This thesis deals with the problem of waste heat, namely, the exhaust gas which are not frequently used. Specifically, it is a design of thermoelectric generators set, power electronics for fan and heat exchanger proposal. The entire system uses the energy of the waste heat to increase the heating efficiency.

<p>Developing the next generation soft optoelectronic materials is of great importance for achieving high-performance, low-cost electronics. These novel material systems bring about new chemistry, physical phenomena, and exciting properties. Organic inorganic hybrid two-dimensional perovskites and organic stable radical molecules are two exciting material systems that bear high expectation and await extensive exploration.</p> <p>Organic inorganic hybrid two-dimensional perovskites are considered one of the solutions to the pressing instability issue of halide perovskites toward commercialization. Moreover, dimension reduction of perovskites creates new opportunities for using two-dimensional perovskites as thermoelectric applications due to the ultralow thermal conductivity. However, two-dimensional perovskite thermoelectric is still at its’ incipient stage of development, therefore a timely proof of potential is required to draw further research interests.</p> <p>In earlier part of this work, the two-dimensional perovskites featuring π-conjugated ligands are synthesized and optimized for high thermoelectric performance. With material design, device engineering, intensive measurements, and careful data analysis, we successfully showed that two-dimensional perovskites are competitive candidate for the emerging thermoelectric materials. Furthermore, temperature and carrier concentration dependencies on thermoelectric properties were also established, giving future researchers a generalized optimization strategy. </p> <p>Organic stable radical molecules are promising for organic electronics as stable radicals don’t require high conjugation for efficient solids-state charge transport. Thanks to their unique redox capability and the unpaired electrons, organic radicals have many unique electronic and magnetic properties that could be useful in spin-related applications. However, the understanding in charge transport mechanisms as well as structure-to-properties correlation remain shallow.</p> <p>In later part of this work, we achieved the highest recorded long channel electrical conductivity of non-conjugated radicals. Meanwhile, the important role of close packing between radical sites was demonstrated by slightly changing chemical design that resulted in drastic change in electrical conductivity. Finally, we concluded that the solid-state charge transport in non-conjugated species is governed by variable range hopping mechanisms. </p>

Thermoelectric materials are playing a larger role in the global effort to develop diverse, efficient, and sustainable energy technologies: primarily through power-generating thermoelectric modules. The principal components of thermoelectric modules are solid-state thermoelectric materials – typically heavily doped semiconductors – that convert heat directly into electricity. However, this conversion efficiency is too low to supplant traditional energy technologies – severely limiting the distribution of clean and sustainable thermoelectric energy technologies. Efforts to enhance thermoelectric efficiency, which have been underway for decades, have been slow to realize appreciable gains in thermoelectric efficiency. However, a key advance in improving efficiency – the New Paradigm in thermoelectric material research – has been the development of thermoelectric nanocomposites. Thermoelectric nanocomposites show improved efficiency; however, they are often synthesized from highly toxic elements via energetically intense and costly synthesis procedures. Therefore, this research focuses on the discovery and development of a novel procedure for synthesizing thermoelectric nanocomposites – attrition enhanced nanocomposite synthesis – from open cage-like skutterudite-based materials. With further optimization, high-performance power-generating thermoelectric materials can be produced via this technique. Therefore, attrition-enhanced nanocomposite synthesis may play a small, though instrumental, role in achieving sustainable electrical power. / Graduation date: 2012 / Access restricted to the OSU Community at author's request from Jan. 6, 2012 - Jan. 6, 2013

