Imbibition describes the rate of mass transfer between the rock and the fractures. Therefore, understanding the imbibition process and the key parameters that control the imbibition process is crucial. Capillary imbibition experiments usually take a long time, especially when we need to vary some parameters to investigate their effects. Therefore, this research presented the numerical studies with the matrix block surrounded by the wetting phase for better understanding the characteristic of spontaneous imbibition, and also evaluated dimensionless time for validating the scheme of upscaling laboratory imbibition experiments to field dimensions. Numerous parametric studies have been performed within the scope of this research. The results were analyzed in detail to investigate oil recovery during spontaneous imbibition with different types of boundary conditions. The results of these studies have been upscaled to the field dimensions. The validity of the new definition of characteristic length used in the modified scaling group has been evaluated. The new scaling group used to correlate simulation results has been compared to the early upscaling technique. The research revealed the individual effects of various parameters on imbibition oil recovery. Also, the study showed that the characteristic length and the new scaling technique significantly improved upscaling correlations.

Le BUT de ma thèse est d’étudier les mécanismes fondamentaux du mélange d’une poudre avec un liquide : Au début du mélange, la poudre et le liquide sont versés dans le mélangeur, des agrégats de poudre communément appelés grumeaux se forment. Ensuite chaque agrégat va évoluer par l’action de plusieurs phénomènes : l’imbibition, phénomène spontané qui désigne l’infiltration d’un liquide dans un milieu poreux par capillarité ; et le phénomène forcé de rupture sous contraintes d’écoulement. A l’état final la poudre est dispersée finement et de façon homogène dans le liquide. Ma thèse est alors structurée en deux parties : l’étude de la cinétique d’imbibition d’un agrégat sphérique immergé ; et l’étude de la rupture d’un agrégat sous contrainte extérieure. La REUSSITE de l’étude provient des expériences approfondies: de la création d’un nouveau procédé de fabrication d’un agrégat grâce à l’impression 3D, jusqu’à la détermination de lois empiriques de nouveaux phénomènes mis en évidence. / The GOAL of my PhD is to study the fundamental mechanisms of mixing a powder with a liquid. The mix of focus proceeds as follows:At start, as the powder and the liquid are filled in the mixer, powder aggregates form.Then each powder aggregate evolves under the influence of several phenomena: imbibition, spontaneous phenomenon corresponding to the infiltration of a liquid inside a porous medium by capillarity; and the forced phenomenon of rupture under flow. At last the powder is finely and homogeneously dispersed in the liquid. My PhD is thus organized in two parts: the study of the imbibitions kinetics of a spherical aggregate, and the study of the rupture of an aggregate under flow.The SUCCESS of the study relies on the thorough experiments: from creating a new aggregate manufacturing process using 3D printing, to determining empirical laws corresponding to new phenomena.

This thesis presents procedures to properly simulate naturally fractured reservoirs using dual-porosity models. The main objectives of this work are to: (1) determine if the spontaneous imbibition can be simulated using a two phase CMG simulator and validate it with laboratory experiments in the literature; (2) study the effect of countercurrent imbibition in field scale applications; and (3) develop procedures for using the dual-porosity to simulate fluid displacement in a naturally fractured reservoir. Reservoir simulation techniques, analytical solutions and numerical simulation for a two phase single and dual-porosity are used to achieve our objectives. Analysis of a single matrix block with an injector and a producer well connected by a single fracture is analyzed and compared with both two phase single and dual-porosity models. Procedures for obtaining reliable results when modeling a naturally fractured reservoir with a two phase dual-porosity model are presented and analyzed.

