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At least 55 records · Page 3

CO oxidation over ceria supported Au 22 nanoclusters: Shape effect of the support

Gold (Au) nanoclusters have recently emerged as ideal models for understanding Au catalysis, because the nanosized Au particles have precise atomic numbers and uniform size. Here, in this work, we studied for the first time the support shape effect on the catalysis of Au nanoclusters by using CO oxidation as a model reaction. Au 22 (L 8 ) 6 (L = 1,8-bis(diphenylphosphino) octane) nanoclusters were supported on CeO 2 rods or cubes, then pretreated at different temperatures (up to 673 K), allowing the gradual removal of the organic phosphine ligands. CO oxidation test over these differently pretreated samples shows that CeO 2 rods are much better supports than cubes for Au 22 nanoclusters in enhancing the reaction rate. In situ IR spectroscopy coupled with CO adsorption indicates that the shape of CeO 2 support can impact the nature and quantity of exposed Au sites, as well as the efficiency of organic ligand removal. Although CeO 2 rods are helpful in exposing a greater percentage of total Au sites upon ligands removal, the percentage of active Au sites (denoted by Au δ+ , 0 < δ < 1) is lower than that on CeO 2 cubes. The in situ extended X-ray absorption spectroscopy (EXAFS) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) results show that the Au nanoclusters bound more strongly to the CeO 2 rods than to the cubes where the Au nanoclusters show more sintering. Considering the typical redox mechanism for CO oxidation over supported Au nanoclusters and nanoparticles, it is concluded that the reactivity of the lattice oxygen of CeO 2 is the determining factor for CO oxidation over Au 22 /CeO 2 . Lastly, CeO 2 rods offer more reactive lattice oxygen and abundant oxygen vacancies than the cubes and thus make the rods a superior support for Au nanoclusters in catalyzing low temperature CO oxidation.

36 MATERIALS SCIENCE↗

The effects of supports on the flow behind a body

Two cases in a supersonic flow with a turbulent boundary layer are studied in order to determine the effects of supports on models with a flat base. The first concerns the effect of various obstacles situated upstream of the two dimensional base, at Mach 2. The second relates to a body of revolution passing through the throat of the jet from upstream to downstream. The interference of obstacles simulating supporting masts is examined for the base, both bare and with a sting, at Mach 1.94. Without any support, the drag of a conical-cylindrical body of revolution was measured by means of the ONERA magnetic suspension. The interference of various stings was studied at Mach 2.4 with a laminary boundary layer and with a separated turbulent boundary layer. The mechanism of the interference of a sting, progressively approached axially to the base, was determined.

Rebuffet, P.↗

Jet exhaust and support interference effects on the transonic aerodynamic characteristics of a fighter model with two widely spaced engines

Jet exhaust, nozzle installation, and model support interference effects on the longitudinal aerodynamic characteristics of a twin-engine fighter model were determined. Realistic jet exhaust nozzle configurations and a reference configuration with a simulated vertical-tail support were tested. Free-stream Mach number was varied from 0.6 to 1.2, and model angle of attack from 0 deg to 9 deg. The jet exhaust affected drag more than it affected lift and pitching moment. The largest effects occurred at a Mach number of 0.9 and for the afterburning mode of exhaust nozzle operation. The combined differences between the aerodynamic characteristics of the realistic and reference configurations (which were due to afterbody and nozzle contours, jet operation, and simulated reference support interference) were considerably different from those for the jet interference alone.

Compton, W. B., III↗

Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes

Support plays a complex role in catalysis by supported metal oxides and the exact support effect still remains elusive. One of the approaches to gain fundamental insights into the support effect is to utilize model support systems. In this study, we employed for the first time titania nanoshapes as the model supports and investigated how the variation of surface structure of the support (titania, TiO 2 ) impacts the catalysis of supported oxide (vanadia, VO x ). TiO 2 truncated rhombi, spheres and rods were synthesized via hydrothermal method and characterized with XRD and TEM. These TiO 2 nanoshapes represent different mixtures of surface facets including [1 0 1], [0 1 0] and [0 0 1] and were used to support vanadia. The structure of supported VO x species was characterized in detail with in situ Raman spectroscopy as a function of loading on the three TiO 2 nanoshapes. Oxidative dehydrogenation (ODH) of isobutane to isobutene was used as a model reaction to test how the support shape influences the activity, selectivity and activation energy of the surface VO x species. It was shown that the shape of TiO 2 support does not pose evident effect on either the structure of surface VO x species or the catalytic performance of surface VO x species in isobutane ODH reaction. Finally, this insignificant support shape effect was ascribed to the small difference in the surface oxygen vacancy formation energy among the different TiO 2 surfaces and the multi-faceting nature of the TiO 2 nanoshapes.

