Aerated treatment wetlands are an increasingly recognized nature–based technology for thetreatment of domestic and industrial wastewater. As biodegradation is the most importanttreatment mechanism in aerated wetlands, these systems heavily rely on mechanical aerationmediated oxygen transfer to supply the dissolved oxygen demand of the associated microbialcommunity. In the last decade, research on aerated wetlands has evolved, however, majorquestions on aeration, the associated oxygen transfer and the quantitative link to treatmentperformance still remain unknown. Answering these questions can further improve aeratedwetland design to optimize treatment efficacy and economical efficiency. This dissertation investigated the link of oxygen transfer to the air flow rate of aerationand elucidated the associated impact on treatment performance for organic carbon and nitrogenin horizontal flow aerated wetlands. Therefore, a numerical process model includingone dimensional reactive transport was developed. This model describes the main processesinvolved in horizontal flow aerated wetlands: water flow, heat transport, transport of solubleand particulate wastewater pollutants, biodegradation by a network of bacterial communitiesand oxygen transfer through mechanical aeration. For model calibration and validation, pilot–scale experiments in horizontal flow aerated wetlands treating real wastewater were conducted.These included conservative tracer experiments as well as monitoring steady–state operationat variable air flow rates and aeration interruption. In general, the model was able to simulate conservative tracer transport as well as treatmentperformance for organic carbon and nitrogen at steady–state operation and aeration interruptionwith sufficient accuracy. A local sensitivity analysis of the calibrated parameters revealedporosity, hydraulic permeability and dispersion length as well as the oxygen transfer coefficientkLa as most important. When operating the wetland systems at steady–state, aeration provideda mostly aerobe environment, except at the influent zone. However, when aeration wasinterrupted, anaerobe process started to take over and treatment performance declined within3–4 days. The modeling elucidated that methanogenic and sulphate reducing bacteria can playa significant role for organic carbon removal during aeration interruption. Moreover, the modelrevealed a non–linear declining relationship of the air flow rate with oxygen transfer coefficientkLa and of kLa with treatment performance. The alteration of oxygen transfer by wastewaterpollutant concentration was then investigated in a laboratory–scale column experiment. Basedon this experiment, an empirical equation describing the inhibitory effect of soluble chemicaloxygen demand (CODs) on the oxygen transfer coefficient kLa was derived and incorporatedinto the process model. With the extended model several simulation scenarios were analyzedto quantify the impact of the inhibited oxygen transfer on treatment performance. It turnedout that the reduction of oxygen transfer by CODs will, most likely, be relevant only at highinfluent wastewater strength (CODs 300 mg L-1), low aeration (air flow rate 50 L m-2h-1) or when the aerated wetland design includes zoned aeration. With respect to secondarytreatment of domestic effluents at similar strength using a spatially uniform aeration, an airflow rate of approximately 150–200 L m-2 h-1 can be recommended as a reasonable compromisebetween treatment efficiency and robustness. If zoned aeration is intended (e.g. to create a redox zonation), however, the air flow rate should be increased to approximately 400 L m-2 h-1 to supress the inhibition of oxygen transfer by CODs concentration. Furthermore, the air flow rate at steady–state operation (50–500 L m-2 h-1) did not substantially affect the response in effluent concentrations for organic carbon and nitrogen. This means that at steady–state air flow rates of 50–500 L m-2 h-1 operation, treatment efficacy during aeration interruption will deteriorate and recover in a similar time. In conclusion, this dissertation provides quantitative insights into the mechanisms of aeration and treatment performance for organic carbon and nitrogen in horizontal flow aerated treatment wetlands. The findings obtained can support aerated treatment wetland design for research experiments and engineering applications. Therefore, this dissertation represents a significant advancement in the field of aerated treatment wetland research.

