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1.
The materials typically used for oxygen transport membranes, Ba0.5Sr0.5Co0.8Fe0.2O3?δ (BSCF) and La0.6Sr0.4Co0.2Fe0.8O3 (LSCF) tend to decompose due to their low thermochemical stability under reducing atmosphere. Fe- and Co-doped SrTiO3 (SrTi1-x-yCoxFeyO3-δ, x + y ≤ 0.35) (STCF) materials showing an oxygen transport comparable to LSCF have great potential for application in ion-transport-devices. In this study, the thermochemical stability of pure perovskite-structured STCF was investigated after annealing in a syngas atmosphere at 600–900 °C. The phase composition of the materials after annealing was characterized by means of X-ray diffraction (XRD). The thermodynamic activities of SrO, FeO, and CoO in the STCF materials were evaluated using Knudsen effusion mass spectrometry (KEMS). Co-doped SrTiO3 (STC) materials were not stable after annealing in the syngas atmosphere above 5 mol% Co-substitution. Ruddlesden-Popper-like phases and SrCO3 were detected after annealing at 600 °C. In contrast, Fe substitution (STF) showed good stability after annealing in syngas upto 35 mol% substitution.  相似文献   
2.
This review summarizes recent advances in the field of gold-catalyzed synthesis of pharmaceutically relevant aza-heterocycles via in situ generated α-imino gold carbene complexes as intermediates.  相似文献   
3.
Mouse double minute 2 (MDM2) is a main and direct inhibitor of the crucial tumor suppressor p53. Reports from initial clinical trials showed that blocking this interaction with a small-molecule inhibitor can have great value in the treatment of cancer for patients with p53 wild-type tumors; however, it also revealed dose-limiting hematological toxicities and drug-induced resistance as main issues. To overcome the former, an inhibitor with superior potency and pharmacokinetic properties to ultimately achieve full efficacy with less-frequent dosing schedules is required. Toward this aim, we optimized our recently reported spiro-oxindole inhibitors by focusing on the crucial interaction with the amino acid side chain of His96MDM2. The designed molecules required the targeted synthesis of structurally complex spiro[indole-3,2′-pyrrolo[2,3-c]pyrrole]-2,4′-diones for which we developed an unprecedented intramolecular azomethine ylide cycloaddition and investigated the results by computational methods. One of the new compounds showed superior cellular potency over previously reported BI-0252. This finding is a significant step toward an inhibitor suitable to potentially mitigate hematological on-target adverse effects.  相似文献   
4.
5.
The fundamental nature of charge transport in highly ordered organic semiconductors is under constant debate. At cryogenic temperatures, effects within the semiconductor such as traps or the interaction of charge carriers with the insulating substrate (dipolar disorder or Fröhlich polarons) are known to limit carrier motion. In comparison, at elevated temperatures, where charge carrier mobility often also decreases as function of temperature, phonon scattering or dynamic disorder are frequently discussed mechanisms, but the exact microscopic cause that limits carrier motion is debated. Here, the mobility in the temperature range between 200 and 420 K as function of carrier density is explored in highly ordered perylene‐diimide from 3 to 9 nm thin films. It is observed that above room temperature increasing the gate electric field or decreasing the semiconducting film thickness leads to a suppression of the charge carrier mobility. Via X‐ray diffraction measurements at various temperatures and electric fields, changes of the thin film structure are excluded as cause for the observed mobility decrease. The experimental findings point toward scattering sites or traps at the semiconductor–dielectric interface, or in the dielectric as limiting factor for carrier mobility, whose role is usually neglected at elevated temperatures.  相似文献   
6.
7.
We present the evolution and current state of the Mr. Racer car racing controller that excelled at the corresponding TORCS competitions of the last years. Although several heuristics and black-box optimization methods are employed, the basic idea of the controller architecture has been to take over many of the mechanisms human racing drivers apply. They learn the track geometry, plan ahead, and wherever necessary, adapt their plans to the current circumstances quickly. Mr. Racer consists of several modules that have partly been adapted and optimized separately, where the final tuning is usually done with respect to a certain racing track during the warmup phase of the TORCS competitions. We also undertake an experimental evaluation that investigates how the controller profits from adding some of the modules to a basic configuration and which modules are most important for reaching the best possible performance.  相似文献   
8.