36 MATERIALS SCIENCE↗

Support System Effects on the DLR-F6 Transport Configuration in the National Transonic Facility

An experimental investigation of the DLR-F6 generic transport configuration was conducted in the NASA NTF for use in the Drag Prediction Workshop. As data from this experimental investigation was collected, a large difference in drag values was seen between the NTF test and an ONERA test that was conducted several years ago. After much investigation, it was determined that this difference was likely due to a sting effect correction applied to the ONERA data which NTF does not use. This insight led to the present work. In this study, a computational assessment has been undertaken to investigate model support system interference effects on the DLR-F6 transport configuration. The configurations computed during this investigation were the isolated wing-body, the wing-body with the full support system (blade and sting), the wing-body with just the blade, and the wing-body with just the sting. The results from this investigation show the same trends that ONERA saw when they conducted a similar experimental investigation in the S2MA tunnel. Computational results suggest that the blade contributed an interference type of effect, the sting contributed a general blockage effect, and the full support system combined these effects.

Rivers, Melissa B.↗

Effect of Support on Iron-Based Catalyst Toward CO2-Free H2 Production From Methane Pyrolysis

The global demand for low-emission hydrogen production is increasing rapidly due to the potential for hydrogen to substitute conventional fossil fuels in energy-related applications. Among practical technologies such as steam reforming of methane (SMR), water electrolysis, and methane pyrolysis, methane pyrolysis has the most potential to produce economical- and near-zero-emission hydrogen. The reaction during methane pyrolysis produces a solid carbon by-product that can be monetized to offset production costs. However, this route is not without research challenges, and the selective formation of high-value carbon remains a critical issue. Supported nickel, iron, and cobalt, have been widely investigated for methane pyrolysis. Although iron-based catalysts are less active than Ni, iron catalysts offer less resistance to coke formation, are inexpensive, and have a longer lifetime. One area not sufficiently explored is the effect of support materials other than Al2O3 for the iron-based catalysts. Therefore, we investigated a detailed variation of support materials to study their influence on the catalytic performance. Moreover, this study offers a fair and direct comparison among all catalytic materials which were synthesized and studied under identical conditions. This direct comparison of the obtained results is important because results reported in different publications are often not comparable due to very different reaction conditions.

Gull, Nathan↗

Effect of Support on Iron-Based Catalyst Toward CO2-Free H2 Production From Methane Pyrolysis

The global demand for low-emission hydrogen production is increasing rapidly due to the potential for hydrogen to substitute conventional fossil fuels in energy related applications. Among all the current practical technologies – Steam Reforming of Methane (SMR), Water Electrolysis, and Methane Pyrolysis – methane pyrolysis has the potential to produce economical- and near-zero-emission hydrogen because the reaction produces a solid carbon by-product that can be monetized to offset production costs. However, this route is not without research challenges, and the selective formation of high-value carbon remains a critical issue. Supported nickel, iron, and cobalt, have been widely investigated for methane pyrolysis. Although iron-based catalysts are less active than Ni, iron catalysts offer less resistance to coke formation, are inexpensive, and have a longer lifetime. One area not sufficiently explored is the effect of support materials other than Al2O3 for the iron-based catalysts. Therefore, in this study we investigated a detailed variation of support material to study their influence on the catalytic performance. Moreover, this study offers a fair comparison because all catalytic materials were synthesized and studied under identical conditions, allowing a direct comparison of the obtained results; this is important because results reported in different publications in literature are often not comparable, due to very different reaction conditions.

