The scope of the present thesis is the development of a Computational Fluid Dynamics model to describe the multiphase flow inside a structured packing absorber for postcombustion carbon capture. The work focuses mainly on two flow characteristics: the interface tracking and the reactive mass transfer between the gas and the liquid. The interface tracking brings the possibility of studying the liquid maldistribution phenomenon, which strongly affects the mass transfer performance. The development of a user-defined function to account for the reactive mass transfer between phases constitutes the second major concept considered in this thesis. Numerical models found in the literature are divided into three scales due to the current computational capacity: small-, meso- and large-scale. Small-scale has usually dealt with interface tracking in 2D computational domains. Meso-scale has usually been considered to assess the dry pressure drop performance of the packing (considering only the gas phase). Large-scale studies the liquid distribution over the whole column assuming that the structured packing behaves as a porous medium. This thesis focuses on small- and meso-scale. The novelty of this work lies in expanding the capabilities of the aforementioned scales. At small-scale, the interfacial tracking is implemented in a 3D domain, instead of 2D. The user-defined function that describes the reactive mass transfer of CO2 into the aqueous MEA solution is also included to assess the influence of the liquid maldistribution on the mass transfer performance. At the meso-scale, the Volume of Fluid method for interface tracking is included (instead of only the gas phase) to describe flow characteristics such as the liquid hold-up, the interfacial area and the mass transfer. At the theoretical level, this model presents the particularity of including both a mass and a momentum source term in the conservation equations. A comprehensive mathematical development shows the influence of the mass source terms on the momentum equation.

Les recherches s’inscrivent dans une prospection qui étudie la viabilité de la valorisation du CO2 d’un incinérateur de déchets industriels. Plusieurs licences commerciales existent pour le captage du CO2 dans des gaz de combustion mais il n’existe pas de référence pour le traitement de fumées d’incinérateur de déchets. Les travaux évaluent, à l’aide d’une installation pilote, la viabilité du captage du CO2 en postcombustion par absorption/désorption avec un solvant à 30 % massique en monoéthanolamine (MEA). Tout d’abord, une synthèse bibliographique identifie les verrous technologiques. Puis, le fonctionnement de l’installation est détaillé. Ensuite, une étude paramétrique a évalué les performances de captage du CO2 et la consommation énergétique du pilote. Enfin, des expériences sur une période de 5 jours ont étudié la résistance chimique du solvant face des gaz de combustion. Les travaux de recherche ont permis une première validation du procédé pour un incinérateur de déchets. / This research is part of a survey designed to establish the viability of the CO2 recovery as a raw material from an industrial waste incinerator.. Several commercial licenses are available to capture CO2 in flue gas, but there are no references for incinerators. This work studies with a pilot the post-combustion CO2 capture from incinerator flue gas using absorption/desorption process with 30 %wt monoethanolamine (MEA). A literature review identifies the technology gaps. Then, the pilot setup was described. A parametric study has evaluated the pilot performance for CO2 capture and energy consumption. Finally, Long runs (5 days) have studied the solvent chemical stability in front of incinerator flue gas. The laboratory experiments show that CO2 capture form incinerator flue gas is possible.