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L'augmentation du prix du pétrole ainsi qu'une possible future réglementation des émissions de CO2 encourage les fabricants de véhicules industriels à trouver de nouvelles solutions pour améliorer encore la performance de la chaine cinématique. Dans ce cadre, deux solutions de récupérations d'énergie prometteuses sont très souvent rapportées dans la littérature: le système de récupération d'énergie par cycle de Rankine et le générateur thermoélectrique. Après un rappel des conditions limites du fonctionnement d'un camion long routier, cette thèse démontre tout d’abord la modélisation 0-D et 1-D (logiciels commerciaux utilisés) de ces deux systèmes de récupération d’énergie. Pour le générateur thermoélectrique, des études paramétriques (hauteur de jambe thermoélectrique, prix, puissance électrique produite) sont effectuées se basant principalement sur l'utilisation de deux matériaux prometteurs. Une conception du système Rankine est présentée et modélisée avec le solveur 1-D. Des validations partielles sont réalisées sur les composants (turbine). Ce modèle a ensuite permis d'étudier les transitoires du système ainsi que la charge en réfrigérant et un système de contrôle possible. Cette étude montre que le générateur thermoélectrique n’est pas encore mature pour son utilisation dans un camion long routier. Le système Rankine doit quant à lui être testé sur un camion prototype pour pouvoir véritablement estimer son potentiel final / Fuel price increase as well as future fuel consumption regulations lead truck manufacturers to further enhance the current powertrain. In such a context, two waste heat recovery technologies appear as promising: the Rankine system as well as the thermoelectric generator. After a reminding of truck boundary conditions, this thesis work defines 0-D and 1-D modeling (commercial tool used) for both systems.For the thermoelectric generator , parametric 1-D studies are done on the integration/design (number of thermoelements, price, electrical power) of a thermoelecric generator upstream the existing engine exhaust gas recirculation cooler. Main studies are done with thermoelectric materials but other materials are also considered. A Rankine system design is presented and modeled under a 1-D solver. Preliminary validations are presented. Transient aspects are evaluated to better understand the behavior of the system and its bottlenecks. The amount of refrigerant in the circuit and the control schematic are also addressed.From these studies, it appears that the thermoelectric generator technology is not yet mature for a long haul truck due to the low performance of thermoelectric materials. The Rankine system technology should handle a complete truck prototype testing to estimate its potential

Cette thèse porte sur le mouvement de particules colloïdales induit par l’effet thermoélectrique (ou effet Seebeck). Dans un électrolyte soumis à un gradient de température, les ions ont tendance à migrer à des vitesse qui différent d'une espèce à l'autre. On observe alors une accumulation de charge aux bords de l’échantillon. Ce déséquilibre induit un champ électrique qui agit sur les colloïdes chargés présents dans la solution. Cette contribution électrophorétique dans le champ de Seebeck s'additionne à la contribution directe de thermodiffusion. Comme résultat principal,nous obtenons la vitesse phorétique en fonction de la fraction volumique des particules et, dans le cas de polyélectrolytes, du poids moléculaire. Dans la seconde partie, nous étudions l’effet thermoélectrique pour une particule chauffée par absorption d’un faisceau laser. Le gradient de température est alors radial et l’effet Seebeck induit une charge nette dans le voisinage de la particule. Enfin, nous discutons les applications possibles de ce phénomène de thermocharge / In this work we study the motion induced in a colloidal dispersion by thethermoelectric or Seebeck effect. As its basic principle, the ions of the electrolytesolution start moving in a temperature gradient. In general, the velocity of one iondiffers from another. As a result, one observes a charge separation and a macroscopicelectric field. This thermoelectric field, in turn, acts upon the charged colloidalparticle present in the solution. Thus thermophoresis of the particle comprises of anelectrophoretic motion in the thermoelectric or Seebeck field. As an important result,we derive how the corresponding velocity of a colloidal particle depends upon thecolloidal volume fraction or on molecular weight for polymers. In a second part, westudy the thermoelectric effect due to a hot colloidal particle where a radialtemperature gradient is produced by the particle itself. In this temperature gradientthe same Seebeck effect takes place in the electrolyte solution. We find that the hotparticle carries a significant amount of charge around it. Whereas the amount ofsurface charges present at the boundaries of the sample container in the onedimensionalcase is rather insignificant. Possible applications of this thermochargingphenomenon are also discussed.

