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Synthese und Charakterisierung neuartiger, gemischter Tetrahydridoborate für die Wasserstoffspeicherung / Synthesis and characterisation of novel mixed tetrahydroborates for hydrogen storageLindemann, Inge 02 July 2014 (has links) (PDF)
Im Rahmen dieser Arbeit wurden neuartige, gemischte Tetrahydridoborate (Borhydride), die für die Wasserstoffspeicherung im Festkörper für die mobile Anwendung geeignet sein könnten, synthetisiert und vollständig charakterisiert. Entscheidende Materialanforderungen für die Kombination mit einer Tieftemperaturbrennstoffzelle sind die hohe Wasserstoffspeicherkapazität von min. 6 m% bei einer Wasserstoffdesorption unterhalb von 100°C. Um beide dieser Hauptkriterien zu erfüllen, wurden Li-Al- und Na-Al-Borhydrid entsprechend dem Konzept von Nakamori u.a. ausgewählt. Beide Borhydride desorbieren unterhalb von 100°C, wobei das synthetisierte Li-Al-Borhydrid aufgrund des hohen Wasserstoffgehalts (17,2 m% H2) die vielversprechendsten Eigenschaften zeigte. Beide Systeme wurden mittels Pulverdiffraktometrie am Synchrotron hinsichtlich Ihrer Struktur aufgeklärt, wobei die Struktur der einzelnen komplexen Ionen anhand von Schwingungsspektroskopie (Infrarot-, Ramanspektroskopie) ebenfalls bestätigt werden konnte. Mit Hilfe verschiedener kombinierter Desorptionsanalysen war es möglich den Zersetzungspfad, insbesondere die Bildung instabiler Desorptionsprodukte, aufzuklären. So erfolgt die Zersetzung des Li-Al-Borhydrids über die Bildung von Lithiumborhydrid in der Festphase, das mittels in-situ Ramanspektroskopie in einer speziellen Ramanzelle beobachtet werden konnte. Die Infrarotspektroskopie des Desorptionsgases zeigte zunächst die Freisetzung von Aluminiumborhydrid, dass wiederrum Diboran und Wasserstoff desorbiert. Weiterhin wurden verschiedene Möglichkeiten verfolgt, wie der Zusatz von Kohlenstoff oder das Nanoconfinement von Lithiumalanat, um den Zersetzungsweg hinsichtlich ausschließlicher Wasserstofffreisetzung zu modifizieren und somit Reversibilität zu ermöglichen. Es konnte jedoch kein reversibles System mit hoher gravimetrischer Wasserstoffspeicherdichte und Desorption unterhalb von 100°C erzeugt werden. / Aim of the work was the synthesis and characterisation of novel mixed tetrahydroborates (borohydrides) for solid state hydrogen storage suitable for mobile applications. The combination with a PEM fuel cell requires a material with at least 6 wt% hydrogen combined with hydrogen desorption below 100°C. To fulfill both criteria, Li-Al- und Na-Al-borohydride were selected according to Nakamori’s concept. Both mixed borohydrides desorb well below 100°C whereas the mixed Li-Al-borohydride showed the most promising properties due to its high gravimetric hydrogen content (17.2 wt% H2). The crystal structures were examined by powder diffraction with a synchrotron source. The symmetry of the containing complex cations and anions was confirmed with vibrational spectroscopy (infrared, raman spectroscopy). The desorption pathway was clarified using a variety of combined thermal analysis techniques. Especially the desorption of unstable products of the most promising Li-Al-borohydride was possible via spectroscopy. Hence the desorption of Li-Al-borohydride leads to the formation of lithium borohydride in the solid state which was monitored via in-situ raman spectroscopy in a special raman cell. Infrared spectroscopy of the desorbed gas showed the initial desorption of aluminium borohydride which desorbs diborane and hydrogen in the following. Different options were examined in order to modify this desorption pathway by carbon addition or nanoconfinement of lithium alanate. However, none of the materials showed high hydrogen content combined with exclusive hydrogen desorption below 100°C and reversibility.
