To support the large­scale integration of renewables in electricity grids, power­to­X­to­power (P2X2P) systems have been proposed. These systems serve to increase the flexibility of thermal power plants while potentially providing both economic and environmental benefits by allowing power from the plant to be redirected into an electrolyzer and converted to a gaseous energy carrier. In this study, the feasibility of a P2X2P system consisting of a combined cycle gas turbine (CCGT) power plant coupled with a PEM electrolyzer in the Italian power sector has been investigated. A dynamic technoeconomic model has been developed for both hydrogen and ammonia­based systems together with a profit maximizing dispatch strategy for operation in both day­-ahead and balancing electricity markets. As a part of this, a PEM electrolyzer model was also developed and validated against experimental data. Notable technical improvements were observed as a consequence of the implementation of a P2X2P system in the form of avoided shutdowns and a more even power output. However, any economic and environmental benefits of such improvements were not observed as the addition of the P2X2P system led to a reduction in net present value as well as higher specific emissions of carbon dioxide. When the gaseous energy carrier was utilized as fuel in the CCGT, similar technical performances were achieved by the hydrogen­based and ammonia­based systems. Due to the increased investment cost demanded by the ammonia production process the hydrogen­based system thus seems most suitable for this setup. / För att möjliggöra en storskalig utbyggnad av förnyelsebar energi har power­to­X­to­power­system (P2X2P) föreslagits som en potentiell lösning. Genom att omdirigera electricitet från kraftverket till en elektrolysator och därmed omvandla denna till vätgas kan dessa system förbättra den tekniska flexibiliten hos värmekraftverk samtidigt som de har potential att medföra både ekonomiska och miljömässiga fördelar. Detta examensarbete har undersökt den tekno­ekonomiska potentialen hos ett P2X2P­system bestående av ett gaskombikraftverk i anslutning till en elektrolysator i det italienska kraftnätet. En dynamisk, tekno­ekonomisk modell av både vätgas­ och ammoniakbaserade P2X2P­system samt en vinstmaximerande kontrollstrategi har utvecklats. En modell över en PEMelektrolysator har även utvecklats och validerats gentemot experimentella data. Införandet av ett P2X2P­system till kraftverket påvisade en teknisk förbättringspotential genom ett minskat antal uppstarter samt en mer jämn uteffekt. Huruvida denna tekniska förbättring också medför ekonomisk and miljömässig förbättring eller ej kvarstår att påvisa. Detta då nuvärdet minskade samtidigt som koldioxidutsläppen per producerad kilowatttimme ökade vid införandet av P2X2P­systemet. Då den producerade energibäraren, i form av vätgas eller ammoniak, enbart användes för att ersätta fossilgas som bränsle i kraftverket påvisades marginell skillnad i presetanda mellan de två systemen. De större kostnaderna som medförs av ett ammoniak­baserat system pekar därför på att ett vätgas­baserat system vore att föredra under sådana förutsättningar.

Cette thèse s'inscrit dans le contexte de la production et de l'utilisation du vecteur énergétique hydrogène dont le potentiel est très prometteur dans un paysage énergétique renouvelé. Plus exactement, cette étude traite des électrolyseurs et des piles à combustible de technologie PEM (membranes échanges de protons) fonctionnant à basse température. Dans une très large majorité, les études présentées ici se sont inscrites en partenariat étroit avec HELION Hydrogen Power, notamment dans le cadre du projet ANR AIRELLES (2008- 2011). Tout d'abord sont posées les bases de modèles (quasi-statique, dynamique petits signaux, dynamique forts signaux) génériques et applicables à une pile à combustible et à un électrolyseur. Les méthodologies de caractérisation ainsi que les techniques de paramétrisation de ces modèles utilisées sont ensuite exposées. L'intérêt de croiser toutes ces approches pour caractériser au plus juste les composants est illustré. A partir de cette vision commune des deux composants, le document est scindé en trois parties : - Une première partie porte sur une validation et une exploitation des modèles proposés via différentes études sur des piles à combustible alimentées en H2/air : 1) La recherche de signatures d'un engorgement et d'un assèchement d'une pile alimentée en H2/air. Ces signatures sont comparées à celles d'une pile alimentée en H2/02. 2) L'analyse des impacts d'harmoniques de courant hautes fréquences (représentatives d'un convertisseur continu-continu de type boost) sur un coeur de pile. Ces travaux s'inscrivent dans le cadre d'une collaboration avec le laboratoire FEMTO-ST/FCLAB (projet CNRS CO-CONPAC). - Une seconde partie porte sur la validation et la paramétrisation des modèles proposés pour l'électrolyseur. Deux techniques originales ont été proposées et testées : la première consiste en une approche multispectres d'impédance et la seconde en une approche multibalayages basses fréquences. - Une troisième partie décrit les moyens d'essais qui ont été conçus et déployés au cours de cette thèse aboutissant à une plateforme significative de tests dédiée à l'hydrogène sur le site l'INPT (Toulouse Labège). / This thesis is part of the production and use of hydrogen energy vector whose potential is very promising in a renewable energy landscape. More precisely, this study focuses on electrolysers and fuel cell using PEM technology (proton exchange membrane) operating at low temperature. Almost all the studies presented here were executed in close partnership with HELION Hydrogen Power; particularly in the context of the ANR project "AIRELLES" (2008-2011). Firstly are presented bases for models (steady-state, small signal dynamics, large signal dynamics) that are generic and applicable to a fuel cell and an electrolyzer. The characterization methodologies and parameterization techniques used are then presented. The interest to interbreed all these approaches to exactly characterize the components is illustrated. Using this common view of the two components, the document is divided into three parts: - The first part focuses on validation and exploitation of the proposed models through various studies on H2/air fuel cells: 1) The search for signatures of a flooding or a drying stack fuelled in H2/air. These signatures are compared with stack fuelled in H2/02. 