportionation. It was suggested that protons on the external surface were preferentially replaced by Cs cations.
It was observed that the Cs modifications did not provide improved p-xylene selectivity at conversions close to that of the H-form. The remaining unaffected proton sites in the 10 MR channels
are considered as responsible for secondary xylene isomerization proceeding upon toluene disproportionation.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献