Global carbon emissions are higher than ever before and in the last decade of 21st century, focus has shifted on reducing these emissions in various ways possible. Carbon capture, utilization and storage (CCUS) has been identified as one of the important ways to reduce carbon emissions and meet climate targets. For a long time, Sweden has promoted the use of biomass as fuel for heat and power generation which has enabled it to meet its climate targets earlier than projected. Now, major Swedish energy companies are looking into coupling exiting biomass fired heat and power plants with CCUS. This opens up the possibility of attaining negative emissions, also known as Bio Energy Carbon Capture and Storage (BECCS). With the right policy framework in place, BECCS can be a major boon and help Sweden attaining net zero carbon emissions. As a contribution in meeting net zero targets, this thesis is aimed to evaluate the installation of a carbon capture plant to abate flue gas emissions from District heating facility in Jordbro which is a ~70 MW (fuel) CHP plant running on biomass.  Among the available carbon capture technologies, Calcium oxide-based carbon capture has been expected to show great promise due to its lower environmental impacts and possibility to extract high quality energy when installed. Hence a concept system for integration calcium looping at Jordbro has been developed through the use of modeling tools like ASPEN. A techno economic assessment was needed to be performed to give conclusive results on the overall viability of the process. Further, key process indicators like energy penalty, plant footprint and cost of capture per tonne of CO2 were identified for making the final evaluation. Finally, through a strategic collaboration with SaltX, major process improvements were introduced and applied to the modeled process.  It was concluded that with the current average flowrates at Jordbro it was possible to capture 154,000 tonnes of CO2 annually. The required amount of energy input to the calciner is 48MW (7.29 MW/kg-CO2 captured) which is one of the major findings of this study. Even though a significant amount of heat is recovered, the main boiler is not capable of producing heat over 900 οC and additional biomass needs to be combusted, leading to an additional CO2 emission of about 125 000 tonnes annually. Considering an optimal integration, the energy penalties became 6.25 %.  However, the plant footprint increased substantially due to requirement for burning additional biomass in the regeneration reactor and addition of several auxiliary units that come along with calcium-based carbon capture. Further, the total capital investment for this project is 1,219 MSEK with reactor costs being most capital intensive. Assuming a plant life of 25 years, the cost of capture per tonne of CO2 (excluding the costs for carbon transport and storage) was evaluated at 988 SEK, which is 58% higher than the reference Mono-ethanol amine based chemical absorption case. The innovative improvements from SaltX substantially reduced the plant footprint but capture costs did not reduce since material transport costs proved to be the major bottleneck.  Upon comparison of this technology with the amine-based technology it was found that Calcium oxide-based carbon capture would need further research and improvements to be more viable than amine-based carbon capture. Integration of thermal energy storage and process intensification can be the possible paths for further improvement.

Stålindustrin är kraftigt energi och utsläppsintensiv och står för upp till cirka 7% av de globala 𝐶𝑂2-utsläppen. Den huvudsakliga utsläppskällan utgörs av masugnsprocessen där järnmalm reduceras till råjärn med hjälp av fossilt kol i den malmbaserade processvägen. Flera tidigare studier har visat att den mest effektiva metoden för att minska industrins utsläpp av 𝐶𝑂2 och därmed bidrag till klimatförändringar är att öka andelen skrot i kolfärskningsprocessen för att på så sätt minska behovet av råjärn.  Syftet med studien var att undersöka möjligheterna att minska stålindustrins utsläpp av 𝐶𝑂2 genom en ökad andel skrot i kolfärskningsprocessen. Rapporten delades upp i två delar, inledningsvis en litteraturstudie som ge en bild över vilka metoder som finns tillgängliga samt vilken potentiell effekt dessa har. Den andra delen baserades på analyser av produktionsdata från SSAB Oxelösund. Tillsammans med resultatet från litteraturstudien användes analyserna för att ta reda på hur mycket råstålets 𝐶𝑂2-avtryck skulle kunna minskas med användning av metoder relevanta för det specifika stålverkets förutsättningar, förbättringsområden och framtida planer.  Parametrarna som undersöktes utgjordes av effekt på skrotinsmältning samt övriga utmaningar och fördelar kopplat till industrins klimatpåverkan. Resultatet från litteraturstudien visade att det fanns ett flertal effektiva metoder för att öka skrotinsmältningskapaciteten i kolfärskningsprocessen och att dessa vid kombinerad användning har en addidativ effekt och har potential att höja skrotinsmältningen avsevärt. Effekten av dessa är dock till stor del beroende på utgångspunkt och produktionsspecifika förutsättningar och måste undersökas vidare genom exempelvis industriförsök.  Eftersom stålverket ställer om produktionen till 2026 kan inte några större investeringar för att minska utsläppen från den äldre produktionen anses vara motiverbar både gällande utsläpp av 𝐶𝑂2 och investeringskostnad. Analyserna av produktionsdata tillsammans med resultatet från litteraturstudierna visade att det fanns flera förbättringsområden och rimliga metoder för stålverket att öka sin skrotinsmältning med syfte att minska utsläppen av 𝐶𝑂2. Genom implementering av dessa metoder som skulle skrotinsmältningen kunna ökas med 2,3 % vilket skulle resultera i en relativ minskning av råstålets 𝐶𝑂2-avtryck med 2,8%.

