Les injections de CO2 à l'échelle industrielle, dans les aquifères salins profonds, vont affecter le système naturel en induisant des perturbations des gradients de pression à court et à moyen terme.Des études prévisionnelles sont nécessaires pour évaluer les risques de contamination (fuites de CO2, déplacement des fluides natifs) et les risques d'interférences entre projets d'injection ou entre utilisations du sous-sol.Les aquifères salins étant généralement peu caractérisés, les incertitudes géologiques sont à considérer lors de l'étude de faisabilité du stockage et des risques associés puisque les paramètres géologiques influencent la réponse du système à l'injection.Nous nous sommes intéressés aux incertitudes résultantes en termes de prévisions de perturbations de pression et de migration de CO2 et à leurs conséquences sur la faisabilité des projets de stockage.Dans un premier temps, les incertitudes de modélisation (changement d'échelle, résolution de la variabilité spatiale des propriétés pétrophysiques) et géologiques (propriétés pétrophysiques de la formation d'injection et de la couverture) ont été étudiées sur des modèles 2D conceptuels. L'objectif étant de balayer les champ d'incertitudes pour des modèles peu coûteux en temps de calcul, pour ensuite, réduire les évaluations à effectuer dans le cadre de la modélisation 3D régionale du système souterrain et y appliquer des méthodes simplifiées, validées en deux dimensions.Des centaines de réalisations stochastiques sont utilisées pour évaluer l'influence de la variabilité spatiale de la perméabilité. Pour limiter le nombre de simulations d'écoulement à effectuer, des méthodes de sélection de réalisations, à partir de "proxy-response" (i.e. approximation de la réponse par une méthode de calcul simplifiée) ont été testées et validées.Ensuite, les modèles 3D sont construits à partir des données d'un modèle hydrogéologique du bassin parisien. Différents scénarios d'injection sont envisagés. La sensibilité de la réponse est étudiée principalement par rapport à la variabilité spatiale de la perméabilité et à la compressibilité des pores. Cette dernière étape permet de mieux appréhender les risques d'interférences en fonction des incertitudes majeures, d'une part des paramètres géologiques, et d'autre part des paramètres physiques liés à l'injection. / This thesis studies the regional-scale response of an aquifer system to a massive CO$_2$ injection. Industrial-scale CO$_2$ injections into deep saline aquifers affect natural groundwater systems by generating short-term to medium-term pressure gradient perturbations. To evaluate contamination risks and interference risks between injection projects or other uses of underground space, modelling studies become necessary. The geological parameters of underground formations are also to be taken into consideration as they certainly influence the injection reponse. But, saline aquifers are generally poorly-characterized which adds uncertainties to an already complex system. This thesis aims to explore uncertainties in pressure perturbations and CO$_2$ migration predictions, and their consequences in terms of CO$_2$ storage feasibility studies. Firstly, modelling and geological uncertainties have been tested on 2D conceptual models. This step, based on simpler models than 3D ones, allows a fast uncertainties discrimination and save computational time. Hundreds of stochastic realizations are generated to define the influence of permeability spatial variability. To limit the number of flow simulations, selection procedures of realizations are applied and tested. Selections are derived from fast-calculations methods called "`proxy-response"'. Secondly, once these methods have been 2D tested and validated, and once a number of uncertainties have been eliminated, these methods and related ones are applied to the underground system 3D modelling. The 3D models have been built based on available data from an existing Paris Basin hydrogeological model. Several injection scenarios have been considered and tested. Permeability spatial variability and pore compressibility are the two main parameters chosen to evaluate the injection response. This last step allows a better definition of interference risks between the major uncertainties from geological parameters and injection-related physical parameters.