The mixing of polymers and nanoparticles makes it possible to give advantageous macroscopic material performance by tailoring the microstructure of composites. In this thesis, five combinations of nano inclusion and polymer matrix have been investigated. The first type of composites is titanium dioxide/ polyaniline combination. The effects of 4 different doping-acids on the microstructure, morphology, thermal stability and thermoelectric properties were discussed, showing that the sample with HCl and sulfosalicylic dual acids gave a better thermoelectric property. The second combination is titanium dioxide/polystyrene composite. Avrami equation was used to investigate the crystallization process. The best fit of the mass derivative dependence on temperature has been obtained using the double Gaussian dependence. The third combination is titanium dioxide/polyaniline/ polystyrene. In the titanium dioxide/polyaniline/ polystyrene ternary system, polystyrene provides the mechanical strength supporting the whole structure; TiO2 nanoparticles are the thermoelectric component; Polyaniline (PANI) gives the additional boost to the electrical conductivity. We also did some investigations on Polyethylene odide-TiO2 composite. The cubic anatase TiO2 with an average size of 13nm was mixed with Polyethylene-oxide using Nano Debee equipment from BEE international; Single wall carbon nanotubes were introduced into the vinyl acetate-ethylene copolymer (VAE) to form a connecting network, using high pressure homogenizer (HPH). The processing time has been reduced to 1/60 of sonication for HPH to give better sample quality. Theoretical percolation was derived according to the excluded volume theory in the expression of the threshold as a function of aspect ratio.

Une des préoccupations majeures de la recherche dans le domaine de l’énergie est la diminution de la production des gaz à effet de serre et la réduction de notre empreinte écologique. Les générateurs thermoélectriques participent à une démarche globale d’efficacité énergétique en convertissant directement une partie de l’énergie thermique qui les traverse en énergie électrique. Ces derniers sont encore peu utilisés et rares sont les travaux qui traitent de leur optimisation. Ce travail a permis d’explorer les stratégies d’intégration des modules thermoélectriques dans les ensembles définis par les utilisateurs finaux en utilisant une méthodologie basée sur une modélisation complète des systèmes du flux de chaleur à la production électrique. Un code numérique couplant les équations de la thermique, de la thermoélectricité et de l’électricité a été développé et permet d’observer l’influence de plusieurs paramètres sur la production d’électricité (débit et température de la source chaude, débit et température de la source froide, type de modules thermoélectriques, emplacement des modules,…). La validation de ce modèle a nécessité la réalisation et l’instrumentation de plusieurs prototypes expérimentaux dont le plus conséquent est une boucle d’air à haute température alimentant un prototype de générateur thermoélectrique modulable. La conception et la réalisation de convertisseurs électriques dédiés, à recherche du point de fonctionnement maximal (MPPT), a permis de tester ces prototypes au point d’adaptation optimale. Enfin, une méthode d’optimisation appliquée au modèle nous délivre le nombre de modules ainsi que leur emplacement pour une production électrique maximale. Un outil de dimensionnement et d’optimisation de générateurs thermoélectriques est maintenant disponible. Il nous a permis tout d’abord d’étudier la faisabilité d’une production d’électricité en zones isolées au travers d’un prototype de cuisinière à bois thermoélectrique. Puis nous avons analysé la faisabilité dans le domaine de l’automobile en se plaçant à un point de fonctionnement précis correspondant au gaz d’échappement. / A major concern of research in the field of energy is the decrease in the production of greenhouse gas emissions and reducing our ecological footprint. Thermoelectric generators participate in a comprehensive approach to energy efficiency by directly converting a part of the thermal energy that flows through in electricity. This work explore strategies for integrating thermoelectric modules in sets defined by end users using a methodology based on a complete systems modelling from heat flow to power generation. A numerical code coupling equations of heat transfers and thermoelectricity was developed and used to observe the influence of several parameters on the production of electricity (flow and temperature of the hot source, flow and temperature of the cold source, type of thermoelectric modules, module location...). The validation of this model has necessitated the construction and the instrumentation of several experimental prototypes which for the most important is a hot air loop supplying a prototype flexible thermoelectric generator. The design and the realization of dedicated electrical converters to research the maximum operating point (MPPT) was performed to test these prototypes optimal adaptation issue. Finally, an optimization method applied to the model delivers us the number of modules and their location for maximum power production. A tool for design and optimization of thermoelectric generators is now available. It has allowed us to study the feasibility of an integrated thermoelectric generation in a variety of systems such as the automobile using exhaust gas or a specific cook stove for developing countries.