2) The analysis of the impacts of high frequency current harmonics (representative of a DC-DC boost converter) on a cell heart. This work is part of collaboration with the laboratory FEMTO-ST/FCLAB (CNRS project CO-CONPAC). - A second part focuses on the validation and parameterization of models proposed for the electrolyzer. Two new techniques have been proposed and tested: the first one is a multispectral impedance approach and the second one a low frequencies multi sweep approach. - The third part describes the test facilities that have been designed and implemented in this thesis leading to a significant test platform dedicated to hydrogen on INPT site (Toulouse Labège).

Un système hybride multi-source est étudié dans cette thèse pour la génération dispersée basée sur des sources d’énergie renouvelable et des systèmes de stockage d’énergie. Il comprend un générateur éolien comme source d’énergie primaire, des super-condensateurs comme système de stockage à dynamique rapide, des piles à combustible et des électrolyseurs comme système de stockage sur le long terme sous forme d’hydrogène. Ils sont tous connectés à un bus continu commun et un onduleur est utilisé pour la connexion du système entier au réseau. Dans ce mémoire, nous avons présenté la modélisation du système, la conception du contrôle y compris des stratégies de répartition des flux de puissance et la gestion énergétique. Cette centrale hybride peut finalement générer des puissances lissées et contrôlables comme la plupart des générateurs classiques. Les performances ont été testées en simulation numérique et aussi sur un prototype expérimental. Les contributions scientifiques principales de cette thèse sont les suivantes : l’utilisation et l’adaptation des formalismes pour la modélisation des systèmes complexes et la conception de leur commande ; la conception et la réalisation expérimentale des émulateurs pour réduire le temps et le cout du développement du prototype expérimental ; la proposition et la validation de deux stratégies de gestion des puissances pour la régulation du bus continu et le contrôle des puissances transitées au réseau et enfin la proposition des stratégies de supervision énergétique avec la définition des modes de fonctionnement pour le générateur actif éolien afin d’assurer une disponibilité énergétique / A hybrid power system is studied in this thesis for the distributed generation based on renewable energy resources and energy storage systems in microgrid applications. It consists of a wind generator as primary energy source, super-capacitors as fast-dynamic storage system, fuel cells and electrolyzers as long-term storage system in hydrogen. They are all connected to a common DC bus and an inverter is used for the connection of the whole system to the grid. In this thesis, we have presented the system modeling, the control design including the power balancing and energy management strategies. This hybrid power system can finally supply controllable smooth powers as most conventional power plants. The performances have been tested in numerical simulations and also on an experimental test bench. As result, it is able to provide ancillary services to the microgrid. The main scientific contributions of this thesis are: the use and the adaptation of the graphical tools for the modeling of complex systems and their design; the design and the experimental implementation of real-time emulators in order to reduce the time and the cost of an experimental platform; the proposition and the validation of two power balancing strategies for the DC-bus voltage regulation and the grid power control and finally the proposition of energy management strategies for the active wind generator to ensure the energy availability

This dissertation thesis revolves around hydrogen economy and energy-storage electrochemical systems. More specifically, it investigates the possibility of using magnetron sputtering for deposition of efficient thin-film anode catalysts with low noble metal content for proton exchange membrane water electrolyzers (PEM-WEs) and unitized regenerative fuel cells (PEM-URFCs). The motivation for this research derives from the urgent need of minimizing the price of mentioned electrochemical devices should they enter mass production. Numerous experiments were carried out, correlating the actual in-cell performance with the varying position of thin-film catalyst within the membrane electrode assembly, with the composition of high-surface support sublayer and with the chemical structure of the catalyst itself. The wide arsenal of analytical methods ranging from electrochemical impedance spectroscopy through scanning electron microscopy to photoelectron spectroscopy allowed us to describe complex phenomena behind different obtained efficiencies. Consequent systematic optimizations led to the design of novel PEM-WE anode thin-film iridium catalyst with thickness of just 50 nm, supported on optimized TiC-based sublayer which performed similarly to standard counterparts despite using just a fraction of their noble metal...

