No description available.

Porous media affect hydrate stability by forcing hydrate-liquid interfaces to form high curvature geometries and by forcing the molecules of the hydrate, liquid, and sedimentary particles that compose the medium to interact where they are in close proximity. To evaluate these effects we first create synthetic spherical packings to approximate pore space geometry. We use the synthetic pore space to calculate the perturbation to the chemical potential caused by the geometrical constraints. Our model predictions agree with published data for ice-water and water-vapor systems. When particles are well-approximated as spheres, our model fits the data with R-squared values that range between about 80% to over 99%. However, our model needs to be improved for porous media that contain a significant fraction of non-equant particles such as clay. Lastly, we demonstrate how our model can be used in predictions for the evolution of hydrate saturation. This thesis includes unpublished co-authored material.

Saline water evaporation from porous media with the associated salt precipitation patterns is frequently observed in a number of industrial and environmental applications and it is important in a variety of topics including, but not limited to, water balance and land-atmosphere interaction, terrestrial ecosystem functioning, geological carbon storage, and preservation of historical monuments. The excess accumulation of salt in soil is a global problem and is one of the most widespread soil degradation processes. Thus, it is important to understand the dominant mechanisms controlling saline water evaporation from porous media. This process is controlled by the transport properties of the porous medium, the external conditions, and the properties of the evaporating fluid. During saline water evaporation from porous media, the capillary induced liquid flow transports the solute towards the evaporation surface while diffusive transport tends to spread the salt homogeneously thorough the porous medium. Therefore, the solute distribution is influenced by the competition between the diffusive and convective transport. As water evaporates, salt concentration in the pore space increases continually until it precipitates. The formation of precipitated salt adds to the complexity of the description of saline water evaporation from porous media. In this dissertation, the effects of salt concentration, type of salt, and the presence of precipitated salt, on the evaporation dynamics have been investigated. The obtained results show that the precipitated salt has a porous structure and it evolves as the drying progresses. The presence of porous precipitated salt at the surface causes top-supplied creeping of the evaporating solution, feeding the growth of subsequent crystals. This could be visualized by thermal imaging in the form of appearance and disappearance of cold-spots on the surface of the porous medium, brought about by preferential water evaporation through the salt crust. My results show that such a phenomenon influences the dynamics of saline water evaporation from porous media. Moreover, a simple but effective tool was developed in this dissertation capable of describing the effects of ambient temperature, relative humidity, type of salt and its concentration, on the evaporative fluxes. Additionally, pore-scale data obtained by synchrotron x-ray tomography was used to study ion transport during saline water evaporation from porous media in 4D (3D space + time). Using iodine K-edge dual energy imaging, the ion concentration at pore scale with a high temporal and spatial resolution could be quantified. This enabled us to reveal the mechanisms controlling solute transport during saline water evaporation from porous media and extend the corresponding physical understanding of this process. Within this context, the effects of particle size distribution on the dispersion coefficient were investigated together with the evolution of the dispersion coefficient as the evaporation process progresses. The results reported in this dissertation shed new insight on the physics of saline water evaporation from porous media and its complex dynamics. The results of this dissertation have been published in 3 peer-reviewed journal papers together with one additional manuscript which is currently under review.

