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Fuel Reforming for Hydrogen Production in Heavy-Duty Vehicle ApplicationsGranlund, Moa. Z. January 2015 (has links)
The depletion of fossil fuels together with growing environmental concerns have created incitement for developing a more energy-efficient and environmentally-friendly vehicle fleet. The development towards cleaner heavy-duty vehicles started already in the 80’s with the introduction of emission legislations. Initially, engine optimization was enough for reaching the legislated levels of emissions. However, at present engine optimization is not enough but exhaust aftertreatment has become an essential part of heavy-duty vehicles, in order to meet the emission standards. Today, the total emissions are targeted which means that there is an interest in decreasing the idling emissions as well as the emissions during operation. To reduce the overall emissions several states in the USA have introduced idling legislations. Due to the limitations in idling time alternative solutions for power generation during rests are requested. A possible alternative is a fuel cell auxiliary power unit, combining a fuel cell with a fuel reformer (FC-APU). The focus of this thesis is the development of the fuel reformer for an FC-APU, in which the hydrogen to the fuel cell is generated from diesel in a high-temperature catalytic process. The produced hydrogen can also be used in other heavy-duty vehicle applications i.e. selective catalytic reduction of NOx (HC-SCR), where addition of hydrogen is essential for reaching high conversion at low temperatures. The effect of using hydrogen from a fuel reformer in HC-SCR is included in this work. The catalytic material development is focused on developing promoted materials with lower rhodium content but with catalytic activity comparable to that of materials with higher rhodium content. This includes evaluation and extensive characterization of both fresh and aged promoted materials. The work also includes reactor design where a micro reactor with multiple air inlets is evaluated. This work has contributed to increased knowledge of catalytic materials suitable for reforming of diesel. By changing the support material from the traditionally used alumina to ceria-zirconia, increased H2 yield was achieved. In addition, the ceria-zirconia supported material was less prone to coke. By promoting the material with cobalt or lanthanum it was possible to decrease the rhodium content by 2/3 with enhanced catalytic performance. It was also discovered that promotion with lanthanum decreased the tendency for coking even further. Additionally, the lanthanum-promoted material had higher thermal stability as well as a stable highly dispersed rhodium phase. Furthermore, the work has contributed to an increased knowledge concerning the fuel reformer’s effect on HC-SCR. The work displays clear evidence of benefits with using hydrogen-rich gas from a fuel reformer instead of pure hydrogen. The benefits are derived from the content of low molecular weight hydrocarbons present in the hydrogen-rich gas, which are strong reducing agents increasing the NOx reduction. This finding proves that fuel reforming in combination with HC-SCR is a viable option for NOx abatement. / <p>QC 20150202</p>
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Síntese de compostos α-amino-1,3-dicarbonílicos em microrreator de fluxo contínuo e suas aplicações / Synthesis of α-amino-1,3-dicarbonyl compounds in continuous flow micro-reactor and their applications.Pereira, Evelin Fornari 19 May 2017 (has links)