<p>The electric arc furnace (EAF) is a critical steelmaking facility that melts the scrap by the heat produced from electrodes and burners. The migration to EAF steelmaking has accelerated in the steel industry over the past decade owing to the consistent growth of the scrap market and the goal of "green" steel production. The EAF production already hit a new high in 2018, contributing to 67% of total short tons of U.S. crude steel produced. The EAF steelmaking process involves dynamic complex multi-physics, in which electric arc plasma and coherent jets coexist resulting in an environment with local high temperature and velocity. Different heat transfer mechanisms are closely coupled and the phase change caused by melting and re-solidification is accompanied by in-bath chemical reactions and freeboard post-combustion, which further creates a complicated gas-liquid-solid three-phase system in the furnace. Therefore, not all conditions and phenomena within the EAF are well-understood. The traditional experimental approach to study the EAF is expensive, dangerous, and labor-intense. Most of the time, direct measurements and observations are impossible due to the high temperature within the furnace. To this fact, the numerical model has aroused great interest worldwide, which can help to gain fundamental insights and improve product quality and production efficiency, greatly benefiting the steel industry. However, due to the complexity of the entire EAF steelmaking process, the relevant computational fluid dynamics (CFD) modeling and investigations of the whole process have not been reported so far. </p> <p><br></p> <p>The present study was undertaken with the aim of developing the modeling methodologies and the corresponding comprehensive EAF CFD models to simulate the entire EAF steelmaking process. Two state-of-the-art comprehensive EAF CFD models have been established and validated for both the lab-scale direct current (DC) EAF and the industry-scale alternating current (AC) EAF, which were utilized to understand the physical principles, improve the furnace design, optimize the process, and perform the trouble-shootings.</p> <p><br></p> <p>For the lab-scale DC EAF, a direct-coupling methodology was developed for its comprehensive EAF CFD model which includes the solid steel melting model based on the enthalpy-porosity method and the electric arc model (for lab-scale DC arc) based on the Magneto Hydrodynamics (MHD) theory, so that the dynamic simulation of the steel ingot melting by DC arc in the lab-scale furnace can be achieved, which considered the continuous phase changing of solid steel, the ingot surface deformation, and the phase-to-phase interaction. Both stationary DC arc and the arc-solid steel interface heat transfer and force interaction were validated respectively against the experimental data in published literature. For the given lab-scale furnace, the DC arc behavioral characteristics with varying arc lengths generated by the moving electrode were analyzed, and the effects of both the initial arc length and the dynamic electrode movement on the steel ingot melting efficiency were revealed.</p> <p><br></p> <p>For the industry-scale AC EAF, an innovative integration methodology was proposed for its comprehensive EAF CFD model, which relies on the stage-by-stage approach to simulate the entire steelmaking process. Six simulators were developed for simulating sub-processes in the industry-scale AC EAF, and five models were developed for the above four simulators, including the scrap melting model, the electric arc model (for industry-scale AC arc), the coherent jet model, the oxidation model, and the slag foaming model, which can be partially integrated according to the mass, energy, and momentum balance. Specifically, the dual-cell approach and the stack