Green hydrogen produced through electrolysis of excess renewable energy is a promising seasonal energy storage solution with the potential to decarbonize the energy sector. However, it has physical properties that make it difficult to store and transport on a large scale for grid scale storage applications. An alternative to storing excess renewable energy in hydrogen is converting the hydrogen to synthetic fuel that has an industrially mature production process and an established transportation, storage and distribution infrastructure. This study aims to conduct a feasibility analysis to compare the cost and compatibility of green hydrogen, ammonia, methane and methanol as seasonal energy storage. The production of each fuel and the barriers to their commercialization as energy vectors is discussed. The hydrogen storage technologies holding the most potential are identified as salt cavern and lined rock cavern storage however type I-IV pressure vessel storage is also included in the analysis due to its prevalence within the industry The outcome of the study is a conceptual model calculating the levelized cost of storage of each fuel considering the storage system size, compression energy required and annualized CAPEX and OPEX of compression and storage. Three cases are developed to analyse the storage system, A- seasonal discharging, B-weekly discharging and C- daily discharging. The results identify that the most feasible seasonal storage option for hydrogen is utilizing a salt cavern. If building a salt cavern is infeasible due to geographical constraints, a lined rock cavern is more cost-effective as compared to utilizing pressure vessel storage. For shorter storage periods or smaller scale applications it is more beneficial to employ low pressure (200-300 bar) pressure vessel storage since geological storage becomes expensive as compared to the seasonal case. Low pressure storage is better suited for smaller applications as compression costs account for a significant share of the total annual cost of each storage system in the weekly and daily cases. The most suitable hydrogen storage option is highly dependent on the end use application. Overall, methanol storage provided the lowest levelized cost of storage in all scenarios. / Grönt väte som produceras genom elektrolys av överskott av förnybar energi är en lovande säsongsbaserad energilagringslösning med potential att koldioxidutlösa energisektorn. Det har dock fysiska egenskaper som gör det svårt att lagra och transportera i stor skala för lagringsapplikationer i nätskala. Ett alternativ till att lagra överskott av förnybar energi i väte är att omvandla vätgas till syntetiskt bränsle som har en industriellt mogen produktionsprocess och en etablerad transport-, lagrings- och distributionsinfrastruktur. Denna studie syftar till att genomföra en genomförbarhetsanalys för att jämföra kostnaden och kompatibiliteten för grönt väte, ammoniak, metan och metanol som säsongsbetonad energilagring. Produktionen av varje bränsle och hindren för deras kommersialisering som energivektorer diskuteras. De tekniker för lagring av väte som har störst potential identifieras som lagring av saltrum och fodrad bergrum, men lagring av tryckkärl av typ I-IV ingår också i analysen på grund av dess förekomst inom industrin Resultatet av studien är en konceptuell modell som beräknar den utjämnade kostnaden för lagring av varje bränsle med hänsyn till lagringssystemets storlek, kompressionsenergi som krävs och årlig CAPEX och OPEX för kompression och lagring. Tre fall är utvecklade för att analysera lagringssystemet, A-säsongsurladdning, B-veckotursning och C-daglig urladdning. Resultaten visar att det mest möjliga säsongsbetonade lagringsalternativet för väte är att använda en saltgrotta. Om det är omöjligt att bygga en salthåla på grund av geografiska begränsningar, är en fodrad berghåla mer kostnadseffektiv jämfört med att använda tryckkärlslagring. För kortare lagringsperioder eller tillämpningar i mindre skala är det mer fördelaktigt att använda lågtrycks (200-300 bar) tryckkärllagring eftersom geologisk lagring blir dyr jämfört med säsongsfallet. Lågtryckslagring är bättre lämpad för mindre applikationer eftersom kompressionskostnaderna står för en betydande del av den totala årliga kostnaden för varje lagringssystem i vecko- och dagliga fall. Det mest lämpliga vätgaslagringsalternativet är starkt beroende av slutanvändningsapplikationen. Sammantaget gav metanollagring den lägsta utjämnade kostnaden för lagring i alla scenarier.

