944 resultados para HETEROGENEOUS CATALYSIS
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Peer reviewed
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Peer reviewed
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Gold nanoparticles (Au NPs) with diameters ranging between 5-60 nm have been synthesised in water, and further stabilized with polyethylene glycol-based thiol polymers (mPEG-SH). Successful PEGylation of the Au NPs was confirmed by Dynamic Light scattering (DLS) and Zeta potential measurements. PEG coating of the Au NPs is the key of their colloidal stabilty, and its successful applications. Catalytic efficiency testing of the PEG-AuNPs were carried out on homocoupling of boronic acid. PEG-Au NPs with AuNps diameter < 30 nm were useful as catalyst in water. Finally, the PEG-Au NPs were also shown to be stable in biological fluid and not cytotoxic on B16.F10 cell line, making them attractive for further studies.
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The development of economical heterogeneous catalysts for the activation of methane is a major challenge for the chemical industry. Screening potential candidates becomes more feasible using rational catalyst design to understand the activity of potential catalysts for CH4 activation. The focus of the present paper is the use of density functional theory to examine and elucidate the properties of doped CeO2. We dope with Cu and Zn transition metals having variable oxidation state (Cu), and a single oxidation state (Zn), and study the activation of methane. Zn is a divalent dopant and Cu can have a +1 or +2 oxidation state. Both Cu and Zn dopants have an oxidation state of +2 after incorporation into the CeO2 (111) surface; however a Hubbard +U correction (+U = 7) on the Cu 3d states is required to maintain this oxidation state when the surface interacts with adsorbed species. Dissociation of methane is found to occur locally at the dopant cations, and is thermodynamically and kinetically more favorable on Zn-doped CeO2 than Cu-doped CeO2. The origins of this lie with the Zn(II) dopant moving towards a square pyramidal geometry in the sub surface layer which facilitates the formation of two-coordinated surface oxygen atoms, that are more beneficial for methane activation on a reducible oxide surface. These findings can aid in rational experimental catalyst design for further exploration in methane activation processes.
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Global connectivity is on the verge of becoming a reality to provide high-speed, high-quality, and reliable communication channels for mobile devices at anytime, anywhere in the world. In a heterogeneous wireless environment, one of the key ingredients to provide efficient and ubiquitous computing with guaranteed quality and continuity of service is the design of intelligent handoff algorithms. Traditional single-metric handoff decision algorithms, such as Received Signal Strength (RSS), are not efficient and intelligent enough to minimize the number of unnecessary handoffs, decision delays, call-dropping and blocking probabilities. This research presents a novel approach for of a Multi Attribute Decision Making (MADM) model based on an integrated fuzzy approach for target network selection.
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The advances in low power micro-processors, wireless networks and embedded systems have raised the need to utilize the significant resources of mobile devices. These devices for example, smart phones, tablets, laptops, wearables, and sensors are gaining enormous processing power, storage capacity and wireless bandwidth. In addition, the advancement in wireless mobile technology has created a new communication paradigm via which a wireless network can be created without any priori infrastructure called mobile ad hoc network (MANET). While progress is being made towards improving the efficiencies of mobile devices and reliability of wireless mobile networks, the mobile technology is continuously facing the challenges of un-predictable disconnections, dynamic mobility and the heterogeneity of routing protocols. Hence, the traditional wired, wireless routing protocols are not suitable for MANET due to its unique dynamic ad hoc nature. Due to the reason, the research community has developed and is busy developing protocols for routing in MANET to cope with the challenges of MANET. However, there are no single generic ad hoc routing protocols available so far, which can address all the basic challenges of MANET as mentioned before. Thus this diverse range of ever growing routing protocols has created barriers for mobile nodes of different MANET taxonomies to intercommunicate and hence wasting a huge amount of valuable resources. To provide interaction between heterogeneous MANETs, the routing protocols require conversion of packets, meta-model and their behavioural capabilities. Here, the fundamental challenge is to understand the packet level message format, meta-model and behaviour of different routing protocols, which are significantly different for different MANET Taxonomies. To overcome the above mentioned issues, this thesis proposes an Interoperable Framework for heterogeneous MANETs called IF-MANET. The framework hides the complexities of heterogeneous routing protocols and provides a homogeneous layer for seamless communication between these routing protocols. The framework creates a unique Ontology for MANET routing protocols and a Message Translator to semantically compare the packets and generates the missing fields using the rules defined in the Ontology. Hence, the translation between an existing as well as newly arriving routing protocols will be achieved dynamically and on-the-fly. To discover a route for the delivery of packets across heterogeneous MANET taxonomies, the IF-MANET creates a special Gateway node to provide cluster based inter-domain routing. The IF-MANET framework can be used to develop different middleware applications. For example: Mobile grid computing that could potentially utilise huge amounts of aggregated data collected from heterogeneous mobile devices. Disaster & crises management applications can be created to provide on-the-fly infrastructure-less emergency communication across organisations by utilising different MANET taxonomies.
Wireless Rotating Disk Electrode (wRDE) for assessing Heterogeneous Water Oxidation Catalysts (WOCs)
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A novel method for assessing the activity of a powdered water oxidation catalyst (WOC) is described, utilising an easily-prepared wireless rotating disc electrode of the WOC, thereby allowing its activity to be probed, via the observed kinetics of water oxidation by Ce(IV) ions, and so provide invaluable electrochemical information.