Many engineering and scientific applications of flow in porous media are characterized by transport phenomena at multiple spatial scales, including pollutant transport, groundwater remediation, and acid injection to enhance well production. Carbon sequestration in particular is a multiscale problem, because the trapping and leakage mechanisms of CO2 in the subsurface occur from the sub-pore level to the basin scale. Quantitative and predictive pore-scale modeling has long shown to be a valuable tool for studying fluid-rock interactions in porous media. However, due to the size limitation of the pore-scale models (10-4-10-2m), it is impossible to model an entire reservoir at the pore scale. A straightforward multiscale approach would be to upscale macroscopic parameters (e.g. permeability) directly from pore-scale models and then input them into a continuum-scale simulator. However, it has been found that the large-scale models do not predict in many cases. One possible reason for the inaccuracies is oversimplified boundary conditions used in this direct upscaling approach. The hypothesis of this work is that pore-level flow and upscaled macroscopic parameters depends on surrounding flow behavior manifested in the form of boundary conditions. The detailed heterogeneity captured by the pore-scale models may be partially lost if oversimplified boundary conditions are employed in a direct upscaling approach. As a result, extracted macroscopic properties may be inaccurate. Coupling the model to surrounding media (using finite element mortars to ensure continuity between subdomains) would result in more realistic boundary conditions, and can thus improve the accuracy of the upscaled parameters. To test the hypothesis, mortar coupling is employed to couple pore-scale models and also couple pore-scale models to continuum models. Flow field derived from mortar coupling and direct upscaling are compared, preferably against a true solution if one exists. It is found in this dissertation that pore-scale flow and upscaled parameters can be significantly affected by the surrounding media. Therefore, using arbitrary boundary conditions such as constant pressure and no-flow boundaries may yield misleading results. Mortar coupling captures the detailed variation on the interface and imposes realistic boundary conditions, thus estimating more accurate upscaled values and flow fields. An advanced upscaling tool, a Super Permeability Tensor (SPT) is developed that contains pore-scale heterogeneity in greater detail than a conventional permeability tensor. Furthermore, a multiscale simulator is developed taking advantage of mortar coupling to substitute continuum grids directly with pore-scale models where needed. The findings from this dissertation can significantly benefit the understanding of fluid flow in porous media, and, in particular, CO2 storage in geological formations which requires accurate modeling across multiple scales. The fine-scale models are sensitive to the boundary conditions, and the large scale modeling of CO2 transport is sensitive to the CO2 behavior affected by the pore-scale heterogeneity. Using direct upscaling might cause significant errors in both the fine-scale and the large-scale model. The multiscale simulator developed in this dissertation could integrate modeling of CO2 physics at all relevant scales, which span the sub-pore or pore level to the basin scale, into one single simulator with effective and accurate communication between the scales. The multiscale simulator provides realistic boundary conditions for the fine scales, accurate upscaled information to continuum-scale, and allows for the distribution of computational power where needed, thus maintaining high accuracy with relatively low computational cost. / text

Local displacement efficiency in miscible floods is significantly affected by mixing taking place in the medium. Laboratory experiments usually measure flow-averaged ("cup mixed") effluent concentration histories. The core-scale averaged mixing, termed as dispersion, is used to quantify mixing in flow through porous media. The dispersion coefficient has the contributions of convective spreading and diffusion lumped together. Despite decades of research there remain questions about the nature and origin of dispersion. The main objective of this research is to understand the basic physics of solute transport and mixing at the pore scale and to use this information to explain core-scale mixing behavior (dispersion). We use two different approaches to study the interaction between convective spreading and diffusion for a range of flow conditions and the influence of their interaction on dispersion. In the first approach, we perform a direct numerical simulation of pore scale solute transport (by solving the Navier Stokes and convection diffusion equations) in a surrogate pore space. The second approach tracks movement of solute particles through a network model that is physically representative of real granular material. The first approach is useful in direct visualization of mixing in pore space whereas the second approach helps quantify the effect of pore scale process on core scale mixing (dispersion). Mixing in porous media results from interaction between convective spreading and molecular diffusion. The converging-diverging flow around sand grains causes the solute front to stretch, split and rejoin. In this process the area of contact between regions of high and low solute concentrations increases by an order of magnitude. Diffusion tends to reduce local variations in solute concentration inside the pore body. If the fluid velocity is small, diffusion is able to homogenize the solute concentration inside each pore. On the other hand, in the limit of very large fluid velocity (or no diffusion) local mixing because of diffusion tends to zero and dispersion is entirely caused by convective spreading. Flow reversal provides insights about mixing mechanisms in flow through porous media. For purely convective transport, upon flow reversal solute particles retrace their path to the inlet. Convective spreading cancels and echo dispersion is zero. Diffusion, even though small in magnitude, causes local mixing and makes dispersion in porous media irreversible. Echo dispersion in porous media is far greater than diffusion and as large as forward (transmission) dispersion. In the second approach, we study dispersion in porous media by tracking movement of a swarm of solute particles through a physically representative network model. We developed deterministic rules to trace paths of solute particles through the network. These rules yield flow streamlines through the network comparable to those obtained from a full solution of Stokes' equation. In the absence of diffusion the paths of all solute particles are completely determined and reversible. We track the movement of solute particles on these paths to investigate dispersion caused by purely convective spreading at the pore scale. Then we superimpose diffusion and study its influence on dispersion. In this way we obtain for the first time an unequivocal assessment of the roles of convective spreading and diffusion in hydrodynamic dispersion through porous media. Alternative particle tracking algorithms that use a probabilistic choice of an out-flowing throat at a pore fail to quantify convective spreading accurately. For Fickian behavior of dispersion it is essential that all solute particles encounter a wide range of independent (and identically distributed) velocities. If plug flow occurs in the pore throats a solute particle can encounter a wide range of independent velocities because of velocity differences in pore throats and randomness of pore structure. Plug flow leads to a purely convective spreading that is asymptotically Fickian. Diffusion superimposed on plug flow acts independently of convective spreading causing dispersion to be simply the sum of convective spreading and diffusion. In plug flow hydrodynamic dispersion varies linearly with the pore-scale Peclet number. For a more realistic parabolic velocity profile in pore throats particles near the solid surface of the medium do not have independent velocities. Now purely convective spreading is non-Fickian. When diffusion is non-zero, solute particles can move away from the low velocity region near the solid surface into the main flow stream and subsequently dispersion again becomes asymptotically Fickian. Now dispersion is the result of an interaction between convection and diffusion and it results in a weak nonlinear dependence of dispersion on Peclet number. The dispersion coefficients predicted by particle tracking through the network are in excellent agreement with the literature experimental data. We conclude that the essential phenomena giving rise to hydrodynamic dispersion observed in porous media are (i) stream splitting of the solute front at every pore, thus causing independence of particle velocities purely by convection, (ii) a velocity gradient within throats and (iii) diffusion. Taylor's dispersion in a capillary tube accounts for only the second and third of these phenomena, yielding a quadratic dependence of dispersion on Peclet number. Plug flow in the bonds of a physically representative network accounts for the only the first and third phenomena, resulting in a linear dependence of dispersion upon Peclet number. / text