The geological sequestration of carbon dioxide (CO2) is one of the options of controlling the greenhouse gas emissions. However, leakage of CO2 from the storage reservoir is a risk associated with geological sequestration. Over longer times, large-scale groundwater motion may cause leakage of dissolved CO2 (CO2aq). The objectives of this thesis are twofold. First, the modelling study analyzes the leakage of CO2aq along the conducting pathways. Second, a relatively safer mode of geological storage is investigated wherein CO2aq is injected in a carbonate reservoir. A reactive transport model is developed that accounts for the coupled hydrological transport and the geochemical reactions of CO2aq in the porous media. The study provides a quantitative assessment of the impact of advection, dispersion, diffusion, sorption, geochemical reactions, temperature, and heat transport on the fate of leaking CO2aq. The mass exchange between the conducting pathway and the rock matrix plays an important role in retention and reactions of leaking CO2aq. A significant retention of leaking CO2aq is caused by its mass stored in aqueous and adsorbed states and its consumption in reactions in the rock matrix along the leakage pathway. Advection causes a significant leakage of CO2aq directly from the reservoir through the matrix in comparison to the diffusion alone in the rock matrix and advection in a highly conducting, but thin fracture. Heat transport by leaking brine also plays an important role in geochemical interactions of leaking CO2aq.  Injection of CO2aq is simulated for a carbonate reservoir. Injected CO2-saturated brine being reactive causes fast dissolution of carbonate minerals in the reservoir and fast conversion of CO2aq through considered geochemical reactions. Various parameters like dispersion, sorption, temperature, and minerals reaction kinetics are found to play important role in the consumption of CO2aq in reactions. / <p>Research Funders:</p><p>(i) Higher Education Commission (HEC) of Pakistan</p><p>(ii) Lars Erik Lundberg Scholarship Foundation, Sweden</p>

A necessidade atual do mercado brasileiro para aumentar a oferta de gás incentiva a comunidade científica nacional no desafio de desenvolvimento de novas rotas tecnológicas, visando aumentar o aproveitamento do gás natural. Tal desafio é acompanhado por uma demanda mundial dos países signatários do Protocolo de Quioto (ratificado em 2005) para a redução das emissões de gases de efeito estufa. Apesar de o Brasil não apresentar nenhuma meta de redução, no primeiro período deste Protocolo (2008 a 2012), o setor do petróleo (atividade de E&P), através de suas companhias operadoras, que atuam no país, já estabeleceram metas corporativas para emissão evitada de gases de efeito estufa, em suas instalações de produção (maior predominância das unidades marítimas de produção). O presente trabalho aborda a análise técnica e econômica de um processo proposto de separação e captura de dióxido de carbono (CO2), através de estudo de caso (Primeira e Segunda Proposição) de simulação de processo, em uma instalação marítima de produção de petróleo, comparativamente a sua ausência (Caso Base). A Primeira Proposição considera a separação e a captura do CO2 oriundo tanto do gás natural produzido, quanto do gás de queima de uma turbina a gás. A Segunda Proposição considera a separação e a captura do CO2 oriundo somente do gás natural produzido. Até o momento, no Brasil, ainda não foram desenvolvidas tecnologias adequadas para a captura do CO2, em instalações marítimas de produção de petróleo. Adicionalmente a regulação atual (Portaria nº104/2002 da ANP) limita o potencial de utilização do CO2 que existe na composição do gás natural comercializado no país, pelo fato de não diferenciar em sua especificação técnica, os usos deste importante combustível. Os resultados obtidos nesta tese, com a utilização de simulador de processo de uso comercial mostraram emissões evitadas de CO2 para atmosfera de 55 % (caso Segunda Proposição que apresentou maior viabilidade econômica), em relação ao resultado obtido para o Caso Base. Este relevante resultado equivale a uma emissão evitada de aproximadamente 241 x 103 t/ano, para uma única unidade piloto proposta. De acordo com o estudo de análise econômica apresentado, a Segunda Proposição (VPL US$ 15,3 x 106) foi melhor do que a da