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1
Ramkumar, Shwetha. "CALCIUM LOOPING PROCESSES FOR CARBON CAPTURE." The Ohio State University, 2010. http://rave.ohiolink.edu/etdc/view?acc_num=osu1274882053.
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Phalak, Nihar. "Calcium Looping Processes for Pre- and Post-Combustion Carbon Dioxide Capture Applications." The Ohio State University, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=osu1366802833.
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Griffiths, Owen Glyn. "Environmental life cycle assessment of engineered nanomaterials in carbon capture and utilisation processes." Thesis, University of Bath, 2014. https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.629663.
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CO2 is a waste product from a number of human activities such as fossil fuel power generation, industrial manufacturing processes, and transport. The rising concentration of CO2 in the atmosphere is heating the planet’s surface via the well-established greenhouse effect; a mechanism for many irreversible climate change impacts. Coupled to this is the ever-increasing global pressure over the availability and access to fossil fuel reserves; the foundations of modern society. In recognition of this CO2 is gaining renewed interest as a carbon feedstock, a changing of attitude viewing it as an asset rather than waste. Carbon capture and utilisation (CCU) technologies are attempting to make use of it. However, little quantitative assessment work has been done to assessand verify such potentials. This thesis applies the principles and framework of the life cycle assessment (LCA) - environmental management tool to early stage CO2 utilisation laboratory processes. All processes employ engineered nanomaterials (ENM) to perform this function, a material class leading the way in the challenges of efficient and feasible CO2 chemistry. The LCA contribution in this thesis acts as a measuring and a guiding tool for technology developers, in the first instance to document the cradle-to-gate impacts of a number of formed ENMs. Appreciating the net environmental benefits of ENM uptake within society has yet to be wholly established, and the unavailability of data is recognised as a major factor. The work of this thesis will thus contribute to knowledge gaps, and be informative to wider community seeking to quantify technical performance benefits of ENMs in the context of net life cycle impact burdens. Finally the actual CCU processes are assessed, initially within the confines of the laboratory but further expanded for consideration at more industrially relevant scales. The potential for sound CCU performance were found achievable under best case conditions, with net GHG impact reductions over the life cycle, and the potential for lower impact carbon products, even carbon negative. However other environmental impacts such as ozone depletion, toxic emissions and the consumption of precious metalores are impacts that require consideration in the use of such technologies.
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HARO, HERBERTH ARTURO VASQUEZ. "NUMERICAL INVESTIGATION OF AMINE BASED ABSORPTION PROCESSES FOR CARBON DIOXIDE CAPTURE IN CCS PROJECTS." PONTIFÍCIA UNIVERSIDADE CATÓLICA DO RIO DE JANEIRO, 2009. http://www.maxwell.vrac.puc-rio.br/Busca_etds.php?strSecao=resultado&nrSeq=15511@1.
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COORDENAÇÃO DE APERFEIÇOAMENTO DO PESSOAL DE ENSINO SUPERIOR<br>Absorção é um processo no qual os componentes de uma corrente
gasosa são separados através do uso de um solvente líquido. O
processo pode ser simplesmente físico ou seguido por uma reação
química. Na indústria, um processo de absorção importante é a remoção
de dióxido de carbono (CO2), usando uma solução aquosa de
monoethanolamina (MEA), dos gases de combustão expelidos pelas
plantas alimentadas por combustíveis fosseis tais como: as usinas de
geração de energia, a indústria farmacêutica, a indústria de petróleo, etc.
Os projetos desenvolvidos por grandes corporações usualmente são
cercados de sigilo, e as companhias evitam a divulgação de suas
soluções tecnológicas. Além disso, no Brasil pouco tem-se publicado a
respeito. Neste trabalho, apresenta-se um modelo simples que simula a
absorção de CO2 em solução aquosa de MEA. O modelo envolve as
equações de conservação de massa, quantidade de movimento e
energia, podendo predizer o comportamento geral do processo de
absorção. Os resultados das simulações da absorção de CO2 em
contracorrente com uma coluna de filme líquido foram comparados com
dados experimentais disponíveis apresentando uma boa concordância.<br>Absorption is a process where the components of a gaseous
stream are separated through the use of a liquid solvent. The process
may be simply physical or be followed by a chemical reaction. In industry,
one of the most important absorption processes is the removal of carbon
dioxide (CO2), by using an aqueous solution of monoethanolamine
(MEA), from flue gases exhausted by fossil-fuel-fired power plants, the
pharmaceutical industry, the petroleum industry, etc. The projects
developed by large companies usually are surrounded by secrecy and the
companies avoid dissemination of their technological solutions. In
addition, there is almost nothing published in Brazil about this subject. In
this work, we present a simple model that simulates the absorption of
CO2 by a MEA based aqueous solution. The model involves the
equations for the conservation of mass, momentum, and energy, and may
predict the general behavior of the absorption process. Results for the
simulation of the absorption of CO2 in a countercurrent liquid film
contactor were compared with available experimental data, presenting
good agreement.
5
Bocciardo, Davide. "Optimisation and integration of membrane processes in coal-fired power plants with carbon capture and storage." Thesis, University of Edinburgh, 2015. http://hdl.handle.net/1842/10560.
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This thesis investigates membrane gas separation and its application to post-combustion carbon capture from coal-fired power plants as alternative to the conventional amine absorption technology. The attention is initially focused on membrane module modelling, with the aim of obtaining more detailed predictions of the behaviour of the separation though spiral-wound and hollow-fibre modules. Both one- and bi-dimensional models are implemented, compared and tested for different separations. Module geometry is investigated as well as the effect on the performances due to possible fabrication defects. A key part of the work involves the integration of the customised models into UniSim® Design, the Honeywell process simulator. Thanks to the developed interface, multi-stage process designs are developed, compared with the available literature and linked to a rigorous economic analysis. In particular, a long-term indicator such as the Levelised Cost Of Electricity (LCOE) is evaluated and parametric analyses are conducted with respect to both material and process parameters.
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Di, Biase Emanuela. "Systematic development of predictive molecular models of high surface area activated carbons for the simulation of multi-component adsorption processes related to carbon capture." Thesis, University of Edinburgh, 2015. http://hdl.handle.net/1842/16155.
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Adsorption in porous materials is a promising technology for CO2 capture and storage. Particularly important applications are adsorption separation of streams associated with the fossil fuel power plants operation, as well as natural gas sweetening. High surface area activated carbons are a promising family of materials for these applications, especially in the high pressure regimes. As the streams under consideration are generally multi-component mixtures, development and optimization of adsorption processes for their separation would substantially benefit from predictive simulation models. In this project we combine experimental data and molecular simulations to systematically develop a model for a high surface area carbon material, taking activated carbon Maxsorb MSC-30 as a reference. Our study starts from the application of the well-established slit pore model, and then evolves through the development of a more realistic model, based on a random packing of small graphitic fragments. In the construction of the model, we introduce a number of constraints, such as the value of the accessible surface area, concentration of the surface groups and pore volume, to bring the properties of the model structure close to the reference porous material. Once a plausible model is developed, its properties are further tuned through comparison between simulated and experimental results for carbon dioxide and methane. The model is then validated by predictions for the same species at different conditions and by prediction of other species involved in the carbon capture processes. The model is applied to simulate the separations involved in pre and post combustion capture processes and sweetening of sour natural gas, using realistic conditions and compositions for the multicomponent mixtures. Finally, it is used to explore the effect of water in pre and post combustion separations.
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Garcia-Gutierrez, Pelayo. "Carbon Capture and Utilisation processes : a techno-economic assessment of synthetic fuel production from CO2." Thesis, University of Sheffield, 2016. http://etheses.whiterose.ac.uk/14369/.
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Carbon Capture and Utilisation (CCU) is seen globally as one of the available technologies that can contribute to avoiding the effects of global warming while securing energy supply by utilising CO2 as a carbon source for chemical and fuel production. This thesis has measured the technical and economic performance of seven Carbon Capture and Utilisation (CCU) process designs (Base Case Models) based on best available technology. This was the first attempt to compare different routes of similar Technology Readiness Level to manufacture a liquid fuel from CO2. In addition, this thesis also examines the techno-economic feasibility of selective CO2 capture processes from biogas streams using ionic liquids as physical absorbents to assess the potential improvements that this developing technology could have on process performance. The selected Base Case Models were modelled using the process simulation software Aspen Plus to determine mass and energy balances. In addition, an economic assessment was developed using Aspen Plus Economic Analyzer (APEA) and MS Excel to determine capital, operating and production costs. The results revealed that the synthetic route based on CO2 capture and steam methane reforming was the most promising CO2-to-fuels route since it was able to achieve the highest overall plant energy efficiency (17.9%) and the lowest fuel production costs (£95.46 per GJ [LHV]); however this process cannot currently compete commercially with conventional fossil fuels. Further research in the specific areas suggested in this work is encouraged in order to bring fuel production costs down. It was also demonstrated that the evaluated ionic liquids cannot compete with MEA in terms of bio-methane production costs; however, the simulation methodology developed in this study can be used as a basis for further work in the area since it allows consideration of ionic liquids made of any combination of cation and anion as well as different gas streams.
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Zaragoza, Martín Francisco Javier. "Development and fluid dynamic evaluation of novel circulating fluidised bed elements for low-temperature adsorption based carbon capture processes." Thesis, University of Edinburgh, 2017. http://hdl.handle.net/1842/25482.
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A methodology for the thermodynamic-kinetic evaluation of circulating systems as TSA carbon capture processes is developed and used in the assessment of a novel CFB configuration against a benchmark (co-current riser). The novel CFB features a counter-current adsorber, a counter-current regenerator and a riser, the latter element playing a double role of solids conveyer and co-current adsorber. The advantages sought by using a counter-current adsorber are not only the more efficient gas-solid contact mode with respect co-current, but also a low pressure drop derived from operation at lower gas velocities and hydrostatic head partially supported on the contactor internals. Knowledge of the adsorption equilibrium alone is sufficient to realise the much higher sorbent circulation rates required by co-current configurations –compared to counter-current– to meet the stringent carbon capture specifications of 90% recovery and 95% purity. Higher solids circulation rates imply higher energy requirements for regeneration, and therefore research and development of co-current gas-solid contactors cannot be justified in terms of searching for energy-efficient post-combustion carbon capture processes. Parallel experimental investigation in the operation and fluid dynamics of cold model CFB rigs is carried out with the purposes of: 1) providing information that may impact the process performance and can be fed into the mathematical model used in the theoretical assessment for more realistic evaluation, and 2) determine gas and solids residence time distributions (RTDs), which are used for the estimation of axial dispersion and comparison with published results in similar systems. Gas RTD data is generated using a tracer pulse injection-detection technique, whereas RTD for the solid phase is studied using positron emission particle tracking (PEPT). The PEPT technique proved to be adequate for the identification of flow regimes in the novel design of the counter-current adsorber, featuring inclined orifice trays. At low gas velocities the particles flow straight down through the tray holes, whereas at higher velocities the particles flow down in zig-zag, increasing the residence time of the particles and reducing the particle axial dispersion, both beneficial in terms of separation efficiency.
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Ramirez, Santos Álvaro Andrés. "Application of membrane gas separation processes to CO2 and H2 recovery from steelmaking gases for carbon capture and use." Thesis, Université de Lorraine, 2017. http://www.theses.fr/2017LORR0272.
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L’acier est produit aujourd’hui principalement en faisant appel à une technologie basée sur le procédé haut fourneau-convertisseur à l’oxygène, conduisant à trois types d’émissions principales: le gaz de haut fourneau (BFG), le gaz de cokerie (COG), et le gaz de convertisseur (BOFG). Dans le cadre du projet VALORCO, une analyse des possibilités de réduction des émissions carbonées, associée à une valorisation des émissions de la sidérurgie, a été réalisée. Une des voies étudiées est la production de composés d’intérêt industriel tel que méthanol, pouvant être produit par transformation chimique du CO et/ou CO2 contenus dans les émissions, associé à de l’hydrogène. L’objectif principal de ce travail de thèse consiste à évaluer les possibilités offertes par le procédé de perméation gazeuse, appliqué à la récupération sélective de ces composés dans les 3 types d’émissions. Dans un premier temps, un état de l’art des différents projets dédiés à la capture (CCS) et à la valorisation (CCU) des émissions dans l’industrie de l’acier est présenté, avec une attention particulière aux différentes technologies de séparation des gaz. Des mesures expérimentales de sélectivité et de perméance pour différentes conditions de température et de pression, réalisées sur banc dédié avec deux matériaux membranaires disponibles commercialement et sélectif à l’hydrogène (vitreux) et au CO2 (élastomère) ont permis une étude paramétrique systématique par simulation des performances de séparation du procédé appliqué au BFG, COG et BOFG. Une comparaison des procédés basés sur un seul ou plusieurs étages de perméation, y compris avec des boucles de recirculation, a ensuite été entreprise dans un environnement de type Process System Engineering (PSE, logiciel Aspen Plus). L’influence des paramètres opératoires (rapport de pression, température, taux de prélèvement) sur les performances de séparation a été réalisée, conduisant à une cartographie des compositions atteignables. La consommation énergétique et la surface membranaire nécessaires pour chaque configuration permettent au final une optimisation techno-économique du procédé, sur la base d’un modèle économique intégré aux conditions de simulation<br>Steel is produced today mainly in a blast furnace-oxygen converter process, leading to three main types of emissions: blast furnace gas (BFG), coke oven gas (COG), and converter gas (BOFG). In the framework of the VALORCO project, an analysis of the possibilities for reducing carbon emissions, combined with the valorization of emissions from the steel industry, was carried out. One of the routes studied is the production of compounds of industrial interest such as methanol, which can be produced by chemical transformation of the CO and / or CO2 contained in the emissions associated with hydrogen. The main objective of this thesis work is to evaluate the possibilities offered by the gas permeation process applied to the selective recovery of these compounds in the three types of emissions. Initially, a state of the art of the various projects dedicated to the capture (CCS) and the valorization (CCU) of the emissions in the steel industry is presented, with particular attention to the different gas separation technologies. Experimental measurements of selectivity and permeance for different temperature and pressure conditions, carried out on a dedicated bench with two commercially available membrane materials, one selective to hydrogen (glassy) and one to CO2 (rubbery), allowed a systematic parametric study by simulation of the separation performance of the process applied to the BFG, COG and BOFG. A comparison of the processes based on one or more permeation stages, including recirculation loops, was then undertaken in a Process System Engineering (PSE) environment (Aspen Plus software). The influence of the operating parameters (pressure ratio, temperature, stage cut) on the separation performance was evaluated, leading to a mapping of attainable compositions. The energy consumption and the membrane surface required for each configuration allow a techno-economic optimization of the process, on the basis of an economic model integrated to the simulation conditions
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Haider, Syed Kumail. "Oxygen carrier and reactor development for chemical looping processes and enhanced CO2 recovery." Thesis, Cranfield University, 2016. http://dspace.lib.cranfield.ac.uk/handle/1826/10014.
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This thesis’s main focus is a CO2 capture technology known as chemical looping combustion (CLC). The technology is a novel form of combustion and fuel processing that can be applied to gas, solid and liquid fuels. By using two interconnected fluidised-bed reactors, with a bed material capable of transferring oxygen from air to the fuel, a stream of almost pure CO2 can be produced. This stream is undiluted with nitrogen and is produced without any direct process efficiency loss from the overall combustion process. The heart of the process is the oxygen carrier bed material, which transfers oxygen from an air to fuel reactor for the conversion of the fuel. Oxygen carrier materials and their production should be of low relative cost for use in large-scale systems. The first part of this research centres on development and investigative studies conducted to assess the use of low-cost materials as oxygen carriers and as supports. Mixed-oxide oxygen carriers of modified manganese ore and iron ore were produced by impregnation. While copper (II) oxide supported on alumina cement and CaO have been produced by pelletisation. These oxygen carriers were investigated for their ability to convert gaseous fuels in a lab-scale fluidised bed, and characterised for their mechanical and chemical suitability in the CLC process. The modified ores and pelletised copper-based oxygen carriers’ mechanical properties were enhanced by their production methods and in the case of the modified iron ore, significant oxygen uncoupling was observed. The copper-based oxygen carriers particularly those containing alumina cement showed high conversion rates of gaseous fuels and improved mechanical stability. The second part of this research thesis focuses on the design philosophy, commissioning and operation of a dual-fast bed chemical looping pilot reactor. Based on the operational experience, recommendations for modifications to the CLC system are discussed. In support, a parallel hydrodynamic investigation has been conducted to validate control and operational strategies for the newlydesigned reactor system. It was determined that the two fast bed risers share similar density and pressure profiles. Stable global circulation rate is flexible and could be maintained despite being pneumatically controlled. Reactor-reactor leakage via the loop-seals is sensitive to loop seal bed-height, and inlet fluid velocity but can be maintained as such to ensure no leakage is encountered.
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Chung, Elena Yin-Yin. "Investigation of Chemical Looping Oxygen Carriers and Processes for Hydrocarbon Oxidation and Selective Alkane Oxidation to Chemicals." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1469182957.