The problem of global warming is becoming more and more serious, and carbon dioxide is one of the main causes of climate problems. Therefore, in order to re-duce CO2 emissions, the use of mineralization to store CO2 has become one of the potential methods. In addition, due to the high mineralization rate of peridotite, it will become the research object of this study. This study uses COMSOL Multiphysics to simulate the changing characteristics of carbon dioxide after injection into peridotite. Sensitivity analysis is performed by changing the porosity of the rock and the rate of CO2 injection to further understand the impact on CO2. The results show that at a lower injection rate, the pressure distribution is relatively uniform, the CO2 concentration range is also small, and the saturation increases slowly. On the other hand, when the porosity decreases, the pressure will increase significantly, the diffusion range of CO2 will be relatively expanded, and the saturation will increase. In addition, no matter which factor, it will tend to decrease with the increase of distance and time, and eventually stabilize. Therefore, in order to avoid the possibility of formation rupture and potential leakage of CO2, it is necessary to combine these influencing factors to seek a stable and effective CO2 storage solution. / Problemet med den globala uppvärmningen blir mer och mer allvarligt och kol-dioxid är en av huvudorsakerna till klimatproblemen. Därför, för att minska CO2 utsläppen, har användningen av mineralisering för att lagra CO2 blivit en av de möjliga metoderna. Dessutom, på grund av den höga mineraliseringshastigheten för peridotit, kommer det att bli forskningsobjektet för denna studie. Denna studie använder COMSOL Multiphysics för att simulera de förändrade egenskaperna hos koldioxid efter injektion i peridotit. Känslighetsanalys utförs genom att ändra bergartens porositet och hastigheten för CO2 injektion för att ytterligare förstå påverkan på CO2. Resultaten visar att vid en lägre injektionshastighet är tryckfördelningen relativt jämn, koncentrationsområdet CO2 är också litet och mättnaden ökar långsamt. Å andra sidan, när porositeten minskar, kommer trycket att öka av-sevärt, diffusionsområdet för CO2 kommer att vara relativt expanderat, och mättnaden kommer att öka. Dessutom, oavsett vilken faktor, kommer den att tendera att minska med ökningen av avstånd och tid, och så småningom stabiliseras. Därför, för att undvika risken för formationsbrott och potentiellt läckage av CO2, är det nödvändigt att kombinera dessa påverkande faktorer för att söka en stabil och effektiv CO2 förvaringslösning.

Ce travail vise à étudier le couplage entre écoulement et interactions physico-chimiques dans les sols, dans différentes conditions de saturation en eau, afin d’améliorer la prédiction du devenir des polluants. Il s’agit de comprendre en quoi le taux de saturation du milieu affecte la réactivité du sol vis-à-vis des polluants, et d’évaluer le pouvoir prédictif du transport de solutés réactifs étudié en milieu saturé sur la réactivité en conditions non saturées. Différents processus sont considérés : l’échange de cations calcium-zinc sur un milieu poreux modèle (sable-kaolinite), la sorption et désorption d’un composé organique sur une terre non contaminée, le transport de polluants prioritaires tels que les HAP sur une terre de friche industrielle. Dans chaque cas, des expériences en colonne de laboratoire ont été conduites en conditions d’écoulement saturé et non saturé permanent, permettant tout d’abord la caractérisation de l’hydrodynamique, puis l’étude du couplage avec la réactivité. Les courbes de percée obtenues ont été ensuite modélisées avec des codes tels que CXTFIT. On a montré l’influence de la teneur en eau du milieu sur le transport réactif, variable suivant le type de réaction considéré, la structure des milieux jouant également un rôle important. L’échange d’ions sur le milieu modèle n’est globalement pas affecté par la teneur en eau, dans une gamme proche de la saturation. En revanche, une plus forte sorption et une plus faible mobilisation des polluants organiques ont été observées en conditions non saturées. Le transport réactif de ces composés ne peut donc pas être prédit en conditions non saturées à partir de mesures en milieu saturé, qui peuvent surestimer le transport / The aim of this work was to study the link between water flow and physical and chemical interactions in soils under variably water flow conditions, in order to improve the prediction of contaminants fate. It deals with understanding how the porous media water content can modify soil reactivity towards contaminants, and assessing the possibility to predict reactivity under unsaturated conditions with reactive solute transport studied in saturated porous media. Various processes were considered: cations exchange calcium-zinc on a model porous media (sand-kaolinite), sorption and desorption of an organic compound on a non polluted soil, transport of priority contaminants such as PAHs on an industrial contaminated soil. In each case, experiments