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Optimally-Sized Design of a Wind/Diesel/Fuel Cell Hybrid System for a Remote CommunityVafaei, Mehdi 29 September 2011 (has links)
Remote communities, characterized by no connection to the main power grid, traditionally get their power from diesel generators. Long geographical distances and lack of suitable roads make the fuel transportation difficult and costly, increasing the final cost of electricity. A microgrid using renewable energy as the main source can serve as a viable solution for this problem with considerable economical and environmental benefits. The focus of this research is to develop a microgrid for a remote community in northern Ontario (Canada) that combines wind, as a renewable source of energy, and a hydrogen-based energy storage system, with the goal of meeting the demand, while minimizing the cost of energy and adverse effect on the environment. The existing diesel generators remain in the system, but their use is minimized.
The microgrid system studied in this research uses a wind turbine to generate electricity, an electrolyser to absorb the excess power from the wind source, a hydrogen tank to store the hydrogen generated by the electrolyser, a fuel cell to supply the demand when the wind resource is not adequate, and a diesel generator as a backup power.
Two scenarios for unit-sizing are defined and their pros. and cons. are discussed. The economic evaluation of scenarios is performed and a cost function for the system is defined. The optimization problem thus formulated is solved by solvers in GAMS. The inputs are wind profile of the area, load profile of the community, existing sources of energy in the area, operating voltage of the grid, and sale price of electricity in the area. The outputs are the size of the fuel cell and electrolyser units that should be used in the microgrid, the capital and running costs of each system, the payback period of the system, and cost of generated electricity. Following this, the best option for the microgrid structure and component sizes for the target community is determined.
Finally, a MATLAB-based dynamic simulation platform for the system under study with similar load/wind profile and sizing obtained in optimization problem is developed and the dynamic behaviour of microgrid at different cases is studied.
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Amélioration et compréhension du mécanisme d'activation de l'alliage FeTi dopé avec de l'hafnium, pour le stockage de l'hydrogène / Enhancement and study of activation process of FeTi alloy doped with hafnium, for hydrogen storageRazafindramanana, Volatiana 20 December 2017 (has links)
La problématique de la première absorption (i.e. étape d’activation) de l’intermétallique FeTi, pour le stockage de l’hydrogène est souvent un frein pour son industrialisation. Le challenge réside dans la conception d’un « nouveau matériau » dont la première étape d’hydrogénation, s’effectue dans les mêmes conditions de température et de pression modérées, que lors de l’hydrogénation réversible. Une solution est de faire appel aux performances d’un élément dopant et/ou à la technique du broyage mécanique. Dans ce manuscrit, nous proposons l’utilisation de l’hafnium comme dopant. Ce projet complète les études qui ont été effectuées sur le zirconium (e.g. le zirconium commercial contient toujours une certaine quantité d’hafnium). L’ajout d’une faible quantité d’hafnium induit la formation d’une phase secondaire, « riche » en hafnium et en fer. Grâce à la présence de cette phase, la cinétique de première absorption est considérablement améliorée, et ce, sans traitement thermique préalable. L’étape d’activation comprend un seul mécanisme lorsque la taille des particules est faible. A contrario, un second mécanisme est mis en évidence, pour des particules de taille supérieure à 0,5 mm. La mécanosynthèse a permis non seulement d’obtenir la phase principale FeTi, mais aussi de favoriser la première absorption d’hydrogène. Des paramètres d’élaboration méticuleusement optimisés ont rendu possible la conception d’un matériau « modèle », par pulvérisation cathodique magnétron, sous forme de couche mince. Ce matériau modèle pourrait servir à étudier et à comprendre la diffusion de l’hydrogène à l’interface de la matrice FeTi et du dopant Zr ou Hf. / The issue of the first hydrogenation (i.e. activation process) of the intermetallic FeTi for the storage of hydrogen is often a brake for its use in industry. The challenge lies in the design of a "new material" whose first hydrogenation is carried out under the same conditions of moderate temperature and pressure, as during reversible absorption. Efficient solutions are to use a doping element and/or mechanical alloying process. In this work, we propose to use hafnium as a dopant. This project completes the studies that have been carried out on zirconium (e.g. commercial zirconium always contains a certain amount of hafnium). The addition of a small amount of hafnium induces the formation of a secondary phase, "rich" in hafnium and iron. Thanks to the presence of this phase, the kinetics of activation process is improved, without prior heat treatment. The activation process consists of a single step, when the particle size is small. However, a second step appears, for particles bigger than 0.5 mm. The mechanical alloying allowed the formation of the main phase FeTi, and also enhanced the activation process. An accurate control of deposition conditions allow us to design a ″model″ material by magnetron sputtering as thin layers. This ″model″ material can be used to study and understand the hydrogen diffusion, at the interface of the matrix (FeTi) and the dopant (Zr or Hf).