Primeira Proposição (VPL: US$ 13,9 x 106) ambos usando o Caso Base como referência. Dentre os ganhos esperados com o uso desta nova tecnologia destacam-se: redução do consumo interno e das perdas de gás natural, emissão evitada de CO2 e hidrocarbonetos para a atmosfera, além do aumento das práticas de armazenamento de gás e CO2, em reservatórios geológicos depletados de petróleo. Estima-se que num cenário futuro, com a implantação deste novo processo proposto, em instalações marítimas de produção de petróleo, uma relevante contribuição de emissões evitadas de gases de efeito estufa possa ocorrer na área de E&P de petróleo no Brasil. / The current Brazilian market needs to increase the natural gas supply to incentive the national scientific community to the challenge of developing new technologies routes aiming increase the utilization of the produced natural gas. Such challenge is followed by a world demand from signatory countries of the Kyoto Agreement (ratified in 2005) to reduce the greenhouse gas emissions. In spite of, the Brazil does not have any reduction goal, in the first period (2008 to 2012) the oil sector (E&P activity), by their oil operators companies that works in our country, has already established corporative goals to avoided greenhouse gas emissions in their production facilities (bigger predominance of offshore production unities). The present work approaches the economic and technical evaluation of a carbon dioxide (CO2) separation and capture proposal process (First and Second Proposal Case) comparatively your absence (Base Case). The First Case consider the CO2 separation and capture both the produced gas and exhausted gases of one turbine driven by gas. The Second Case consider only the CO2 separation and capture from the produced gas. At the present, in Brazil, it has not been developed yet suitable technologies, for such use, and the CO2 is normally disposal to the atmosphere. Moreover, the present Regulation (104/2002 ANP Decree) limit the potential of CO2 use existing in the gas composition that is marketed in the country, due to not differentiate the uses of this important fuel. The results obtained of this thesis, by using a process simulator of commercially use showed CO2 avoided emissions of 55 % to the atmosphere (Second Proposal Case that shows the best economic evaluation) related to the result obtained from the Base Case. This relevant result is equivalent in mass flow, to the avoidance emission of roughly 241 x 103 tons per year, for a single pilot unity proposal. According the economic evaluation study, the Second Proposal Case (VPL:US$ 15,3 x 106) was better than the First Case (VPL: US$ 13,9 x 106), using the Case Base as reference. Within the benefits expected with the use of this new technology are the following: reduction both the internal gas consumption and natural gas losses (atmospheric disposal), emissions avoided of CO2 and hydrocarbons, beyond the increase of CO2 and gas storage practices in offshore depleted oil fields. It is estimated, in future scenery, with the implantation of this new proposal process in offshore production unities, relevant contribution of avoided greenhouse gases emissions can occur in oil E&P tasks in Brazil.

A necessidade atual do mercado brasileiro para aumentar a oferta de gás incentiva a comunidade científica nacional no desafio de desenvolvimento de novas rotas tecnológicas, visando aumentar o aproveitamento do gás natural. Tal desafio é acompanhado por uma demanda mundial dos países signatários do Protocolo de Quioto (ratificado em 2005) para a redução das emissões de gases de efeito estufa. Apesar de o Brasil não apresentar nenhuma meta de redução, no primeiro período deste Protocolo (2008 a 2012), o setor do petróleo (atividade de E&P), através de suas companhias operadoras, que atuam no país, já estabeleceram metas corporativas para emissão evitada de gases de efeito estufa, em suas instalações de produção (maior predominância das unidades marítimas de produção). O presente trabalho aborda a análise técnica e econômica de um processo proposto de separação e captura de dióxido de carbono (CO2), através de estudo de caso (Primeira e Segunda Proposição) de simulação de processo, em uma instalação marítima de produção de petróleo, comparativamente a sua ausência (Caso Base). A Primeira Proposição considera a separação e a