H2 Green Steel AB was founded in 2020 to build a large-scale green steel factory in Boden, Norrbotten, Sweden. The factory consists of green hydrogen production, iron production and steel production. In 2030, the factory’s annual steel production will be 5 million tonnes annually. The objective of the thesis was to build a concept to improve a recommendation for a Hydrogenproduction site in an early stage of engineering. It included improving the understanding and basis for three criteria. The first criteria consisted of technical and customer requirements, seeing the requirements for the specific application of hydrogen as the critical factor. The second criteria consisted of further investigating how existing interfaces and utilities can be used in hydrogen production and building the basis for qualification. The third criteria consisted of adapting the concept to existing internal design tools by building it forward compatible. The thesis was initiated by bench-marking possible activities related to the recommendation acting as technical support and extensions to existing solutions. The research approach used was Design Research Methodology (DRM), held as the framework for execution. The result from the thesis delivers a database model built upon three linked packages providing a methodology of increased technical information, forward compatibility and a modular approach for design.

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<p dir="ltr">Catalyzing a green hydrogen economy can accelerate progress towards achieving the goal of a sustainable energy map with net-zero carbon emissions by rapid strides. An environmentally benign electrochemical energy conversion system is the Polymer Electrolyte Fuel Cell (PEFC) which uses hydrogen as a fuel to produce electricity and is notably used in a variety of markets such as industries, commercial setups, and across the transportation sector, and is gaining prominence for use in heavy-duty vehicles such as buses and trucks. Despite its potential, the commercialization of PEFCs needs to address several challenges which are manifested in the form of mass transport limitations and deleterious mechanisms at the interfacial scale under severe operating conditions. Achieving a robust electrochemical performance in this context is predicated on desired interactions at the triple-phase boundary of the electrochemical engine of the PEFC – the porous cathode catalyst layer (CCL) where the principal oxygen reduction reaction (ORR) takes place. The liquid water produced as a byproduct of the ORR helps minimize membrane dehydration; however, excess water renders the reaction sites inactive causing reactant starvation. In addition, the oxidation of the carbonaceous support in the electrode and loss of valuable electrochemically active surface area (ECSA) pose major barriers that need to be overcome to ameliorate the life expectancy of the PEFC.</p><p dir="ltr">In this thesis, the multimodal physicochemical interactions occurring inside the catalyst layer are investigated through a synergistic blend of visualization and computational techniques. The spatiotemporal dynamics of capillary force-driven liquid transport that ensues concentration polarization thereby affecting the desired response will be probed in detail. The drop in efficacy of the ORR due to competing catalyst aging mechanisms and the impact of degradation stressors on chemical potential-induced instability will be examined. The reaction-transport-mechanics interplay in core-shell nanoparticles, a robust class of electrocatalysts that promises better mass activity compared to the single metal counterparts is further highlighted. Finally, the influence of electrode microstructural attributes on the electrochemical performance of the reverse mode of fuel cell operation, i.e., Proton Exchange Membrane Water Electrolyzers (PEMWEs) is investigated through a mesoscale lens.</p>

There has recently been an increased interest in hydrogen, both as a solution for seasonal energy storage but also for implementations in various industries and as fuel for vehicles. The transition to a society less dependent on fossil fuels highlights the need for new solutions where hydrogen is predicted to play a key role. This project aims to investigate technical and economic outcomes of different strategies for production and storage of hydrogen based on hydrogen demand and source of electricity. This is done by simulating the operation of different systems over a year, mapping the storage level, the source of electricity, and calculating the levelized cost of hydrogen (LCOH). The study