were carried out with soil columns at the laboratory scale under saturated and unsaturated steady-state flow conditions, in order to characterize at first hydrodynamics and then to study the link with reactivity. Modeling of the breakthrough curves was then performed with codes such as CXTFIT. We showed an influence of porous media water content on reactive transport which was different as a function of the interaction. Porous media structure must also be taken into account. Ions exchange on a model porous media was not globally modified by the water content varying in a range close to saturation. On the contrary, higher sorption and lower migration of organic contaminants were observed under unsaturated conditions. Reactive transport of these compounds cannot therefore be predicted under unsaturated conditions with tests performed on saturated porous media which may overestimate transport

L'atténuation du changement climatique est l'un des défis majeurs de notre époque. Les émissions anthropiques de gaz à effet de serre ont augmenté de façon continue depuis la révolution industrielle, provoquant le réchauffement climatique. Un ensemble de technologies très diverses doivent être mises en œuvre pour respecter les accords internationaux relatifs aux émissions de gaz à effet de serre. Certaines d'entre elles ont recours au sous-sol pour le stockage de diverses substances. Cette thèse traite plus particulièrement de la dynamique du stockage souterrain du dioxyde de carbone (CO2) et de l'hydrogène (H2). Des modèles numériques de transport réactif et multiphasiques ont été élaborés pour mieux comprendre la migration et les interactions des fluides dans des milieux poreux de stockage souterrain. Ils fournissent des recommandations pour améliorer l'efficacité, la surveillance et la sécurité du stockage. Trois modèles sont présentés dans ce document, dont deux dans le domaine du captage et du stockage du CO2 (CCS pour Carbon Capture and Storage), et le troisième s'appliquant au stockage souterrain de l'hydrogène (UHS pour Underground Hydrogen Storage). Chacun d'entre eux traite plus spécifiquement un aspect de la recherche : Modèle multiphasique appliqué au CCS L'efficacité et la sécurité à long terme du stockage du CO2 dépend de la migration et du piégeage du panache de CO2 flottant. Les grandes différences d'échelles temporelles et spatiales concernées posent de gros problèmes pour évaluer les mécanismes de piégeage et leurs interactions. Dans cet article, un modèle numérique dynamique diphasique a été appliqué à une structure aquifère synclinale-anticlinale. Ce modèle est capable de rendre compte des effets de capillarité, de dissolution et de mélange convectif sur la migration du panache. Dans les aquifères anticlinaux, la pente de l'aquifère et la distance de l'injection à la crête de l'anticlinal déterminent la migration du courant gravitaire et, donc, les mécanismes de piégeage affectant le CO2. La structure anticlinale arrête le courant gravitaire et facilite l'accumulation du CO2 en phase libre, en dessous de la crête de l'anticlinal, ce qui stimule la mise en place d'une convection et accélère donc la dissolution du CO2. Les variations de vitesse du courant gravitaire en raison de la pente de l'anticlinal peuvent provoquer la division du panache et une durée différente de résorption du panache en phase libre, qui dépend de l'endroit de l'injection. / Climate change mitigation is one of the major challenges of our time. The anthropogenic greenhouse gases emissions have continuously increased since industrial revolution leading to global warming. A broad portfolio of mitigation technologies has to be implemented to fulfill international greenhouse gas emissions agreements. Some of them comprises the use of the underground as a storage of various substances. In particular, this thesis addresses the dynamics of carbon dioxide (CO2) and hydrogen (H2) underground storage. Numerical models are a very useful tool to estimate the processes taking place at the subsurface. During this thesis, a solute transport in porous media module and various multiphase flow formulations have been implemented in COMSOL Multiphysics (Comsol, 2016). These numerical tools help to progress in the understanding of the migration and interaction of fluids in porous underground storages. Three models that provide recommendations to improve the efficiency, monitoring and safety of the storages are presented in this manuscript: two in the context of carbon capture and storage (CCS) and one applied to underground hydrogen storage (UHS). Each model focus on a specific research question: Multiphase model on CCS. The efficiency and long-term safety of underground CO2 storage depend on the migration and trapping of the buoyant CO2 plume. The wide range of temporal and spatial scales involved poses challenges in the assessment of the trapping mechanisms and the interaction between them. In this chapter a two-phase dynamic numerical model able to capture the effects of capillarity, dissolution and convective mixing on the plume migration is applied to a