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Flack, Kyle M. "Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents." Diss., Georgia Institute of Technology, 2012. http://hdl.handle.net/1853/44802.
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Green chemistry principles have been applied to the enhancement of two industrial chemistry problems. An industrially used reaction to form alcohols from aldehydes and ketones, the Meerwein-Ponndorf-Verley reduction, was improved by introducing a new catalyst Al(OtBu)₃. Due to the lower state of aggregation of this catalyst versus the conventional Al(OiPr)₃ catalyst, reduction rates were found to be faster in both pure iPrOH and mixed solvent systems for three model compounds: benzaldehyde, acetophenone, and a complex, chiral ketone, (S)-CMK. This allowed for the successful implementation of two important milestones; lowering the amount of catalyst needed necessary to complete the reactions (an economic benefit and lower waste) and the conversion from traditional batch reactions to continuous flow (a processing benefit) whereby reactions can be scaled-out rather than scaled-up. Another industrially important field of research that was focused on was CO₂ capture. High energy demands from current CO₂ capture methods such as aqueous amine solvents, specifically from coal-fired power plant flue gas, led to the development of non-aqueous reversible ionic liquids based on silylated amines. Structural modifications of the substitution around the silicon atom, the length of the alkyl chain bonding the silicon and amine, branching along the alkyl backbone, and investigating secondary and primary amines within this class of silylated amines were completed. These amines were reacted with CO₂ and the CO₂ capacity, the ionic liquid viscosity, reversal temperature and reaction enthalpy were all considered as a function of structure. In all cases the capacity was found to be not only greater than that of monethanolamine, an industrial standard, but higher than theoretical predictions through the formation of carbamic acid. Viscosity, reversal temperature, and reaction enthalpy were all found to be tunable through structure. These modifications gave significant insight into the necessary direction for optimization of these solvents as energy-efficient replacements of current CO₂ capture technology.
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Villar, I. Comajoan Laia. "Simulation of stripper modifications for bioenergy carbon capture by absorption." Thesis, KTH, Kemiteknik, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-299891.
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Att koldioxidutsläppen neutraliseras är avgörande för att begränsa klimatförändringarna. Bioenergi i kombination med separation och lagring av koldioxid (BECCS) är en Teknik som kan generera negativa utsläpp. Det största hindret för dess storskaliga genomförande är de höga energikraven för processen. Detta projekt syftar till att kvantifiera energistraffen för lean solvent flash och modifikationer för multitrycksstrippning för att förbättra prestandan av koldioxidavskiljning (CC) i en kraftvärmeverksanläggning för förbränning av biomassa. En jämviktsmodell utvecklades och validerades för att simulera en fullskalig CC genom kemisk absorption i Aspen Plus med kaliumkarbonat som lösningsmedel. Båda layoutändringarna resulterar i energipåföljder på 18-21 % för en kraftvärmeverk, medan energistraffet för baslinjeprocessen är 5 %. För ett kraftverk går straffen från 32 till 62 %. Detta visar hur en förbättring av processen kan minska kostnaderna för CCS, särskilt om värme anses vara en värdefull produkt. CCS i kraftvärmeverk har en mycket lägre energipåverkan än i kraftverk där värme inte återvinns.<br>Bio-energy with carbon capture and storage (BECCS) is a technology that can generate negative emissions. Hence it is recognized as a solution for becoming carbon neutral, which is essential for climate change mitigation. The main obstacle for its large scale implementation is the high energy requirements of the process. This thesis aims at quantifying the energy penalties for lean solvent flash and multi-pressure stripper layout modifications to improve the performance of carbon capture (CC) by means of absorption with a liquid solvent in a biomass-fired CHP plant. The work focuses on K2CO3 based solvents operated in a mixed temperature swing/pressure swing cycle witch is deemed advantageous for heat recovery. An equilibrium model was developed and validated to simulate a full-scale CC by chemical absorption in Aspen Plus using potassium carbonate as solvent. Both layout modifications result in energy penalties of 18-21 % for a CHP plant, while the energy penalty for the baseline process is 28 %. For a power plant, the penalties go from 32 % to 62 % for the lean solvent flash and the multi-pressure stripper respectively. This shows how improving the process can reduce the costs of CCS, especially if heat is considered a valuable product. CCS in CHP plants has a much lower energy impact than in power plants where heat is not recovered.
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Kritzinger, Liaan Rudolf. "Establishing a pilot plant facility for post combustion carbon dioxide capture studies." Thesis, Stellenbosch : Stellenbosch University, 2013. http://hdl.handle.net/10019.1/80143.
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Thesis (MScEng)--Stellenbosch University, 2013.<br>ENGLISH ABSTRACT: Carbon dioxide (CO2) is seen as one of the main contributors to global warming. The use of fossil fuels for power production leads to large quantities of carbon dioxide being released into the atmosphere. The released CO2 can, however, be captured by retrofitting capture units downstream from the power plant called Post Combustion Carbon Dioxide Capturing.
Post combustion CO2 capture can involve the reactive absorption of CO2 from the power plant flue gas steam. Reactive solvents, such as monoethanolamine (MEA), are used for capturing the CO2 and the solvent is regenerated in a desorber unit where the addition of heat drives the reverse reaction, releasing the captured CO2. However, the large energy requirement for solvent regeneration reduces the viability of employing CO2 capture on an industrial scale.
This study focused on establishing a facility for CO2 capture studies – the main aim being the construction and validation of the results produced by the pilot plant facility. A secondary aim of this study was developing an Aspen Plus® Simulation method that would simplify simulating the complex CO2 capture process. Results from the simulation were to be compared to that of the pilot plant experiments.
A pilot plant facility with a closed gas system, allowing gas recycling from both the absorber and the stripping columns, was set up. The absorber column (internal diameter = 0.2 m) was set up to allow one to obtain information regarding gas- and liquid temperatures and compositions at various column heights. Online gas analysers are used for analysing the gas composition at various locations in the absorber column.
The pilot plant was initially commissioned with 20 weight % MEA in aqueous solution; however the main validation experiments were conducted with 30 weight % MEA in aqueous solution. 30 weight % MEA (aq) is generally used as the reference solvent for pilot plant studies. Pilot plant results with regards to the carbon dioxide concentration profiles for the absorber column as well as the regeneration energy requirement and capture rates compared well to literature data.
The Aspen Plus® simulation was also set up and validated using published pilot plant data. The comparison of the pilot plant results from this study, to the results from the Aspen Plus® Simulation, showed good agreement between the two. The Aspen Plus® Simulation could further be used to validate pilot plant data that has been gathered outside the range of reported CO2 capture efficiencies.
The Aspen Plus®model was evaluated at liquid-to-gas ratios of 1.7 and regeneration energies matching the pilot plant results. It was found that the model under predicts the capture efficiency of CO2 with an average of 4.0%. The model was corrected for this error at liquid-to-gas ratios of 2 and the fit of the model to pilot plant results improved considerably (R2-value = 0.965).
Pilot plant repeatability was investigated with both 20 weight %- and 30 weight % MEA in aqueous solution. Temperature- and gas concentration profiles from the absorber column showed good repeatability. The maximum deviation of the regeneration energy and the capture efficiency from the calculation means were ±0.72% and ±1.40% respectively.
The aims of this study have been met by establishing, and validating the results of a pilot plant facility for carbon dioxide capture studies. It has been shown that the pilot plant produces repeatable results. Results from the Aspen Plus® Simulation were validated and also match results from the established pilot plant setup. The simulation may prove to provide valuable information regarding the optimal operating conditions for the pilot plant and may aid in performing a full parametric study on the CO2 capture process.<br>AFRIKAANSE OPSOMMING: Koolstofdioksied (CO2) word geklassifiseer as een van die bekendste kweekhuisgasse wat ʼn groot bydra lewer tot aardverwarming. Die gebruik van fossielbrandstowwe om na die energiebehoeftes van die mens om te sien lei daartoe dat groot hoeveelhede koolstofdioksied, hoofsaaklik vanaf kragstasies, vrygestel word in die atmosfeer. Daar is verskeie maniere hoe die CO2 uit die uitlaatgas van kragstasies verwyder kan word – die vernaamste hiervan is bekend as die Na-verbranding opvangs metode.
Die opvangs van CO2 na verbranding van fossielbrandstowwe vir kragproduksie kan vermag word deur van reaktiewe absorpsie tegnieke gebruik te maak. Mono-etanol-amien (MEA) kan vir hierdie doeleindes aangewend word deur dit, in ʼn absorpsiekolom, in kontak te bring met die CO2. Die gereageerde oplosmiddel word geregenereer deur die oplosmiddel te verhit in ʼn stropingskolom. ʼn Bykans suiwer CO2 stroom word vrygestel. Die implementering van hierdie opvangtegniek op industriële skaal lei egter tot groot energieverliese vir die kragstasies. Die hoofrede hiervoor is die hoeveelheid energie wat benodig word om die oplosmiddel te regenereer vir hergebruik.
Die hoofdoel van hierdie studie was gemik op die oprigting en inwerkstelling van 'n navorsingsfasiliteit vir studies aangaande die na-verbranding opvangs van CO2. Dit het behels die ontwerp, konstruksie en stawing van gelewerde resultate met resultate in die literatuur. 'n Sekondêre doel van hierdie studie was die metode-ontwikkeling vir die opstel van 'n Aspen Plus® Model wat die simulasie van die CO2 opvangsproses met ʼn reaktiewe oplosmiddel, MEA, vereenvoudig. Gesimuleerde resultate is vergelyk met resultate uit die literatuur.
Die toetsaanleg, met 'n geslote gas stelsel, maak voorsiening vir die hersirkulering van gas wat vir eksperimentele doeleindes gebruik word. Die absorpsie kolom (interne diameter van 0,2 m) is opgestel sodat informasie aangaande die gas- en vloeistof temperature, sowel as gas- en vloeistof komposisies vanaf verskillende kolomhoogtes, bekom kan word. ʼn Aanlyn CO2 analiseerder word gebruik om vir CO2 in die prosesgas te analiseer.
Die toetsaanleg is aanvanklik in bedryf gestel met ʼn 20 massa % MEA in waterige oplossing; die hoof eksperimente is egter uitgevoer deur van 30 massa % MEA in waterige oplossing gebruik te maak. Die laasgenoemde oplosmiddel word algemeen gebruik in die CO2 opvangs verwante navorsingsveld. Die resultate van die toetsaanleg, vergelyk goed met resultate in die literatuur.
Die gesimuleerde Aspen Plus® resultate is ook vergelyk met resultate in die literatuur en die gevolgtrekking is gemaak dat die simulasie gebruik kan word om redelike akkurate voorspellings van die werklike prosesresultate te gee. Die simulasie is verder ook gebruik om resultate, verkry vanaf die opgerigte toetsaanleg, te verifieer en ʼn goeie ooreenstemming tussen die gesimuleerde en die eksperimentele resultate is waargeneem. ʼn Verder gevolgtrekking aangaan die Aspen Plus® simulasie metode was dat dit in die toekoms ʼn groot doel kan dien in die optimeringsproses van toetsaanlegte waar navorsing aangaande die na-verbranding opvang van CO2 gedoen word.
Die Aspen Plus® model is geëvalueer by ‘n vloeistof-tot-gas-verhouding van 1,7 en ooreenstemmende toetsaanleg resultate, aangaande die hoeveelheid energie wat ingesit is vir die regenerasie van die oplosmiddel. Die onakkuraathede in die model, met betrekking tot die voorspelling van die hoeveelheid CO2 wat vasgevang sal word, is hierdeur bepaal en die model is daarvoor aangepas. Resultate van die verbeterde model vergelyk baie goed met die toetsaanleg resultate – ʼn R2-waarde van 0.965.
Die herhaalbaarheid van die toetsaanleg resultate is ondersoek en ʼn goeie herhaalbaarheid van die temperatuur- en CO2 konsentrasieprofiele is verkry. Die toetsaanleg dui ook goeie herhaalbaarheid met betrekking tot die effektiwiteit waarmee die CO2 uit ʼn gasstroom verwyder word (± 1,40%), sowel as die hoeveelheid energie wat benodig word vir regenerering van die oplosmiddel (± 0,72%).
Die doelwitte van hierdie studie is bereik deur die oprigting en verifiëring van resultate gelewer deur 'n toetsaanleg vir studies aangaande die na-verbrandingsopvang van CO2. Die herhaalbaarheid van toetaanleg resultate is bewys. Resultate van die Aspen Plus® simulasie stem ooreen met resultate in die literatuur sowel as resultate van die toetsaanleg wat opgerig is in hierdie studie.
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Higgins, Stuart James. "Design and Optimization of Post-Combustion CO2 Capture." Diss., Virginia Tech, 2016. http://hdl.handle.net/10919/80003.
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This dissertation describes the design and optimization of a CO2-capture unit using aqueous amines to remove of carbon dioxide from the flue gas of a coal-fired power plant. In particular we construct a monolithic model of a carbon capture unit and conduct a rigorous optimization to find the lowest solvent regeneration energy yet reported.
Carbon capture is primarily motivated by environmental concerns. The goal of our work is to help make carbon capture and storage (CCS) a more efficient for the sort of universal deployment called for by the Intergovernmental Panel on Climate Change (IPCC) to stabilize anthropomorphic contributions to climate change, though there are commercial applications such as enhanced oil recovery (EOR).
We employ the latest simulation tools from Aspen Tech to rigorously model, design, and optimize acid gas systems. We extend this modeling approach to leverage Aspen Plus in the .NET framework through Microsoft's Component Object Model (COM).
Our work successfully increases the efficiency of acid gas capture. We report a result optimally implementing multiple energy-saving schemes to reach a thermal regeneration energy of 1.67 GJ/tonne. By contrast, the IPCC had reported that leading technologies range from 2.7 to 3.3 GJ/tonne in 2005. Our work has received significant endorsement for industrial implementation by the senior management from the world's second largest chemical corporation, Sinopec, as being the most efficient technology known today.<br>Ph. D.
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Cruz, Rui Vogt Alves da. "Estudo da utilização de microalgas e cianobactérias para a captura de dióxido de carbono e produção de matérias-primas de interesse industrial." Universidade de São Paulo, 2011. http://www.teses.usp.br/teses/disponiveis/3/3137/tde-21032012-131813/.
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O uso de microalgas e cianobactérias para a produção de biocombustíveis e outros produtos e matérias-primas de interesse comercial tem sido amplamente divulgado como uma tecnologia sustentável bastante promissora, em função das elevadas produtividades areais, potencial para fixação de CO2, uso de terras não adequadas para cultivo e possibilidade de utilizar fontes alternativas de nutrientes, tais como água salobra ou efluentes agroindustriais. A produção comercial de cianobactérias em tanques abertos em formato de pista foi estudada combinando-se a modelagem matemática do crescimento nos tanques com a avaliação técnica, econômica e de sustentabilidade do processo. Construiu-se um macromodelo para a simulação dos tanques, que permitiu determinar o impacto de variáveis ambientais como, por exemplo, temperatura e luminosidade, e otimizar condições de operação e coleta. A análise econômica detalhada demonstrou o impacto dos custos de capital, operação e consumo de energia pelo processo, também destacando a importância da receita de produtos de alto valor agregado para a viabilidade do sistema, com base na tecnologia atual. Os valores de transformidade e índices de sustentabilidade e carga ambiental, obtidos através da análise emergética, são comparáveis com outros processos para obtenção de biocombustíveis de segunda geração, mas os elevados custos de construção e operação e grande consumo de energia nas etapas de coleta e extração representam ainda grandes desafios à sua sustentabilidade. A análise de sensibilidade para as principais variáveis de processo e estudos de caso para melhorias e modelos de negócio alternativos permitiram priorizar áreas para pesquisa futura com base no impacto econômico e ambiental.<br>The use of microalgae and cyanobacteria for the production of biofuels and other substances of commercial interest has been widely advertised as an extremely promising sustainable technology, due to the high areal productivity, potential for fixation of CO2, possibility of using non-arable land and alternative sources of nutrients such as brackish water and agricultural and industrial effluents. The commercial production of cyanobacteria in open raceway ponds was studied through the combination of a mathematical model for the algal growth with technical, economical and sustainability evaluations. A macromodel was developed to simulate the ponds, and it was used to assess the impact of environmental variables, such as light and temperature, and to optimize the process conditions for operation and harvesting. A detailed economic analysis demonstrated the impact of capital, operation costs and energy consumption, also highlighting the importance of revenue from high value products to process viability, considering the current technology. The transformity, emergy sustainability and environmental loading indices obtained by emergy analysis are comparable to other second generation biofuels, but the high construction and operation costs and energy consumption by the harvesting and extraction steps still represent major challenges to sustainability. The sensitivity analysis and evaluation of both technology improvements and alternative business models enabled the prioritization of future research areas, based on economic and environmental impact.
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Ingvarsdóttir, Anna. "Comparison of direct air capture technology to point source CO2 capture in Iceland." Thesis, KTH, Kemiteknik, 2020. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-289164.