approach were proposed for the scrap melting model to treat the scrap pile as the porous medium and simulate the scrap melting together with its dynamic collapse process. The statistical sampling method, the CFD-compatible Monte Carlo method, and the electrode regulation algorithm were proposed for the electric arc model to estimate the total AC arc power delivery, the arc radiative heat dissipation, and the instantaneous electrode movement. The energetic approach was proposed to determine the penetration of the top-blown jet in the molten bath based on the results from the coherent jet model. The source term approach was proposed in the oxidation model to simulate the in-bath decarburization process, where the oxidation of carbon, iron, and manganese as well as the effect of those exothermic reactions on bath temperature rising was considered. Moreover, corresponding experiments were performed in the industry-scale EAF to validate the proposed simulators. The quantitative investigations and analyses were conducted afterward to explore and understand the coherent jet performance, the AC arc heat dissipation, the burner preheating characteristics, the scrap melting behavior, the in-bath decarburization efficiency, and the freeboard post-combustion status.</p> <p><br></p>

The Paris Agreement has ambitious targets to limit the global warming below 1.5 °Cin the 21st century. This goal is reflected in the national climate targets, for example, Sweden aims to achieve net zero greenhouse gas emissions by 2045, and thereafter achieve negative emissions. One of the pivotal ways to achieve these goals is by applying the mature bioenergy with carbon capture and storage (BECCS) technology to large-scale industries that emit CO2. Around 6% of the global emissions arise from the pulp and paper industry making them one of the largest localized emitters of biogenic CO2. This makes them suitable for retrofitting BECCS technologies and post-combustion capture (PCC) is one among them. This study presents a techno-economic assessment of an absorption-based PCC unit in SCA Östrand pulp mill. Chemical absorption using MEA and chilled ammonia process (CAP) using NH3 as the solvent are considered in this study. For both the processes, mass and energy balances using Aspen HYSYS were done and validated against published data in literature. Heat integration by applying excess or waste heat from the mill is also considered in this work. CO2 capture from flue gas originating from various emission sources in the mill (recovery boiler, lime kiln and multi-fuel boiler) are considered in different combinations in the analysis. The main key performance indicator (KPI) evaluated in this work is the cost of CO2capture for all the different cases for both the MEA- and chilled NH3-based absorption processes. The minimum cost of CO2 capture for MEA-based absorption process was found to be in the range 37-41 €/tCO2 and for CAP, it was found to be in the range 73-81 €/tCO2. For MEA-based absorption process, the excess low pressure steam from the mill satisfies the steam demand in all the cases, except the one where CO2 is captured from all the three emission sources. For CAP, sufficient excess low pressure steam is present in the mill for all the capture cases due to a lower reboiler duty compared to MEA-based absorption process. An optimal process configuration and capture scenario for the existing design conditions in the mill are derived and justified. A sensitivity analysis was carried out to find the associated bottlenecks from the breakdown of the cost of CO2 capture for each process. The overall BECCS cost is also sensitive to CO2 transport &amp; storage costs. However, it is also clear that incentives for negative emissions will make BECCS an attractive solution for the pulp and paper industry.