syncline-anticline aquifer structure. In anticline aquifers, the slope of the aquifer and the distance of injection to anticline crest determine the gravity current migration and, thus, the trapping mechanisms affecting the CO2. The anticline structure halts the gravity current and promotes free-phase CO2 accumulation beneath the anticline crest, stimulating the onset of convection and, thus, accelerating CO2 dissolution. Variations on the gravity current velocity due to the anticline slope can lead to plume splitting and different free-phase plume depletion time is observed depending on the injection location. Injection at short distances from the anticline crest minimizes the plume extent but retards CO2 immobilization. On the contrary, injection at large distances from anticline crest leads to large plume footprints and the splitting of the free-phase plume. The larger extension yields higher leakage risk than injection close to aquifer tip; however, capillary trapping is greatly enhanced, leading to faster free-phase CO2 immobilization. Reactive transport model on convective mixing in CCS. Dissolution of carbon-dioxide into formation fluids during carbon capture and storage (CCS) can generate an instability with a denser CO2-rich fluid located above the less dense native aquifer fluid. This instability promotes convective mixing, enhancing CO2 dissolution and favouring the storage safety.

Parmi les options en cours d’investigation, le stockage souterrain de l'hydrogène dans les formations sédimentaires comme les grès pourrait offrir un potentiel unique pour stocker de grandes quantités d'énergie. L'évaluation des modalités de stockage souterrain de l'hydrogène nécessite donc à la fois une connaissance précise des transformations minéralogiques dues à la présence de l'hydrogène et l’acquisition de données sur le comportement hydrodynamique des fluides. Par conséquent, cette étude se composera de trois parties : 1- Etude des interactions géochimiques de l’hydrogène dans des formations sédimentaires gréseuses : Les produits expérimentaux portent la marque d'une réaction très limitée entre les minéraux du grès et l'hydrogène. Si les résultats expérimentaux sont combinés aux résultats numériques, l’étude démontre que l'hydrogène, une fois injecté, peut être considéré comme relativement inerte. De façon globale, nos résultats renforcent la faisabilité du confinement de l'hydrogène dans des réservoirs géologiques comme les grès. 2- Etude de la migration de l'hydrogène dans les grès : détermination de la perméabilité relative et de la pression capillaire du système hydrogène-eau : Afin de fournir des données quantitatives pour le développement du stockage souterrain de l'hydrogène, la pression capillaire et la perméabilité relative ont été mesurées pour le système hydrogène-eau en deux conditions potentielles. Les résultats indiquent que les données obtenues sont applicables à l’ensemble des conditions de stockage de l'hydrogène. 3- Modélisation numérique d’un site de stockage géologique d’hydrogène : La simulation numérique a été effectuée pour caractériser l'évolution dynamique d’un site de stockage d'hydrogène pur. Une fluctuation saisonnière du fonctionnement du réservoir et l'effet des fuites d'hydrogène dus aux réactions ont été pris en compte. / Underground hydrogen storage has been introduced as storage solution for renewable energy systems as it offers a unique potential to store large amounts of energy, especially in sedimentary formations such as sandstones. However, evaluating the underground hydrogen storage requires a precise knowledge of the hydrodynamic behavior of the fluids and of mineralogical transformations due to the presence of hydrogen that may affect the storage properties. Therefore, this study is consists in three parts: 1- Study of geochemical reactivity of hydrogen in sandstone sedimentary formations: The experimental products bear the mark of only very limited reaction between sandstone minerals and hydrogen. Taken together with the numerical results, this study demonstrates that hydrogen, once injected, can be considered as relatively inert. Overall, our results support the feasibility of hydrogen confinement in geological reservoirs such as sandstones. 2- Study of the migration of hydrogen in sandstone: determination of relative permeability and capillary pressure of hydrogen-water system: To provide quantitative data for the development of underground hydrogen storage, capillary pressures and relative permeabilities of hydrogen-water system have been measured at two potential conditions. The interpretation of the results would suggest that the obtained data are applicable for the entire range of hydrogen storage conditions. Interfacial tensions and contact angles for the hydrogen-water system have been also derived. 3- Numerical simulation of a geological hydrogen storage site: The numerical simulation was performed to characterize the evolution of pure hydrogen storage, by considering the seasonal fluctuation of renewable energy and the effect of hydrogen loses due to the biotic reactions.