captura do CO2 oriundo tanto do gás natural produzido, quanto do gás de queima de uma turbina a gás. A Segunda Proposição considera a separação e a captura do CO2 oriundo somente do gás natural produzido. Até o momento, no Brasil, ainda não foram desenvolvidas tecnologias adequadas para a captura do CO2, em instalações marítimas de produção de petróleo. Adicionalmente a regulação atual (Portaria nº104/2002 da ANP) limita o potencial de utilização do CO2 que existe na composição do gás natural comercializado no país, pelo fato de não diferenciar em sua especificação técnica, os usos deste importante combustível. Os resultados obtidos nesta tese, com a utilização de simulador de processo de uso comercial mostraram emissões evitadas de CO2 para atmosfera de 55 % (caso Segunda Proposição que apresentou maior viabilidade econômica), em relação ao resultado obtido para o Caso Base. Este relevante resultado equivale a uma emissão evitada de aproximadamente 241 x 103 t/ano, para uma única unidade piloto proposta. De acordo com o estudo de análise econômica apresentado, a Segunda Proposição (VPL US$ 15,3 x 106) foi melhor do que a da Primeira Proposição (VPL: US$ 13,9 x 106) ambos usando o Caso Base como referência. Dentre os ganhos esperados com o uso desta nova tecnologia destacam-se: redução do consumo interno e das perdas de gás natural, emissão evitada de CO2 e hidrocarbonetos para a atmosfera, além do aumento das práticas de armazenamento de gás e CO2, em reservatórios geológicos depletados de petróleo. Estima-se que num cenário futuro, com a implantação deste novo processo proposto, em instalações marítimas de produção de petróleo, uma relevante contribuição de emissões evitadas de gases de efeito estufa possa ocorrer na área de E&P de petróleo no Brasil. / The current Brazilian market needs to increase the natural gas supply to incentive the national scientific community to the challenge of developing new technologies routes aiming increase the utilization of the produced natural gas. Such challenge is followed by a world demand from signatory countries of the Kyoto Agreement (ratified in 2005) to reduce the greenhouse gas emissions. In spite of, the Brazil does not have any reduction goal, in the first period (2008 to 2012) the oil sector (E&P activity), by their oil operators companies that works in our country, has already established corporative goals to avoided greenhouse gas emissions in their production facilities (bigger predominance of offshore production unities). The present work approaches the economic and technical evaluation of a carbon dioxide (CO2) separation and capture proposal process (First and Second Proposal Case) comparatively your absence (Base Case). The First Case consider the CO2 separation and capture both the produced gas and exhausted gases of one turbine driven by gas. The Second Case consider only the CO2 separation and capture from the produced gas. At the present, in Brazil, it has not been developed yet suitable technologies, for such use, and the CO2 is normally disposal to the atmosphere. Moreover, the present Regulation (104/2002 ANP Decree) limit the potential of CO2 use existing in the gas composition that is marketed in the country, due to not differentiate the uses of this important fuel. The results obtained of this thesis, by using a process simulator of commercially use showed CO2 avoided emissions of 55 % to the atmosphere (Second Proposal Case that shows the best economic evaluation) related to the result obtained from the Base Case. This relevant result is equivalent in mass flow, to the avoidance emission of roughly 241 x 103 tons per year, for a single pilot unity proposal. According the economic evaluation study, the Second Proposal Case (VPL:US$ 15,3 x 106) was better than the First Case (VPL: US$ 13,9 x 106), using the Case Base as reference. Within the benefits expected with the use of this new technology are the following: reduction both the internal gas consumption and natural gas losses (atmospheric disposal), emissions avoided of CO2 and hydrocarbons, beyond the increase of CO2 and gas storage practices in offshore depleted oil fields. It is estimated, in future scenery, with the implantation of this new proposal process in offshore production unities, relevant contribution of avoided greenhouse gases emissions can occur in oil E&P tasks in Brazil.

