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41.
Nicholas C. Nelson Linxiao Chen Debora Meira Libor Kovarik Jnos Szanyi 《Angewandte Chemie (International ed. in English)》2020,59(40):17657-17663
The application of single‐atom catalysts (SACs) to high‐temperature hydrogenation requires materials that thermodynamically favor metal atom isolation over cluster formation. We demonstrate that Pd can be predominantly dispersed as isolated atoms onto TiO2 during the reverse water–gas shift (rWGS) reaction at 400 °C. Achieving atomic dispersion requires an artificial increase of the absolute TiO2 surface area by an order of magnitude and can be accomplished by physically mixing a precatalyst (Pd/TiO2) with neat TiO2 prior to the rWGS reaction. The in situ dispersion of Pd was reflected through a continuous increase of rWGS activity over 92 h and supported by kinetic analysis, infrared and X‐ray absorption spectroscopies and scanning transmission electron microscopy. The thermodynamic stability of Pd under high‐temperature rWGS conditions is associated with Pd‐Ti coordination, which manifests upon O‐vacancy formation, and the artificial increase in TiO2 surface area. 相似文献
42.
A new procedure, based on combustion to sulphate and ion chromatography for the analysis of elemental sulphur in sediments 总被引:1,自引:0,他引:1
Summary A procedure exploiting the bomb preparation method for the analysis of total sulphur in organic materials has been developed
for the determination of zero-valent sulphur (So) in sediments. Sediment samples were dried over magnesium oxide and sonicated in the presence of toluene to extract So. Toluene solutions were directly oxidized by combustion in a bomb containing sodium carbonate-bicarbonate buffer, which trapped
sulphur species generated from So as sulphate ions. These were in turn analysed by suppressed anion chromatography with ion-conductivity detection. The method
was used to determine the distribution of So in saltmarsh sediment cores. 相似文献
43.
Piotr Dobrzynski Daniele Fabbri Cristian Torri Janusz Kasperczyk Bozena Kaczmarczyk Malgorzata Pastusiak 《Journal of polymer science. Part A, Polymer chemistry》2009,47(1):247-257
A hydroxylactone ((1R,5S)‐1‐hydroxy‐3,6‐dioxabicyclo [3.2.1] octan‐2‐one, abbreviated as LAC) obtained from catalytic pyrolysis of cellulose was investigated as a monomer in the synthesis of polyesters by ring‐opening polymerization (ROP) with L ‐lactide. Although stannous octoate resulted inactive, ROP initiated by zirconium (IV) acetylacetonate afforded novel copolyesters from LAC and lactide mixtures in the bulk at 110 °C. Copolymers were obtained with different LAC content (from 19 to 45%) with a random microstructure as established by detailed NMR analysis. FTIR spectrometry confirmed the presence in the polymer chain of the OH groups originally present in LAC, which do not react during polymerization due to steric hindrance and inter/intramolecular hydrogen bonding. Reaction with trichloroacetylisocyanide proved that OH groups of the polyesters can be readily derivatized. The application of LAC as a comonomer enables the insertion of the alcohol functionality in polylactide avoiding protection/deprotection steps and potentially expanding the realm of biomaterials affordable from carbohydrate feedstock. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 247–257, 2009 相似文献
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Juliana S Luz Celso RR Ramos Márcia CT Santos Patricia P Coltri Fernando L Palhano Debora Foguel Nilson IT Zanchin Carla C Oliveira 《BMC biochemistry》2010,11(1):22
Background
The archaeal exosome is formed by a hexameric RNase PH ring and three RNA binding subunits and has been shown to bind and degrade RNA in vitro. Despite extensive studies on the eukaryotic exosome and on the proteins interacting with this complex, little information is yet available on the identification and function of archaeal exosome regulatory factors. 相似文献46.
Emiliana Fabbri Isaac Markus Lei BiDaniele Pergolesi Enrico Traversa 《Solid State Ionics》2011,202(1):30-35
BaZr0.8 − xPrxY0.2O3 − δ (BZPYx, 0.1 ≤ x ≤ 0.4) perovskite oxides were investigated for application as cathode materials for intermediate temperature solid oxide fuel cells based on proton conducting electrolytes (protonic-SOFCs). The BZPYx reactivity with CO2 and water vapor was evaluated by thermogravimetric and X-ray diffraction analyses, and good chemical stability was observed for each BZPYx composition. Conductivity measurements of BZPYx sintered pellets were performed as a function of temperature and pO2 in humidified atmospheres, corresponding to cathode operating condition in protonic-SOFCs. Different conductivity values and activation energies were measured depending on the Pr content, suggesting the presence of different charge carriers. For all the compositions, the partial electronic conductivity, calculated from conductivity measurements at different pO2, increased with increasing the temperature from 500 to 700 °C. Furthermore, the larger the Pr content, the larger the electronic conductivity. BaZr0.7Pr0.1Y0.2O3 − δ and BaZr0.4Pr0.4Y0.2O3 − δ showed mostly pure proton and electron conductivity, respectively, whereas the intermediate compositions showed mixed proton/electronic conductivity. Among the two mixed proton/electronic conductors, BaZr0.6Pr0.3Y0.2O3 − δ presented the larger conductivity, which coupled with its good chemical stability, makes this perovskite oxide a candidate cathode materials for protonic-SOFCs. 相似文献
47.
Human movement, as for example human gait, can be considered as an optimal realization of some given task. However, the criterion for which the naturally performed human motion is optimal, is generally not known. In this article we formulate an inverse optimal control problem to study the relevance of four different optimization criteria in human locomotion. As a walking model we use an actuated three dimensional spring loaded inverted pendulum (3D-SLIP), which is able to mirror the typical shape of the center of mass trajectory in human gait. Using a direct all-at-once approach, the weighting of the optimization criteria and the position of the footsteps are optimized in such a way, that the center of mass trajectory of the resulting optimal state fits real motion capture data as good as possible. Numerical experiments show, that whereas the so called capture point seems to have a great impact on human walking, minimization of the vertical center of mass movement does not show any relevance at all. (© 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
48.
Starting from the spectral analysis of g-circulant matrices, we study the convergence of a multigrid method for circulant and Toeplitz matrices with various size reductions. We assume that the size n of the coefficient matrix is divisible by g≥2 such that at the lower level the system is reduced to one of size n/g, by employing g-circulant based projectors. We perform a rigorous two-grid convergence analysis in the circulant case and we extend experimentally the results to the Toeplitz setting, by employing structure preserving projectors. The optimality of the two-grid method and of the multigrid method is proved, when the number θ∈ℕ of recursive calls is such that 1<θ<g. The previous analysis is used also to overcome some pathological cases, in which the generating function has zeros located at “mirror points” and the standard two-grid method with g=2 is not optimal. The numerical experiments show the correctness and applicability of the proposed ideas, both for circulant and Toeplitz matrices. 相似文献
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We have developed a fully adaptive optimization environment suitable to solve complex optimal control problems restricted by partial differential algebraic equations (PDAEs) and pointwise constraints on the control [1, 2]. This contribution is devoted to the inclusion of pointwise constraints on the state within the optimization environment. To this end we first give a brief introduction into the architecture of the environment and the inclusion of pointwise constraints on the state by Moreau-Yosida regularization. Then, we test the new tool by applying it to an optimal boundary control problem for the cooling of hot glass down to room temperature, modeled by radiative heat transfer and semi-transparent boundary conditions. (© 2012 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献