Flow and transport phenomena in the subsurface often span a wide range of length (nanometers to kilometers) and time (nanoseconds to years) scales, and frequently arise in applications of CO₂ sequestration, pollutant transport, and near-well acid stimulation. Reliable field-scale predictions depend on our predictive capacity at each individual scale as well as our ability to accurately propagate information across scales. Pore-scale modeling (coupled with experiments) has assumed an important role in improving our fundamental understanding at the small scale, and is frequently used to inform/guide modeling efforts at larger scales. Among the various methods, there often exists a trade-off between computational efficiency/simplicity and accuracy. While high-resolution methods are very accurate, they are computationally limited to relatively small domains. Since macroscopic properties of a porous medium are statistically representative only when sample sizes are sufficiently large, simple and efficient pore-scale methods are more attractive. In this work, two Eulerian pore-network models for simulating single-phase flow and solute transport are developed. The models focus on capturing two key pore-level mechanisms: a) partial mixing within pores (large void volumes), and b) shear dispersion within throats (narrow constrictions connecting the pores), which are shown to have a substantial impact on transverse and longitudinal dispersion coefficients at the macro scale. The models are verified with high-resolution pore-scale methods and validated against micromodel experiments as well as experimental data from the literature. Studies regarding the significance of different pore-level mixing assumptions (perfect mixing vs. partial mixing) in disordered media, as well as the predictive capacity of network modeling as a whole for ordered media are conducted. A mortar domain decomposition framework is additionally developed, under which efficient and accurate simulations on even larger and highly heterogeneous pore-scale domains are feasible. The mortar methods are verified and parallel scalability is demonstrated. It is shown that they can be used as “hybrid” methods for coupling localized pore-scale inclusions to a surrounding continuum (when insufficient scale separation exists). The framework further permits multi-model simulations within the same computational domain. An application of the methods studying “emergent” behavior during calcite precipitation in the context of geologic CO₂ sequestration is provided. / text

[Truncated abstract] As mineral deposits continue to be mined, the non economic gangue materials such as sulphides (e.g. pyrite) that are extracted as part of the ore body or overburden are deposited within the waste rock and/or milled tailings. As a result of natural weathering processes, these reactive materials represent a potential hazard to surrounding environments. A major consequence, resulting from mine-waste impoundments containing sulphidic materials, relates to the offsite movement of low pH leachates containing elevated concentrations of metal ions posing a contamination threat. The processes and mechanisms acting in the formation of acid mine drainage (AMD) are highly variable and, to a high extent, controlled by climatic conditions as the main driver of water flow and wetness of the system which in turn determines the availability of oxygen as well as water for pyrite weathering. In particular, this thesis is based on the hypothesis that in semiarid and arid climates the acid production may be water … The experiments were repeated at different water contents ranging from 0.24 to 0.33 cm3 cm-3. Breakthrough curves (BTC) of Li+, K+, Ca2+, Mg2+, Na+ and pH were measured and described with models of different complexities. This included the use of a simple linear and non-linear isotherms for Li+ alone, a binary Li+ - K+ ion exchange, and a complete multicomponent chemical equilibrium description of ion transport. The latter, by including dissolution of primary minerals which released base cations such as Mg2+, Ca2+ and K+ explained some of the elution patterns of base cations for which the Li+ - K+ exchange was the dominant process. Furthermore, under unsaturated water flow conditions, retardation of Li+ increased with decreasing water content. Thus solute mobility in mafic rock tailings appears to decrease under strongly unsaturated water flow conditions.