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Hydrogen absorption property of nanocrystalline-magnesium filmsUchida, Helmut Takahiro 27 November 2015 (has links)
No description available.
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Preparation and Characterization of Nanoscopic Solid State Hydrogen Storage Materials / Herstellung und Charakterisierung nanoskopischer Festkörper-WasserstoffspeicherSurrey, Alexander 05 July 2017 (has links) (PDF)
Die Speicherung von Wasserstoff in Form von Hydriden im festen Aggregatzustand hat den Vorteil einer hohen volumetrischen und gravimetrischen Wasserstoffspeicherdichte, die sowohl für die stationäre als auch die mobile Anwendung nötig ist. Um die Anforderungen dieser Anwendungen erfüllen zu können, müssen die Speichereigenschaften dieser Materialien weiter verbessert werden. Als zentrales Konzept dieser Dissertation wird die Nanostrukturierung verfolgt, die eine vielversprechende Strategie zur Modifizierung der thermodynamischen und kinetischen Eigenschaften von Hydriden darstellt. Die Transmissionselektronenmikroskopie (TEM) stellt dabei eine unverzichtbare Untersuchungsmethode solch nanoskopischer Materialien dar. Als problematisch erweist sich dabei die durch Radiolyse hervorgerufene Zersetzung der meisten Hydride bei der Beleuchtung mit dem abbildenden Elektronenstrahl.
Im ersten Teil dieser Arbeit wird eine Methodik entwickelt um dieses Phänomen quantitativ mit Hilfe von Valenzelektronenenergieverlustspektroskopie zu untersuchen. Hierzu kommt kugelgemahlenes MgH2 als Modellsystem zum Einsatz. Die Dehydrierung kann quantitativ durch die inelastische Streuung der hochenergetischen Elektronen am MgH2-Plasmon erklärt werden. Eine Lösung dieses grundlegenden Problems wird theoretisch an Hand von Multislice TEM-Kontrastsimulationen untersucht. Hierbei wird ein TEM Experiment unter Wasserstoff bei Umgebungsdruck anstatt unter Vakuum simuliert, was mit Hilfe eines speziellen TEM Halters, in dem das Gas durch elektronentransparente Fenster eingeschlossen ist, realisiert werden kann.
Im zweiten Teil wird der Einfluss des Nanoconfinements (Nanoeinschließung), einer speziellen Form der Nanostrukturierung, des komplexen Hydrids LiBH4 auf dessen Wasserstoffspeichereigenschaften untersucht, wofür eine neuartige nanoporöse aerogel-ähnliche Kohlenstoff-Gerüststruktur zum Einsatz kommt. Diese wird durch Salt Templating synthetisiert - einer simplen und nachhaltigen Methode zur Herstellung nanoporöser kohlenstoffbasierter Materialien mit großen Porenvolumina. Es wird gezeigt, dass durch das Nanoconfinement die Wasserstoffdesorptionstemperatur, die für makroskopisches LiBH4 bei über 400 °C liegt, auf 310 °C sinkt und die Desorption bereits bei 200 °C einsetzt. Eine teilweise Rehydrierung ist unter moderaten Bedingungen (100 bar und 300 °C) möglich, wobei die Reversibilität durch eine partielle Oxidation des amorphen Bor gehemmt ist. Im Gegensatz zu Beobachtungen einer aktuellen Veröffentlichung von in hoch geordnetem, nanoporösen Kohlenstoff eingebetteten LiBH4 deuten die in-situ TEM-Heizexperimente der vorliegenden Arbeit darauf hin, dass beide Reaktionsprodukte (B und LiH) in den Poren des aerogel-ähnlichen Kohlenstoffs verbleiben. / Storing hydrogen in solid hydrides has the advantage of high volumetric and gravimetric hydrogen densities, which are needed for both stationary and mobile applications. However, the hydrogen storage properties of these materials must be further improved in order to meet the requirements of these applications. Nanostructuring, which represents one of the central approaches of this thesis, is a promising strategy to tailor the thermodynamic and kinetic properties of hydrides. Transmission electron microscopy (TEM) is an indispensable tool for the structural characterization of such nanosized materials, however, most hydrides degrade fast upon irradiation with the imaging electron beam due to radiolysis.