examines two main cases. The first case is a system integrated with offshore wind power for production of hydrogen to fuel the operations in the industrial port Gävle Hamn. The second case examines a system for independent refueling stations where two locations with different electricity prices and traffic flows are analyzed. Factors such as demand, electricity prices, and component costs are investigated through simulating cases as well as a sensitivity analysis. Future potential sources of income are also analyzed and discussed. The results show that using an alkaline electrolyzer (AEL) achieves the lowest LCOH while PEM electrolyzer is more flexible in its operation which enables the system to utilize more electricity from the offshore wind power. When the cost of wind electricity exceeds the average electricity price on the grid, a higher share of wind electricity relative to electricity from the grid being utilized in the production results in a higher LCOH. The optimal design of the storage depends on the demand, where using vessels above ground is the most beneficial option for smaller systems and larger systems benefit financially from using a lined rock cavern (LRC). Hence, the optimal design of a system depends on the demand, electricity source, and ultimately on the purpose of the system. The results show great potential for future implementation of hydrogen systems integrated with wind power. Considering the increased share of wind electricity in the energy system and the expected growth of the hydrogen market, these are results worth acknowledging in future projects.

Ce travail de thèse est consacré à l’étude des nickelates La2-xPrxNiO4+δ, comme nouveaux matériauxde cathodes pour piles à combustible haute température, SOFC, et en particulier à la caractérisationde leur stabilité chimique et leur comportement en fonctionnement. En effet, du fait de leurpropriété de conduction mixte ionique et électronique, MIEC, les nickelates de structure typeK2NiF4, Ln2NiO4+δ (Ln = La, Pr, Nd), correspondant au terme n = 1 de la série de Ruddlesden-Popper (An+1MnO(3n+1)), sont des matériaux prometteurs pour des fonctionnements à températureintermédiaire, IT-SOFC (T < 800 °C). Compromis entre la stabilité chimique de La2NiO4+δ et lestrès bonnes performances électrochimiques de Pr2NiO4+δ, les phases La2-xPrxNiO4+δ, ont étésynthétisées et leurs propriétés physico-chimiques, de transport et électrochimiques ont étédéterminées. L’étude approfondie des caractéristiques des électrodes par spectroscopied’impédance en cellules symétriques a été réalisée à courant nul et sous polarisation anodique etcathodique sur des périodes d’un mois. De façon surprenante, même après la dissociation complètede Pr2NiO4+δ en PrNiO3-δ, Pr4Ni3O10+δ et Pr6O11, la résistance de polarisation ne montre pas dechangement significatif. L’étude de PrNiO3-δ et Pr4Ni3O10+δ, comme matériau de cathode pour pilesà combustible, démontre l’excellent comportement de la phase Pr4Ni3O10+δ et ceci en cellulesymétrique (Rp (Pr4Ni3O10+δ) = Rp (Pr2NiO4+δ) = 0.15 Ω.cm² à 600 ° C) et cellule complète (1.6W.cm-2 at 800 °C). / This PhD work is dedicated to stability and ageing studies of Praseodymium based nickelates ascathodes for Solid Oxide Fuel Cells (SOFCs). With this respect Ln2NiO4+δ (Ln=La, Pr or Nd)compounds with the K2NiF4 type structure act as alternative cathode materials for IT-SOFC due totheir mixed ionic and electronic conductivity (i.e. MIEC properties). Pr2NiO4+δ shows excellentelectrochemical properties at intermediate temperature (i.e. low polarization resistance Rp value, Rp= 0.03 Ω.cm² at 700 °C), while La2NiO4+δ exhibits higher chemical stability. So, the properties ofLa2-xPrxNiO4+δ nickelates were investigated with the aim to find best compromise between chemicalstability and electrochemical performances. After synthesis, the physical and chemical properties aswell as their transport and electrochemical properties have been determined. Measurements of thepolarization resistance of symmetrical half-cells have been carried out by impedance spectroscopy.Then, the chemical stability and the electrochemical performance of the materials have been studiedfor duration up to one month. As an interesting point, even after complete dissociation of Pr2NiO4+δinto PrNiO3-δ,Pr4Ni3O10+δ and Pr6O11, the polarization resistance does not show significant change.So finally, two new materials PrNiO3-δ and Pr4Ni3O10+δ were investigated as SOFCs cathodeshowing very promising results for Pr4Ni3O10+δ in symmetrical cell (Rp (Pr4Ni3O10+δ) = Rp(Pr2NiO4+δ) = 0.15 Ω.cm² à 600 ° C) and complete cell (1.6 W.cm-2 at 800 °C).