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Det är välkänt att klimatförändringar på grund av global uppvärmning är en av de största kriserna som hotar jorden. Det är en enorm utmaning för mänskligheten att minska koldioxidutsläppen, den främsta orsaken till global uppvärmning. Enkelt genomförbara åtgärder är inte tillräckliga och teknik för att ta bort koldioxid från atmosfären anses nödvändig för att temperaturökningen inte ska överstiga de 1,5 °C som anges i Parisavtalet. Direkt infångning av koldioxid från luft (vanligen kallad direkt luftinfångning, (Eng. Direct air capture - DAC)) är en ny teknik som kan ta bort koldioxid direkt från atmosfären. För närvarande är denna metod dyr; upp till 1000 USD per ton avlägsnad koldioxid. Denna höga kostnad beror främst på den relativt låga koldioxidkoncentrationen i luften, vilket leder till att en stor anläggning behövs för att fånga upp gasen och därmed stora investeringar. Tekniken är mycket energiintensiv, antingen elektrisk eller termisk, och för att göra en direkt infångning effektivare, måste anläggningen drivas med energi som inte har några eller mycket låga koldioxidutsläpp. Energin på Island är billig och dess produktion innebär ett mycket lågt koldioxidavtryck. Syftet med arbetet i denna avhandling är att utforska om metoden för direkt infångning av koldioxid från luft kommer att vara en mer genomförbar metod än koldioxidinfångning från punktkällor (eng. point source - PS) på Island på grund av god tillgång till billig och ren energi. Lärandekurvan för direkt luftfångning studerades tillsammans med scenarier för metodens tekniska utveckling. Tre olika fall med punktkällor på Island studerades för jämförelse. Två olika direkta luftinfångningstekniker analyserades också, en som drivs av en stor mängd elektricitet och en som drivs mestadels av termisk energi. Det resulterade i att i bästa fall, där inlärningshastigheten är hög och tekniska förbättringar är signifikanta, så skulle produktionskostnaden för direkt luftinfångning (levelized cost of energy, LCOC) vara lägre än motsvarande för infångning från en punktkälla. Energikostnaden påverkar LCOC för DAC idag men med teknisk utveckling förväntas energibehovet minska och därför kommer energikostnadens påverkan att bli lägre. Det är dock fortfarande viktigt, med tanke på bidraget till att minska globala uppvärmningen, att energin som driver DAC-anläggningen har ett lågt koldioxidavtryck, vilket kan garanteras på Island. Tvärtom, om inlärningshastigheten för DAC-tekniken är låg och inga tekniska förbättringar sker i lösningsmedel eller sorbenter, är och kommer DAC-tekniken att bli dyrare än infångning från punktkällor om båda anläggningarna finns på Island. En hög inlärningshastighet och teknikutveckling är beroende av trycket att nå målen i Parisavtalet. Det är därför mycket viktigt för DAC att efterfrågan på koldioxidinfångning ökar. Dessutom har DAC mer potential att påverka klimatförändringarna eftersom DAC kan vara en kolnegativ teknik om den kombineras med permanent lagring av koldioxid. PS-avskiljningen kan endast vara en kolneutral teknik och detta om den kombineras med permanent lagring av koldioxid.<br>It is well known that climate change due to global warming is one of the greatest crises facing the Earth. It is a huge challenge for mankind to reduce CO2 emissions, the major cause of global warming. Mitigation measures are not enough. Technologies to remove the CO2 from the atmosphere are considered necessary, so the temperature rise does not exceed 1.5°C as stated in the Paris Agreement. Direct air capture (DAC) is a new technology that can remove carbon dioxide directly from the atmosphere. Currently, this method is expensive, up to 1000 USD per ton CO2 removed. This high cost is mostly due to the relatively low concentration of CO2 in the ambient air, leading to a large unit to capture the gas and therefore high capital investment. The technology is very energy-intensive, either electrical or thermal, and to make direct air capture more efficient the plant needs to be powered with energy that has no or very low CO2 emissions. The energy in Iceland is low cost and its production has a very low carbon footprint. This thesis aims to find out if the direct air capture method will be more feasible than a point source CO2 capture in Iceland due to good access to low-cost and clean energy. The learning curve for direct air capture was studied along with scenarios for its technological development. Two different direct air capture technologies were analyzed, one that is powered by a large amount of electricity and one powered mostly by thermal energy. Three different point source cases in Iceland were studied for comparison. For the best-case scenario, where the learning rate is high and technological improvements are significant, the levelized cost of direct air capture is lower than levelized cost of point source capture. The cost of energy affects the levelized cost of direct air capture today but with technical development, the energy needed is expected to go down, and therefore the effect of energy cost will be lower. However, it is still important, concerning contribution to reducing global warming, that the energy powering the direct air capture plant has a low carbon footprint, which can be assured in Iceland. On the contrary, if the learning rate of the direct air capture technology is low and no technical improvements occur in solvents or sorbents the direct air capture technology is and will be more expensive than point source capture considering both located in Iceland. The high learning rate and development in technology are dependent on the pressure to reach the goals of the Paris Agreement. It is therefore vital for direct air capture that the demand for carbon removal measures is enhanced due to pressure to reach the Paris Agreement goals. Furthermore, direct air capture has more potential to affect climate change than point source capture as direct air capture can be a carbon-negative technology if coupled with the permanent storage of CO2. The point source capture can only be a carbon-neutral technology if coupled with the permanent storage of CO2.
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Anselmi, Hélène. "Modélisation et évaluation environnementale d’une unité de captage de CO₂ intégrée à un procédé industriel." Thesis, Université de Lorraine, 2019. http://www.theses.fr/2019LORR0080.
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Limiter les émissions de dioxyde de carbone (CO2) est devenu un enjeu d’envergure internationale, notamment pour les industries des secteurs énergétique, chimique et métallurgique. À cette fin, des technologies de captage de CO2 ont été développées durant ces dernières décennies. Dans cette étude, nous nous intéressons à trois types de technologies de captage de CO2 : par absorption chimique à la MEA, par séparation membranaire et par adsorption sur charbon actif. Le CO2 considéré est émis par une centrale à charbon puis directement valorisé au sein d’un procédé de fabrication sur le même site. L’objectif de cette étude est de quantifier les bénéfices environnementaux de l’installation d’une technologie de captage de CO2, en comparaison à la configuration actuelle, sans captage du CO2. Notre approche associe modélisation systémique des procédés et analyse de cycle de vie (ACV). La méthodologie adoptée consiste à modéliser le système complet (la centrale, le procédé de fabrication et les différentes unités de captage) en utilisant un logiciel de diagrammes de flux (Aspen Plus), puis à déterminer les impacts environnementaux par une ACV. Les résultats montrent que le procédé par adsorption chimique à la MEA est fortement pénalisé par l’utilisation du solvant, tant en ce qui concerne la consommation énergétique que les impacts environnementaux. Le procédé membranaire montre des impacts environnementaux importants, malgré une consommation énergétique bien plus faible, en raison de l’utilisation massive de polymères (matériaux membranaires). Enfin, le procédé par adsorption au charbon actif présente des impacts environnementaux moins élevés que les deux autres procédés dans la grande majorité des catégories d’impact<br>Limiting carbon dioxide (CO2) emissions is a major global issue, particularly for the energy, chemical and metallurgical industries. To this end, CO2 capture technologies have been developed in recent decades. In this study, we focused on three types of CO2 capture technologies: chemical absorption by MEA, membrane separation and activated carbon adsorption. The CO2 considered is emitted by a coal-fired power station and then directly valorized within a manufacturing process on the same site. The objective of this study was to quantify the environmental benefits of installing a CO2 capture technology in comparison to the current configuration, without CO2 capture. Our approach combined process modeling and life cycle assessment. The methodology adopted was to model the complete system (the power plant, the manufacturing process and the various capture units) using a flowsheeting software (Aspen Plus), then to determine the environmental impacts by LCA. The results show that the MEA chemical adsorption process is strongly penalized by the use of the solvent, both regarding the energy consumption and the environmental impacts. The membrane process exhibits significant environmental impacts, despite a much lower energy consumption, due to the massive use of polymers (membrane materials). Finally, the activated carbon adsorption process has lower environmental impacts than the other two processes in the vast majority of impact categories
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Karthikeyan, Tejas Latha. "Investigation of the absorption solvent for bioenergy carbon capture and storage (BECCS) through pilot plant trials." Thesis, KTH, Kemiteknik, 2020. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-289165.
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Att begränsa globala uppvärmningen till 1,5°C kommer kräva negativa koldioxidutsläpp. En metod för att generera negativa koldioxidutsläpp är så kallad Bio-Energy Carbon Capture and Storage (BECCS). En direkt implementering av BECCS är att fånga in CO2 från rökgas som genereras vid förbränning av biomassa i en så kallad post-combustion capture-konfigurering. Post-combustion BECCS har skapat en stor resonans hos kraftverksoperatörer och pappersproducenter. Stockholm Exergi, som ägs av Fortum och Stockholms Stad, siktar på att fånga in upp till 800 kt CO2 per år från deras biomass-eldade CHP-anläggning i Värtaverket vid 2024. Planen är att fånga in CO2 från rökgasen genom en absorptionsprocess och sedan skeppa det till Norge för geologisk förvaring. Mastersexamensarbetet följde en experimentskampanj driven av Stockholm Exergi som siktade på att uppnå experimentell validering av en absorptionsprocess för koldioxidinfångning från rökgas vid förbränning av biomassa. En testenhet konstruerades och tester genomfördes från december 2019 till maj 2020. Examensarbetet fokuserade på rollen absorptionsmedlet hade på infångningshastigheten. Tester med tre olika lösningsmedel genomfördes och de experimentella resultaten analyserades genom en kombination av jämviktsmodeller och Murphree-effektiviteter. Resultatet visar att ett absorptionsmedel baserat på vattenlöslig K2CO3 är kompatibel med rökgas från förbränning av biomassa, eftersom infångningshastigheter mellan 5 och 13 % uppmättes. De undersökta hastighetspromotorerna (3 vikt% H3BO3 + 1 vikt% V2O5) visade dock inte den förväntade effekten på infångningshastigheter, och på grund av tidsbegränsningar testades inte olika vikt% av promotorn under det här examensarbetet. Ingen tydlig slutsats drogs därför med hänsyn till promotorer. Baserat på Murphree-effektiviteterna som beräknats genom experimenten med konstant förhållande mellan vätske- och gasflöde uppskattas en 28–35 m hög kolonn fånga 90% av CO2 i rökgasen.<br>Limiting global warming to 1.5°C will require negative carbon emissions. One way for generating negative carbon emissions is through bio-energy carbon capture and storage (BECCS). A direct implementation of BECCS is to capture CO2 from the flue gas originating from the combustion of biomass in a post-combustion capture configuration. Post-combustion BECCS has generated considerable resonance among power plant operators and paper manufactures. Stockholm Exergi, owned by Fortum and Stockholm Stad, aims at capturing up to 800 kt CO2 per year from their biomass-fired CHP plant in Värtaverket by 2024. The plan foresees to capture CO2 from the flue gas utilizing an absorption process and shipment of the captured CO2 to Norway for geological storage. The Master thesis project followed an experimental campaign run by Stockholm Exergi that aimed at experimental validation of an absorption process for carbon capture from flue gas originating from the combustion of biomass. A test unit was constructed, and test trials were run from Dec. 2019 to May 2020. The thesis focused on the role of the absorption solvent on the capture rate. Test trails with three different solvents were conducted, and the experimental results were analyzed using equilibrium models combined with Murphree efficiencies. The results show that an absorption solvent based on aqueous K2CO3 is compatible with the flue gas derived from biomass combustion, i.e., capture rates ranging from 5 to 13 % were measured. However, the investigated rate promoters (3 wt.% H3BO3 + 1 wt.% V2O5) did not show the expected effect with regards to capture rates and due to time constrain different wt.% of the promoter were not tested within the scope of this thesis. Therefore, no firm conclusion was given with regards to promoters. Based on the Murphree efficiency calculated from the experiment with keeping a constant liquid to gas flow ratio, a column height of 28-35 m is estimated to capture 90% of CO2 from the flue gas.
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Preso, Davide Bernardo. "Application of an ammonia-based process with controlled solid formation for post-combustion CO2 capture." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2019. http://amslaurea.unibo.it/17505/.
Full textAbstract:
CO2 capture and storage is needed to reduce the carbon footprint related to industrial activities. Among the different available technologies, CO2 removal from power/cement plant’s flue gases is of particular interest due to its versatility and retrofit opportunities for existing plants. In this framework, the Chilled Ammonia Process (CAP) is a promising technology for post-combustion CO2 capture. Besides its competitive energetic performance compared to conventional amines, the use of aqueous NH3 as a solvent offers advantages concerning global availability, environmental footprint and cost compared to most amine processes.
A new ammonia-based process for CO2 capture from flue gas has been developed, which found its origin in the Controlled Solid Formation - Chilled Ammonia Process (CSF-CAP). A controlled solid precipitation carried in a dedicated unit of the plant lead to a reduction of the energy penalty of the process without hindering its operability, since the mass flow rate sent to regeneration can be substantially reduced by means of CO2 concentration in the solid phase rather than the liquid phase.
Differently from the original CSF-CAP, where ammonium bicarbonate has been exploited in the crystallization section, in this new process ammonium carbonate monohydrate is formed, which promises numerous advantages in terms of the overall energy efficiency of the process.
Initially, the process synthesis has been performed, followed by a rigorous optimization and performance evaluation. The work have been carried out coupling Aspen Plus V8.6 and Matlab. The speciation model developed by Thomsen has been used for the calculations in the CO2-NH3-H2O system.
Under the assumptions considered in this work, the new CSF-CAP has been found to require 0.84 MJ/kgCO2 of electrical energy, which corresponds to a reduction of 5\% of the overall energy duty of the plant, compared to the original CSF-CAP, which needs 0.89 MJ/kgCO2.
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James, David William. "Failing Drop CO2 Deposition (Desublimation) Heat Exchanger for the Cryogenic Carbon Capture Process." BYU ScholarsArchive, 2011. https://scholarsarchive.byu.edu/etd/2930.
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Cryogenic carbon capture removes CO2 and other pollutants from flue and waste stream gases produced from the combustion of fossil fuels such as coal, natural gas, and oil and the production of cement. A transient, 1-dimensional numerical model was developed to study the temperature profile within a counter-current surface CO2 desublimation-falling liquid or solid heat exchanger. Effects of desublimation heat and mass transfer as well as convective and conductive heat transfer relationships were taken into account. Experiments show that CO2 can be captured on a falling spherical particle when appropriate column operating conditions are met.
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Retief, Frederik Jacobus Gideon. "A novel approach to solvent screening for post-combustion carbon dioxide capture with chemical absorption." Thesis, Stellenbosch : Stellenbosch University, 2012. http://hdl.handle.net/10019.1/19964.
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Thesis (MScEng)--Stellenbosch University.<br>ENGLISH ABSTRACT: Carbon dioxide (CO2) is classified as the main greenhouse gas (GHG) contributing to global warming.
Estimates by the Intergovernmental Panel on Climate Change (IPCC) suggest that CO2 emissions must be
reduced by between 50 to 85% by 2050 to avoid irreversible impacts. Carbon capture and storage (CCS)
strategies can be applied to de-carbonize the emissions from fossil-fueled power plants. Compared to
other CCS techniques, post-combustion capture (PCC) is most likely to be implemented effectively as a
retrofit option to existing power plants. At present however CCS is not yet commercially viable. The
main challenge with CCS is to reduce the inherent energy penalty of the CO2 separation stage on the
host plant.
Seventy-five to eighty percent of the total cost of CCS is associated with the separation stage. There are
several technologies available for separating CO2 from power plant flue gas streams. Reactive absorption
with aqueous amine solutions has the ability to treat low concentration, low pressure and large flux flue
gas streams in industrial-scale applications. It is most likely to be the first technology employed
commercially in the implementation of CCS. The energy required for solvent regeneration however, is
high for the standard solvent used in reactive absorption processes, i.e. MEA. This leads to a reduction in
thermal efficiency of the host plant of up to 15%. Alternative solvent formulations are being evaluated in
an attempt to reduce the energy intensity of the regeneration process.
The main objective of this study was to establish a novel, simplified thermodynamic method for solvent
screening. Partial solubility parameters (PSPs) were identified as the potential basis for such a method.
The major limitation of this approach is that the model doesn’t account for effects from chemical
reaction(s) between materials, e.g. CO2 reacting with aqueous alkanolamine solutions; considering only
the effects from dissolution. The EquiSolv software system was developed based on PSP theory. The
Hansen 3-set PSP approach was used to describe the equilibrium behaviour of CO2 absorbing in task
specific solvents. The Hansen theory was expanded to a 4-set approach to account for contributions
from electrostatic interactions between materials. The EquiSolv program was used successfully to screen
large sets of solvent data (up to 400 million formulations) in the search for suitable alternative solvent
formulations for CO2 absorption.
The secondary objective of this study was to evaluate the ability of the proposed PSP model to
accurately predict suitable alternative solvents for CO2 absorption through preliminary experimental
work. A series of CO2 absorption experiments were conducted to evaluate the absorption performance
of predicted alternative solvent formulations. The predicted alternative solvent formulations exhibited a
significant improvement in absorption performance (up to a 97% increase in the measured absorption
capacity) compared to conventional solvent formulations. Statistical analysis of the experimental results
has shown that there is a statistically significant concordant relationship between the predicted and
measured rankings for the absorption performance of the predicted solvent formulations. Based on this
it was concluded that PSP theory can be used to accurately predict the equilibrium behaviour of CO2
absorbing in task specific solvents.