In the first part of this work, a methodology is developed to quantitatively investigate this phenomenon using valence electron energy loss spectroscopy on ball milled MgH2 as a model system. The dehydrogenation can be quantitatively explained by the inelastic scattering of the incident high energy electrons by the MgH2 plasmon. A solution to this fundamental problem is theoretically studied by virtue of multislice TEM contrast simulations of a windowed environmental TEM experiment, which allows for performing the TEM analysis in hydrogen at ambient pressure rather than vacuum.
In the second part, the effect of the nanoconfinement of the complex hydride LiBH4 on its hydrogen storage properties is investigated. For this, a novel nanoporous aerogel-like carbon scaffold is used, which is synthesized by salt templating - a facile and sustainable technique for the production of nanoporous carbon-based materials with large pore volumes. It is shown that the hydrogen desorption temperature, which is above 400 °C for bulk LiBH4, is reduced to 310 °C upon this nanoconfinement with an onset temperature as low as 200 °C. Partial rehydrogenation can be achieved under moderate conditions (100 bar and 300 °C), whereby the reversibility is hindered by the partial oxidation of amorphous boron. In contrast to recent reports on LiBH4 nanoconfined in highly ordered nanoporous carbon, in-situ heating in the TEM indicates that both decomposition products (B and LiH) remain within the pores of the aerogel-like carbon.
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Étude de l'influence d'éléments d'addition sur les propriétés de stockage de l'hydrogène dans le système Ti-V-Fe / Study of the influence of alloying elements on hydrogen storage properties in the Ti-V-Fe systemDenis, Jean-Benoît 22 September 2016 (has links)
Cette thèse s'inscrit dans la thématique du stockage de l'hydrogène sous forme d'hydrure métallique. Pour pallier aux coûts importants des éléments utilisés pour l'élaboration des matériaux hydrurables, il est possible d'utiliser des alliages de pureté moindre comme précurseurs. Cela implique la présence d'éléments supplémentaires dans matériaux. Le matériau étudié appartient à la famille des composés intermétalliques Ti-V-Fe de structure cubique centrée. Cette structure est connue pour donner de fortes capacités réversibles d'absorption d'hydrogène durant une utilisation dans des conditions proches de l’ambiant. Grâce à une modélisation des principaux paramètres des hydrures formés à partir de ces alliages, il est apparu que le composé Ti15V71Fe14 présente des pressions d’équilibre intéressantes à température ambiante. Toutes les propriétés de ce matériau de référence ont été mesurées par diffraction des rayons X, microsonde de Castaing, microscopie à balayage électronique et banc d’hydruration. Une petite quantité des éléments d’addition est ajoutée individuellement puis ensemble dans la composition du matériau référent. Les échantillons sont analysés et les résultats sont comparés à ceux obtenus avec le référent. Il apparait que l’aluminium forme une solution solide de structure cubique centrée simple et améliore la capacité d’absorption du matériau référent. Il en est de même pour le silicium malgré un comportement plus complexe avec l’apparition de plusieurs phases supplémentaires. En contrepartie la vitesse d’absorption de l’hydrogène dans le matériau est diminuée / This Ph.D takes place on the hydrogen storage theme in metal hydride. In order to reduce the cost of the elements used for the preparation of hydridable materials, it is possible to use lower purity alloys as precursors. The compound selected belongs to the body centered cubic family consisting of Ti, V and Fe. This structure is known to store reversibly good quantities of hydrogen in conditions close to ambient. Thanks to modeling of the main parameters, it appears that the compound Ti15V71Fe14 presents interesting equilibrium pressure at room temperature. All properties of this reference material are measured by X-ray diffraction, EPMA, scanning electron microscopy and hydriding apparatus. A small amount of alloying elements has then been added individually then together in the composition of the reference material. Samples are analyzed and the results are compared to the referent. It appears that aluminum forms a solid solution of body centered cubic structure and improves the absorption capacity of the reference material. It is the same for silicon despite more complex behavior with the formation of several additional phases. In return the absorption kinetic of the material is reduced
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Materials For Hydrogen Generation, Storage, And CatalysisKalidindi, Suresh Babu 01 1900 (has links) (PDF)
Hydrogen, nature’s simple and the most abundant element has been in the limelight for the past few decades from the stand point of the so-called hydrogen economy. With a high calorific value (142 MJ/kg) that is three times as large as the liquid hydrocarbons, hydrogen has emerged as a promising and environmentally friendly source of energy for the future generations. However, on-board hydrogen storage is one of the bottlenecks for its widespread usage for mobile applications. Storing hydrogen in liquid or compressed form is extremely difficult because of its low density. One of the best alternatives is to store hydrogen in a chemical form. Despite extensive work in this area, none of the materials seem to satisfy the essential criteria of reversible hydrogen storage with high gravimetric content. With regard to chemical hydrogen storage, apart from metal hydrides, ammonia borane (H3N•BH3, AB) is a promising prospect with a very high gravimetric storage of 19.6 wt% of hydrogen. Objectives
1) Develop cost-effective and active first-row transition metal based catalysts for the generation of hydrogen from AB in protic solvents 2) Study the dehydrogenation of AB in fluorinated alcohols and acids in order to realize compounds that are suitable for regeneration.