Experimental results for methane and carbon dioxide diffusion in coal, as reported in the literature, often lead to diffusion rates of CO2 appearing to be much greater than that of CH4. The interpretation sometimes offered that the diffusion coefficient for CO2 is 1–2 orders of magnitude higher than that of CH4, violates fundamental principles. Nevertheless, the experimental observations require explanation. In this article, we: (a) Develop simplified models for the fast estimation of transport coefficients. These are compared with comprehensive grand canonical Monte Carlo (GCMC) and molecular dynamic (MD) simulations, collectively defined as molecular simulations (MS), which provide theoretical adsorption isotherms and various transport coefficients based on multicenter potential energy equations. The simplified models are shown to have acceptable accuracies. (b) Use the simplified models to compare diffusivities of CO2 and CH4 in carbon nanopores. For all cases examined, the diffusivity of CH4 is always larger than that of CO2. (c) Offer two explanations for the apparently contradictory experimental observations (that CO2 sometimes appears to diffuse much faster than the CH4 molecule, even though CH4 is lighter and has smaller adsorption affinity): (i) CH4 mobility could be significantly reduced by directional forces resulting from irregular pore geometries; and (ii) if pores contain throats with sizes close to the CH4 molecular diameter, the energy barrier that the methane molecules must overcome to proceed through is much larger than that required for CO2. (d) Demonstrate that both mobility and connectivity issues can be addressed using kinetic theory in association with percolation analysis. Furthermore, this method of understanding pore networks provides a number of important quantitative measures including percolation threshold, size of largest cluster, shortest path and tortuosity. Separating different transport mechanisms, as we propose here, provides improved insights into the complex transport phenomena that occur in carbonaceous porous media. In many cases, diffusivities reported in the literature with mixed mechanisms are better named “apparent transport coefficients,” because they lump in other unrelated phenomena, violating the fundamental basis of, or mathematical assumptions imposed on, the definition of diffusion. © 2011 American Institute of Chemical Engineers AIChE J, 2012  相似文献   
9.
A novel nanoporous carbon/electrolyte hybrid material is reported for use in actuation. The nanoporous carbon matrix provides a 3D network that combines mechanical strength, light weight, and low cost with an extremely high surface area. In contrast to lower dimensional nanomaterials, the nanoporous carbon matrix can be prepared in the form of macroscopic monolithic samples that can be loaded in compression. The hybrid material is formed by infiltrating the free internal pore volume of the carbon with an electrolyte. Actuation is prompted by polarizing the internal interfaces via an applied electric bias. It is found that the strain amplitude is proportional to the Brunauer‐Emmett‐Teller (BET) mass specific surface area, with reversible volume strain amplitudes up to the exceptionally high value of 6.6%. The mass‐specific strain energy density compares favorably to reported values for piezoceramics and for nanoporous metal actuators.  相似文献   
10.
The creep behavior of La0.58Sr0.4Co0.2Fe0.8O3?δ (LSCF) perovskite was studied in the temperature range 750–950 °C in air and vacuum (PO2  4 mbar). A transition in the apparent activation energy was found between 800 and 850 °C for both oxygen partial pressures. The apparent activation energy is ~250 kJ mol?1 for the temperature range 700–800 °C under vacuum (PO2  4 mbar) and ~480 kJ mol?1 for 850–950 °C in both atmospheres. Above 850 °C, the creep rate of LSCF is higher in vacuum than in air although the same cubic structure exists. The stress exponent of the creep law is in the range 1.9–2.5 for all temperatures, which excludes a transition of creep mechanism. It is suggested that, below 800 °C, cation vacancies originate from the necessary balance with the substituted cations in LSCF, and the determined activation energy reflects the energy barrier for cation migration via these vacancies. Above 850 °C, additional vacancies appear to be formed intrinsically, and the activation energy represents the sum of the thermally activated formation energy of cation vacancies and migration energy of cations.  相似文献   
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