Recently ionic liquids (ILs) have been identified as potential alternatives to alkanolamine solutions
conventionally used for CO2 absorption. Absorption experiments were conducted as a preliminary
assessment of the absorption performance of ILs. Results have shown ILs to have significantly improved
performance compared to conventional alkanolamine solvents; up to a 96% increase in the measured
absorption capacity compared to conventional solvents. Future work should focus on developing task
specific ionic liquids (TSILs) in an attempt to reduce the energy intensity of solvent regeneration in CO2
absorption processes.<br>AFRIKAANSE OPSOMMING: Koolsuurgas (CO2) word geklassifiseer as die vernaamste kweekhuis gas (GHG) wat bydra to globale
verwarming. Beramings deur die Interregeringspaneel oor Klimaatsverandering (IPKV) toon aan dat CO2
emissies teen 2050 verminder moet word met tussen 50 en 85% om onomkeerbare invloede te vermy.
Verskeie koolstof opvangs en bergings (KOB) strategieë kan toegepas word ten einde die koolstof
dioksied konsentrasie in die emissies van kragstasies wat fossielbrandstowwe gebruik, te verminder. Naverbranding
opvangs (NVO) is die mees aangewese KOB tegniek wat effektief toegepas kan word op
bestaande kragstasies. Tans is KOB egter nog nie kommersieël lewensvatbaarvatbaar nie. Die hoof
uitdaging wat KOB in die gesig staar is om die energie boete inherent aan die CO2 skeidingstap te
verminder.
Tussen vyf-en-sewentig en tagtig persent van die totale koste van KOB is gekoppel aan die skeidingstap.
Daar is verskeie metodes beskikbaar vir die skeiding van CO2 uit die uitlaatgasse van kragstasies.
Reaktiewe absorpsie met waterige oplossings van amiene kan gebruik word om lae konsentrasie, lae
druk en hoë vloei uitlaatgasstrome in industriële toepassings te behandel. Dit is hoogs waarskynlik die
eerste tegnologie wat kommersieël aangewend sal word in die toepassing van KOB. Die oplosmiddel wat
normalweg vir reaktiewe absorpsie gebruik word (d.w.s. MEA) benodig egter ‘n groot hoeveelheid
energie vir regenerasie. Dit lei tot ‘n afname in die termiese doeltreffendheid van die voeder aanleg van
tot 15%. Alternatiewe oplosmiddelstelsels word tans ondersoek in ‘n poging om the energie intensiteit
van die regenerasieproses te verminder.
Die hoof doelwit van hierdie studie was om ‘n nuwe, ongekompliseerde termodinamiese metode te
vestig vir die keuring van alternatiewe oplosmiddels. Parsiële oplosbaarheidsparameters (POPs) is
geïdentifiseer as ‘n moontlike grondslag vir so ‘n metode. Die model beskryf egter slegs die ontbindings
gedrag van materiale. Die effekte van chemise reaksie(s) tussen materiale, bv. die tussen CO2 en
waterige oplossings van alkanolamiene, word nie in ag geneem nie. Die POP teorie het gedien as
grondslag vir die ontwerp van die EquiSolv sagteware stelsel. Die Hansen stel van drie POPs is gebruik
om die ewewigsgedrag te beskryf van CO2 wat absorbeer in doelgerig-ontwerpte oplosmiddels. Die
Hansen teorie is verder uitgebrei na ‘n stel van vier POPs om die bydrae van elektrostatiese wisselwerking tussen materiale in ag te neem. Die EquiSolv program is verskeie kere met groot sukses
gebruik vir die sifting van groot stelle data (soveel as 400 miljoen formulasies) in die soektog na
alternatiewe oplosmiddels vir CO2 absorpsie.
Die sekondêre doelwit van die studie was om die vermoë van die voorgestelde POP model om geskikte
alternatiewe oplosmiddels vir CO2 absorpsie akkuraat te voorspel, te ondersoek deur voorlopige
eksperimentele werk. ‘n Reeks CO2 absorpsie eksperimente is gedoen ten einde die absorpsie
werkverrigting van die voorspelde alternatiewe oplosmidels te ondersoek. ‘n Verbetering in absorpsie
werkverrigting van tot 97% is gevind vir die voorspelde oplosmiddels vergeleke met die van
oplosmiddels wat tipies in die industrie gebruik word. Statistiese ontleding van die eksperimentele
resultate het getoon dat daar ‘n beduidende ooreenstemming tussen die voorspelde en gemete
rangskikking van die voorspelde oplosmiddels se werkverrigting bestaan. Dus kan POP teorie gebruik
word om die absorpsie van CO2 in doelgerig-ontwerpte oplosmiddels akkuraat te beskryf.
Ioniese vloeistowwe (IVs) is onlangs geïdentifiseer as moontlike alternatiewe oplosmidels vir die
alkanolamien oplossings wat normaalweg gebruik word vir CO2 absorpsie. Absorpsie eksperimente is
gedoen ten einde ‘n voorlopige raming van die absorpsie werkverrigting van IVs te bekom. Daar is
bevind dat IVs ‘n beduidende verbetering in werkverrigting toon in vergelyking met die alkanolamien
oplosmiddels wat normaalweg gebruik word. ‘n Verbetering in absorpsie werkverrigting van tot 96% is
gevind vir die voorspelde IV-bevattende oplosmiddels vergeleke met die van oplosmiddels wat tipies in
die industrie gebruik word. Die fokus van toekomstige navorsing moet val op die ontwikkeling van
doelgemaakte ioniese vloeistowwe (DGIVs) in ‘n poging om die energie intensiteit van oplosmiddel
regenerasie in CO2 absorpsie prosesse te verminder.
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Gharaie, Mona. "Design and optimization of energy systems with effective carbon control." Thesis, University of Manchester, 2013. https://www.research.manchester.ac.uk/portal/en/theses/design-and-optimization-of-energy-systems-with-effective-carbon-control(12eab9ec-f647-4d5a-b74e-2ac729dc88ca).html.
Full textAbstract:
Environmental concerns about the effect of greenhouse gases have led governments to regulate industrial CO2 emissions, including through emissions caps, trading and penalties, thus creating economic incentives to reduce CO2 emissions. This research focuses on strategies to reduce CO2 emissions from energy systems in the context of the process industries. In the process industries, energy systems consume fuel to generate steam and power for site process units. Improving energy efficiency can reduce costs of energy generation and use, as well as CO2 emissions. This research develops an integrated design and optimisation methodology for energy systems, allowing effective capture and control of carbon dioxide emissions. The first focus of this study is to develop a systematic approach to evaluate combinatorial strategies for reducing CO2 emissions, based on a techno-economic analysis. A conceptual design procedure with hierarchical decision-making is introduced to combine CO2 emissions reduction strategies, accounting for interactions between site components, including the heat exchanger network and utility system. CO2 emissions reduction options considered in development of this procedure include process integration techniques for improving the energy efficiency of the site and fuel switching. The proposed approach considers trade-offs between the economy of energy retrofit and CO2 emissions penalties. Opportunity for reducing the CO2 penalty is included in the economic evaluation of the combined emissions reduction strategies. A mathematical model for simultaneous optimization of emissions reduction strategies is developed. In addition to emissions reduction strategies, options for trading CO2 allowances are considered in the model. The proposed mathematical method applies Mixed Integer Non Linear Programming (MINLP) optimization, which employs a superstructure of the strategies for CO2 reduction. The proposed mathematical model relates the selected options to their operating and capital costs and to their associated CO2 emissions, allowing the optimizer to search for the optimal combination of emissions reduction strategies. While the reduction in CO2 emissions through process integration techniques is based on the existing configuration of a site and the associated structural limitations, integration of Carbon Capture and Storage (CCS) technologies can provide greater mitigation of CO2 emissions from a site. However, important challenges of implementing CCS in the process industries are the energetic and economic impact of the CCS plant on the integrated site. In the second part of this study, these energy-economic issues are explored. The CCS technologies addressed in this thesis include post- and pre-combustion CO2 capture techniques. Simulation of each capture technique is carried out in process simulation software to characterize the energy performance of the CO2 capture plant. Sensitivity analyses are carried out for key parameters of the CO2 capture plant. The relationship between these key parameters and the energy balance of the capture plant is represented using a simple energy performance model for the CO2 capture plant. This model allows the integration of the CO2 capture plant with the site utility system to be explored. Interactions between the utility system and CO2 capture plant are considered. The site utility system, together with the CO2 capture plant, is optimized for minimum operating cost. The proposed procedures are illustrated by application to a case study of a medium-scale oil refinery. The results illustrate that to reduce CO2 emissions, heat integration, utility system optimization and fuel switching provide more cost-effective solutions than integrating CCS technologies. The mathematical model allows more cost-effective solutions to be identified than using sequential, conceptual methods, but the value of the conceptual method for developing insights is also illustrated. The results demonstrate that, depending on the potential of the site for increasing heat recovery and the type of fuel used on site, solutions that combine energy efficiency and fuel switching can provide up to 40% reduction in site CO2 emissions. Integrating a post-combustion CO2 capture plant with the site utility system can provide up to 90 mol% pure CO2 for sequestration; however, the high capital cost of the capture plant reduces the economic performance of the integrated site. The high heat demand of post-combustion CO2 capture for solvent regeneration increases the fuel consumption of the site and its utility system, which in turn reduces the recovery of CO2. The results reveal that pre-combustion CO2 capture can provide opportunities for heat and power generation to improve the techno-economic performance of the overall integrated site.
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El, Gemayel Gemayel. "Integration and Simulation of a Bitumen Upgrading Facility and an IGCC Process with Carbon Capture." Thèse, Université d'Ottawa / University of Ottawa, 2012. http://hdl.handle.net/10393/23274.
Full textAbstract:
Hydrocracking and hydrotreating are bitumen upgrading technologies designed to enhance fuel quality by decreasing its density, viscosity, boiling point and heteroatom content via hydrogen addition. The aim of this thesis is to model and simulate an upgrading and integrated gasification combined cycle then to evaluate the feasibility of integrating slurry hydrocracking, trickle-bed hydrotreating and residue gasification using the Aspen HYSYS® simulation software. The close-coupling of the bitumen upgrading facilities with gasification should lead to a hydrogen, steam and power self-sufficient upgrading facility with CO2 capture. Hydrocracker residue is first withdrawn from a 100,000 BPD Athabasca bitumen upgrading facility, characterized via ultimate analysis and then fed to a gasification unit where it produces hydrogen that is partially recycled to the hydrocracker and hydrotreaters and partially burned for power production in a high hydrogen combined cycle unit. The integrated design is simulated for a base case of 90% carbon capture utilizing a monoethanolamine (MEA) solvent, and compared to 65% and no carbon capture scenarios. The hydrogen production of the gasification process is evaluated in terms of hydrocracker residue and auxiliary petroleum coke feeds. The power production is determined for various carbon capture cases and for an optimal hydrocracking operation. Hence, the feasibility of the integration of the upgrading process and the IGCC resides in meeting the hydrogen demand of the upgrading facility while producing enough steam and electricity for a power and energy self-sufficient operation, regardless of the extent of carbon capture.
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Signorini, Virginia. "Hybrid polymer-based membranes with graphene oxide nanoparticles for carbon dioxide capture." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2019.
Find full textAbstract:
The project focuses on the development of hybrid polymer/inorganic membranes with aligned nanoparticles within the polymeric matrix for CO2 separation membrane fabrication. The investigated polymer is the PEG3A, while the inorganic particles are the Graphene Oxide (GO).
The addition of the GO nanoparticles is done due to a UV-light cross-linking reaction between the polymer, the polymer solvent and the solvent in which nanoparticles are dispersed in different concentration. The solvents used for the incorporation of GO into the membrane matrix are Water, Ethanol and Acetone since these fillers are considered non-toxic for human being.
The membrane alignment is expected to improve the performance for CO2/N2 and CO2/He separation application which had been calculated by testing each membrane with the Single Gas Apparatus with the same operative condition.
The compatibility of the polymers and nanoparticles will be characterized by using different techniques such as SEM, TGA and DSC, in order to develop the optimal hybrids for the carbon capture.
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Kong, Fanhe. "Chemical Looping Partial Oxidation and Hydrogen Production: Process Simulation, Exergy Analysis and Life Cycle Assessment." The Ohio State University, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=osu1587591727870495.
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Zaidiza, David Ricardo Albarracin. "Modelling of Hollow Fibre Membrane Contactors : Application to Post-combustion Carbon Dioxide Capture." Thesis, Université de Lorraine, 2016. http://www.theses.fr/2016LORR0035/document.
Full textAbstract:
La capture du dioxyde de carbone (CO2) en postcombustion est une stratégie importante pour la limitation de l’effet de serre. Le procédé de référence est l’absorption du CO2 dans des solutions aqueuses aminées, suivie par une étape de stripage du solvant. La technologie mature associée à ce procédé est la colonne à garnissage. Toutefois, afin de rendre le procédé plus attractif, il convient de l’intensifier en réduisant le volume des équipements et le coût énergétique associé. Les contacteurs membranaires à fibres creuses (CMFC) constituent une alternative aux colonnes à garnissage. Les CMFC permettent de développer d’importantes aires spécifiques conduisant potentiellement à une intensification des transferts gaz-liquide. Ainsi, l’utilisation des CMFC réduirait la taille des installations, mais aussi diminuerait la consommation énergétique par la diminution de la quantité de vapeur de stripage. Cependant, l’utilisation de CMFC dans les étapes d’absorption et de stripage dans des conditions industrielles a été peu étudiée. Afin de combler cette lacune, des modèles à différents niveaux de complexité : monodimensionnel, bidimensionnel, isotherme et adiabatique ont été développés, comparés et validés. Ceci afin d’identifier le niveau de complexité approprié. Les résultats de simulation ont mis en évidence le potentiel d’intensification des CMFC dans l’étape d’absorption et aussi de stripage, se traduisant par une réduction en volume de 4 à 10 fois par rapport aux colonnes à garnissage. Néanmoins, les CMFC peuvent difficilement réduire le coût énergétique du procédé étant donné que l’étape de stripage fonctionne dans des conditions très proches de la limite thermodynamique<br>Post-combustion CO2 capture (PCC) is an important strategy in mitigating greenhouse effect. The reference process in PCC is the CO2 absorption into amine aqueous solutions, followed by the regeneration (or stripping) of the solvent. The robustness of packed columns makes it the standard technology for both absorption and stripping steps. However, the treatment of large quantities of flue gases requires itself equipment of a large size. Hollow fibre membrane contactors (HFMC) are considered as one of the most promising strategies for intensified CO2 absorption process, due to their significantly higher interfacial area than that of packed columns, allowing to reduce the equipment size. In addition, this would reduce the energy penalty of the process by reducing the required amount of stripping steam. However, despite the potential advantages of HFMC, very few investigations have studied implementing this technology for PCC within an industrial framework. To fill this lack, the performances of both absorption and stripping steps using HFMC under industrial conditions were estimated by modelling and simulation. To identify the optimal modelling strategy, transfer models with different levels of complexity were developed ranging from one-dimensional isothermal single-component to two-dimensional adiabatic multi-component. Simulation results of both absorption and stripping steps revealed that, compared to traditional packed columns, contactor volume reduction factors comprised between 4 and 10 might be achieved using HFMC. However, since the stripping operating conditions are very close to thermodynamic equilibrium, HFMC can hardly reduce the energy consumption of the process
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Lalsare, Amoolya Dattatraya. "High Pressure Steam Reactivation of Calcium Oxide Sorbents For Carbon Dioxide Capture Using Calcium Looping Process." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1462444410.
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Ozcan, Dursun Can. "Techno-economic study of the calcium looping process for CO2 capture from cement and biomass power plants." Thesis, University of Edinburgh, 2014. http://hdl.handle.net/1842/10455.