Aireddy, Divakar Reddy↗

The effect of support functions in a computerized procedure system on interface management tasks - 235

By adapting digital and computer technology, the design of main control rooms (MCR) in nuclear power plants has been changed. When operators operate a nuclear power plant, the tasks using soft controls in advanced MCRs include primary tasks and secondary tasks. Primary tasks are to control nuclear power plant devices and secondary tasks are to find appropriate screens or devices by screen navigations and selections before performing the primary task. The secondary task including interface management tasks is newly introduced in advanced MCRs. In this paper, the tasks are analyzed based on the simulation data of APR1400 which is one of the digitalized nuclear power plants. For analyzing tasks, the unit tasks are divided into three types: navigation, manipulation, and acknowledgement. The primary task represents the manipulation of devices and the secondary task indicates the navigating screens, opening control panels, closing control panels, and confirming the acknowledging alarms. To analyze the effect of support functions of a computerized procedure system (CPS), one of the functions which is expected to have a significant effect on the secondary tasks was considered, that is 'related screen link button.' Two factors, 'ratio of screen alteration' and 'ratio of using screen link button', were used to see the effect of 'related screen link button'. From the task analysis result, it was observed that the secondary tasks which is one of the unique features in advanced MCRs have a quite much portion than that of the primary tasks. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Further Investigation of the Support System Effects and Wing Twist on the NASA Common Research Model

An experimental investigation of the NASA Common Research Model was conducted in the NASA Langley National Transonic Facility and NASA Ames 11-foot Transonic Wind Tunnel Facility for use in the Drag Prediction Workshop. As data from the experimental investigations was collected, a large difference in moment values was seen between the experiment and computational data from the 4th Drag Prediction Workshop. This difference led to a computational assessment to investigate model support system interference effects on the Common Research Model. The results from this investigation showed that the addition of the support system to the computational cases did increase the pitching moment so that it more closely matched the experimental results, but there was still a large discrepancy in pitching moment. This large discrepancy led to an investigation into the shape of the as-built model, which in turn led to a change in the computational grids and re-running of all the previous support system cases. The results of these cases are the focus of this paper.

Rivers, Melissa B.↗

Wind tunnel blockage and support interference effects on winged-body models at Mach numbers from 0.6 to 1.0

Three sting-mounted winged-body models with tunnel blockages of 0.1, 1.0, and 2.0 percent were tested in the Lewis Research Center's 8- by 6- Foot Supersonic Wind Tunnel. Fuselage pressures were obtained over a Mach number range of 0.6 to 1.0 at angles of attack from 0 deg to 4 deg. Two other types of model support were investigated, which included simulated wing-tip and fuselage support-strut mountings. The effects of tunnel porosity and sidewall geometry were also investigated. Model blockage effects were small up to M sub 0 = 0.95. At higher speeds the major blockage effect observed was a displacement of the local transonic terminal shocks on the model. The effects of the wing-tip type of model support were small up to M sub 0 = 0.95, but disturbances were observed on the fuselage at higher speeds. Changes in local tunnel porosity were effective in reducing the disturbances up to M sub 0 = 0.975, but a change in sidewall geometry was not.

Blaha, B. J.↗

Support System Effects on the NASA Common Research Model

An experimental investigation of the NASA Common Research Model was conducted in the NASA Langley National Transonic Facility and NASA Ames 11-Foot Transonic Wind Tunnel Facility for use in the Drag Prediction Workshop. As data from the experimental investigations was collected, a large difference in moment values was seen between the experimental and the computational data from the 4th Drag Prediction Workshop. This difference led to the present work. In this study, a computational assessment has been undertaken to investigate model support system interference effects on the Common Research Model. The configurations computed during this investigation were the wing/body/tail=0deg without the support system and the wing/body/tail=0deg with the support system. The results from this investigation confirm that the addition of the support system to the computational cases does shift the pitching moment in the direction of the experimental results.

Rivers, S. Melissa B.↗

Designing for Maintainability and System Availability

The final goal for a delivered system (whether a car, aircraft, avionics box or computer) should be its availability to operate and perform its intended function over its expected design life. Hence, in designing a system, we cannot think in terms of delivering the system and just walking away. The system supplier needs to provide support throughout the operating life of the product. Here, supportability requires an effective combination of reliability, maintainability, logistics and operations engineering (as well as safety engineering) to have a system that is available for its intended use throughout its designated mission lifetime. Maintainability is a key driving element in the effective support and upkeep of the system as well as providing the ability to modify and upgrade the system throughout its lifetime. This paper then, will concentrate on maintainability and its integration into the system engineering and design process. The topics to be covered include elements of maintainability, the total cost of ownership, how system availability, maintenance and logistics costs and spare parts cost effect the overall program costs. System analysis and maintainability will show how maintainability fits into the overall systems approach to project development. Maintainability processes and documents will focus on how maintainability is to be performed and what documents are typically generated for a large scale program. Maintainability analysis shows how trade-offs can be performed for various alternative components. The conclusions summarize the paper and are followed by specific problems for hands-on training.