Le présent manuscrit de thèse présente l'étude de différents phénomènes dans un convertisseur d?acier, grâce au développement de deux modèles distincts. Le premier modèle décrit la cavité produite à la surface libre du bain de métal par l'impact du jet d'oxygène supersonique. Il est basé sur le découpage du domaine de calcul en deux régions. Les effets de compressibilité du gaz sont pris en compte uniquement dans la région du jet où la vitesse est élevée, alors que partout ailleurs, le gaz est considéré comme incompressible. La méthode Volume Of Fluid (VOF) est utilisée pour suivre la déformation de la surface libre du bain. Les résultats de simulations sont présentés pour des systèmes bi- et triphasés et comparés à des données expérimentales obtenues dans diverses maquettes froides. L'influence sur la taille et la forme de la cavité de différents paramètres (parmi lesquels les conditions aux limites en sortie de la lance d'injection, le schéma d'advection de la méthode VOF et le modèle de turbulence) est étudiée. Le modèle est ensuite utilisé pour simuler l'interaction entre un jet supersonique d'oxygène et la surface libre d'un bain d'acier liquide dans un convertisseur de taille pilote. Le second modèle se focalise sur l'écoulement du gaz, le transfert de chaleur et la réaction de postcombustion dans la phase gazeuse au-dessus du bain de métal. Il utilise l'algorithme Simple Chemical Reaction Scheme pour décrire le transport des espèces chimiques, et prend en compte l'absorption d'oxygène dans le bain et les transferts thermiques par rayonnement. Les prédictions numériques sont en assez bon accord avec les mesures recueillies dans une expérience de laboratoire et dans un four à l'échelle pilote / The present thesis treats different phenomena taking place in a steelmaking converter through the development of two separate models. The first model describes the cavity produced at the free surface of the metal bath by the high speed impinging oxygen jet. It is based on a zonal approach, where gas compressibility effects are taken into account only in the high velocity jet region while elsewhere the gas is treated as incompressible. The Volume Of Fluid (VOF) method is employed to follow the deformation of the bath free surface. Calculations are presented for two- and three-phase systems and compared against experimental data obtained in various cold model experiments. The influence on the size and shape of the cavity of various parameters (including the jet inlet boundary conditions, the VOF advection scheme and the turbulence modelling) is studied. Next, the model is used to simulate the interaction of a supersonic oxygen jet with the surface of a liquid steel bath in a pilot-scale converter. The second model concentrates on fluid flow, heat transfer and the post-combustion reaction in the gas phase above the metal bath. It uses the Simple Chemical Reaction Scheme approach to describe the transport of the chemical species and takes into account the consumption of oxygen by the bath and thermal radiative transfer. The numerical predictions are in reasonable agreement with measurements collected in a laboratory experiment and in a pilot-scale furnace

Les explosions sphériques entraînent des perturbations importantes de l'interface entre les produits de détonation et l'air. Ces instabilités jouent un rôle dominant dans la détermination du volume de la "boule de feu". Un calcul sphérique unidimensionnel classique conduit un volume de sphère très inférieur à celui mesuré expérimentalement. De plus, des réactions de post-combustion peuvent avoir lieu dans la zone de mélange, libérant une énergie deux fois supérieur à celle de la détonation, déjà considérable. À une échelle suffisamment petite, on distingue les longueurs d'onde des instabilités et les tailles de jets, mais à une échelle plus globale, on observe une couche de mélange où la forme précise de l'interface n'est plus visible. Les deux phases (produits détonation et de l'air) s'interpénètrent, et par conséquent, l'interface devient une zone de mélange. Pour calculer correctement chacune des instabilités, une approche multidimensionnelle semble s'imposer. Cependant, un grand nombre de cellules est nécessaire pour calculer une structure unique de la zone de mélange. En outre, pour une instabilité isolé, le maillage entraînent des instabilités parasites qui dépendent fortement de la viscosité numérique du schéma utilisé. L'approche multidimensionnelle, basée sur la simulation numérique directe, présente donc des difficultés. En réalité, nous ne voulons pas calculer la forme exacte des instabilités de l'interface, mais seulement l'épaisseur de la couche de mélange et les champs de concentrations des phases dans celle-ci. Ainsi, une approche unidimensionnelle peut être suffisante. L'objectif est d'écrire un modèle unidimensionnel décrivant le phénomène d'interpénétration. Trois modèles ont alors été construits à partir du modèle diphasique de l'Baer et Nunziato (1986). Nous obtenons des résultats intéressants avec les deux premiers sur des problématiques d'épaississement d'interface, mais ils sont insuffisants. Le dernier modèle, qui dérive des deux premiers, a été validé sur des tests d'explosions sphériques.