No description available.

Reactive Transport Models (RTMs) provide quantitative tools to analyze the interaction between transport and biogeochemical processes in subsurface environments such as aquatic sediments and groundwater flow. A tremendous amount of research has shown the role and impact of scaling behavior of the reactive systems which stems from geologic heterogeneity. Depending on the kinetics of the reactions, different types of formulations have been proposed to describe reactions in RTMs. We introduce a novel quantitative criteria on the range of validity of local equilibrium assumption (LEA) in aquatic sediments with irreversible heterogeneous sorption reactions. Then we present a one-dimensional (1-D) early diagenetic module, MATSEDLAB, developed in MATLAB. The module provides templates for representing the reaction network, boundary conditions and transport regime, which the user can modify to fit the particular early diagenetic model configuration of interest. We describe the theoretical background of the model and introduce the MATLAB pdepe solver, followed by calibration and validation of the model by a number of theoretical and empirical applications. Finally, we introduce a new pore-scale model using lattice Boltzmann (LB) approach. It uses an iterative scheme for the chemical transport-reaction part and recent advances in the development of optimal advection-diffusion solvers within the lattice Boltzmann method framework. We present results for the dissolution and precipitation of a porous medium under different dynamical conditions, varying reaction rates and the ratio of advective to diffusive transport (Pe, Peclet number) for linear reactions. The final set of calculations considers sorption reactions on a heterogeneous porous medium. We use our model to investigate the effect of heterogeneity on the pore-scale distribution of sorption sites and the competition between three different sorption reactions.