Les activités humaines dans la subsurface se développent rapidement (stockage de déchets,nouvelles techniques minières, stockage à haute fréquence de l’énergie), alors que dans le même temps les attentes du public et des autorités s’intensifient. L’évaluation de chaque étape de ces opérations souterraines repose sur des études détaillées de la sûreté et des impacts environnementaux.Elles reposent sur des simulateurs élaborés et sur de la modélisation multiphysique. Avec leur approche orientée processus, les simulations en transport réactifs proposent une méthode efficace pour comprendre et prévoir le comportement de ces systèmes complexes, à différentes échelles de temps et d’espace.Le but de ce travail est d’intégrer la résolution de l’écoulement diphasique compressible dans le cadre de codes de transport réactifs à l’aide d’une méthode de séparation d’opérateurs. Un module multiphasique a été créé dans le code de transport réactif HYTEC. Une nouvelle approche a ensuite été développée pour coupler écoulement multicomposant multiphasique compressible, description de propriétés thermo-dynamiques complexes pour les fluides, avec des codes de transport réactif. La méthode a été intégrée dans HYTEC. Des cas de validation sont proposés, puis des exemples d’application pour la simulation du stockage souterrain de CO2 et des impuretés associées. / Human activity in the subsurface has rapidly been expanding and diversifying (waste disposal, new mining technologies, high-frequency storage of energy), while the public and regulatory expectations keep growing. The assessment of each step of underground operations requires careful safety and environmental impact evaluations. They rely on elaborate simulators and multiphysics modeling. With its process-based approach, reactive transport simulation provides an effective way to understand and predict the behavior of such complex systems at different time and spatial scale.This work aims at incorporating a compressible multiphase flow into conventional reactive transport framework by an operator splitting approach. A multiphase flow module is developed in the HYTEC reactive transport software. A new approach is then developed to fully couple multiphase multicomponent compressible flow, the complex thermodynamic description of the fluid properties, with existing reactive transport codes. The method is implemented in HYTEC. Some validation is provided, before application to the simulation of underground storage of CO2 and associated impurities.

Dans cette thèse, nous développons le modèle phénoménologique optimisé de lessivage chimique in situ (ISL) de l'uranium par l'injection d'acide sulfurique, en prenant en compte la précipitation des espèces non-solubles telles que le gypse, qui réduisent la récupération de l'uranium. Le modèle proposé décrit le transport de masse avec des réactions chimiques hétérogènes entre le liquide et les roches solides, qui mènent à la dissolution des oxydes d'uranium et à la récupération de l'uranium sous forme liquide. Ce modèle comprend à la fois des réactions utiles, qui décrivent la dissolution de divers types d'oxydes d'uranium, et les réactions néfastes qui conduisent à la précipitation des sédiments solides (gypse), dont les flocons couvrent la surface de canaux poreux et réduisent l'efficacité des réactions utiles. Parmi les résultats qualitatifs, nous avons révélé l'existence d'un taux critique de sédimentation de gypse, en dessous duquel la récupération ultime de l'uranium est complète. En revanche, elle tend à une valeur limite inférieure à 100% lorsque le taux de sédimentation est supérieur à la valeur critique. Ce taux de récupération limite dépend de divers paramètres du processus. La théorie et la méthodologie développées dans ce travail peuvent être facilement étendues et appliquées aux autres types de minerais qui sont récupérés par la méthode de lessivage in situ, et autres types de solvant / In the present thesis we develop the optimized phenomenological model of in-situ chemical leaching (ISL) of uranium by the injection of sulfuric acid, with special account for the precipitation of non-soluble species as gypsum, which reduces the uranium recovery. The suggested model describes the mass transport with heterogeneous chemical reactions