Le stockage géologique du CO2 est une stratégie prometteuse pour limiter la concentration de CO2anthropique dans l’atmosphère. Les aquifères salins (AS) ont été identifiés comme des optionsviables car ils possèdent de grandes capacités potentielles de stockage. Toutefois, les processusrelatifs au piégeage du CO2 souffrent d’un manque de connaissances fondamentales car il existe peude méthodes d’expérimentation rapides et reproductibles, travaillant dans les conditions du stockagegéologique. Ainsi, nous avons développé des microréacteurs haute pression, véritables laboratoiresgéologiques sur puce (GLoCs), recréant les conditions de porosité et de perméabilité des AS pour :(i) Mesurer la solubilité du CO2 dans l’eau et les saumures via un couplage microsystèmes /spectroscopie Raman ;(ii) Etudier les mécanismes d’invasion du CO2 dans les formations géologiques, incluantnotamment les écoulements diphasiques en milieux poreux, les séparations de phases etla précipitation des carbonates. / CO2 geological storage is a promising strategy to control the anthropogenic CO2 concentration in theatmosphere. Deep saline aquifers (DSA) were identified as viable options since they exhibit largestorage capacity. However, processes inherent to CO2 trapping suffer from a lack of fundamentalknowledge, since there are too few fast and reproducible experimental approaches able to work atgeological storage conditions. Therefore, to address these limitations, we have developed highpressure microreactors, so-called “geological labs on a chip” - GloCs – allowing mimicking porosityand permeability conditions of DSA for:(i) Measuring solubility of CO2 in water and brine through the combination of microsystemsand confocal Raman spectroscopy,(ii) Studying invasion mechanisms of CO2 in geological formations, including in particularbiphasic flows in porous media, phase separation and carbonates precipitation.

In spite of the large number of research works on carbon capture and sequestration (CCS), the migration and behaviour of CO2 in the subsurface (i. e. strata below the earth's surface) still needs further understanding and investigations with the aim of encouraging the governmental policy makers to adopt CCS technology as one of the most viable means to tackle the global warming threats. In this research work, a series of numerical simulations has been carried out using STOMP-CO2 simulation code to determine the flow behaviour and ultimate fate of the injected supercritical carbon dioxide (scCO2) into saline aquifers in medium terms of storage (i. e. few thousand years). The characteristics of the employed simulator, including the mathematical algorithm, governing equations, equations of states and phase equilibria calculations are explained in details.

[pt] Os mecanismos envolvidos na produção de metano e no sequestro de CO2 no carvão são complexos, tendo em vista grande quantidades de fatores envolvidos no processo. O entendimento do comportamento mecânico do carvão assim como a caracterização de sistema poroso é de fundamental importância para o êxito de um projeto de explotação. Esse trabalho visou à caracterização de amostras de carvão oriundas da camada Barro Branco. A fim de caracterizar o sistema poroso do material, uma campanha de análises foi programada como: microtomógrafo, microscopia eletrônica de varredura (MEV), micropermiametria e porosimetria por injeção a mercúrio. Ensaios mecânicos foram realizados visando à caracterização mecânica do material e a validação de um modelo constitutivo. O carvão apresentou comportamentos mecânicos de resistência e deformabilidade consistentes e com pouca variabilidade, o que permitiu um ajuste confiável da envoltória de resistência de Mohr-Coulomb bem como o do modelo constitutivo elastoplástico de Lade-Kim. / [en] Mechanisms involved in geological storage of CO2 and eventual production of methane are complex due to a number of different factors involved. One of the important factors to be taken into account is the geomechanical behaviour of coal, key to the success of the exploration as well as the characterization of the pore structure of the material.Coal can be regarded as a sedimentary rock possessing two perpendicular families of microfissures called cleats.This work presents results of an experimental program aiming at the characterization of the mechanical properties of coal from the Barro Branco formation. A constitutive model (Lade-Kim s model) was tested in order to check its validity in the representation of the stress-strain-strength behaviour of the coal. Lade-Kim s model is well accepted for the representation of the mechanical behaviour of soft rocks. Furthermore, in order to characterize the porous structure of the material, a number of tests were performed such as: X Ray Micro CT scan, scanning electron microscopy, minipermeameter determination of permeability and mercury injection porosimetry.

