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11.
12.
Tromp M van Bokhoven JA Arink AM Bitter JH van Koten G Koningsberger DC 《Chemistry (Weinheim an der Bergstrasse, Germany)》2002,8(24):5667-5678
Herein we describe a structural characterisation with EXAFS of copper(I) arenethiolate complexes in both the solid and liquid state. Previously noted difficulties in the detection of the Cu-Cu interaction have been attributed to anti-phase behaviour of different Cu-Cu neighbour contributions. A data analysis procedure solely based on EXAFS parameters is presented which resolves these problems. A careful analysis of the individual coordination shells and the use of different k-weightings during the data analysis are shown to be an absolute necessity to obtain reliable results. During R-space fitting, the difference file technique is used to separate, examine and compare the individual contributions. Using this technique their statistical significance and correctness can be determined. Anti-phase behaviour can be detected and accounted for in this way. An additional mixed organocopper aggregate [Cu4(SAr)2(Mes)2] with different Cu sites is analysed, which proves the value of the analysis procedure described above. Moreover, this newly developed EXAFS data analysis procedure is applicable to any other EXAFS spectrum obtained. The structural analysis of these organocopper complexes with EXAFS provides information about their actual structure and dynamic behaviour in solution. The technique can now be used to obtain insights into the reactivity of these complexes and the way in which they form catalytic reaction intermediates. 相似文献
13.
This paper describes the stereoselective outcome of the intramolecular Diels-Alder furan (IMDAF) reaction of substituted (2S,3S)-ethanolamides 9-13, which were synthesised from a furyl substituted cyanohydrin. The latter was obtained from 2-furaldehyde with high enantioselectivity by an oxynitrilase catalysed addition of hydrogen cyanide. The stereochemistry of the IMDAF products was shown to be dependent on the size of the ethanolamide substituents R. Small substituents (H, Me, CN) gave exclusively exo-cycloaddition, whereas more bulky ones (Ph, Et) gave both evo- and endo-addition, the larger phenyl substituent giving a high endo-exo-ratio. 相似文献
14.
Multiphase flow metering with operationally robust, low-cost real-time systems that provide accuracy across a broad range of produced volumes and fluid properties, is a requirement across a range of process industries, particularly those concerning petroleum. Especially the wide variety of multiphase flow profiles that can be encountered in the field provides challenges in terms of metering accuracy. Recently, low-field magnetic resonance (MR) measurement technology has been introduced as a feasible solution for the petroleum industry. In this work, we study two phase air-water horizontal flows using MR technology. We show that low-field MR technology applied to multiphase flow has the capability to measure the instantaneous liquid holdup and liquid flow velocity using a constant gradient low flip angle CPMG (LFA-CPMG) pulse sequence. LFA-CPMG allows representative sampling of the correlations between liquid holdup and liquid flow velocity, which allows multiphase flow profiles to be characterized. Flow measurements based on this method allow liquid flow rate determination with an accuracy that is independent of the multiphase flow profile observed in horizontal pipe flow for a wide dynamic range in terms of the average gas and liquid flow rates. 相似文献
15.
Time‐Resolved,In Situ DRIFTS/EDE/MS Studies on Alumina‐Supported Rhodium Catalysts: Effects of Ceriation and Zirconiation on Rhodium–CO Interactions
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Dr. Anna B. Kroner Dr. Mark A. Newton Prof. Dr. Moniek Tromp Dr. Otello M. Roscioni Prof. Andrea E. Russell Prof. Andrew J. Dent Dr. Carmelo Prestipino Prof. John Evans 《Chemphyschem》2014,15(14):3049-3059
The effects of ceria and zirconia on the structure–function properties of supported rhodium catalysts (1.6 and 4 wt % Rh/γ‐Al2O3) during CO exposure are described. Ceria and zirconia are introduced through two preparation methods: 1) ceria is deposited on γ‐Al2O3 from [Ce(acac)3] and rhodium metal is subsequently added, and 2) through the controlled surface modification (CSM) technique, which involves the decomposition of [M(acac)x] (M=Ce, x=3; M=Zr, x=4) on Rh/γ‐Al2O3. The structure–function correlations of ceria and/or zirconia‐doped rhodium catalysts are investigated by diffuse reflectance infrared Fourier‐transform spectroscopy/energy‐dispersive extended X‐ray absorption spectroscopy/mass spectrometry (DRIFTS/EDE/MS) under time‐resolved, in situ conditions. CeOx and ZrO2 facilitate the protection of Rh particles against extensive oxidation in air and CO. Larger Rh core particles of ceriated and zirconiated Rh catalysts prepared by CSM are observed and compared with Rh/γ‐Al2O3 samples, whereas supported Rh particles are easily disrupted by CO forming mononuclear Rh geminal dicarbonyl species. DRIFTS results indicate that, through the interaction of CO with ceriated Rh particles, a significantly larger amount of linear CO species form; this suggests the predominance of a metallic Rh phase. 相似文献
16.
We present new results obtained with medium energy ion beam crystallography on the clean Si (100)?(2 × 1) surface. This study, meant to discriminate between symmetric and asymmetric dimer models for the reconstruction, shows that symmetric dimers are not consistent with our results. We conclude that the Si (100)?(2 × 1) surface is reconstructed in asymmetric dimers, accompanied by extensive subsurface distortions. 相似文献
17.
Thayer GE Sadowski JT Meyer zu Heringdorf F Sakurai T Tromp RM 《Physical review letters》2005,95(25):256106
We show that the orientation of pentacene molecules is controlled by the electronic structure of the surface on which they are deposited. We suggest that the near-Fermi level density of states above the surface controls the interaction of the substrate with the pentacene pi orbitals. A reduction of this density as compared to noble metals, realized in semimetallic Bi(001) and Si(111)(5 x 2)Au surfaces, results in pentacene standing up. Interestingly, pentacene grown on Bi(001) is highly ordered, yielding the first vertically oriented epitaxial pentacene thin films observed to date. 相似文献
18.
Dislocation interactions play a critical role in plasticity and heteroepitaxial strain relaxation. We use real time transmission electron microscopy observations of the interaction between threading and misfit dislocations in SiGe heterostructures to investigate interactions quantitatively. In addition to the expected long-range blocking of threading segments, we observe a new short-range mechanism which is significantly more effective. Simulations show that this reactive blocking occurs when two dislocations with the same Burgers vector reconnect. 相似文献
19.
Three-dimensional islanding is generally assumed to proceed through nucleation and growth. Here we present studies showing the growth of Si1-xGex islands (0.2相似文献
20.
Subbiah Meenakshisundaram RM. Sockalingam 《Journal of molecular catalysis. A, Chemical》2000,160(2):269-275
Catalytic activity of Os(VIII) in the oxidation of some twenty organic sulfides with sodium salt of N-chlorobenzenesulfonamide (CAB) has been investigated in alkaline (pH8.7) t-butanol–water (1:1 v/v) medium. Significant retarding influence of [OH−] on the reactivity is exhibited. The catalysed reaction is strongly accelerated in the presence of Hg(II). Imperfections are observed in the linear Hammett relationship in the case of –NO2 substituents. 相似文献