Une meilleure performance économique du séchage industriel consiste à la fois en l'amélioration de la qualité des produits et de l’optimisation énergétique. Plusieurs technologies peuvent être appliquées pour intensifier le processus de séchage. Ce travail s’intéresse à l'effet des vibrations, qui peuvent accélérer le séchage via un échauffement par dissipation visqueuse, une amélioration de la migration de l’eau liquide et de la vapeur à l'intérieur du milieu poreux et une augmentation des coefficients de transferts externes de chaleur de masse. Toutefois, malgré les études numériques et expérimentales antérieures, l'évaluation de l'importance relative de ces mécanismes d'intensification doit encore être améliorée.Ce travail porte sur l'échelle du pore, simulée par un tube capillaire, partiellement rempli d'eau soumis à des vibrations sinusoïdales. Un dispositif expérimental complet a été conçu, développé et utilisé. Grâce à une procédure de traitement d'images pertinente, le comportement de l'eau à l'intérieur du tube (déplacement et le rayon du ménisque) ont été étudiés pour différentes configurations de vibrations (fréquence, amplitude, taille du tube). Les expériences avec des géométries symétriques et asymétriques sont destinées à imiter le transfert d'humidité pendant le séchage d'un milieu poreux. Quelle que soit la configuration étudiée, l'intensification du séchage a été clairement confirmée.Pour la configuration symétrique, une nouvelle cartographie 2D basée sur des nombres adimensionnels est définie pour résumer les effets capillaires et visqueux, et ainsi expliquer le comportement de l'eau en fonction des conditions vibratoires (rayon du tube, fréquence et amplitude). Pour la configuration asymétrique, les résultats expérimentaux sont discutés et comparés aux simulations obtenues avec deux modèles numériques (un modèle 0-D et un modèle 1-D). Le potentiel de la modélisation a été mis en évidence, mais il est encore limité par les hypothèses physiques aux interfaces. D'autres développements sont proposés afin d'augmenter la plage de validité et d'approfondir l'étude de ce système physique. / A better economic performance of industrial drying consists both in product quality improvement and energy efficiency enhancement. Several technologies can be applied to intensify the drying process. This work is focused on the effect of vibration that can assist the drying through heating-up due to viscous dissipation, enhancement of liquid and vapor migration inside the porous medium and the increase of the external heat and mass transfer. However, despite previous numerical and experimental studies, the assessment of the relative importance of these intensification mechanisms has still to be improved.This work is focused on the pore scale, simulated by a capillary tube, partially filled with water subjected to sinusoidal vibrations. A full experimental device was conceived, developed and used. Thanks to a relevant image processing chain, the behavior of water inside the tube (displacement and meniscus radius), was investigated for various vibration configurations (frequency, amplitude, tube size). Experiments with both symmetrical and asymmetrical geometries are intended to mimic the moisture transfer during drying of a porous medium. Whatever the configuration, the drying intensification was clearly confirmed.For the symmetrical configuration, a new 2D dimensionless number map is set to summarize the capillary and viscous effects and thus to explain the water behavior depending on vibration conditions (tube radius, frequency and amplitude). For the asymmetrical configuration, the experimental results are discussed and compared to the simulations obtained with two computational models (a 0-D model and 1-D model). The potential of modeling was evidenced but still limited by the surrounding physical assumptions. Further developments are proposed to increase the validity range and further investigate this physical system

Geological Carbon Storage (GCS) is considered as one of the key techniques to reduce the rate of atmospheric emissions of CO2 and thereby to contribute to controlling the global warming. A successful application of a GCS project requires the capability of the formation to trap CO2 for a long term. In this context, processes related to CO2 trapping and also possible leakage of CO2 to the near surface environment need to be understood. The overall aim of this thesis is to understand the flow and transport of CO2 through porous media in the context of geological storage of CO2. The entire range of scales, including the pore scale, the laboratory scale, the field experiment scale and the industrial scale of CO2 injection operation are addressed, and some of the key processes investigated by means of experiments and modeling.  First, a numerical model and laboratory experimental setup were developed to investigate the CO2 gas flow, mimicking the system in the near-surface conditions in case a leak from the storage formation should occur. The system specifically addressed the coupled flow and mass transport of gaseous CO2 both in the porous domain as well as the free flow domain above it. The comparison of experiments and modelling results showed a very good agreement indicating that the model developed can be applied to evaluate monitoring and surface detection of potential CO2 leakage. Second, the field scale CO2 injection test carried out in a shallow aquifer in Maguelone, France was analyzed and modeled. The results showed that Monte Carlo simulations accounting for the heterogeneity effects of the permeability field did capture the key observations of the monitoring data, while a homogeneous model could not represent them. Third, a numerical model based on phase-field method was developed and model simulations carried out addressing the effect of wettability on CO2-brine displacement at the pore-scale. The results show that strongly water-wet reservoirs provide a better potential for the dissolution trapping, due to the increase of interface between CO2 and brine with very low contact angles. The results further showed that strong water-wet conditions also imply a strong capillary effect, which is important for residual trapping of CO2. Finally, numerical model development and model simulations were carried out to address the large scale geological storage of CO2 in the presence of impurity gases in the CO2 rich phase. The results showed that impurity gases N2 and CH4 affected the spatial distribution of the gas (the supercritical CO2 rich phase), and a larger volume of reservoir is needed in comparison to the pure CO2 injection scenario. In addition, the solubility trapping significantly increased in the presence of N2 and CH4.