Oxide materials exhibit a wide variety of structures and properties. In particular, transition metal oxides tend to be highly stable while exhibiting a wide range of properties that can be used for numerous applications. This work focuses on investigating how the structures��� of 4d and 5d transition metal oxides influences their properties. Specifically oxides of Ru, Rh and Ir were investigated. A complete solid solution was found between isostructural Pb���Mn���O������ and Pb���Rh���O������. Pb���Rh���O������ shows a Verwey-type transition at 185 K. This transition remains with a 3 % substitution of Mn for Rh but disappears with a 4 % substitution of Mn for Rh. The structure was found to expand in the direction perpendicular to the layers of the structure, which is the c-axis, despite a contracting unit cell. Bi for Pb substitution in Pb���Mn���O������ was found to be limited as compared to in Pb���Rh���O������. Alkali metal substitution on the A-site of the orthorhombic perovskite SrRuO��� showed only low substitution levels were possible. Nonetheless, the substituted phases showed decreased ferromagnetic Curie temperatures, increased electrical resisitivity and relatively unchanged Seebeck coefficients. Thermoelectric studies of Sr[subscript 2-x]La[subscript x]CoRuO��� perovskite phases showed Sr���.���La���.���CoRuO��� with the best thermoelectric performance. This system showed possible correlations between cation ordering on the B-site and the charge carrier transport. A similar thermoelectric study of (RhV)[subscript 1+x]Ti[subscript 1-2x]O��� phases crystallizing in a disordered trirutile structure was done. Electron carriers were found to be dominant and dependent on Ti content. The electron carriers appear to become diminished at higher temperatures. Sr���IrO��� crystallizes in a K���NiF���-type structure. Effects of Ti, Fe and Co substitution for Ir were investigated. A complete Sr���Ir[subscript 1-x]Ti[subscript x]O��� solid solution was synthesized and characterized while limited solubility was found for Fe and Co substitutions. All substitutions showed a decrease in the c-cell parameter coupled with a decrease in octahedral tilting. All substitutions also showed a decrease in magnetic susceptibility and an increase in the paramagnetic effective moment was observed for Co and Fe doped samples. An incomplete solid solution was formed for Sr���Ti[subscript 1-x]Rh[subscript x]O��� phases; however effects of increased octahedral tilting with higher Rh content were observed. / Graduation date: 2013

It is generally believed that one of the key parameterscontrolling the normal state and superconducting properties ofhigh temperature superconductors is the charge carrierconcentrationpin the CuO2planes.By changing the non-isovalent dopingconcentration on the RE site as well as the oxygen content in(RE)Ba2Cu3O7−δ, an excellent tool is obtained tovary the hole concentration over a wide range from theunderdoped up to the overdoped regime.In the present thesis thefocus is on the doping effects on the structural and normalstate electrical properties in Nd-123 doped with Ca, La, Pr,Ca-Pr, and Ca-Th.T he effects of doping have been investigatedby X-ray and neutron powder diffraction, and by measurements ofthe resistivity, thermoelectric powerS, and Hall coefficient RH.T he thermoelectric power is a powerful tool forstudies of high temperature superconductivity and is highlysensitive to details of the electronic band structure.Sas a function of temperature has been analyzed in twodifferent two band models.The parameters of these models arerelated to charactristic features of the electron bands and asemiempirical physical description of the doping dependence ofSis obtained.So me important results are following: (i)The valence of Pr in the RE-123 family.Results from thestructural investigations, the critical temperature Tc, and thethermoelectric power indicated a valence +4 at low dopingconcentration, which is in agreement with results of chargeneutral doping in the RE-123 family.(ii)Hole localization. The results of bond valence sum (BVS)calculations from neutron diffraction data showed that holelocalization on the Pr+4site was the main reason for the decrease of thehole concentration p.Differ ent types of localization wereinferred by S measurements for Ca-Th and Ca-Pr dopings.(iii)Competition between added charge and disorder. Theresults of RH measurements indicated that Ca doping introduceddisorder in the CuO2planes in addition to added charge.This could bethe main reason for the observed small decrease of thebandwidth of the density of states in the description of aphenomenological narrow band model.(iv) Empirical parabolic relation between γ and p.S data were analyzed and well described by a two-band modelwith an additional linear T term, γT.An empiricalparabolic relation for γ as a function of holeconcentration has been found. <b>Key words:</b>high temperature superconductors, criticaltemperature, resistivity, thermoelectric power, Hallcoefficient, X-ray diffraction, Neutron diffraction, NdBa2Cu3O7−δ, hole concentration,substitution.