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The first detailed systematic investigation of a cement plant with various carbon capture technologies has been performed. The calcium looping (Ca-looping) process has emerged as a leading option for this purpose, since this process applied to a cement plant provides an opportunity to use the CaO purge for clinker production. The Ca-looping process is comprised of two interconnected reactors where the carbonator captures CO2 from flue gases and the calciner regenerates the CaCO3 into CaO by oxy-combustion. Fully integrated process flowsheets have been developed and simulated in UniSim Design Suite from Honeywell. The detailed carbonator model has been implemented using Matlab and incorporated into UniSim to provide a full flowsheet simulation for an exemplary dry-feed cement plant as a user-defined operation. The base cement plant simulation was also modified to integrate three different carbon capture processes: membrane; indirect calcination; and amine-scrubbing. Furthermore, an advanced configuration of Ca-looping process has been investigated where the energy intensive air separation unit was replaced with a chemical looping combustion (CLC) cycle. Each case has been optimised to minimise its energy consumption and compared in terms of levelised cost of cement and its resulting cost of CO2 avoided at the same CO2 avoidance rate. The proposed integration of the Ca-looping process is capable of achieving over 90% CO2 avoidance with additional fuel consumption of 2.5 to 3.0 GJth/ton CO2 avoided. By using an advanced configuration of the Ca-looping process with a CLC cycle, the additional fuel consumption can be reduced to 1.7 GJth/ton CO2 avoided, but the cost of the oxygen carrier is the major concern for this system. Among the other CO2 capture options, the membrane process is a promising alternative for the Ca-looping process since it has a potential of achieving the target CO2 avoidance rate and purity requiring lower energy consumption. The indirect calcination process provides moderate levels of CO2 avoidance (up to 56%) without a need of an external capture process whereas the integration of the amine process in a cement plant is challenging as a result of the requirement of steam for solvent regeneration. Furthermore, considering zero net CO2 emissions associated with biomass combustion systems, a novel concept has been analysed to capture of CO2 in-situ with the Ca-looping process while operating the combustor of a dedicated biomass power plant at sufficiently low temperature. This process is capable of achieving 84% overall CO2 capture rate with an energy penalty of 5.2% when a proper heat exchanger network is designed with the support of a pinch analysis. The techno-economic performance of the biomass power plant with in-situ Ca-looping CO2 capture process was compared with that of the alternative biomass-air-fired and biomass-oxy-fired power plants.
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Boscherini, Mattia. "Adsorbimento dinamico di CO2 in compositi innovativi a base geopolimerica." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2020.
Find full textAbstract:
Fra le alternative proposte per la riduzione delle emissioni di CO2, le tecniche di Carbon Capture si presentano come un’efficace soluzione per il breve e medio termine. Fra queste, l’adsorbimento su fase solida per la rimozione di CO2 da correnti gassose si prospetta come una valida alternativa rispetto al convenzionale assorbimento ad umido. Questo lavoro di tesi si è occupato della sintesi di un composito a base geopolimerica presso l’ISTEC/CNR di Faenza, da impiegare per l’adsorbimento di CO2 a bassa temperatura, e dell’analisi del suo comportamento in regime di adsorbimento dinamico. Tale materiale è stato sintetizzato tramite attivazione con soluzione alcalina di metacaolino 1200S addizionato con polveri di zeolite Na13X. Esso costituisce una opzione interessante per la cattura di CO2, mostrando capacità di adsorbimento superiori a 1 mmol/g per concentrazioni di CO2 del 14% (a pressione atmosferica), simili a quelle presenti in molti processi industriali. Le prestazioni in regime dinamico risultano inoltre simili a quelle registrate nel regime statico.
Le prove sperimentali hanno evidenziato la criticità della rigenerazione del materiale, in particolare riguardo all’eliminazione dell’acqua. Una temperatura di 130°C si mostra adatta per ottenere un’elevata rigenerazione del materiale, con rimozione sia di CO2 che dell’umidità adsorbita. Dalle prove svolte è risultato evidente come non sia conveniente operare con desorbimenti a temperatura ambiente e pressione atmosferica, ma sia necessario operare combinando swing di pressione e temperatura. È stato inoltre valutato l’effetto di una più bassa temperatura di adsorbimento (2°C), che porta ad un aumento della capacità del materiale.
Sviluppi futuri in questo campo potrebbero essere la produzione di monoliti geopolimerici a porosità strutturate tramite tecniche innovative quali il freeze-casting e l’utilizzo di compositi integrati con additivi che ne migliorino le performance in termini di conducibilità termica.
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Sissman, Olivier. "Séquestration minérale du CO2 dans les basaltes et les roches ultrabasiques : impact des phases secondaires silicatées sur le processus de carbonatation." Paris, Institut de physique du globe, 2013. http://www.theses.fr/2013GLOB0001.
Full textAbstract:
La formation de carbonates constitue une option pérenne de séquestration géologique du dioxyde de carbone (CO2), susceptible de participer significativement à la réduction des émissions d’origine anthropique. Or, notre compréhension du mécanisme de carbonatation, ainsi que des blocages cinétiques rencontrés au cours de cette réaction chimique, n’est encore que peu développée. Bien qu’il existe de nombreuses études portant sur les cinétiques de dissolution des silicates basiques et de précipitation de carbonates, peu de travaux se sont intéressés à l’impact que la formation de phases secondaires non carbonatées pouvait produire sur ces cinétiques réactionnelles. C’est le parti pris par ce travail de thèse, dans la mesure où seule une bonne connaissance du mécanisme global de carbonatation pourra rendre ce procédé prédictible et efficace. Des données expérimentales de dissolution et carbonatation en réacteur fermé ont ainsi été obtenues sur des minéraux et roches pertinents. Dans une première partie, nous nous intéressons à la carbonatation de l’olivine, phase majeure des péridotites et mineure des basaltes, à 90°C et sous une pression de CO2 de 280 bars. L’altération d’olivine de San Carlos (Mg1. 76Fe0. 24SiO4) est inhibée par la formation d’un gel de silice en surface du minéral, dès lors que le milieu atteint la saturation vis de la silice amorphe (SiO2am). Le transport des espèces, qui se poursuit par un mécanisme de diffusion intra-solide à travers la couche de silice, devient l’étape limitante, ralentissant le processus de dissolution de l’olivine de San Carlos de cinq ordres de grandeur. En revanche, cette passivation des surfaces ne se produit pas lors de l’altération de calcio-olivine (Ca2SiO4), malgré la formation d’une couche de silice. Cette comparaison démontre que ce n’est pas la structure du silicate primaire qui contrôle les propriétés de transport de la silice, mais sa composition chimique. Le second volet se focalise sur la dynamique de formation des phases secondaires, en explorant les effets produits par l’ajout de ligands organiques, ainsi que par des variations de température. L’ajout de citrate à 90°C accélère bien la dissolution d’olivine de San Carlos d’un ordre de grandeur, et permet de libérer du magnésium en concentration suffisante pour former des carbonates avant que la silice ne précipite depuis la solution et passive les surfaces de l’olivine. Une expérience à 120°C en eau pure met en évidence le rôle de la valence du fer (et donc de la fugacité d’oxygène du système) sur les propriétés de transport de la silice, et le fait qu’un environnement réduit doit être nécessaire pour rendre viable la carbonatation de l’olivine. Enfin, une expérience similaire à 170°C montre, par la formation d’un phyllosilicate ferreux en remplacement de la silice, que la minéralogie et les propriétés passivantes des couches interfaciales évoluent avec la température. Le troisième volet de ce travail s’intéresse à la carbonatation d’une roche totale, un basalte provenant d’un site pilote de stockage de CO2 (Hellisheidi, Islande), composé de plagioclases calciques, de pyroxènes, d’oxydes de fer et d’olivines ferromagnésiennes. L’analyse minéralogique et chimique des produits de réaction à 150°C montre que c’est essentiellement l’olivine qui se carbonate. Cette étude confirme le rôle de la fO2 dans la formation de phases passivantes transitoires, et montre que le fer, lorsqu’il ne se situe pas dans le silicate, peut agir efficacement pour réduire le système et initier la formation de carbonates ferromagnésiens.
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Rodriguez, Machine Carla Thais. "Raman spectroscopic study of CO2 capture and separation by semi-clathrate hydrates crystallization and investigation of exchange processes in hydrates." Electronic Thesis or Diss., Université de Lille (2018-2021), 2021. http://www.theses.fr/2021LILUR003.
Full textAbstract:
Aujourd’hui, les combustibles fossiles sont largement brûlés pour répondre aux besoins énergétiques croissants des populations humaines et aux enjeux industriels. De grandes quantités de gaz à effet de serre sont ainsi rejetées dans l’atmosphère et contribuent au réchauffement de la planète. Pour cette raison, des techniques d’atténuation du dioxyde de carbone (CO2) efficaces et respectueuses de l’environnement sont nécessaires, comme le captage et de stockage du carbone (CCS) en post-combustion, notamment à l’aide du processus de séparation à base d’hydrates (HBSP). Le HBSP consiste en l’encapsulation de petites molécules de gaz (e.g. CO2, azote (N2), méthane (CH4)) dans des composés cristallins semblables à de la glace, formant des hydrates de clathrate ou hydrates. Des travaux antérieurs ont montré que l’ajout de promoteurs tels que le bromure de tetrabutylammonium (TBAB) améliore considérablement le mécanisme de piégeage du gaz dans l’hydrate de semi-clathrate (sc). C’est pourquoi le HBSP peut s’avérer être une technique appropriée pour le captage sélectif du CO2 et la récupération d’énergie, bien qu’il soit encore nécessaire d’approfondir les connaissances fondamentales que nous avons des processus impliqués avant de pouvoir considérer un déploiement routinier à grande échelle. Ce travail vise à mieux comprendre les processus de séparation et de capture du CO2 à l’aide de l’hydrate sc, ainsi qu’à explorer les processus d’échange dans les hydrates de clathrate pour ouvrir une perspective vers les applications industrielles.Tout d’abord, une revisite des propriétés vibrationnelles de clathrates de CO2 est effectuée par spectroscopie Raman ex-situ à haute résolution pour révéler la distribution de cette molécule dans les hydrates en fonction des paramètres composition, pression et température. Seule une étude a rapporté la répartition des molécules de CO2 dans les petites et grandes cages des hydrates, mais avec une interprétation contestable, probablement due à l’effet de la résonance de Fermi qui en complique l’interprétation. Une des nouveautés de ce travail est l’identification des changements de fréquence en fonction de l’environnement structurel du CO2, améliorant ainsi notre connaissance des mécanismes d’encapsulation. De plus, des analyses Raman à haute résolution corroborées par mesures de diffraction de neutrons sont effectuées sur des sc de TBAB à base de CO2 à des fins de caractérisation.Par la suite, l’étude se concentre sur l’influence du protocole de formation (cristallisation rapide ou lente) sur les mécanismes d’encapsulation, la structure et la sélectivité de CO2+N2-TBAB par mesures Raman in-situ. Un nouveau point de dissociation est obtenu et nos résultats Raman mettent en évidence une performance variable du système sur la sélectivité en CO2 loin de ce point, alors qu’un meilleur résultat est obtenu proche de la dissociation. De même, les facteurs de séparation atteignent leurs plus grandes valeurs proches de la dissociation, en fonction toutefois de la structure du cristal de sc. La variation morphologique de la surface est suivie par microscopie optique et présente une transformation continue avec la température (cristaux polygonaux ou empilés évoluant en cristaux de TBAB-sc cylindriques). De plus, l’influence de la cinétique de formation sur la séparation et la sélectivité du CO2 est explorée.Enfin, une application potentielle de la séparation et du captage du CO2 par HBSP est abordée en étudiant le mécanisme d’échange lors de l’exposition d’un hydrate de clathrate de CO2 à l’azote gazeux. Même si les hydrates de CO2 et de N2 cristallisent respectivement dans les structures sI et sII, après injection de N2, ils forment une structure sI avec une occupation préférentielle des petites cages par les molécules de N2. Ensuite, la cinétique d’échange est analysée avec une perspective supplémentaire de récupération de méthane par injection de CO2 et de CO2+N2<br>Nowadays, fossil fuels are constantly burnt to fulfill the increasing human and industrial demand in energy, and as a consequence, large quantities of greenhouse gases such as carbon dioxide (CO2) are released in the atmosphere and contribute to global warming. It is therefore pressing to develop efficient post-combustion CO2 mitigation techniques that are also efficient and environment-friendly, and as such, Carbon Capture and Storage (CCS) technologies involving the Hydrate-Based Separation Process (HBSP) have attracted a lot of attention. HBSP consists in encapsulating small gas molecules (e.g. CO2, nitrogen (N2), methane (CH4)) within crystalline ice-like compounds known as clathrate hydrates or hydrates. Previous works have shown that promoters like tetra-n-butyl ammonium bromide (TBAB) considerably improves the guest-gas trapping mechanism in semi-clathrate hydrate (sc). Hence, while HBSP proves to be a suitable technique for selective CO2 capture and energy recovery, advancing the fundamental understanding of processes at play is still needed before large-scale practical applications can be routinely considered. This work aims to better comprehend CO2 separation and capture processes using sc-hydrate technology, while also exploring exchange processes in hydrates to open a perspective towards industrial applications.First, the guest distribution in the hydrate phases of CO2¬-based clathrate hydrates as a function of parameters (initial composition, p, T) is revisited and elucidated by ex-situ high-resolution Raman spectroscopy. Up to now, there is a gap in the literature regarding the discrimination of the contribution of the small and large cages in CO2-based hydrates, mainly due to the Fermi resonance effect. So far, only a single study has attempted to distinguish these contributions in CO2-clathrates, however with a questionable interpretation. One of the novelties of the present work is to revisit the vibrational properties of CO2-clathrates to identify distinct frequency shifts depending on the structural environment of CO2 molecules, thereby improving our knowledge of CO2 encapsulation mechanisms in hydrates. High-resolution Raman analysis and neutron diffraction analyses are additionally performed in CO2-based TBAB-semi-clathrates for characterization purposes.Second, the influence of two different formation protocols (quick and slow crystallization protocols, commonly used in hydrate formation) on the encapsulation mechanisms, the structure, and the selectivity of CO2+N2-TBAB compounds is investigated by in-situ Raman spectroscopy. A new dissociation point (pressure and temperature) is obtained and our results highlight that slow hydrates formation rates exert a variable performance on CO2 selectivity at temperatures far from the dissociation point, while a better performance is observed when approaching dissociation. Similarly, separation factors reach their greatest values close to the dissociation, depending however on the sc crystal structure formed. Surface morphology variation is monitored by optical microscopy and exhibits a continuous transformation with temperature, starting from a rough surface coated with polygonal or stacked shaped crystals to the formation of columnar TBAB-sc crystals near dissociation. Moreover, the influence of the formation kinetics on CO2 separation and selectivity is explored.Finally, a potential application of CO2 separation and capture by HBSP is addressed through the investigation of the exchange mechanism when exposing CO2 clathrate hydrates to N2 gas. Even though CO2 and N2 hydrates crystallize in structure sI and sII, respectively, it is a CO2-N2 mixed hydrate with a preferential occupation of the small cages by N2 molecules that forms upon N2 injection. The exchange kinetics is analyzed from the perspective of methane recovery from CO2 and CO2+N2 injections
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Zeng, Liang. "Multiscale Study of Chemical Looping Technology and Its Applications for Low Carbon Energy Conversions." The Ohio State University, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=osu1354722135.
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Daval, Damien. "Processus de carbonation de basaltes et de roches ultrabasiques en conditions de subsurface." Paris 7, 2009. http://www.theses.fr/2009PA077136.
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Le piegeage mineral du co2 par carbonatation est un procede potentiellement perenne dont les cinetiques et mecanismes reactionnels sont peu connus. Ce travail a eu pour but d'identifier les principaux facteurs affectant les vitesses d'alteration et de carbonatation de silicates modeles de roches (ultra)basiques. L'influence des phases secondaires sur la cinetique d'alteration des silicates a ete etudiee. Si la formation d'une couche epaisse et poreuse de silice amorphe en surface de wollastonite ne constitue pas un obstacle a sa dissolution, l'alteration de forsterite est en revanche inhibee par une couche de silice passivante. La reaction continue alors par diffusion a l'etat solide, un processus 100000 fois plus lent que celui de dissolution. Un autre parametre controlant la vitesse d'alteration des silicates (r) est l'ecart a l'equilibre (Δg) auquel elle se deroule. Nous avons montre que la loi liant r a Δg implementee dans les codes geochimiques surestime la vitesse de dissolution du diopside d'un ordre de grandeur sur une vaste gamme de ag. Cet ecart est a l'origine d'une erreur substantielle du taux de carbonatation de diopside modelise, que nous avons calculee et corrigee. Un 3eme facteur affectant la cinetique d'alteration des mineraux provient du co2 lui-meme : son effet (distinct du ph) sur la dissolution de lizardite est intrinsequement accelerateur, surement en raison de la complexation en surface de ligands hco3'. Enfin, les interactions eau-co2-silicates ferreux peuvent conduire a la reduction du co2, un flux entrant en competition avec celui de carbonatation. L'acquisition preliminaire de donnees originales de dissolution de fayalite aidera a traiter cet aspect<br>Mineral trapping of co2 by carbonation is possibly a way to store co2 permanently. However, little is known aboutthe reaction kinetics and mechanisms of this process. Our work aimed at identifying the main parameters/dontrolling the weathering and carbonation rates of model silicates of (ultra)basic rocks. The influence of secondary phases on silicate weathering rates received detailed attention. Whereas the formation of thick and mesoporous coatings of amorphous silica onto the surface of wollastonite weakly affects wollastonite dissolution, forsterite dissolution is inhibited by a passivating silica layer. In this latter case, the reaction continues through solid-state diffusion, a process which is ~ 5 orders of magnitude slower than an interfacial dissolution mechanism. Another parameter which controls the weathering rate of silicates (r) is the distance from equilibrium (Δgr) at which it takes place. We showed that the law implemented into geochemical codes and which links r to Δgr overestimates diopside dissolution rate by one order of magnitude on a wide range of Δgr. This difference is responsible for a substantial error on the modeling of carbonation rate of diopside, which we calculated and corrected. A third factor which affects the weathering rate of minerals is due to the c02 itself: its effect (apart from that of ph) intrinsically promûtes lizardite dissolution kinetics, presumably because of the formation of surface complexes involving hco3" species. Finally, co2-h2o-fe-silicates interactions can lead to the reduction of co2, a flux which could compete with that of carbonation. Preliminary experiments of fayalite dissolution will help to resolve this question
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Zanobetti, Francesco. "Development of a multi-objective optimisation approach for the assessment of techno-economical and environmental performances of pipeline-based Carbon Capture and Storage (CCS) systems." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2021.