Lalli, Vincent R.↗

High-performance of CrOx/HZSM-5 catalyst on non-oxidative dehydrogenation of C 2 H 6 to C 2 H 4 : Effect of supporting materials and associated mechanism

Ethane (C 2 H 6 ) is an important inexpensive and widely available fuel resource. High-value use of C 2 H 6 has become increasingly important. Catalytic dehydrogenation of C 2 H 6 to ethylene (C 2 H 4 ) has attracted much attention in recent years due to its high energy efficiency. The direct non-oxidative ethane dehydrogenation (EDH) to ethylene is a promising strategy to produce ethylene and hydrogen at the same time. In this research, Cr/HZSM-5 catalyst with superior stability was synthesized and exhibited an C 2 H 6 converting activity of 1.47 µmol/(g·s) with the corresponding C 2 H 6 conversion and C 2 H 4 selectivity of 37.3% and 90%, respectively. Herein, the synergistic effects of Si and Al in supporting materials were investigated by comparing Cr/HZSM-5 with SBA-15, SiO 2 and Al 2 O 3 supported ones, which contains either Al or Si with different structures. Characterization results indicated that the intimate interactions between Cr and support significantly improved the catalytic performance. The presence of Al in the support promoted the formation of more active Cr 6+ species by forming the aluminum-chromium-chromate (Cr-O-Al) structures which were more efficient to active C-H bond and form (Cr, Al)-OH groups during the reaction. Meanwhile, the formation of internal silanol group with the dissociative adsorbed H* could stabilized the active Cr phase to achieve a stable dehydrogenation activity.

03 NATURAL GAS↗

Electron injection study of photoexcitation effects on supported subnanometer Pt clusters for CO 2 photoreduction

In this paper, using density functional theory, we study the effect of injected electrons (simulating photoexcited electrons) on the energetics, structures, and binding sites available to CO 2 molecules on subnanometer Pt clusters decorated onto anatase TiO 2 (101) surfaces, shedding light on the first and key step of CO 2 photoreduction. Upon the addition of one, two, or three electrons, the O–C–O angles of adsorbed CO 2 become progressively smaller in binding sites that directly contact Pt clusters, while no significant change is found in the intra bond length of the adsorbed CO 2 and in the bonding distances between the adsorbed CO 2 and supported clusters. The extra electrons lead to the stabilization of adsorption sites identified on neutral slabs, including previously metastable configurations, suggesting the enhancement of accessible CO 2 binding sites. Furthermore, supported clusters are able to populate the electronic states of adsorbed CO 2 species, facilitating the formation of the CO 2 - anion. To help interpret experimentally observed frequencies, conversion factors are proposed to gain insight into the charge state and O–C–O angle of the adsorbed CO 2 . Interestingly, upon electron addition, cluster reconstruction may exist due to the bonding inclination between CO 2 and atoms in the Pt cluster, further stabilizing the intermediate complexes. In conclusion, the rate-limiting step (C–O bond cleavage) in the CO 2 dissociation to CO is slightly reduced by the introduction of an extra electron. Our results show that subnanometer metal cluster based photocatalysts are good candidates for CO 2 photoreduction.

74 ATOMIC AND MOLECULAR PHYSICS↗

Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

The optimization of supported metal catalysts predominantly focuses on engineering the metal site, for which physical insights based on extensive theoretical and experimental contributions have enabled the rational design of active sites. Although it is well known that supports can influence the catalytic properties of metals, insights into how metal–support interactions can be exploited to optimize metal active-site properties are lacking. Here in this paper, we utilize in situ spectroscopy and microscopy to identify and characterize a support effect in oxide-supported heterogeneous Rh catalysts. This effect is characterized by strongly bound adsorbates (HCO x ) on reducible oxide supports (TiO 2 and Nb 2 O 5 ) that induce oxygen-vacancy formation in the support and cause HCO x -functionalized encapsulation of Rh nanoparticles by the support. The encapsulation layer is permeable to reactants, stable under the reaction conditions and strongly influences the catalytic properties of Rh, which enables rational and dynamic tuning of CO 2 -reduction selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