Les simulations numériques à l'échelle du pore sont fréquemment utilisées pour étudier le comportement des écoulements multiphasiques largement rencontrées dans phénomènes naturels et applications industrielles. Dans ce travail, la morphologie de structures liquides et l'action capillaire sont examinées à l'échelle des pores par la méthode de Boltzmann sur réseau (LBM) à plusieurs composants selon le modèle de Shan-Chen. Les résultats numériques obtenus sont en bon accord avec les solutions théoriques. Les simulations numériques sont étendues à microstructures complexes au-delà du régime pendulaire.La LBM a été utilisée pour modéliser l'écoulement multiphasique à travers un milieu poreux idéalisé dans des conditions de drainage primaire quasi-statique. Les simulations LBM ont fourni une excellente description du déplacement de l'interface fluide-fluide à travers les grains. Pendant le drainage, les simulations LBM sont capables de reproduire la déconnexion d'une phase dans le milieu granulaire sous la forme de ponts pendulaires ou structures liquides complexes. Malheureusement, le temps de calcul nécessaire pour ce type de simulations est assez élevé. Afin d’optimiser les ressources de calcul, nous présentons un modèle 2D (modèle Throat-Network) basé sur des solutions analytiques pour décrire l'écoulement biphasique à travers un ensemble de disques dans un temps de calcul très réduit, donc le modèle 2D est susceptible de remplacer les simulations LBM lorsque les ressources de calcul sont limitées. L'approche souligne l'importance de simuler le problème a l'échelle de la gorge du pore pour obtenir les relations volume - pression capillaire locales. Le modèle Throat-Network est un point de départ pour le modèle hybride proposé pour résoudre les problèmes en 3D. Le modèle hybride combine l’efficacité de l’approche réseau de pores et la précision du LBM à l’échelle des pores. Le modèle hybride est basé sur la décomposition de l’échantillon en petits sous-domaines, dans lesquels des simulations LBM sont effectuées pour déterminer les propriétés hydrostatiques principales (pression capillaire d'entrée, courbe de drainage primaire et morphologie du liquide pour chaque gorge du pore). Malgré la réduction significative des temps de calcul obtenus avec le modèle hybride, le temps n’est pas négligeable et les modélisations numériques d'échantillons de grandes tailles ne sont pas réalistes. Les approximations données par les méthodes Incircle et MS-P, qui prédisent les propriétés hydrostatiques, sont comparées à celles de LBM et du modèle hybride. / Numerical simulations at the pore scale are a way to study the behavior of multiphase flows encountered in many natural processes and industrial applications. In this work, liquid morphology and capillary action are examined at the pore-scale by means of the multicomponent Shan-Chen lattice Boltzmann method (LBM). The accuracy of the numerical model is first contrasted with theoretical solutions. The numerical results are extended to complex microstructures beyond the pendular regime.The LBM has been employed to simulate multiphase flow through idealized granular porous media under quasi-static primary drainage conditions. LBM simulations provide an excellent description of the fluid-fluid interface displacement through the grains. Additionally, the receding phase trapped in the granular media in form of pendular bridges or liquid clusters is well captured. Unfortunately, such simulations require a significant computation time. A 2D model (Throat-Network model) based on analytical solutions is proposed to mimic the multiphase flow with very reduced computation cost, therefore, suitable to replace LBM simulations when the computation resources are limited. The approach emphasizes the importance of simulating at the throat scale rather than the pore body scale in order to obtain the local capillary pressure - liquid content relationships. The Throat-Network model is a starting point for the a hybrid model proposed to solve 3D problems. The hybrid model combines the efficiency of the pore-network approach and the accuracy of the LBM at the pore scale to optimize the computational resources. The hybrid model is based on the decomposition of the granular assembly into small subsets, in which LBM simulations are performed to determine the main hydrostatic properties (entry capillary pressure, capillary pressure - liquid content relationship and liquid morphology for each pore throat). Despite the reduction of computation time, it is still not negligible and not affordable for large granular packings. Approximations by the Incircle and the MS-P method, which predict hydrostatic properties, are contrasted with the results provided by LBM and the hybrid model. Relatively accurate predictions are given by the approximations.