Na primeira parte deste trabalho apresentamos uma forma eficiente para sintetizar quinze novos compostos α-amino-1,3-dicarbonílicos através da reação multicomponente de Ugi. Para estas sínteses foi utilizado o microrreator de fluxo contínuo, um aparelho que possibilita uma excelente transferência de calor, de massa e alta relação superfície / volume. Algumas das vantagens em se utilizar um microrreator de fluxo contínuo na síntese são: redução do tempo de reação, aumento de rendimento, seletividade das reações e menor geração de resíduos. Foi possível assim estudar as reações químicas em condições inéditas, variando parâmetros como: temperatura, pressão, tempo de residência e relação estequiométrica. Um comparativo de rendimento da síntese de quatro moléculas foi realizado e pôde-se notar a eficiência do equipamento utilizado, pois os rendimentos obtidos foram superiores quando as mesmas moléculas foram sintetizadas através da reação one-pot. Um scale-up da reação de Ugi também foi realizado e apresentou um resultado satisfatório. Na segunda parte alguns destes compostos foram utilizados como intermediários na formação de uma ligação amídica e também aplicamos a metodologia relacionada à cicloadição catalisada por cobre entre alquinos e azidas na síntese de cinco novos compostos 1,2,3-triazóis. Este foi o primeiro trabalho realizado no Laboratório de Compostos Heterocíclicos da Faculdade de Ciências Farmacêuticas utilizando o microrreator de fluxo contínuo e este equipamento atendeu as necessidades deste trabalho com efetividade. / The first part of this work we present an efficient way to synthesize fifteen new α-amino-1,3-dicarbonyl compounds through the multicomponent Ugi reaction. For these syntheses was used the continuous flow micro-reactor, an equipment that allows an excellent transfer of heat, mass and high surface / volume ratio. Some of the advantages of using a continuous flow micro-reactor in the synthesis are: reduction of reaction time, increase of yield, selectivity of reactions and less generation of residues. It was possible to study the chemical reactions under new conditions, varying parameters such as: temperature, pressure, residence time and stoichiometric ratio. A yield comparison of the synthesis of four molecules was carried out and it was possible to note the efficiency of the equipment used, because the obtained yields were superior when the same molecules were synthesized through the one-pot reaction. A scale-up of the Ugi reaction was also performed and presented a satisfactory result. In the second part some of these compounds were used as intermediates in the formation of an amide bond and we also apply the methodology related to the copper catalyzed cycloaddition between alkynes and azides in the synthesis of five new 1,2,3-triazoles compounds. It was the first work performed in the Laboratory of Heterocyclic Compounds of the Faculty of Pharmaceutical Sciences using the continuous flow micro-reactor and this equipment met the needs of this work with effectiveness.
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Active and Passive Mixing for Immiscible Liquid-Liquid Systems: A Performance Evaluation of Novel Micro-ReactorsMongeon, Sébastien January 2018 (has links)
Continuous flow reaction using micro-reactors is a valued technology due to its excellent mass and heat transfer performance, reduced reactor volume, handling capacity of hazardous reactions, and many other process intensifications. These intensifications opportunities interest the fine chemicals, pharmaceuticals producers and other multiphase reaction users who currently use batch processes or already use continuous flow. In this thesis, elements of passive and active mixing are investigated for the application of immiscible liquid-liquid systems.
In the first study, the effects of geometrical arrangements of a residence time between mixing units on the interphase mass transfer rates are evaluated with four different immiscible liquid-liquid systems. A presentation of an algorithm for the optimal selection of a reactor and its operating conditions is given in order to enable easy and improved use of one’s micro-reactor.
In the second study, the impact of a secondary pulse flow on interphase mass transfer is investigated. A coil without internal baffles is used as the oscillatory-flow coil reactor with a continuous active mixing source. The best application for the reactor is determined using a comparison to other complementary continuous flow platforms in the toolbox approach.
The novel advancements presented here will help lead new molecular discoveries and connect the laboratory science scale to the process engineering production scale.