3) Study the interaction of Cu2+ with AB in non-aqueous medium using 11B NMR spectroscopy and powder XRD techniques. 4) Generation of highly pure hydrogen from ammonia borane in the solid state under mild conditions in the presence of late first row transition metal salts.
5) Synthesis of highly monodisperse ultrasmall colloidal Mg nanoparticles using the Solvated Metal Atom Dispersion (SMAD) method and digestive ripening technique; study the effect of size on the desorption temperature of MgH2.
6) Synthesize Cu/ZnO and Cu/MgO nanocomposites from the individual metal nanoparticles using co-digestive ripening technique and establish the structure of the composites using TEM, EF-TEM, and powder XRD techniques.
Significant results
Hydrogen generation from AB in protic solvents was realized using first-row transition metal catalysts. Initial studies were carried out using Cu nanocatalyst synthesized by the solvated metal atom dispersion method (SMAD). The activity order was found to be Cu2O > Cu@Cu2O > Cu. In addition, the late first-row transition metal ions, Co2+, Ni2+, and Cu2+ ions were also found to be highly active towards AB hydrolysis. These ions assisted AB hydrolysis via in-situ formation of metal atoms/clusters. Cu2+ assisted the hydrolysis of AB via the in-situ generation of both H+ and Cu clusters. At higher concentrations of AB, hydrolysis resulted in the evolution of NH3 in addition to H2 whereas, methanolysis afforded pure H2. In the case of methanolysis, for catalyst/AB = 0.2, three equiv of H2 were liberated in 2.5, 4.2, and 1.5 min when Co-Co2B, Ni-Ni3B, and Co-Ni-B nanopowders were used as catalysts, respectively.
Dehydrogenation of ammonia borane (AB) was carried out in 2,2,2-trifluoroethanol and trifluoroacetic acid in order to realize compounds that are suitable for regeneration. The final byproduct obtained after the catalytic dehydrogenation of AB in 2,2,2-trifluoroethanol was NH4+B(OCH2CF3)4–. The FTIR data showed that the B-O bond in NH4+B(OCH2CF3)4 is slightly weaker compared to that in boric acid. Dehydrogenation of AB in trifluoroacetic acid in a controlled manner resulted in the formation of [CF3COO]–[BH2NH3]+ as the final by-product. Ammonia-borane was regenerated from [CF3COO]–[BH2NH3]+ by its reaction with LiAlH4, which served as the hydride source.
Dehydrogenation of AB in non-aqueous medium and in the solid state were studied in hydrogen storage point of view. Cu2+ was found to activate the B–H bond in amine boranes in non-aqueous medium even at room temperature. As a result of the B–H bond cleavage in AB, [H3N•BH2]Cl species is formed. This compound reacts with unreacted AB via 3 separate pathways one involving hydrogen evolution, a second involving formation of a stable diammoniate of diborane cation [(NH3)2BH2]Cl without hydrogen evolution, and the third involving the formation of [H2NBH2]n and BNHx polymers accompanied by the generation of H2. Mechanisms of these pathways have been elaborated using 11B NMR spectroscopy and powder X-ray diffraction methods. These studies demonstrate that Cu(II) salts can be used as effective initiators for the dehydrogenation of amine boranes.