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It is widely recognized that Carbon Capture and Storage (CCS) may be playing a key role in decarbonising industrial and power generation processes and meeting net zero emission targets by 2050. However, the successful large-scale development of CCS is still hindered by a wide lack of reliable techno-economic and environmental assessment methodologies. In the present work, a CFD code developed by UCL Chemical Engineering, named PipeTech, was first used to simulate CO2 pipeline transport performances with respect to variations of main design and operational parameters. Based on these results, a multi-objective optimisation methodology for CCS pipelines is proposed to minimise economic and environmental footprints while reliably simulating fluid flow behaviour. Then, the Decision Maker (DM) is supposed to select one or more trade-offs that best suit his preferences. Three potentially most effective solutions were determined by applying the mathematical Level Diagrams technique. Uncertainty affecting CO2 transport cost modelling is assessed by employing a Monte Carlo simulation approach, which also provides the DM with a probabilistic tool to compare the different alternatives. Lastly, a quantitative methodology is applied to convert multi-criteria optimisation results in impact indicators weighting economic and environmental issues. Results were then compared with those given by the single minimisation of two additional indices. These are presented as a “CO2 avoided transport cost”, which considers an apparent transported flow rate decreased by emitted GHG expressed as CO2 equivalents, and as a “market-based transport cost”, which applies a carbon pricing to the greenhouse gas emissions according to carbon markets. Overall, this approach provided a route to flexibly weigh environmental and economic concerns according to DM preferences, whereas the two aggregated indices give a lower visibility to the environmental footprint of the system.
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Melendez-Ceballos, Arturo. "Adéquation de nouvelles compositions d'électrolytes et de revêtements protecteurs nanostructurés de la cathode pour les piles à combustible à carbonates fondus TiO2 protective coating processed by Atomic Layer Deposition for the improvement of MCFC cathode Electrochemical properties of Atomic layer deposition processed CeO2 as a protective layer for the molten carbonate fuel cell cathode." Thesis, Paris 6, 2017. http://www.theses.fr/2017PA066103.
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Dans ce travail, nous développons deux grands axes de recherche liés aux carbonates fondus. Le premier est l'optimisation des piles à combustible à base de carbonates fondus, avec deux approches : (i) l'amélioration de la durée de vie de la cathode grâce à des couches ultra-minces d'oxydes métalliques élaborés par la technique de dépôt de couches atomiques; (ii) la modification des électrolytes Li-K et Li-Na par addition de Cs ou de Rb. Le second est consacré à la valorisation du CO2 par sa réduction électrochimique dans les électrolytes à carbonates fondus, où nous analysons la réduction du CO2 par chronopotentiométrie et chronoamperométrie. Finalement, afin de tester les modifications subies par certains des composants analysés dans les deux premières parties, nous avons installé et adapté une configuration de cellule complète couplée à la chromatographie en phase gazeuse. Nous avons obtenu quelques résultats significatifs dans l’ensemble des approches abordées ; en ce qui concerne le point (i), nous avons constaté que TiO2 et CeO2 sont appropriés pour protéger la cathode contre la corrosion sans affecter ses propriétés électrochimiques en réduisant presque de moitié la dissolution du Ni. Les résultats obtenus pour le point (ii) sont également fructueux, car nous avons établi une méthode pour comparer deux électrolytes différents en déterminant les coefficients de diffusion des ions superoxyde et du dioxyde de carbone. Nous avons également comparé les performances de la cathode de NiO dans les électrolytes modifiés avec Cs et Rb. De ces études, nous avons constaté que l'addition de Cs améliore significativement le coefficient de diffusion de CO2 en réduisant la résistance de transfert de charge et la résistance totale à l'électrode, étant l'additif le plus prometteur testé ici. En ce qui concerne la réduction du CO2, nous avons constaté que la réaction implique des espèces adsorbées et instables et se produit en deux étapes à un électron ou une étape à deux électrons ; ainsi, il s’agit très probablement d’un mécanisme de réduction simultanée d’espèces adsorbées et dissoutes. Finalement, nous avons effectué les premiers tests sur cellule complète MCFC dans notre laboratoire, obtenant une performance et une puissance acceptables. Cependant, de petites améliorations sont encore nécessaires pour pouvoir tester les composants modifiés de cellule MCFC<br>In this work, we develop two major research routes related to molten carbonates. The first one is the molten carbonate fuel cell optimization, with two approaches: (i) cathode lifetime improvement through ultra-thin layers of metal oxides deposited by atomic layer deposition; (ii) Li-K and Li-Na electrolyte modification by Cs or Rb additions. The second one is dedicated to CO2 valorization through its electrochemical reduction in molten carbonate electrolytes, where we analyze CO2 reduction by means of chronopotentiometry and chronoamperometry. Finally, in order to test some of the component modifications described in the two first parts, we installed and adapted a single-cell setup coupled to gas chromatography. We obtained some significant results in all the approaches; concerning point (i), we found that TiO2 and CeO2 are suitable for cathode corrosion protection without affecting the electrochemical properties of the electrode and reducing almost by half the dissolution of Ni. The results obtained from point (ii) are also fruitful, since we established a method for comparing two different electrolytes and obtained the diffusion coefficients of the superoxides and carbon dioxide. We also compared the performance of the state-of-the-art NiO cathode in Cs and Rb modified electrolytes. From these studies, we found that Cs addition improves significantly the CO2 diffusion coefficient and reduces the charge transfer and total resistance at the electrode, being a promising additive. Regarding CO2 reduction, after all the tests performed, we found that the reaction involves adsorbed and instable species and occurs in two one-electron steps or in two-electron unique step; thus, it follows most probably a mechanism of simultaneous reduction of the adsorbed and dissolved species. Finally, we performed the first MCFC single-cell tests in our laboratory obtaining an acceptable cell performance and output power. However, small improvements are still necessary to be able to test MCFC modified components
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Kathe, Mandar V. "Iron-Based Chemical Looping Gasification Technologies for Flexible Syngas Production from Fossil Fuels with Carbon-di-oxide Capture: Process Systems Simulations, Techno-Economic Analysis." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1460460186.
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Neveux, Thibaut. "Modélisation et optimisation des procédés de captage de CO2 par absorption chimique." Thesis, Université de Lorraine, 2013. http://www.theses.fr/2013LORR0266/document.
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Les procédés de captage de CO2 par absorption chimique engendrent une importante pénalité énergétique sur la production électrique des centrales à charbon, constituant un des principaux verrous technologiques au déploiement de la filière. L'objectif de cette thèse est de développer et valider une méthodologie à même d'évaluer précisément le potentiel d'un procédé de captage aux amines donné. La phénoménologie de l'absorption chimique a été étudiée en détail et représentée par des modèles à l'état de l'art. Le modèle e-UNIQUAC a été utilisé pour décrire les équilibres chimiques et de phases des solutions électrolytiques et les paramètres du modèle ont été régressés pour quatre solvants. Un modèle hors-équilibre a été utilisé pour représenter le transfert couplé de matière et de chaleur, accéléré par les réactions chimiques. Les modèles ont été validés avec succès sur des données expérimentales d'un pilote industriel et d'un pilote de laboratoire. L'influence des phénomènes sur les efficacités de séparation a été explicitée afin d'isoler les phénomènes les plus impactants. Une méthodologie a alors été proposée pour évaluer la pénalité énergétique, incluant les consommations thermiques et électriques, liée à l'installation d'un procédé de captage sur une centrale à charbon supercritique. Une méthode d'estimation du coût de l'électricité est proposée pour quantifier les dépenses opératoires et d'investissement d'un tel procédé. L'environnement de simulation et d'évaluation de procédés obtenu a ensuite été couplé à une méthode d'optimisation afin de déterminer les paramètres opératoires et les dimensions des équipements maximisant les performances énergétiques et économiques<br>CO2 capture processes by chemical absorption lead to a large energy penalty on efficiency of coal-fired power plants, establishing one of the main bottleneck to its industrial deployment. The objective of this thesis is the development and validation of a global methodology, allowing the precise evaluation of the potential of a given amine capture process. Characteristic phenomena of chemical absorption have been thoroughly studied and represented with state-of-the-art models. The e-UNIQUAC model has been used to describe vapor-liquid and chemical equilibria of electrolyte solutions and the model parameters have been identified for four solvents. A rate-based formulation has been adopted for the representation of chemically enhanced heat and mass transfer in columns. The absorption and stripping models have been successfully validated against experimental data from an industrial and a laboratory pilot plants. The influence of the numerous phenomena has been investigated in order to highlight the most limiting ones. A methodology has been proposed to evaluate the total energy penalty resulting from the implementation of a capture process on an advanced supercritical coal-fired power plant, including thermal and electric consumptions. Then, the simulation and process evaluation environments have been coupled with a non-linear optimization algorithm in order to find optimal operating and design parameters with respect to energetic and economic performances
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Chomel, Mathilde. "Sylviculture intensive en région boréale : impact de la mixité des essences sur le processus de décomposition des litières et le stockage de carbone." Thesis, Aix-Marseille, 2014. http://www.theses.fr/2014AIXM4747/document.
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Depuis quelques années la sylviculture intensive prend une grande ampleur afin de rapprocher la source de fibres des usines, d'accroître la productivité des plantations, et de diminuer la pression de coupe sur les forêts naturelles. Toutefois un débat sur le type d'aménagement optimal des plantations oppose l'aménagement mono- et pluri-spécifique. Il est important de mieux comprendre le fonctionnement de ces écosystèmes pour en effectuer une bonne gestion et d'optimiser les services écosystémiques que ces plantations fournissent. La décomposition des litières et le recyclage des nutriments sont des processus complexes essentiels au fonctionnement des écosystèmes. Ainsi mon projet de thèse visait à mieux comprendre l'influence de la mixité de deux essences forestières, à savoir l'épinette blanche et le peuplier hybride, en comparaison à des plantations pures sur le processus de décomposition des litières et le stockage de carbone. Les résultats de cette étude ne montrent pas d'amélioration du processus de décomposition avec le mélange du peuplier et de l'épinette ou de leurs litières. En revanche, le mélange de ces deux espèces en plantation tamponne les effets contrastés du peuplier et de l'épinette observés dans les plantations monospécifiques. De plus, le stockage de carbone et la productivité du peuplier sont améliorés dans les plantations mixtes par rapport aux plantations monospécifiques. Les herbacées semblent être bénéfiques pour la diversité d'organismes et favorisent la libération d'azote des litières d'arbres. Cet aspect pourrait contrebalancer l'effet négatif de la présence d'herbacées qui entrent en compétition avec les arbres pour les ressources<br>The use of trees under intensive management is particularly important for rapid fibre production and for reduce cutting pressure on natural forests in boreal regions. However, a debate on the best type of plantation management opposes the mono-and pluri-specific management. Despite the possible antagonistic effects on productivity, it seems that mixed plantations would have benefits on soil properties, environmental stability, but also to maintain biodiversity and aesthetic value. It is important to better understand the functioning of these ecosystems to make good management in order to optimize ecosystem services of these plantations. Litter decomposition and nutrient cycling are essential process for the ecosystems functioning. My thesis project was to better understand the influence of the mixing of two tree species planted in comparison to monospecific plantations, namely white spruce and hybrid poplar, on the litter decomposition process and carbon storage. The results of this study showed no improvement in the decomposition process with the mixture of poplar and spruce in plantation or by their litters mixture. However, the mixture of the two species in plantation buffers the contrasting effects of poplar and spruce observed in monospecific plantations. In addition, carbon storage and productivity of poplars are improved in mixed plantations compared to monospecific plantations. Herbaceous litter appears to be beneficial for the abundance of organisms and promote the release of nitrogen from tree litter. This could offset the negative effect of the presence of grasses that compete with trees for resources
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Svanberg, Frisinger Maja-Stina. "Technoeconomical evaluation of small-scale CO2 liquefaction using Aspen Plus." Thesis, KTH, Kemiteknik, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-299662.
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Syftet med den här studien är att göra en teknoekonomisk utvärdering av processer för förvätskning av CO2 med hjälp av Aspen Plus. Ett flertal förvätskningsprocesser från tidigare studier jämfördes och från dessa valdes två förvätskningsprocesser ut för fortsatta studier och simuleringar. Dessa två förvätskningsprocesser var ett internt kylt förvätskningssystem och ett externt kylt förvätskningssystem av Øi et al., Energy Procedia 86 (2016) 500-510, som kallats system A, samt av Seo et al., International Journal of Greenhouse Gas Control 35 (2015) 1-12 kallat system B. Dessa två olika processer simulerades för teknisk analys med hjälp av Aspen Plus. Aspen Economical Analyzer (AEA) användes för att göra den ekonomiska analysen. I dessa simuleringar användes ett massflöde på 45 ton/h inkluderat vatteninnehåll, i jämförelse med tidigare studier med högre massflöden runt 100 ton/h. Elektricitet-och kylbehovet undersöktes i ett flertal olika fall med varierande kyltemperatur mellan kompressorerna. Två fall med integrering av fjärrvärme samt två fall med en värmepump undersöktes också med varierande återgående temperatur på fjärrvärmevattnet. Detta gjordes för att undersöka hur mycket värme som kan tillvaratas från förvätskningsprocessen. Vidare bestämdes även investeringskostnader samt driftskostnader med hjälp av AEA. Från detta bestämdes även den årliga kostnaden av kapitalet, CAPEX, och kostnaden att förvätska CO2 räknades ut i form av €/ton. Resultaten visade att integrering av fjärrvärme samt värmepumpar är användbart för att tillvarata på så mycket värme som möjligt från förvätskningssystemen. I de fall med en värmepump samt en återgående temperatur på 47°C i fjärrvärmenätet hade ett COP på 3.07 samt 3.15 för system A samt system B vardera. Kostanden att förvätska CO2 var 17.42 €/ton för system A samt 17.75 €/ton för system B utan använding av en värmepump samt en återgående temperatur på 47°C i fjärrvärmenätet. Vid integrering av en värmepump gick kostnaden av förvätskning upp till 20.85 €/ton för system A samt 21.69 €/ton för system B. Kostnaden av förvätskning dominerades av driftskostnader med kostnaden av kapitalet har en mindre påverkan. Utnyttjandegraden har även en stor påverkan på kostanden av förvätskning, då lägre kapaciteter visade sig leda till markant högre förvätskningskostnader. När intäkterna från fjärrvärmeproduktionen adderades till kostnadskalkylen, minskade kostnaden av förvätskning, speciellt för de system med en värmepump, där priset minskade till 10.26 €/ton för system A eller 10.98 €/ton för system B. I linje med tidigare studier pekar även dessa resultat på att det ekonomiska optimumet sammanfaller med energioptimum. Resultaten visade även att system A, det internt kylda systemet, hade den lägsta förvätskningskostanden och minsta elektricitetsförbrukningen med och utan värmepump, och därför är system A optimalt för småskalig CO2 förvätskning.<br>The aim of this study is to do a technoeconomical analysis on CO2 liquefaction systems using Aspen Plus. Several liquefaction systems from previous studies were compared, and from these, two liquefaction systems were chosen for further studies and simulations. These liquefaction systems were namely an internal liquefaction system and an external liquefaction system by Øi et al., Energy Procedia 86 (2016) 500-510, called system A and Seo et al., International Journal of Greenhouse Gas Control 35 (2015) 1-12, called system B. These systems were simulated for technical analysis using Aspen Plus, and Aspen Economical Analyzer (AEA) was used for economical studies. A small-scale liquefaction system was studied with a mass flow rate of 45 tonne/h including the water content, as compared to other studies with higher mass flow rates of around 100 tonne/h. The electricity demand and cooling demand were studied in several cases of interstage cooling between compressors. Furthermore, two cases of district heating as well as two cases of heat pumps were studied with varying return temperatures of the district heating water. This was done to study how much heat could be recovered from the liquefaction process. Furthermore, the capital expenses as well as the operating expenses were also determined using AEA. From this, the annual CAPEX and the cost of CO2 was calculated in terms of €/tonne CO2. The results showed that district heating and heat pumps can be useful to recover heat from the liquefaction processes. The simulations that included a heat pump and assumed a return temperature of 47°C had a COP of 3.07 and 3.15 for system A and B respectively. The determined cost of production was 17.42 €/tonne for system A and 17.75 €/tonne for system B when not using a heat pump and a return temperature of 47°C in the district heating grid. However, when adding a heat pump the total production cost (TPC) increased to 20.85 €/tonne for system A, and 21.69 €/tonne for system B. It was also shown that the TPC is highly dominated by the operating expenses while the total capital investment has a smaller impact on the TPC. The capacity is also important for the TPC as lower capacities was shown to lead to significantly increased production costs. When taking the revenue streams from district heating into account the TPC was decreased, in particular for the systems including the heat pumps, where the TPC for system A was 10.26 €/tonne while for system B it was 10.98 €/tonne. In accordance with previous studies it was shown that the economical optimum is closely related to the energy optimum. It was concluded that as system A, the internal liquefaction system, had the lowest TPC and electricity input with and without the heat pump and thus it is the optimal configuration for small-scale CO2 liquefaction.