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Síntese de compostos α-amino-1,3-dicarbonílicos em microrreator de fluxo contínuo e suas aplicações / Synthesis of α-amino-1,3-dicarbonyl compounds in continuous flow micro-reactor and their applications.Evelin Fornari Pereira 19 May 2017 (has links)
Na primeira parte deste trabalho apresentamos uma forma eficiente para sintetizar quinze novos compostos α-amino-1,3-dicarbonílicos através da reação multicomponente de Ugi. Para estas sínteses foi utilizado o microrreator de fluxo contínuo, um aparelho que possibilita uma excelente transferência de calor, de massa e alta relação superfície / volume. Algumas das vantagens em se utilizar um microrreator de fluxo contínuo na síntese são: redução do tempo de reação, aumento de rendimento, seletividade das reações e menor geração de resíduos. Foi possível assim estudar as reações químicas em condições inéditas, variando parâmetros como: temperatura, pressão, tempo de residência e relação estequiométrica. Um comparativo de rendimento da síntese de quatro moléculas foi realizado e pôde-se notar a eficiência do equipamento utilizado, pois os rendimentos obtidos foram superiores quando as mesmas moléculas foram sintetizadas através da reação one-pot. Um scale-up da reação de Ugi também foi realizado e apresentou um resultado satisfatório. Na segunda parte alguns destes compostos foram utilizados como intermediários na formação de uma ligação amídica e também aplicamos a metodologia relacionada à cicloadição catalisada por cobre entre alquinos e azidas na síntese de cinco novos compostos 1,2,3-triazóis. Este foi o primeiro trabalho realizado no Laboratório de Compostos Heterocíclicos da Faculdade de Ciências Farmacêuticas utilizando o microrreator de fluxo contínuo e este equipamento atendeu as necessidades deste trabalho com efetividade. / The first part of this work we present an efficient way to synthesize fifteen new α-amino-1,3-dicarbonyl compounds through the multicomponent Ugi reaction. For these syntheses was used the continuous flow micro-reactor, an equipment that allows an excellent transfer of heat, mass and high surface / volume ratio. Some of the advantages of using a continuous flow micro-reactor in the synthesis are: reduction of reaction time, increase of yield, selectivity of reactions and less generation of residues. It was possible to study the chemical reactions under new conditions, varying parameters such as: temperature, pressure, residence time and stoichiometric ratio. A yield comparison of the synthesis of four molecules was carried out and it was possible to note the efficiency of the equipment used, because the obtained yields were superior when the same molecules were synthesized through the one-pot reaction. A scale-up of the Ugi reaction was also performed and presented a satisfactory result. In the second part some of these compounds were used as intermediates in the formation of an amide bond and we also apply the methodology related to the copper catalyzed cycloaddition between alkynes and azides in the synthesis of five new 1,2,3-triazoles compounds. It was the first work performed in the Laboratory of Heterocyclic Compounds of the Faculty of Pharmaceutical Sciences using the continuous flow micro-reactor and this equipment met the needs of this work with effectiveness.
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Study on the Transport Phenomena in Complex Micro-ReactorsMielke, Eric January 2017 (has links)
Continuous processing in the pharmaceutical and fine chemical industries, particularly in micro/milli-scale reactors, has been a topic of interest in literature in recent years due to the advantages offered over batch reactions. One such advantage is the enhanced transport properties of operating at smaller scales, although the quantification of the transport phenomena is not straightforward when wall and entrance effects cannot be neglected.
In the first study presented, various micro-mixer geometries and scales were considered to increase the mixing efficiency in liquid-liquid systems of diverse interfacial tensions for fast reactions. The conditions were varied over different flow regimes; including slug flow, parallel flow, and drop flow. A mass-transfer-limited test reaction was used to evaluate the overall volumetric mass transfer coefficients (Korga) as a function of the average rate of energy dissipation (ε) for each mixer design. The onset of drop flow occurred at a lower ε for the LL-Triangle mixer when compared with the Sickle or LL-Rhombus mixers for low interfacial-tension systems (i.e., n-butanol-water). In the drop flow regime for energy dissipation rates of around 20 to 500 W/kg, Korga values ranged from approximatively 0.14 to 0.35 s-1 and 0.004 to 0.015 s-1 for the relatively low and high interfacial-tension (i.e., toluene-water) systems, respectively.