Copper-induced hydrogen generation from AB in the solid state was also studied: for Cu2+/AB = 0.05, two equiv of H2 were liberated in 6.5 h at 333 K, which is equal to 9 wt% of the system. The 11B MAS NMR studies showed that the reaction proceeds through the intermediacy of [NH4]+[BCl4]– which eliminates the formation of borazine impurity, thereby affording pure H2. The cost effectiveness of CuCl2 makes this reaction scheme extremely attractive for real time applications.
In the context of hydrogen storage in metal hydrides, highly monodisperse colloidal Mg nanoparticles with a size regime of 2–4 nm were synthesized by using the SMAD method followed by digestive ripening technique. The Mg-HDA nanopowder was fully hydrided at 33 bar and 391 K. Onset of hydrogen desorption from MgH2 nanoparticles was observed at a remarkably low temperature, 388 K compared to > 623 K in the case of bulk MgH2. The present study is a step towards realizing hydrogen storage materials that could operate close to ambient conditions.
Colloids of Cu and Zn nanoparticles stabilized by 2-butanone have been prepared by the SMAD method. The as-prepared colloids which are polydisperse in nature have been transformed into highly monodisperse colloids by the digestive ripening process in the presence of hexadecylamine. Using this process, copper nanoparticles of 2.1 ± 0.3 nm and zinc nanoparticles of 3.91 ± 0.3 nm diameters have been obtained. Co-digestive ripening of Cu, Zn and Cu, Mg colloids resulted in the formation of Cu/ZnO and Cu/MgO nanocomposites, respectively. The structures of these nanocomposites were established using UV-visible spectroscopy, TEM, EF-TEM, and powder XRD techniques.
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Modificação superficial de ligas armazenadoras de hidrogênio por óxidos metálicos a partir do método sol-gel / Surface modification on hydrogen storage alloys by metal oxides via sol-gel routeRosangela Bocutti 26 May 2003 (has links)
Este trabalho consiste na análise da modificação superficial da liga armazenadora de hidrogênio, MmNi3,4Co0,8Al0,8, através de óxidos de Cobre, Níquel e Cobalto, utilizando-se para tanto o método sol-gel. As técnicas de caracterização usadas para o recobrimento obtido, Microscopia Eletrônica de Varredura (MEV) e Redução Térmica Programada (RTP), permitiram a observação de uma \"rede\" formada pelos óxidos presentes nos recobrimentos que proporcionam a aglomeração das partículas da liga, sem contudo, impedir a interação de hidrogênio com o material. O estudo do comportamento eletroquímico do recobrimento foi realizado pelas técnicas de Voltametria Cíclica , Ciclos Galvanostáticos de Carga e Descarga e Espectroscopia de Impedância. Foi possível verificar que a camada de óxidos formada pelo recobrimento através do método sol-gel melhora o desempenho da liga: em relação a sua capacidade de descarga que é significativamente aumentada, principalmente no recobrimento por óxido de cobalto e também em relação a proteção contra a pulverização do material, que proporciona maiores números de ciclos de carga e descarga / This work consists in the analysis of the surface modification of the hydrogen storage alloy, MmNi3,4Co0,8Al0,8, threugh Copper, Nickel and Cobalt oxides, using for this the sol-gel method. The characterization techniques used for the obtained surfase modification (SEM and TPR) allowed the observation of a \" net \" formed by the presents oxides in the surface modification that provides the gathering of the alloys particles, without however, to harm the hydrogen interaction with the material. The study of the electrochemical behavior of the surface modification was carried out by the techniques of Cyclic Voltammetry, Charge/Discharge cycles and Electrochemical Impedance. It was possible to verify that the oxides of layer formed by the surface modification for the sol-gel method improves the alloy performance: in relation to its discharge capacity that is significantly increased, mainly in the surface modification by oxide of cobalt, and also in relation to the protection against the deterioration of the material, that provides higher numbers of cycles charge and discharge
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Phase Change Materials for Thermal Management in Thermal Energy Storage ApplicationsJanuary 2020 (has links)