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Pupier, Christophe. "Etude d'un capteur de gaz sensible au monoxyde de carbone et aux oxydes d'azote élaboré à base d'alumine bêta." Phd thesis, Ecole Nationale Supérieure des Mines de Saint-Etienne, 1999. http://tel.archives-ouvertes.fr/tel-00836902.
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Ce travail concerne le développement d'un capteur potentiométrique de gaz permettant la détection sélective du monoxyde de carbone à haute température et du dioxyde d'azote à basse température, destiné au contrôle des émissions automobiles. Le capteur est constitué de deux électrodes, une d'or, l'autre de platine, déposées sur la même face d'un électrolyte solide élaboré à base d'alumine bêta et traité par le dioxyde de soufre, l'ensemble étant plongé dans une même atmosphère de mesure. Une partie de l'étude consiste à caractériser le procédé d'élaboration de l'élément sensible élaboré sous forme de couche épaisse par la technique de sérigraphie. La seconde partie concerne une étude des phénomènes à l'origine du potentiel mesure aux bornes de notre dispositif à partir de l'observation des réponses obtenues sous oxygène. Nous proposerons alors un modèle basé sur l'adsorption compétitive de deux espèces oxygène sur les électrodes métalliques dont une sera considérée comme instable et sur un effet capacitif à l'interphase électrode métallique - électrolyte solide. La différence de potentiel aux bornes du capteur, mesurée en présence de gaz réducteur ou oxydant, est alors représentative de la différence des activités catalytiques propres à chacun des métaux et donc de leur aptitude à consommer ou produire cet espèce à leur surface. Les réponses obtenues à partir de la simulation mathématique du potentiel nous ont donné des résultats satisfaisants, capable de reproduire le comportement du capteur sous air et pour différentes concentrations de monoxyde de carbone ou de dioxyde d'azote dilués dans l'air, dans une grande gamme de températures.
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Arango, Munoz Paty. "Stripper Modification of a Standard MEA Process for Heat Integration with a Pulp Mill." Thesis, KTH, Kemiteknik, 2020. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-289162.
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De 20 största massabruken i Sverige släpper tillsammans ut ungefär 20 miljoner ton CO2 per år. Dessa utsläpp har biogent ursprung och anses därför vara klimatneutrala. Massa- och pappersindustrin är därmed en lämplig kandidat för implementeringen av BECCS (eng. Bioenergy with Carbon Capture and Storage) och har en betydande potential att nå de, av den svenska regeringen, uppsatta klimatmålen som säger att Sverige inte ska några nettoutsläpp av växthusgaser till atmosfären senast år 2045. I detta examensarbete simulerades kemiska absorptions- och desorptionsprocesser med MEA som lösningsmedel genom att tillämpa den hastighetsbaserade metoden i en rigorös modell i Aspen Plus. Stripper- och absorptionsmodellerna validerades innan standardprocessen modifierades till en konfiguration som möjliggör värmeintegration av koldioxidinfångningens överskottsvärme med, exempelvis, ett sulfatmassabruk. Avskiljningsgraden och laddning hos den mättade lösningen användes som prestandaindikatorer för att validera absorptionskolonnerna. Återkokarens energiåtgång och laddning hos den omättade lösningen användes somprestandaindikatorer för att validera stripperkolonnerna. Samtliga kolonner dimensionerades för att erhålla 90 vikt% avskiljningsgrad. Olika flödeshastigheter av lösningsmedlet testades för att säkerställa effektivt nyttjande av packningen i absorptions- och stripperkolonnerna. Lämpliga temperaturnivåer för värmeintegration, inom och utanför, koldioxidinfångningen erhölls genom att utvärdera olika varianter av en stripper-overhead-kompression konfiguration. Utvärderingen av den modifierade MEA processen tog hänsyn till potentialen för ångbesparing och energieffektivisering. Resultat från simuleringarna tyder på att den modifierade strippern skulle kunna ge besparingar på upp emot 11 % i ånganvändning. Energibesparingar i samma storleksordning kunde även erhållas genom värmeintegration mellan koldioxidinfångningen och en särskild process i ett referensbruk. Implementering av BECCS-konceptet på det här sättet skulle därmed kunna bli ett mer attraktivt alternativ för den svenska massa- och pappersindustrin att bekämpa klimatförändringarna.<br>The 20 largest pulp mills in Sweden emit around 20 million tonnes of CO2 per year. These emissions are considered carbon-neutral since they originate from biogenic sources. The pulp and paper industry is therefore a good candidate for the application of BECCS (Bioenergy with Carbon Capture and Storage) and has the potential to play a significant role for reaching the long-term mitigation target set by the Swedish government that Sweden should be climate-neutral by year 2045. In this thesis, a MEA-based chemical absorption and desorption process was rigorously modelled in Aspen Plus using the rate-based method. Validation of the absorber and stripper model was conducted before the standard process was modified to a configuration that enables heat integration of a significant amount of excess heat from the capture process in, for example, a Kraft pulp mill. CO2 removal rate and rich solvent loading were used as performance indicators to validate the absorber columns. The reboiler duty and lean solvent loading served as performance indicators in the stripper validation. The columns were dimensioned considering 90 wt% capture rate. Efficient use of the entire packing in the absorber and stripper columns was ensured by testing different solvent flow rates. Suitable temperature levels for heat integration, within and across the capture plant, were obtained through an assessment of different versions of a stripper overhead compression configuration. The evaluation of the modified MEA processes took into account the steam conservation potential and energy efficiency potential. The simulation results indicate that the modified stripper may lead to savings of up to 11% in steam consumption. Heat integration between the capture plant and a specific process in a reference Kraft pulp mill resulted in energy savings of the same order of magnitude. Thereby, making the BECCS concept a more attractive solution for the Swedish pulp and paper industry to mitigate climate change.
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Contreras, Moreno Viviana. "Captage et valorisation du CO2 par voie chimique : application à la synthèse de carbonates cycliques à partir d’époxydes." Thesis, Rouen, INSA, 2016. http://www.theses.fr/2016ISAM0021/document.
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L'utilisation du CO2 comme matière première pour la synthèse de produits à haute valeur ajoutée, comme les carbonates cycliques, est aujourd'hui l'une des alternatives proposées dans la réduction des émissions gazeuses à effet de serre. Ce travail de thèse vise à comprendre et concevoir un procédé de valorisation de CO2 à partir de la modélisation de la thermodynamique et des cinétiques de transfert de matière et de réactions, qui sont engendrées dans la synthèse de carbonates cycliques à partir des époxydes et un composé hétérocyclique comme catalyseur. Grâce à ce nouveau système, les carbonates cycliques très utilisés dans l'industrie de polymères, cosmétique ou pharmaceutique, sont obtenus avec de bons rendements, dans des conditions opératoires douces et en absence de solvants. Des propriétés thermodynamiques telles que la solubilité et la constante de Henry ont été estimées pour les systèmes binaires CO2/époxyde. L'étude du transfert de matière sans ou avec réactions a permis de déterminer respectivement le coefficient de transfert de matière en phase liquide et le régime de la réaction. Des suivis cinétiques ont été réalisés afin de proposer un modèle cinétique capable de représenter la réaction et d'estimer les paramètres cinétiques. Ces derniers ont été utilisés pour la conception préliminaire et la simulation du procédé de production du carbonate d' épichlorohydrine sur Aspen Hysys<br>Today, the utilisation of CO2 as raw material for the synthesis of high-value added products like cyclic carbonates, is one of the alternatives used for reducing greenhouse gases. This thesis aims to understand and design a CO2 valorisation process by modelling the thermodynamic and the mass transfer/reaction kinetics generated during the cyclic carbonates synthesis from CO2, epoxides and a heterocyclic compound as catalyst. By using this new catalytic system, cyclic carbonates, which are used in the polymeric, pharmaceutic or cosmetic industry, can be produced with good yields at low temperatures and pressures and without any solvent. Thermodynamic properties as solubility and Henry's law constant have been estimated for CO2/epoxide binary systems. Mass transfer occurring without and with reaction has been studied in order to determine respectively the liquid volumetric mass transfer coefficient and the reaction regime. A kinetic study has been performed to propose a model able to represent the reaction and to estimate the kinetic parameters. This information has been used in the design and the simulation of the production process of epichlorohydrin carbonate on Aspen Hysys
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Fascetta, Eliette. "Étude d'un capteur potentiométrique élaboré à partir d'alumine-bêta. Interprétation des phénomènes électrochimiques observés en présence de dioxyde de soufre et de monooxyde de carbone." Phd thesis, Ecole Nationale Supérieure des Mines de Saint-Etienne, 1993. http://tel.archives-ouvertes.fr/tel-00844391.
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Ce travail concerne l'étude d'un dispositif original pour la détection de gaz tels que le dioxyde de soufre et le monooxyde de carbone. Il s'agit d'un capteur électrochimique développé à partir d'un électrolyte solide, l'alumine-bêta, sur lequel sont déposées par pulvérisation cathodique deux électrodes métalliques de propriétés catalytiques différentes: l'une est en or, l'autre est en platine. La force électromotrice mesurée entre les deux électrodes est représentative de la concentration en gaz réducteurs présents dans l'atmosphère. Les performances électriques obtenues sont très nettement améliorées par un prétraitement gazeux au dioxyde de soufre qui assure la formation d'une couche épaisse de sulfate de sodium à la surface de l'alumine-bêta. La stabilité sous air devient tout à fait remarquable et la sensibilité au monooxyde de carbone, par exemple, est multipliée par deux. L'origine des phénomènes électriques obtenus sur un tel dispositif ne comportant qu'un seul compartiment gazeux est proposée sur la base d'un mécanisme cinétique diffèrent au niveau des deux catalyseurs métalliques. Ce modèle permet d'interpréter les influences de la pression du gaz réducteur et de la pression d'oxygène sur les variations de la force électromotrice enregistrée
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Bernachot, Isabelle. "Utilisation des isotopes stables du chlore pour le traçage des processus générés par l'injection de CO2 au sein d'un réservoir géologique." Thesis, Sorbonne Paris Cité, 2017. http://www.theses.fr/2017USPCC016/document.
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L’injection de CO2 dans un réservoir géologique n’a rien d’un processus anodin : les impacts sur la roche hôte peuvent menacer l’intégrité du stockage suite à des modifications des propriétés pétrophysiques. Nous proposons ainsi d’envisager l’utilisation des isotopes stables du chlore comme indicateurs des processus physicochimiques générés par une injection de CO2. L’ion chlorure Cl- est en effet un élément conservatif et ubiquiste dans les eaux des réservoirs, et le rapport δ37Cl est connu pour être modifié par divers processus (diffusion, filtration ionique, précipitation de sel, changements de phase). La méthodologie adoptée a consisté à investiguer les effets de ces différents processus sur le signal isotopique du Cl en conditions P-T d’un réservoir de stockage. Des expériences en autoclaves ont montré que le Cl était solubilisé dans le CO2sc, mais en quantités suffisamment faibles pour ne pas impacter le signal isotopique dans les saumures si fractionnement isotopique il y a. Des expériences de migration d’une saumure réactive par advection (banc de percolation ICARE1, Université de Montpellier) et par diffusion (cellule développée à IFPEN) ont également été réalisées. Aucune évolution de δ37Cl n’a été mesurée au cours de la percolation (transport advectif conservatif) et les effets de la diffusion restent à évaluer et à mettre en relation avec les évolutions de porosité et perméabilité des roches. Les expériences de séchage et de précipitation de sel en milieu poreux ont montré que les concentrations en Cl et les valeurs de δ37Cl permettaient de caractériser les processus de transport en jeu. Ces résultats expérimentaux ont permis d’identifier des processus capables de modifier les abondances isotopiques de Cl et indiquent l’intérêt des isotopes pour le monitoring de site de stockage de CO2<br>CO2 injection in a reservoir leads to physicochemical processes which can have harmful consequences on the reservoir integrity due to porosity and permeability alteration. In this work, we propose to test the possibility that stable chlorine isotopes could be used as a geochemical tool to assess these effects. Indeed, chloride is a conservative and a major component of reservoir brines, and it is already known that several processes can modify the ratio of its two stable isotopes δ37Cl (diffusion, ionic filtration, salt precipitation or phase change). To test this possibility, several types of experiments were performed to investigate the effects generated by a CO2 injection on Cl-isotopes. Autoclave experiments have shown that Cl can be solubilized in CO2SC, but the amounts would be too low to modify the isotopic signal of brines in case of any fractionation process. Reactive brine migration experiments by advection (ICARE1 percolation apparatus in Montpellier University) and diffusion (diffusion cell developed at IFPEN) were also conducted. No δ37Cl was observed during percolation (conservative advective transport) and the effects of diffusion remain to be investigated with regard to the evolution of rock porosity and permeability. Drying and salt precipitation experiments on porous media have shown that Cl concentrations and δ37Cl values can give information about transport processes during water evaporation. These experimental results allowed us to identify the processes capable of modifying the δ37Cl signal, and that Cl-isotopes can be of use for the monitoring of CO2 storage site
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Niva, L. (Laura). "Self-optimizing control of oxy-combustion in circulating fluidized bed boilers." Doctoral thesis, Oulun yliopisto, 2018. http://urn.fi/urn:isbn:9789526221304.
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Abstract Energy production in combustion power plants is a significant source of anthropogenic carbon dioxide emissions. The targets of international climate agreements call for utilizing all available technologies to achieve rapid and cost-effective emission reductions. Carbon capture and storage is one of the possible technical solutions applied in combustion power plants. Circulating fluidized bed boilers have gained increasing popularity due to advantages in availability, emission control, fuel flexibility and option for using challenging fuels, and the possibility of using high-efficiency steam cycles. In the novel process of oxy-combustion, combustion air is replaced by a mixture of oxygen and recycled flue gas to facilitate the capture of carbon dioxide from the flue gas flow. Additional degrees of freedom become available for combustion control as the gas flow and composition can be controlled separately for fluidization and combustion purposes. In the research for this thesis, self-optimizing control was applied for the control structure design of a circulating fluidized bed boiler. Self-optimizing control offers a systematic tool for the early phases of control design, in which decisions have traditionally been made based on intuition, heuristics and previous experience. The self-optimizing control approach searches for controlled variables without a need for constant setpoint optimization when the process is affected by disturbances and implementation errors. Results presented in the thesis show that self-optimizing control can be applied in the control structure design of circulating fluidized bed combustion. A range of control structure alternatives were evaluated using steady-state approximations of a validated process model. For the novel oxy-combustion process, promising control structures were identified and could be dynamically demonstrated<br>Tiivistelmä Energiantuotanto polttovoimalaitoksissa on merkittävä hiilidioksidipäästöjen lähde. Kansainväliset ilmastotavoitteet edellyttävät kaikkien käytettävissä olevien teknologioiden hyödyntämistä päästövähennysten aikaansaamiseksi nopeasti ja kustannustehokkaasti. Hiilidioksidin talteenotto on yksi mahdollisista teknisistä ratkaisuista polttovoimalaitoksissa. Kiertoleijukattilat ovat saavuttaneet kasvavaa suosiota etuinaan hyvä käytettävyys, tehokas päästöjen hallinta, soveltuvuus erilaisten haastavienkin polttoaineiden hyödyntämiseen ja mahdollisuus tehokkaiden höyrykiertojen käyttöön. Uudessa happipolttoprosessissa palamisilma korvataan hapen ja kierrätetyn savukaasun seoksella, mikä mahdollistaa hiilidioksidin talteenoton savukaasuista. Kiertoleijupolton säädön kannalta vapausasteet lisääntyvät, sillä leijutukseen ja polttamiseen käytettävän kaasun määrää ja koostumusta voidaan säätää erikseen. Väitöstutkimuksessa käytettiin itseoptimoivaa säätöä kiertoleijukattilan säätörakenteiden suunnitteluun. Itseoptimoiva säätö tarjoaa systemaattisen menetelmän säätösuunnittelun alkuvaiheeseen, jossa päätöksenteko on perinteisesti tehty esimerkiksi intuition, heuristiikan ja aiempien ratkaisujen perusteella. Menetelmän tavoitteena on löytää säädettävät muuttujat, joiden asetusarvot eivät vaadi jatkuvaa optimointia, vaikka prosessiin vaikuttavat erilaiset häiriöt ja mittausvirheet. Väitöstutkimuksen tulokset osoittavat, että itseoptimoiva säätö soveltuu kiertoleijupolton säätörakenteiden suunnitteluun. Erilaisten säätörakenteiden toimivuutta arvioitiin käyttäen validoidun prosessimallin tasapainotilan approksimaatioita. Uudelle happipolttoprosessille löydettiin lupaavia säätörakenteita, joiden toimintaa voitiin demonstroida myös dynaamisesti
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Rhino, Kévins. "Caractérisation, quantification et modélisation des processus de transfert et des interactions CO₂-eau-roche en milieu poreux non saturé en contexte de forage lors d'un stockage géologique." Thesis, Bordeaux 3, 2017. http://www.theses.fr/2017BOR30040/document.