Dans l'industrie du forage pétrolier, les conditions de travail de plus en plus sévères requièrent sans cesse de nouveaux outils plus résistants à l'usure abrasive et à l'impact. Afin de répondre à ce défi, les travaux présentés ici, ont pour but l'élaboration de matériaux en carbure cémenté à gradient de composition par le procédé d'imbibition réactive. Ce procédé peut être décomposé en deux procédés de gradation, à savoir : l'imbibition et le revêtement réactif. L'imbibition a pour rôle d'enrichir graduellement, en phase liante, le coeur d'une pièce en carbure cémenté dense et repose sur le principe de migration de phase liquide dans un corps solide-liquide. Le revêtement réactif est un procédé qui s'applique également sur un carbure cémenté dense sur lequel est déposé un revêtement de nitrure de bore. Après avoir atteint le liquidus de la phase liante du carbure cémenté, une précipitation de borures ternaires prend place à la surface du matériau et s'étend graduellement sur des distances millimétriques. Dans le cas de pièces industrielles (inserts tricône et supports de taillants PDC (Polycrystalline Diamond Compact)), le traitement d'imbibition réactive permet de générer des gradients de dureté pouvant atteindre 450 HV sur 25 mm. L'élaboration de tels gradients a nécessité une meilleure compréhension des cinétiques ainsi que des phénomènes mis en jeu durant l'imbibition et le revêtement réactif. Dans le cas des taillants PDC, l'influence des paramètres du procédé HPHT de synthèse de la plaquette diamantée, sur le gradient de composition présent dans le support WC-Co après imbibition réactive, a été étudiée. Ces travaux se sont également intéressés à l'effet de ces gradients de composition sur les propriétés des plaquettes diamantées ainsi obtenues. A la suite d'essais mécaniques, les inserts WC-Co et taillants PDC gradués montrent une augmentation significative de leur résistance à l'abrasion (de 30 à 100%) et de leur tenue à l'impact (de 20 à 40%). / In oil drilling industry, harsher working conditions require ever new and more abrasive wear and impact resistant tools. To meet this challenge, the work presented here, is to develop graded cemented carbide materials by reactive imbibition process. This method can be divided into two gradation processes, namely, reactive coating and imbibition. Imbibition gradually enriches the core of dense cemented carbide with binder phase and is based on the principle of liquid phase migration in a solid-liquid body. Reactive coating also takes place in dense cemented carbide on which a boron nitride coating is deposited. After reaction with the WC-Co liquid binder, some ternary boride precipitations take place from surface to several millimeters deep. For industrial parts (inserts for roller cone bits and PDC (Polycrystalline Diamond Compact) cutters substrates), hardness gradients obtained can reach 450 HV on 25 mm. Such gradients development is passed through a better understanding of kinetics and phenomena occurring during imbibition and reactive coating. In case of PDC cutters, influence of HPHT process parameters, allowing diamond table synthesis, on the WC-Co substrate gradient, generated by reactive imbibition, was studied. This work was also interested in gradient effect on the obtained diamond tables properties. After mechanical tests, graded WC-Co inserts and graded PDC cutters show a significant increase of both wear resistance (from 30 to 100%) and impact resistance (from 20 to 40%).

Les milieux poreux sont omniprésents dans le quotidien des hommes du 21ème siècle que ce soit par hasard ou par nécessité. Certains permettent le transport d’une ou plusieurs phases fluides immiscibles, une situation à la fois courante et critique dans de nombreuses applications industrielles. Le transport d’une phase mouillante, l’imbibition, a été largement étudiée mais un certain nombre de problèmes restent ouverts. Dans cette thèse, nous nous sommes concentrés sur trois d’entre eux. La fragmentation de phase induite par la gravité dans une jonction asymétrique a été étudiée. La dynamique et un critère d’apparition ont été prédits analytiquement puis confirmés expérimentalement. Ensuite, l’évolution de l’épaisseur d’un front d’imbibition dans un réseau de capillaires a été simulée numériquement. Les résultats ont permis de lever une controverse de la littérature. Enfin, l’imbibition dans un milieu constitué de lames flexibles déformables a été explorée numériquement et expérimentalement. Il a été montré que la déformabilité des lames induit leur coalescence et agit sur la dynamique de l'imbibition. / Porous media are ubiquitous in today’s society due to chance or necessity. Some of them allow the transportation of one or several immiscible fluid phases simultaneously. This property is both usual and critical in many industrial processes. The transport of a wetting phase, imbibition, has been widely studied but lots of issues remain opened. In this manuscript, three of them are addressed. Gravity induced phase fragmentation has been studied in an asymmetric pore junction. Fragmentation criterion and dynamic are predicted analytically and confirmed experimentally. Then, the broadening of an imbibition front in a capillary network has been investigated numerically. Results resolved a controversy in the literature. Finally, imbibition in a medium made of flexible sheets has been studied both numerically and experimentally. It showed that sheets flexibility induces their clustering and influences the imbibition dynamic.