abstract: Thermal Energy Storage (TES) is of great significance for many engineering applications as it allows surplus thermal energy to be stored and reused later, bridging the gap between requirement and energy use. Phase change materials (PCMs) are latent heat-based TES which have the ability to store and release heat through phase transition processes over a relatively narrow temperature range. PCMs have a wide range of operating temperatures and therefore can be used in various applications such as stand-alone heat storage in a renewable energy system, thermal storage in buildings, water heating systems, etc. In this dissertation, various PCMs are incorporated and investigated numerically and experimentally with different applications namely a thermochemical metal hydride (MH) storage system and thermal storage in buildings. In the second chapter, a new design consisting of an MH reactor encircled by a cylindrical sandwich bed packed with PCM is proposed. The role of the PCM is to store the heat released by the MH reactor during the hydrogenation process and reuse it later in the subsequent dehydrogenation process. In such a system, the exothermic and endothermic processes of the MH reactor can be utilized effectively by enhancing the thermal exchange between the MH reactor and the PCM bed. Similarly, in the third chapter, a novel design that integrates the MH reactor with cascaded PCM beds is proposed. In this design, two different types of PCMs with different melting temperatures and enthalpies are arranged in series to improve the heat transfer rate and consequently shorten the time duration of the hydrogenation and dehydrogenation processes. The performance of the new designs (in chapters 2 and 3) is investigated numerically and compared with the conventional designs in the literature. The results indicate that the new designs can significantly enhance the time duration of MH reaction (up to 87%). In the fourth chapter, organic coconut oil PCM (co-oil PCM) is explored experimentally and numerically for the first time as a thermal management tool in building applications. The results show that co-oil PCM can be a promising solution to improve the indoor thermal environment in semi-arid regions. / Dissertation/Thesis / Doctoral Dissertation Mechanical Engineering 2020
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Hydrogen Storage In Nanostructured MaterialsAssfour, Bassem 28 February 2011 (has links)
Hydrogen is an appealing energy carrier for clean energy use. However, storage of hydrogen is still the main bottleneck for the realization of an energy economy based on hydrogen. Many materials with outstanding properties have been synthesized with the aim to store enough amount of hydrogen under ambient conditions.
Such efforts need guidance from material science, which includes predictive theoretical tools.
Carbon nanotubes were considered as promising candidates for hydrogen storage applications, but later on it was found to be unable to store enough amounts of hydrogen under ambient conditions. New arrangements of carbon nanotubes were constructed and hydrogen sorption properties were investigated using state-of-the-art simulation methods. The simulations indicate outstanding total hydrogen uptake (up to 19.0 wt.% at 77 K and 5.52wt.% at 300 K), which makes these materials excellent candidates for storage applications. This reopens the carbon route to superior materials for a hydrogen-based economy.
Zeolite imidazolate frameworks are subclass of MOFs with an exceptional chemical and thermal stability. The hydrogen adsorption in ZIFs was investigated as a function of network geometry and organic linker exchange. Ab initio calculations performed at the MP2 level to obtain correct interaction energies between hydrogen molecules and the ZIF framework. Subsequently, GCMC simulations are carried out to obtain the hydrogen uptake of ZIFs at different thermodynamic conditions. The best of these materials (ZIF-8) is found to be able to store up to 5 wt.% at 77 K and high pressure.
We expected possible improvement of hydrogen capacity of ZIFs by substituting the metal atom (Zn 2+) in the structure by lighter elements such as B or Li. Therefore, we investigated the energy landscape of LiB(IM)4 polymorphs in detail and analyzed their hydrogen storage capacities. The structure with the fau topology was shown to be one of the best materials for hydrogen storage. Its total hydrogen uptake at 77 K and 100 bar amounts to 7.8 wt.% comparable to the total uptake reported of MOF-177 (10 wt.%), which is a benchmark material for high pressure and low temperature H2 adsorption.
Covalent organic frameworks are new class of nanoporous materials constructed solely from light elements (C, H, B, and O). The number of adsorption sites as well as the strength of adsorption are essential prerequisites for hydrogen storage in porous materials because they determine the storage capacity and the operational conditions. Currently, to the best of our knowledge, no experimental data are available on the position of preferential H2 adsorption sites in COFs. Molecular dynamics simulations were applied to determine the position of preferential hydrogen sites in COFs. Our results demonstrate that H2 molecule adsorbed at low temperature in seven different adsorption sites in COFs. The calculated adsorption energies are about 3 kJ/mol, comparable to that found for MOF systems. The gravimetric uptake for COF-108 reached 4.17 wt.% at room temperature and 100 bar, which makes this class of materials promising for hydrogen storage applications.
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