The second investigation explored the heat transfer properties of a FlowPlate® system by Ehrfeld Mikrotechnik BTS. First, in a non-reactive system with rectangular serpentine channels (d_h<1mm, 400<Re<2000), a Gnielinski-type model was fit to the internal Nusselt number. Using a silver-based thermal paste between the reactor and heat transfer fluid plates proved to reduce the external resistance to heat transfer by ~70%, yielding overall heat transfer coefficients of ~2200 [W/(m^2 K)]. Secondly, a Grignard reaction was highlighted as a test reaction to compare different reactors’ localized heat transfer characteristics (i.e., hotspot formation) with various micro-mixer geometries, materials, injection ports, and channel scales. Lastly, a case study of four reactions utilized the fourth Damköhler number to determine a maximum channel diameter that would remove sufficient heat to avoid hotspot formation.
Each of these studies provides insight to aid in the proper selection of a reactor for a given set of physical properties and reaction kinetics/enthalpies.
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The Application Of Polymer Particles In Industrial ProcessesSteele, John E. January 2019 (has links)
The research in this thesis considers novel innovative developments in established
industrial processes that involve the use of recyclable polymeric particles as a
partial replacement for aqueous media and chemicals. The application of the
technology typically leads to water savings of over 80% and chemical savings of
over 25%. These industrial processes may be characterised in that are considered
inefficient and wasteful but nevertheless are considered economically vital. These
diverse industries including laundry cleaning, leather manufacturing, textile
garment processing, effluent treatment and metal beverage can manufacture.
The outcomes of this research have made significant contributions to industrial
best practice in such industries. In terms of academic research, the knowledge
created in this thesis provides the basis for the application of CFD-DEM modelling
to understand complex multi-phase and multi-component systems. In particular,
the thesis advocates the application of the Free Surface Lattice Boltzmann Method
for creating highly accurate simulations of multi-phase flow. In addition, the thesis
offers opportunities for further research in novel plasma micro-reactors and their
applications in diverse fields such as chemical synthesis, chemical engineering and
biotechnology. The nature of the research is multi-disciplinary, and involved
investigations across several fields including applied mathematics, biochemistry,
chemistry, physics, and engineering. The projects also involved scale up from
laboratory, pilot plant and full commercial scale production trials. Primary
objectives were investigated through a series of six published patents. The three
patents relating to the development of novel leather and textile processes were
solely conceived and executed by the author. The patent related to the
development of the plasma micro-reactor for ozone synthesis was conceived and
executed jointly by the author and Professor Will Zimmerman (Sheffield University).
The two patents related to the development of a novel metal cleaning and
treatment process was conceived and executed jointly by the author and Dr.
Robert Bird (Xeros Technology Group Limited).
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Příprava a studium katalytického systému Cu(O)-CeO2 metodami povrchové analýzy / The preparation and study of catalytic system Cu(O)-CeO2 using surface analytical methodsŠmíd, Břetislav January 2013 (has links)
Title: The preparation and study of catalytic system Cu(O)-CeO2 using surface analytical methods Author: Břetislav Šmíd Department: Department of Surface and Plasma Science Supervisor of the doctoral thesis: Doc. Mgr. Iva Matolínová, Dr. Abstract: This work is concerned with a study of copper/copper oxide - cerium dioxide systems and their interaction with CO and H2O molecules. Investigated samples were prepared in the form of powder catalysts and also as very well defined model inverse systems. The low temperature CO oxidation powder catalysts were studied by means of XPS, XRD, SEM, TEM and in micro-reactor system allowing the CO oxidation examination. The study of H2O adsorption and co-adsorption of H2O with CO were carried out on model inverse systems CeOx(111)/Cu(111) in ultra-high vacuum conditions using X-ray, synchrotron radiation (SRPES), resonant (RPES) photoelectron spectroscopies and LEED. It was observed on the stoichiometric surface water adsorbs molecularly at 120 K while on the reduced surface and surface of CeO2 islands on Cu(111) the H2O adsorption is partially dissociative with formation of OH groups. The increase of Ce3+ species (i.e. surface reduction) observed after H2O adsorption was explained as an electronic effect of the Ce 4f charge accumulation and Ce 5d charge depletion....
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