The effective mass transfer area (a [subscript e]), liquid film mass transfer coefficient (k [subscript L]), and gas film mass transfer coefficient (k [subscript G]) of eleven structured packings and three random packings were measured consistently in a 0.428 m packed column. Absorption of CO₂ with 0.1 gmol/L NaOH with 3.05 m packing was used to measure a [subscript e], while air stripping of toluene from water with 1.83 m packing was used to measure k [subscript L], and absorption of SO₂ with 0.1 gmol/L NaOH with 0.51 m packing was used to measure k [subscript G]. The experiments were conducted with liquid load changing from 2.5 to 75 m³/(m²*h) and gas flow rate from 0.6 to 2.3 m/s. Packings with surface area from 125 to 500 m²/m³ and corrugation angle from 45 to 70 degree were tested to explore the effect of packing geometries on mass transfer. The effective area increases with packing surface area and liquid flow rate, and is independent of gas velocity. The packing corrugation angle has an insignificant effect on mass transfer area. The ratio of effective area to surface area decreases as surface area increases due to the limit of packing wettability. A correlation has been developed to predict the mass transfer area with an average deviation of 11%. [Mathematical equation]. The liquid film mass transfer coefficient is only a function of liquid velocity with a power of 0.74, while the gas film mass transfer coefficient is only a function of gas velocity with a power of 0.58. Both k [subscript L] and k [subscript G] increase with packing surface area, and decrease with corrugation angle. A new concept, Mixing Point Density, was introduced to account for effect of the packing geometry on k[subscript L] and k [subscript G]. Mixing Point Density represents the frequency at which liquid film is refreshed and gas is mixed. The mixing point density can be calculated by either packing characteristic length or by surface area and corrugation angle: [mathematical equation]. The dimensionless k [subscript L] and k [subscript G] models can then be developed based on the effects of liquid/gas velocity, mixing point density, packing surface area: [mathematical equation] [mathematical equation]. Mi is the dimensionless form of Mixing Point Density (M), which is M divided by a [subscript P]³. Because Mi is only a function of corrugation angle (θ), it is a convenient transformation to represent the effect of θ on mass transfer parameters. An economic analysis of the absorber was conducted for a 250 MW coal-fired power plant. The optimum operating condition is between 50 to 80 % of flooding, and the optimum design is to use packing with 200 to 250 m²/m³ surface area and high corrugation angle (60 to 70 degree). The minimum total cost ranges from $4.04 to $5.83 per tonne CO₂ removed with 8 m PZ.

Pour faire face à l'augmentation des émissions de CO2 dans l'atmosphère à cause de la production électrique dans des centrales à charbon, le captage en post-combustion au moyen d'un procédé VSA est une solution envisageable. Les adsorbants utilisés dans notre étude sont la TEPA imprégnée sur SiO2, les oxydes de terre rare et le MOF (Metal Organic Frameworks) SIM-1. Pour chaque adsorbant, une étude du perçage puis de la régénération a été effectuée à partir d'une alimentation composée de 15%vol de CO2 et de N2. De ces essais, les conditions opératoires des cycles VSA ont été établies (durées des phases courtes, pas de circulation de purge). En cycle, les performances sont comparées à celle du procédé d'absorption avec la monoéthénolamine. La pureté du désorbat varie de 89,2%vol à 97,2%vol selon les adsorbants et les conditions opératoires. Elle est inférieure à celle du procédé d'absorption (99%vol) mais est correcte pour le transport et le stockage. Le taux de captage évolue de 87,2% à 94,9% (absorption : 98%). La consommation énergétique est inférieure à celle du procédé avec la MEA (de 1,53 à 3,45 MJ.kgCO2 1 pour notre procédé et 3,7 MJ.kgCO2¬1 pour l'absorption) Enfin la productivité est du même ordre de grandeur que celle d'autres procédés VSA de la littérature. Avec le modèle numérique, une étude locale de l'adsorbeur a été menée. Puis grâce à une étude paramétrique, des conditions optimales en cycle ont été déterminées. Les résultats obtenus ont permis de mettre en évidence des performances comparables avec les autres procédés VSA de la littérature. De plus, notre procédé est beaucoup moins énergivore que le procédé d'absorption mais la pureté du désorbat et le taux de captage en CO2 restent inférieurs.