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FPGAs and GPUs are often used when real-time performance in video processing is required. An accelerated processor is chosen based on task-specific priorities (power consumption, processing time and detection accuracy), and this decision is normally made once at design time. All three characteristics are important, particularly in battery-powered systems. Here we propose a method for moving selection of processing platform from a single design-time choice to a continuous run time one.We implement Histogram of Oriented Gradients (HOG) detectors for cars and people and Mixture of Gaussians (MoG) motion detectors running across FPGA, GPU and CPU in a heterogeneous system. We use this to detect illegally parked vehicles in urban scenes. Power, time and accuracy information for each detector is characterised. An anomaly measure is assigned to each detected object based on its trajectory and location, when compared to learned contextual movement patterns. This drives processor and implementation selection, so that scenes with high behavioural anomalies are processed with faster but more power hungry implementations, but routine or static time periods are processed with power-optimised, less accurate, slower versions. Real-time performance is evaluated on video datasets including i-LIDS. Compared to power-optimised static selection, automatic dynamic implementation mapping is 10% more accurate but draws 12W extra power in our testbed desktop system.
Evaporative Moisture Loss from Heterogeneous Stone: Material- Environment Interactions During Drying
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The complexities of evaporation from structurally and mineralogically heterogeneous sandstone (Locharbriggs Sandstone) are investigated through a laboratory-based experiment in which a variety of environmental conditions are simulated. Data reported demonstrate the significance of material-environment interactions on the spatial and temporal variability of evaporative dynamics. Evaporation from porous stone is determined by the interplay between environmental, material and solution properties, which govern the rate and mode by which water is transmitted to, and subsequently removed from, an evaporating surface. Initially evaporation is marked by high rates of moisture loss controlled by external atmospheric conditions; then, when a critical level of surface moisture content is reached, hydraulic continuity between the stone surface and subsurface is disrupted and the drying front recedes
beneath the surface, evaporation rates decrease and are controlled by the ability of the material to transport water vapour to the surface. Pore size distribution and connectivity, as well as other material properties, control the timing of each stage of evaporation and the nature of the transition.
These experimental data highlight the complexity of evaporation, demonstrating that different regions of the same stone can exhibit varying moisture dynamics during drying and that the rate and nature of evaporative loss differs under different environmental conditions. The results identify the importance of material-environment interactions during drying and that stone micro-environmental conditions cannot be inferred from ambient data alone.
These data have significance for understanding the spatial distribution of stone surface weathering-related morphologies in both the natural and built environments where mineralogical and/or structural heterogeneity creates differences in moisture flux and hence variable drying rates. Such differences may provide a clearer explanation for the initiation and subsequent development of complex weathering responses where areas of significant deterioration can be found alongside areas that exhibit little or no evidence surface breakdown.
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The major part of this thesis concerns the development of catalytic methodologies based on palladium nanoparticles immobilized on aminopropyl-functionalized siliceous mesocellular foam (Pd0-AmP-MCF). The catalytic activity of the precursor to the nanocatalyst, PdII-AmP-MCF is also covered by this work. In the first part the application of Pd0-AmP-MCF in Suzuki-Miyaura cross-coupling reactions and transfer hydrogenation of alkenes under microwave irradiation is described. Excellent reactivity was observed and a broad range of substrates were tolerated for both transformations. The Pd0-AmP-MCF exhibited high recyclability as well as low metal leaching in both cases. The aim of the second part was to evaluate the catalytic efficiency of the closely related PdII-AmP-MCF for cycloisomerization of various acetylenic acids. The catalyst was able to promote formation of lactones under mild conditions using catalyst loadings of 0.3 - 0.5 mol% at temperatures of up to 50 oC in the presence of Et3N. By adding 1,4-benzoquinone to the reaction, the catalyst could be recycled four times without any observable decrease in the activity. The selective arylation of indoles at the C-2 position using Pd-AmP-MCF and symmetric diaryliodonium salts is presented in the third part. These studies revealed that Pd0-AmP-MCF was more effective than PdII-AmP-MCF for this transformation. Variously substituted indoles as well as diaryliodonium salts were tolerated, giving arylated indoles in high yields within 15 h at 20 - 50 oC in H2O. Only very small amounts of Pd leaching were observed and in this case the catalyst exhibited moderate recyclability. The final part of the thesis describes the selective hydrogenation of the C=C in different α,β-unsaturated systems. The double bond was efficiently hydrogenated in high yields both under batch and continuous-flow conditions. High recyclability and low metal leaching were observed in both cases.
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SOUZA, Rodrigo B. ; MEDEIROS, Adelardo A. D. ; NASCIMENTO, João Maria A. ; GOMES, Heitor P. ; MAITELLI, André L. A Proposal to the Supervision of Processes in an Industrial Environment with Heterogeneous Systems. In: INTERNATIONAL CONFERENCE OF THE IEEEOF THE INDUSTRUI ELECTRONICS SOCIETY,32., Paris, 2006, Paris. Anais... Paris: IECON, 2006
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Heterogeneity has to be taken into account when integrating a set of existing information sources into a distributed information system that are nowadays often based on Service- Oriented Architectures (SOA). This is also particularly applicable to distributed services such as event monitoring, which are useful in the context of Event Driven Architectures (EDA) and Complex Event Processing (CEP). Web services deal with this heterogeneity at a technical level, also providing little support for event processing. Our central thesis is that such a fully generic solution cannot provide complete support for event monitoring; instead, source specific semantics such as certain event types or support for certain event monitoring techniques have to be taken into account. Our core result is the design of a configurable event monitoring (Web) service that allows us to trade genericity for the exploitation of source specific characteristics. It thus delivers results for the areas of SOA, Web services, CEP and EDA.