Face aux enjeux énergétiques d’aujourd’hui et de demain, le développement des énergies renouvelables semble inéluctable. Cependant, la production électrique de sources renouvelables prometteuses comme le photovoltaïque ou l’éolien est intermittente et difficilement prévisible du fait de la dépendance de ces sources aux conditions météorologiques. Afin de s’affranchir du caractère discontinu de la production d’électricité et de l’inadéquation de la production avec la consommation, un moyen de stockage de l’énergie électrique est nécessaire. Dans ce contexte, la batterie hydrogène est une des solutions envisagées. Lors de périodes de surproduction d’énergie renouvelable, un électrolyseur produit de l’hydrogène par électrolyse de l’eau. Lorsque cela est nécessaire, une pile à combustible fournit de l’électricité à partir du gaz stocké. Couplé avec des sources d’énergie renouvelable, la batterie hydrogène produit de l’énergie électrique non carbonée, c’est-à-dire non émettrice de gaz à effet de serre. L’intérêt majeur de cette technologie est le découplage entre l’énergie et la puissance du système. Tant que la pile à combustible est alimentée en gaz, elle fournit de l’électricité, l’énergie dépend des réservoirs de gaz. La puissance, quant à elle, dépend des caractéristiques des composants électrochimiques et du dimensionnement des chaînes de conversions de puissance. Les chaînes de conversion de puissance relient les composants électrochimiques au réseau électrique. Dans le cas de la chaîne de conversion sans transformateur qui est ici envisagée, la présence d’un convertisseur DC-DC à haut rendement à fort ratio de conversion est rendue nécessaire de par la caractéristique basse tension fort courant des composants électrochimiques. Avec pour but principal l’optimisation du rendement, deux axes de recherche sont développés. Le premier axe développe un convertisseur multicellulaire innovant à haut rendement à fort ratio de conversion. Les résultats expérimentaux du convertisseur appelé « miroir » obtenus dans deux expérimentations ont démontré la supériorité de cette topologie en terme d’efficacité énergétique par rapport aux convertisseurs conventionnels. Le deuxième axe porte sur de nouveaux composants de puissance en nitrure de gallium (GaN) annoncés comme une rupture technologique. Un convertisseur buck multi-phases illustre les défis technologiques et scientifiques de cette technologie et montre le fort potentiel de ces composants. / Development of renewable energy seems inevitable to face the energy challenge of today and tomorrow. However, the power generation of promising renewable sources such as solar or wind power is intermittent and unpredictable due to the dependence of the these sources to the weather. In order to overcome the discontinuous nature of the electricity production and the mismatch between production and consumption, electrical energy storage is needed. In this context, hydrogen battery is one of the solutions. During periods of overproduction of renewable energy, an electrolyzer produces hydrogen gas by the electrolysis of water. When necessary, a fuel cell provides electricity from the stored gas. Coupled with renewable energy sources, the hydrogen battery produces carbon-free electricity, i.e. without any greenhouse gas emission. The major advantage of this technology is the decoupling between energy and power system. As long as the fuel cell is supplied with gas, it supplies electricity. Like so, the energy depends on the gas tanks and the system power depends on the characteristics of electrochemical components and the design of the power conversion chain. Power converters connect electrochemical components to the grid. In the case of the transformerless conversion system introduce here, a high efficiency high voltage gain DC-DC converter is required given the high-current low-voltage characteristic of electrochemical components. Since the main goal is to optimize the efficiency, two research approaches are developed. The first develops an innovating multicell converter with high efficiency at high voltage conversion ratio. The experimental results of the “mirror” converter obtained in two experiments have demonstrated the superiority of this topology in terms of energy efficiency compared to conventional converters. The second line of research focuses on new gallium nitride (GaN) transistors heralded as a disruptive technology. A multiphase buck converter illustrates the technological and scientific challenges of this technology and shows the potential of these transistors.