[pt] Atrelado aos cenários cada vez mais complexos de extração de energia, o estudo de fenômenos acoplados em meios porosos - notadamente térmicos, hidráulicos, químicos e mecânicos - tem se apresentado como essencial na previsão de comportamento de meios geológicos no que diz respeito à disposição de rejeitos radioativos, armazenamento de dióxido de carbono, engenharia de reservatórios geotérmicos e geomecânica de reservatórios. Assim, este trabalho objetiva desenvolver um esquema de acoplamento termo-hidro-mecânico-químico iterativo visando a simulação do armazenamento geológico de dióxido de carbono, empregando um simulador de fluxo composicional (GEM) e um programa de análise de tensões (ABAQUS ou CHRONOS). A idealização das metodologias de acoplamento foi efetuada através dos processos hidro-mecânico, termo-hidro-mecânico e termo-hidro-mecânico-químico, bem como as validações e aplicações em casos reais. Os casos de validação, realizados empregando modelos simplificados monofásicos, apresentaram resultados satisfatórios quanto ao comportamento hidro-mecânico e termo-hidro-mecânico. Adicionalmente às validações, os esquemas termo-hidro-mecânico e termo-hidro-mecânico-químico foram aplicados em dois casos reais de armazenamento de CO2 apresentados na literatura, projeto In Salah (Argélia) e aquífero Utsira (Noruega), respectivamente. De maneira geral, os resultados encontrados, para ambos os casos estudados, representaram acuradamente as respostas encontradas em campo, fato que evidencia a qualidade, robustez e aplicabilidade dos esquemas de acoplamento propostos neste trabalho. / [en] Considering the increasingly complex scenarios of energy extraction, the study of coupled phenomena in porous media - notably thermal, hydraulic, chemical and mechanical - has been considered as essential in order to predict the behavior of geological media with regard to radioactive waste storage, CO2 geological storage, geomechanics of geothermal reservoirs and reservoir geomechanics. Thus, this work aims to develop a thermo-hydro-mechanical-chemical iterative coupling scheme in order to simulate the geological storage of CO2, employing a compositional flow simulator (GEM) and a stress analysis program (ABAQUS or CHRONOS). The idealization of the coupling methodologies was carried out through the processes hydro-mechanical, thermo-hydro-mechanical and thermo-hydro-mechanical-chemical, as well as the validations and applications in real cases. The validation cases, performed employing simplified single-phase models, presented satisfactory results regarding the hydro-mechanical and thermo-hydro-mechanical behaviors. Additionally to the validations, the thermo-hydro-mechanical and thermo-hydro-mechanical-chemical schemes were applied in two real cases of CO2 geological storage reported by the literature, In Salah project (Algeria) and Utsira aquifer (Norway), respectively. In general, the results found, in both cases studied, accurately represented the behavior observed in the field, which in turn highlights the accuracy, robustness and applicability of the coupling schemes proposed in this work.