Les mélanges de toluène et de tert-butanol sont complètement miscibles dans toutes les compositions à l'échelle macroscopique. Toutefois tert-butanol forme un réseau de liaisons hydrogène à l'échelle nanométrique qui persistent même dans les mélanges liquides binaires tert-butanol/toluène. Des expériences de diffusion de neutrons ont révélé la séparation des phases du mélange dans une structure cœur-gaine sous confinement dans des solides nanoporeux hydrophiles. Le travail effectué dans cette thèse vise à comprendre le rôle joué par la concurrence des interactions intermoléculaires (liaisons hydrogène, Van der Waals) lors de la séparation de phase sous nanoconfinement. Des expériences de RMN révèlent la persistance d'un réseau de liaisons hydrogène dans ces liquides binaires confinés dans des nanopores de silice à des concentrations faibles de tert -butanol, fournissant la preuves d'un autre type de réseau de liaisons hydrogène sous confinement. Des expériences d'adsorption du mélange gazeux dans des nanopores de silice ont aidé à expliquer l'affinité plus élevée des parois de silice polaires pour tert-butanol par une modèle thermodynamique. Le remplacement de la matrice hôte par un analogue hydrophobe est associé à une inversion de la sélectivité, montrant cette fois une plus grande affinité du toluène pour la surface des pores. L'effet des interactions spécifiques avec la surface sur la dynamique d'imbibition spontanée de ces liquides binaires à travers le réseau de silice nanoporeux a également été étudié. Des expériences de radiographie de neutrons ont révélé la séparation des flux à deux composants, au sein d'une dynamique toujours gouvernée par une loi de Lucas-Washburn. / Toluene and tert-butanol mixtures are completely miscible for all compositions at the macroscopic scale. However tert-butanol forms a network of hydrogen-bonded clusters at the nanoscale which persist even in the tert-butanol-toluene binary liquid mixtures. Interpretation of neutron scattering experiments revealed phase separation of the mixture into a core-shell structure inside hydrophilic nanoporous solids, with a tert-butanol shell and a toluene core. The work carried out in this thesis is aimed at understanding the role played by competing intermolecular interactions (hydrogen-bonding, van der Waals) in driving phase separation in confinement. NMR experiments reveal the persistence of a hydrogen-bonding network in these binary liquids confined in silica nanopores even at very low concentrations of tert-butanol, providing evidence of a new kind of hydrogen bonded network under confinement. Vapour sorption isotherms of tert-butanol-toluene binary gas mixtures in silica nanopores helped explain higher affinity of polar silica walls for tert-butanol by a thermodynamic model. Replacing the host matrix by a hydrophobic analogue was found to reverse the selectivity, with toluene showing greater affinity for the pore surface. Effect of surface specific interactions was studied on spontaneous imbibition dynamics of these binary liquids through nanoporous silica network. Neutron radiography experiments revealed the separation of fluxes into a twocomponent flow, generally obeying the Lucas-Washburn law.

Brazing and soldering, as advanced manufacturing processes, are of significant importance to industrial applications. It is widely accepted that joining by brazing or soldering is possible if a liquid metal wets the solids to be joined. Wetting, hence spreading and capillary action of liquid metal (often called filler) is of significant importance. Good wetting is required to distribute liquid metal over/between the substrate materials for a successful bonding. Topographically altered surfaces have been used to exploit novel wetting phenomena and associated capillary actions, such as imbibitions (a penetration of a liquid front over/through a rough, patterned surface). Modification of surface roughness may be considered as a venue to tune and control the spreading behavior of the liquids. Modeling of spreading of liquids on rough surface, in particular liquid metals is to a large extent unexplored and constitutes a cutting edge research topic. In this dissertation the imbibitions of liquid metal has been considered as pertained to the metal bonding processes involving brazing and soldering fillers. First, a detailed review of fundamentals and the recent progress in studies of non-reactive and reactive wetting/capillary phenomena has been provided. An imbibition phenomenon has been experimentally achieved for organic liquids and molten metals during spreading over topographically modified intermetallic surfaces. It is demonstrated that the kinetics of such an imbibition over rough surfaces follows the Washburn-type law during the main spreading stage. The Washburn-type theoretical modeling framework has been established for both isotropic and anisotropic non-reactive imbibition of liquid systems over rough surfaces. The rough surface domain is considered as a porous-like medium and the associated surface topographical features have been characterized either theoretically or experimentally through corresponding permeability, porosity and tortuosity. Phenomenological records and empirical data have been utilized to verify the constructed model. The agreement between predictions and empirical evidence appears to be good. Moreover, a reactive wetting in a high temperature brazing process has been studied for both polished and rough surfaces. A linear relation between the propagating triple line and the time has been established, with spreading dominated by a strong chemical reaction.