between liquid and solid rocks, leading to dissolve uranium oxides and recover uranium in liquid form. It includes both useful reactions, describing the dissolution of various kinds of uranium oxides, and detrimental reactions, leading to the precipitation of solid sediments (gypsum), whose flakes cover the surface of porous channels and reduce the efficiency of useful reactions. Among the qualitative results we revealed the existence of a critical rate of gypsum sedimentation, below which the ultimate uranium recovery is complete. In contrast, it tends to a limit value lower than 100% when the sedimentation rate is higher than the critical value. This limit recovery depends on various parameters of the process. The theory and the methodology developed in this work can be easily extended and applied on other type of ores that are recovered by in-situ leaching method and other types of solvents

En vue de contrôler les émissions de gaz à effet de serre, il est envisagé d’injecter du CO2 dans des réservoirs géologiques. Or le CO2 n'est pas un gaz inerte. En modifiant la composition chimique de l'eau in situ, il est à l'origine d'interactions roche/fluide. Ces réactions géochimiques impactent les propriétés d'écoulement. Aussi, pour s'assurer de la viabilité et de la pérennité du stockage, les opérateurs ont besoin de simulations tenant compte de ces écoulements réactifs. Cependant les paramètres de l'équation macroscopique de transport utilisée sont affectés par les réactions surfaciques. Or, ces spécificités dues au transfert de masse ne sont pas prises en compte actuellement. De même, la loi perméabilité-porosité (K-F) n’est estimée que semi-empiriquement. Le but de cette thèse a été de développer une méthode pour obtenir les coefficients macroscopiques précédents et les relations K-F, en résolvant les équations gouvernant les phénomènes à l'échelle du pore. Pour ce faire, nous avons utilisé l'approche réseau de pores. L'avantage du modèle réseau est qu'il prend en compte explicitement la structure tout en conceptualisant cette dernière à un ensemble de pores et de canaux à la morphologie simplifiée (sphères, cylindres). L'étude est basée sur deux changements d'échelles successifs : du local au pore, puis du pore à la carotte. Le problème de transport réactif est résolu pour des éléments basiques, analytiquement ou numériquement. Puis, en faisant appel aux solutions précédemment trouvées, le transport réactif est traité sur l'ensemble du réseau. Notre model fut validé par des observations sur micromodèles, puis à l'aide d'une expérience d'altération acide / The geological storage of CO2 is considered as an attractive option to reduce the greenhouse gas emissions in the atmosphere. CO2 is not an inert gas, however. Its dissolution in brine forms a weak acid that has the potential to react with the host rock formation. The induced pores structure modification impacts the flow properties. Thus, to ensure the viability and sustainability of CO2 storage, operators need simulations that take into account the specificities of reactive transport. However, the macroscopic coefficients of the reactive transport equation are modified from the values of an inert tracer by surface reactions. These specificities due to mass transfer are currently not considered. Similarly, the permeability-porosity (K-F) relationship is only estimated semi-empirically. The aim of this thesis was to develop a method to obtain the macroscopic coefficients and the K-F laws, by solving the equations governing the pore-scale phenomena. To do this, we used the Pore Network Modelling approach (PNM). The advantage of the PNM is that it explicitly takes into account the pore structure, while conceptualizing the latter to a set of pores and throats whose morphology is simplified into spheres or cylinders for instance. The study is based into two successive upscalings: from local-scale to pore-scale, then from pore-scale to core-scale. The reactive transport problem is solved for basic elements, analytically or numerically. Then, using the solutions previously found at the pore scale, the reactive transport phenomena are treated throughout the network. Our model was validated by observations on micromodels and by a comparison with an acid-induced alteration experiment