En vue de réduire à moyen terme les émissions de gaz à effet de serre d'origine anthropique, le captage-transport-stockage du dioxyde de carbone (CO2) est considéré comme une technologie prometteuse. Plusieurs sites pilotes existent déjà dans le monde. Cependant, avant de développer la technique de façon industrielle, des recherches expérimentales et numériques doivent être menées afin de garantir le succès et la pérennité d'un projet de stockage. Sur un site de stockage, les discontinuités naturelles ainsi que le(s) puits d'injection constituent des chemins préférentiels pour des fuites éventuelles. Ce travail de doctorat s'attache à l'étude des effets de la présence de dioxyde de carbone sur les géomatériaux en présence et, plus particulièrement, sur le ciment du puits d'injection. L'intégrité du puits et donc la garantie de son étanchéité est critique au niveau de la roche de couverture. Après injection et remontée du panache de dioxyde de carbone vers la roche de couverture, le ciment du puits au niveau de la zone triple (puits/réservoir/couverture) est en contact avec un fluide saturé en CO2 dissous. Un tel fluide, au pH acide, est amené à réagir avec les géomatériaux et entraîne diverses réactions de dissolution des minéraux de la matrice cimentaire ainsi que des réactions de précipitation pouvant altérer le matériau. Ce couplage fort existant entre réactions chimiques et comportement poro-mécanique du ciment du puits peut en effet induire un endommagement de la matrice cimentaire, lié aux modifications de la porosité et des caractéristiques de transport, à la dégradation des modules mécaniques, ou encore à la création de surpressions interstitielles localisées. Un modèle constitutif entièrement couplé a été développé pour simuler le comportement chimio-poromécanique du ciment en présence d'un fluide chargé de CO2. Ce modèle a été implémenté dans deux codes numériques, à savoir, un code aux volumes finis d'une part, et un code aux éléments finis, BIL, développé au Laboratoire Navier, d'autre part. La première implémentation se révèle être bien adaptée aux problèmes de transport réactif à front raide, et est utilisée dans ce mémoire pour modéliser une géométrie unidimensionnelle alliant ciment du puits et roche de couverture. La seconde méthode d'implémentation est quant à elle mieux adaptée à la modélisation du comportement poro-mécanique du ciment, mais, comme nous le verrons, nécessite des adaptations numériques a fin d'être convenable pour la modélisation de phénomènes chimiques impliquant des discontinuités. L'endommagement mécanique lié aux phénomènes chimiques est évalué d'une part via une approche micro-mécanique simplifiée, et d'autre part par une théorie de l'endommagement isotrope. En fin, en ce qui concerne la seconde approche, les résultats sont comparés à des tests expérimentaux issus de la littérature scientifique dans le contexte du stockage géologique du CO2 / In order to reduce in medium-term the anthropogenic original greenhouse gas, the processes of capture-transport-storage of carbon dioxide (CO2) is considered as a promising technology. Several pilot sites already exist in the world. However, before developing the technology on an industrial scale, experimental and numerical researches have to be performed in order to ensure the success and the sustainability of a storage project. In a storage site, the natural discontinuities of the rocks and of the injection wells are normally the preferential leak paths of CO2. In this context, the present PhD research focuses particularly on the cement injection wells. The problems of the integrity of the well and thus ensuring its sealing are the critical points of the caprock.After the injection and the ascent of the CO2 plume to the caprock, the cement paste of well at the triple zone (well/ reservoir/caprock) is contacted with a fluid saturated with dissolved CO2. Because of its acidity, such a fluid is reacted with geomaterials and causes diverse reactions of dissolution of the minerals in the cementitious matrix and precipitation reactions that may affect the material. This strong coupling existing between the chemical reactions and poro-mechanical behavior of the cement well can indeed induce damage to the cementitious matrix related to the modifications of the porosity and the transport characteristics, to the degradation of mechanical modulus, or to the development of localized pore pressure.A constitutive model fully coupled has been developed to simulate the chemo-poro-mechanical behaviour of the hard cement paste of the well with the presence of a CO2-rich fluid. This model has been implemented in two numerical codes: on the one hand, a finite volume code, and on the other hand, a finite element code, BIL, developed at the Navier Laboratory. The first implementation was found to be well adapted to the problems of reactive transport with sharp front, and is used in this thesis to modeling an one-dimensional geometry by combining the cement well and the caprock. The second implementation method is best suited to modeling the poro-mechanical behavior of cement, but, as we shall see, requires numerical adaptations in order to be suitable for modeling chemical phenomenon involving discontinuities. The mechanical damage related to chemical phenomena is evaluated firstly via a simplified micro-mechanical approach, and secondly a theory of isotropic damage. Finally, the results are compared to experimental tests from the scientific literature in the context of the CO2 geosequestration