The demand for energy and new oil reservoirs around the world has increased rapidly while oil recovery from depleted reservoirs has become more difficult. Oil production from fractured carbonate reservoirs by water flooding is often inefficient due to the commonly oil-wet nature of matrix rocks. Chemical enhanced oil recovery (EOR) processes such as surfactant-induced wettability alteration and interfacial tension reduction are required to decrease the residual oil saturation in matrix blocks, leading to incremental oil recovery. However, improvement in recovery will depend on the degree of wettability alteration and interfacial tension (IFT) reduction, which in turn are functions of matrix permeability, fracture intensity, temperature, pressure, and fluid properties. The oil recovery from fractured carbonate reservoirs is frequently considered to be dominated by the spontaneous imbibition mechanism which is a combination of viscous, capillary, and gravity forces. The primary purpose of this study is to model wettability alteration in the lab scale for both coreflood and imbibition cell tests using the chemical flooding reservoir simulator. The experimental recovery data for fractured carbonate rocks with different petrophysical properties were history-matched with UTCHEM, The University of Texas in-house compositional chemical flooding simulator, using a highly heterogeneous permeability distribution. Extensive simulation work demonstrates the validity and ranges of applicability of upscaled procedures, and also indicates the importance of viscous and capillary forces in larger fields. The results of this work will be useful for designing field-scale chemical EOR processes. / text

During carbon dioxide (CO₂) sequestration, CO₂ injection suffers from viscous fingering and low sweep efficiency. In addition, the lower density of CO₂ compared to in-situ brine leads to the possibility of sequestered CO₂ rising up through the relatively permeable path in the cap rock and being emitted back out to the atmosphere. This research proposes a mechanism of CO₂-in-brine emulsion stabilization by surface-coated nanoparticles as a potential cure for these problems. This mechanism is studied in detail by conducting a series of core floods to investigate the interactions between nanoparticles and the surroundings such as fluids and rock surfaces during nanoparticle transport in sedimentary rocks. The experiments presented here use n-octane as a low-pressure analog fluid to supercritical CO₂ as they share several key characteristics. Comparisons of pressure drop and CT images from drainage displacement experiments with and without nanoparticles show that nanoparticle-stabilized emulsions were generated in-situ in highly permeable and homogeneous Boise sandstones tested in this study. Roof snap-off is proposed as the key mechanism for generating the emulsions. The imbibition experiment presents a case where Roof snap-off does not occur. The pressure drop for the control experiment and the nanoparticle experiments confirmed that without Roof snap-off nanoparticles do not affect the dynamics of the displacement except for the viscosity increase of the aqueous phase. However, it was inferred from the saturation profiles and effluent concentration history that nanoparticles were traveling faster than the aqueous phase in which they were dispersed and accumulating at the main displacement front. Inaccessible pore volume is proposed as a mechanism responsible for the accelerated transport of nanoparticles. The single-phase flow experiments demonstrate the accelerated transport of nanoparticles in porous media that was invoked to explain observations during imbibition displacement. During these experiments, tracer and nanoparticles were simultaneously injected into a porous medium and their effluent concentrations were monitored using a UV-Vis detector. The results show that nanoparticles traveled faster than the tracer in Boise and Berea sandstones studied in this research. Two-site model developed by Zhang (2012) was used to fit the data. Simulations suggested that the two-site model could replicate the overall shape of the experimental data when a slug of nanoparticle dispersion was injected, but it was not able to accurately predict the leading edge and the trailing edge of the effluent concentration history, where nanoparticles appeared before tracer due to accelerated transport. To account for the enhanced transport of nanoparticles, a modified two-site model with an acceleration factor, E, is proposed. The resulting fit matched the experimental data better than the original two-site model. / text

Spontaneous imbibition of water into Fontainebleau Sandstone matrix because of capillary gradient is an important mechanism for oil recovery from Fontainebleau Sandstone reservoirs. Spontaneous imbibition characteristics of Fontainebleau Sandstone core were determined by measuring the Wettability Index of four Fontainebleau Sandstone core samples under laboratory conditions. This was done by utilizing a combination of a Benchtop Relative Permeameter Flooding System and Amott Cups. The specimen had a diameter of 38mm and a height of 47mm. Permeability and porosity of the cores varied from 12 to 14 mD and 10 to 14% respectively. The fluids and chemicals used were kerosene, synthetic brine and Sodium dodecyl sulphate. Amott’s method was used to measure the wettability index. This method consists of four steps: (1) brine flooding, (2) spontaneous imbibition of brine, (3) kerosene flooding, (4) spontaneous imbibition of kerosene. One core was saturated with kerosene and then flooded with brine, followed by spontaneous imbibition of brine. Similarly, another core was saturated with brine and then flooded with kerosene, followed by spontaneous imbibition of kerosene. Similar procedures were used for other two cores except the addition of surfactant to the synthetic brine. All cores were then cleaned and re-saturated for spontaneous imbibition of kerosene and brine. All Experiments were performed under laboratory temperature conditions. Oil and water wettability values were obtained along with secondary and tertiary oil recoveries. These values were used to calculate the wettability index of Fontainebleau sandstone cores. Spontaneous imbibition characteristics of the cores obtained from the experimental data indicate that Fontainebleau Sandstone formation is a potential candidate for Secondary and Tertiary oil recovery by water injection and spontaneous imbibition.