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Le stockage géologique du carbone est l’une des techniques les plus prometteuses pour réduire le taux de CO₂ dans l’atmosphère. La séquestration géologique possède la capacité et la longévité potentielles pour diminuer les émissions de CO₂ vers l’atmosphère. Dans le cadre d’injections à l’échelle industrielle, les réservoirs carbonatés peuvent faire partie des sites aptes à stocker du CO₂. Toutefois, ces injections à grandes profondeurs sont sujettes à des risques de fuites du piège géologique lui-même ou des infrastructures liés à l’exploitation du site de stockage. Ainsi, il existe principalement deux types de fuite : brutale et diffuse. Dans les deux cas, elles sont susceptibles d’entrainer des risques pour l’environnement et de mettre en danger les populations. Il est ainsi nécessaire de développer des outils capables de prévenir une fuite de CO₂ quel que soit son type. Par ailleurs, il est particulièrement indispensable de comprendre les mécanismes de transport réactif qui rentrent en jeu lors de l’arrivée de cette fuite en contexte de proche surface (zone vadose) et ainsi d’essayer d’étudier comment cette fuite peut s’amortir. Ces travaux de thèse traitent donc de la caractérisation, de la quantification et de la modélisation des processus de transferts et des interactions CO₂-H₂O-CaCO₃ dans la zone vadose en contexte de fuite à partir d’un puits de forage. Cette problématique a été d’abord abordée par une approche expérimentale sur un site pilote à Saint-Emilion. Puis, les interactions CO₂-H₂O-CaCO₃ ont été étudiées au travers d’une approche expérimentale à l’échelle de la carotte en laboratoire. L’approche expérimentale a conduit à la réalisation de deux fuites dans la zone vadose du site pilote : une fuite diffuse et une fuite ultra diffuse. Elles furent réalisées dans la continuité des expériences qui avaient déjà eu lieu auparavant. Une comparaison de l’ensemble des fuites a montré la nécessité d’utiliser des gaz nobles comme précurseurs de l’arrivée en surface du CO₂. Selon le type de fuite, l’hélium peut servir de précurseur temporel du CO₂, tandis que le krypton prévient de l’étendue du panache de gaz durant la fuite. Plus la pression d’injection du CO₂ est importante et plus le gaz migre par advection. Par ailleurs, une pression d’injection importante favorise l’existence de passage préférentiel dans la zone vadose. L’utilisation d’isotopes tels que ceux de l’hélium et du carbone permet de mettre en évidence la présence locale de phases aqueuses dans le massif et de déterminer l’origine biologique ou anthropique du CO₂. Les expériences à l’échelle de la carotte permettent d’estimer le pouvoir tampon des calcaires oligocènes en fonction du faciès de la roche. La perméabilité et la porosité de celle-ci conditionnent la dissolution des calcaires. De même, la réactivité des carbonates en contexte de fuite dépend du pH de la phase aqueuse, du débit qui traverse le réseau poreux, de la saturation en eau et des caractéristiques pétro-physiques des carbonates<br>Carbon storage is one of the most encouraging methods to decrease CO₂ concentration into the atmosphere. Carbon storage provides the longevity and the capacity needed to decrease CO₂ emissions toward the atmosphere. When dealing with storage on an industrial scale, carbonated reservoirs can be among the most suitable storage sites. However, these high depth injections are subject to leakage risks from the geologic trap itself or from the framework created by the establishment of the site. Two main types of leakage exist: brutal and diffusive leakage. In both cases, they are likely to endanger the environment and the population. Therefore, it is essential to develop tools that are able to anticipate any types of CO₂ leakage. Furthermore, it is also necessary to understand the reactive transport mechanism that take place when the leakage arrives in the shallow subsurface (vadose zone)and to see how the leakage can be buffered. This work deals with the characterization, the quantification and the modelling of transfer processes and CO₂-H₂O-CaCO₃ interactions into the vadose zone in a context of a leakage from a drilling well. This issue was first dealt through field experiment on the site of Saint Emilion. Then, the CO₂-H₂O-CaCO₃ interactions were studied through an experimental approach in laboratory. Two leakage experiments were performed on the site: a diffusive leakage and an ultra-diffusive leakage. They were performed as a sequel of former experiments carried on the pilot site. A comparison of all the leakage experiments revealed the necessity to use noble gases as precursor of the CO₂ arrival at the surface. Depending of the type of the leakage, helium can be a temporal precursor while krypton can anticipate the spread of the CO₂ gas plume. The higher the injection pressure, the more the gas migrates through advective flux. Moreover, a high injection pressure favors the existence of preferential paths in the vadose zone. The use of helium and carbon isotopes makes it possible to reveal the presence of a local aqueous phase within the porous media and to identify the origin of CO₂. The core scale experiments lead to the estimation of the buffering power of Oligocene limestone according to the rock facies. The permeability and the porosity influence the dissolution of the limestone. The reactivity of carbonates during a leakage depends on the pH of the aqueous phase, the flow rate that goes through the porous media, the water saturation and petrophysical characteristics of the carbonates
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Piriou, Patrice. "Caractérisation et modélisation d'un procédé pilote de captage de CO2 par carbonatation des saumures alcalines et séparation des phases en colonnes de flottation." Thesis, Université de Lorraine, 2014. http://www.theses.fr/2014LORR0136/document.
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Le procédé Solvay génère d’énormes quantités de saumures résiduaires au pH alcalin contenant portlandite, brucite et silicates de calcium hydratés. La carbonatation conduit à un abaissement du pH, ce qui favorise la formation de deux phases majoritaires : la calcite et le gypse. L’objectif de la thèse est de valoriser les saumures résiduaires carbonatées par séparation des phases en colonne de flottation. L’étude de la carbonatation en réacteur batch, puis en colonne de carbonatation pilote montre qu’il est préférable de ne pas carbonater les saumures résiduaires jusqu’à l’équilibre thermodynamique. En effet, la mise en solution de métaux lourds intervient à partir d’un pH de l’ordre de 7,5, ce qui limiterait les rejets des saumures dans l’environnement. En outre, une carbonatation brusque et incomplète est souhaitable pour une meilleure séparation des phases par flottation. Les essais de flottation réalisés sur une colonne de 7,6 cm de diamètre et de 3 m de haut ont montré une faisabilité de la séparation des deux minéraux calciques avec l’oléate de sodium comme collecteur malgré une abondante littérature incitant à la prudence. La différence entre la taille des particules de carbonates et celle des particules de sulfates et leurs hydratations de surfaces, ainsi qu’une force ionique élevée du milieu permettent une bonne séparation des phases. Une étude des saumures synthétiques permet de mettre en évidence le rôle des cations métalliques (nature, rayon, charge…) sur la coalescence des bulles dans les conditions dynamiques et dans un milieu à forte force ionique. Une étude des paramètre de fonctionnement effectué sur une colonne de 30,5 cm de diamètre et de 10 m de haut ont permis la modélisation du procédé de flottation en colonne dans le but de proposer une procédure de dimensionnement du procédé industriel. La confrontation des résultats de simulation aux résultats réels permet la détermination des intensités des microprocessus de flottation (attachement/détachement), et conduit à la proposition d’une installation industrielle avec deux colonnes de flottation en série<br>Solvay process generates huge amounts of waste brines at alkaline pH containing portlandite, brucite and calcium silicate hydrates. Carbonation leads to lowering of pH which favors formation of two predominant phases: calcite and gypsum. The aim of this thesis is to develop carbonated waste brines valorization by phase separation in flotation column Study of carbonation in a batch reactor and in a carbonation pilot column shows it is preferable not to carbonate waste brines until thermodynamic equilibrium. Indeed dissolution of heavy metals occurs from a pH of about 7.5 thereby limiting discharge of brines in the environment. In addition, a sudden and incomplete carbonation is appropriate for phase separation by flotation. Flotation tests carried out in a 7.6 cm diameter and 3 m high column showed feasibility of the separation of the two calcium minerals using sodium oleate as a collector despite abundant literature for caution. The differences between the particle size of carbonates and sulfates and their surface hydration, as well as the high ionic strength of the medium allow an efficient separation of phases. Study of synthetic brines highlights the role of metal cations (nature, radius, charge…) on bubble coalescence in dynamic conditions in an environment with high ionic strength. Study of operation parameter performed on a 30.5 cm diameter and 10 m high column enabled the modeling of the column flotation process in order to provide a scale-up procedure of industrial process. Comparison of simulation results with actual results allows the determination of intensities of flotation subprocesses (attachment/detachment), and led to the proposal of an industrial plant with two flotation columns in series
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Peuble, Steve. "Caractérisation expérimentale des processus d’hydratation et de carbonatation des roches basiques et ultra-basiques." Thesis, Montpellier 2, 2014. http://www.theses.fr/2014MON20017/document.
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Depuis le milieu des années 90, la minéralisation in situ du CO2 est envisagée comme une solution durable et efficace pour limiter ses émissions anthropiques vers l'atmosphère. Il s'agit de récupérer le CO2 émis par certaines industries pour le piéger en profondeur sous forme minérale (carbonates) dans les aquifères mafiques et ultramafiques naturels (de type basaltes et péridotites). La carbonatation du CO2 a été largement décrite dans les systèmes naturels où elle apparait à travers une série de réactions chimiques couplées au transport des espèces réactives dans le fluide. Plusieurs expériences en réacteurs fermés ont été menées depuis une quinzaine d'années afin de mieux comprendre les paramètres physico-chimiques contrôlant ces réactions. Mais très peu d'études n'ont encore caractérisé les processus de transport-réactif au cours de l'injection et de la minéralisation in situ du CO2 dans ces roches.Ces travaux visent à répondre à 3 principaux objectifs : (i) caractériser l'évolution des chemins réactifs lors de l'injection de CO2 dans des roches (ultra-)mafiques, (ii) mesurer les effets en retour des réactions sur les propriétés hydrodynamiques du milieu et (iii) quantifier le rendement et la pérennité des processus sur le long terme. Ils s'appuient sur le développement de protocoles expérimentaux pour (i) reproduire l'injection de CO2 dans les roches (ultra-)mafiques et (ii) caractériser les réactions à l'aide d'une série d'outils géochimiques et analytiques de l'échelle atomique à centimétrique. Trois séries d'expériences de percolation réactive ont été réalisé sur des agrégats (ultra-)mafiques relativement simples (olivines de San Carlos et d'Hawaii) et plus complexes (basaltes de Stapafell) dans des conditions de P-T-confinement in situ (Ptot=10-25 MPa ; T=180-185°C;Pconf=15-28 MPa).Les résultats obtenus ont permis de différencier plusieurs chemins réactifs dans ces systèmes en fonction du transport du fluide, de la porosité du milieu, des hétérogénéités locales de la roche, de la minéralogie et/ou des variations locales de la composition chimique du fluide. Les calculs du bilan de masse ont révélé une minéralisation efficace du CO2 contrôlée par les propriétés chimiques et hydrodynamiques du milieu. Mais certaines réactions associées à l'altération des roches (ultra-)mafiques (hydratation) ont des effets en retour négatifs sur les propriétés réservoirs de la roche (porosité, perméabilité) pouvant compromettre la pérennité du stockage du CO2 dans les aquifères naturels sur le long terme.Ces nouvelles données permettront aux modèles numériques de mieux simuler la carbonatation des roches (ultra-)mafiques en connaissant les propriétés hydrodynamiques du milieu et les hétérogénéités structurales du réservoir. Elles suggèrent aussi qu'un meilleur contrôle de certains paramètres d'injection, comme le débit ou la composition du fluide injecté (ex: pCO2), permettrait d'améliorer le taux et le rendement de la carbonatation<br>Since the mid-90s, in situ mineralization of CO2 has been considered as a safe and efficient solution to mitigate its anthropogenic emissions to the atmosphere. It is to recover the CO2 emitted by some industries and trap it in the mineral form (carbonates) in mafic and ultramafic aquifers (e.g. basalts and peridotites). The carbonation of CO2 has been widely described in natural systems where it occurs through a series of complex chemical reactions coupled to the transport of reactive species in the fluid. Numerous experiments have been conducted in batch reactors over the past fifteen years to better understand the physico-chemical parameters controlling the carbonation of (ultra-)mafic rocks. But few studies have further characterized the coupling reactive-transport processes during the injection and in situ mineralization of CO2 in these rocks.This work aims to meet 3 main objectives: (i) characterize changes in reaction paths during the injection of CO2 in (ultra-)mafic systems, (ii) measure the feedbacks effects of chemical reactions on the hydrodynamic rock properties and (iii) quantify the efficiency and sustainability of such processes over long time periods. It is based on the development of experimental protocols to (i) reproduce the injection of CO2 into (ultra-)mafic rocks and (ii) characterize the reactions using a series of geochemical and analytical tools from the atomic to the centimetric scale. Three series of reactive percolation experiments have been performed on (ultra-)mafic aggregates from relatively simple (olivines from San Carlos and Hawaii) to more complex samples (basalts from Stapafell) under in situ P-T-containment conditions (Ptot=10-25 MPa; T=180-185°C; Pcont=15-28 MPa).The results allowed us to differentiate several reactions paths in these systems depending on the fluid transport, rock porosity, local hydrodynamic properties, mineralogy and/or local changes in the fluid composition. Mass balance calculations have revealed an efficient mineralization of CO2 in the samples. It is controlled by the chemical and the hydrodynamic properties of the rock at the pore scale. But some reactions associated with the alteration of (ultra-)mafic rocks (e.g. hydration) have negative feedbacks effects on the reservoir rock properties (porosity and permeability) that may compromise the sustainability of CO2 storage in natural aquifers in the long term.These new supporting data will allow numerical models to better simulate the carbonation of (ultra-)mafic rocks knowing the hydrodynamic properties and the structural heterogeneities of the reservoir. They also suggest that a better control of some injection parameters, such as the flow injection rate and the injected fluid composition (e.g. pCO2), would improve the rate and yield of CO2 mineralization in these systems
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Sergienko, Ekaterina. "Adapted reservoir characterization for monitoring and uncertainty analysis of CO2 storage." Toulouse 3, 2012. http://thesesups.ups-tlse.fr/2019/.
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L'analyse de risques du stockage géologique de CO2 consiste à simuler la dynamique du processus de stockage et à évaluer la probabilité de fuites. L'approche proposée dans ce travail consiste à utiliser des surfaces de réponses basées sur les processus Gaussiens, cela permet de réduire le grand nombre d'appels au simulateur de réservoir nécessaire à cette analyse. Dans cette thèse des méthodes innovantes sont étudiées pour résoudre les problèmes suivants: 1. Emplacement des puits d'injection 2. Estimation de la fiabilité 3. Analyse de sensibilité fiabiliste Pour résoudre le premier problème nous proposons une méthode de surface de réponse pour gérer les paramètres discrets (positions des puits) et les sorties fonctionnelles discrètes (évolution de pression du réservoir). Par ailleurs, nous introduisons une nouvelle méthode pour la modélisation des réponses variées dans le temps. Pour cela, la caractérisation des courbes est effectuée en utilisant des modèles à forme invariante. Pour le problème de fiabilité, nous avons développé une approche combinant la méthode de réduction d'ensemble et le krigeage. Un échantillonnage adaptatif est construit afin d'améliorer itérativement l'estimation de la probabilité de défaillance du modèle. Pour répondre au dernier problème, nous proposons une méthode pour l'analyse de sensibilité fiabiliste. Elle est basée sur une perturbation de la distribution de probabilité des variables d'entrée afin de trouver les facteurs qui contribuent le plus à la variabilité de la probabilité de défaillance. Toutes les méthodes proposées ont été testées numériquement sur des exemples analytiques et des cas test de stockage de CO2<br>Risk analysis of CO2 geological storage involves the simulation of the dynamics of the storage process and the evaluation of the probability of the possible leakage events. The approach followed here focuses on Gaussian Process response surface modelling in order to reduce the number of calls to the expensive reservoir simulator. Three major problems related to uncertainty analysis of CO2 storage are addressed: 1. Injection well placement 2. Reliability estimation 3. Reliability sensitivity analysis To tackle the first problem we provide a response surface method to handle discrete parameters (well positions) and discrete functional outputs to treat responses varying trough time (reservoir pressure evolutions). In addition, we introduce a new method for modelling functional outputs based on curves characterization and involving shape invariant model. To address the reliability problem, we introduce a subset simulation algorithm linked with the Gaussian Process model. It involves adaptive experimental design refinement and the model updating. To solve the last problem we suggest a new method for reliability sensitivity analysis. It is based on a perturbation of a probability distribution of input variables in order to evaluate which one contributes the most in the variability of the failure probability. All the proposed methods have been numerically tested on analytical and CO2 storage examples