Carbon dioxide capture and storage (CCS) is considered one of the key technologies for reducing atmospheric emissions of CO₂ from human activities (IPCC, 2005). The scale of potential deployment of CCS is enormous spanning manufacturing, power generation and hydrocarbon extraction worldwide. Uncertainty, cost-benefit challenges, market barriers and failures, and promotion and regulation of infrastructure are the main obstacles for deploying CCS technology in a broad scale. In a CCS project, it is the operator’s responsibility to guarantee the CO₂ containment while complying with environmental regulations and CO₂ contractual requirements with the source emitter. Acquiring new information (e.g. seismic, logs, production data, etc.) about a particular field can reduce the uncertainty about the reservoir properties and can (but not necessarily) influence the decisions affecting the deployment of a CCS project. The main objective of this study is to provide a decision-analysis framework to quantify the Value of Information (VOI) in a CCS project that faces uncertainties about permeability values in the reservoir. This uncertainty translates into risks of CO₂ migration out of the containment zone (or lease zone), non-compliance with contractual requirements on CO₂ storage capacity, and leakage of CO₂ to sources of Underground Source of Drinking Water (USDW). The field under analysis has been idealized based on a real project located in Texas. Subsurface modeling of the upper Frio Formation (injection zone) was conducted using well logs, field-specific GIS data, and other relevant published literature. The idealized model was run for different scenarios with different permeability distributions. The VOI was quantified by defining prior scenarios based on the current knowledge of a reservoir, contractual requirements, and regulatory constraints. The project operator has the option to obtain more reliable estimates of permeability, which will help to reduce the uncertainty of the CO₂ behavior and storage capacity of the formation. The accuracy of the information gathering activities is then applied to the prior probabilities (Bayesian inference) to infer the value of such data. / text

A partnership between oilfield operators and the federal government in the coupled CO₂ enhanced oil recovery (EOR) and storage projects brings long-term benefits for both. We quantify the win-win condition for this partnership in terms of an optimum storage tax credit. We describe the field-scale design optimization of coupled CO₂-EOR and storage operations from the viewpoint of oilfield operators. We introduce a CO₂ market model and investigate two special CO₂ market problems, namely a fixed storage requirement and an integrated asset optimization. The first problem follows an environmental objective by giving priority to the storage element of CO₂-EOR and storage; the second prioritizes the oil recovery and relies on the principles of a free market where CO₂ is a commodity and the commitment to storage is made based on the economic benefits. We investigate the CO₂ market sustainability conditions and quantitatively derive them for the fixed storage requirement and integrated asset optimization problems. Ultimately, we quantify the impact of storage tax credit on the operator benefits, the federal government benefits, and the optimum economic storage capacity of an oilfield. CO₂ EOR-storage projects are long-term and capital-intensive and therefore vulnerable to the risks of the CO₂ market. Two important uncertain economic parameters are investigated, the oil price and the storage tax credit. The government plays an important role in reducing the CO₂ market risks because it has the leverage to regulate the storage tax credit. The stochastic optimization results show that a transparent storage tax credit reinforces the sustainability of the CO₂ market and helps both the government and the oilfield operators boost their long-term benefits. / text

Stacked storage systems are a viable carbon management operation, especially in regions with potential growth in CO₂ enhanced oil recovery (EOR) projects. Under a carbon constrained environment, the industrial Texas Gulf Coast is an ideal area for development of stacked storage operations, with a characteristically high CO₂ intensity and abundance of aging oil fields. The development of EOR along the Texas Gulf Coast is limited by CO₂ supply constraints. A stacked storage system is implemented with an EOR project to manage the temporal differences between the operation of a coal-fired power plant and EOR production. Currently, most EOR operations produce natural CO₂ from geologic formations. A switch to anthropogenic CO₂ sources would require an EOR operator to handle volumes of CO₂ beyond EOR usage. The use of CO₂ in an EOR operation is controlled and managed to maximize oil production, but increasing injection rates to handle the volume of CO₂ captured from a coal plant can decrease oil production efficiency. With stacked storage operations, a CO₂ storage reservoir is implemented with an EOR project to maintain injection capacity equivalent to a coal plant's emissions under a carbon constrained environment. By adding a CO₂ storage operation, revenue can still be generated from EOR production, but it is considerably less than just operating an EOR project. The challenge for an efficient stacked storage project is to optimize oil production and maximize profits, while minimizing the revenue reduction of pure carbon sequestration. There is an abundance of saline aquifers along the Texas Gulf Coast, including the Wilcox, Vicksburg, and Miocene formations. To make a stacked storage system more viable and reduce storage costs, maximizing injectivity is critical, as storage formations are evaluated on a cost-per-ton injected basis. This cost-per-ton injected criteria, also established as injection efficiency, incorporates reservoir injectivity and depth dependant drilling costs to determine the most effective storage formation to incorporate with an EOR project. With regionally adequate depth to maximize injectivity while maintaining reasonable drilling costs, the Vicksburg formation is typically the preferred storage reservoir in a stacked storage system along the Texas Gulf Coast. Of the eleven oil fields analyzed on a net present value basis, the Hastings field has the greatest potential for both EOR and stacked storage operations. / text

Depuis une dizaine d'années, une volonté internationale de réduction des émissions de gaz à effet de serre s'est développée, afin de limiter leur concentration dans l'atmosphère. Ainsi, il est envisagé de récupérer le CO₂ issu d'activités humaines fortement émettrices afin de le réinjecter dans le sous-sol à l'état supercritique. Hors du panache de CO₂ supercritique, ce gaz se dissout dans la saumure et l'acidifie. Deux phénomènes ont alors lieu. Ils constituent la base des études menées au cours de cette thèse : (i) le devenir des espèces chimiques mobilisées par la dissolution des minéraux, et (ii) les variations des propriétés d'écoulements induites par la réactivité de la roche encaissante. Pour étudier ces phénomènes, des expériences ont été menées sur les carbonates de Lavoux et de St-Emilion. Ces deux échantillons naturels ont été sélectionnés pour leur composition minérale modèle qui assure une forte réactivité dans le contexte de l'étude, et l'absence d'argile et de matière organique qui limite la complexité du système géochimique. Les expériences menées sont de deux types. En autoclave, la compétition entre dissolution et sorption des éléments traces est mise en avant et permet d'investiguer des conditions variant de celles de la surface (20°C – 1 atm) à celles d'un site de stockage (40°C – 90 bar de CO₂) en passant par des intermédiaires de pression (30 et 60 bar). Les effets de la salinité de la saumure, de la concentration initiale en cations divalents ainsi que de l'état de l'échantillon solide (poudre, plug) sont étudiés. D'autre part, un dispositif expérimental a été développé au cours de cette thèse. Il permet d'étudier les propriétés de diffusion d'éléments traces à travers une carotte dans des conditions représentatives de celles d'un réservoir de stockage de CO₂. Les résultats expérimentaux obtenus mettent en évidence à la fois l'impact de la dissolution sur la mobilisation des espèces chimiques, la compétition entre différents cations pour la sorption et les conséquences de cette sélectivité sur le transport et la disponibilité des espèces chimiques. L'étude pétrophysique des échantillons réagis met en évidence une augmentation de la porosité, et une tendance à l'uniformisation du réseau de pore. Les données obtenues dans les expériences en batch permettent d'obtenir par simulation les paramètres de sorption du système pour les différents éléments traces, en fonction des conditions de pression. Grâce à ces différents résultats, la surveillance de sites de stockage géologique de CO₂ est possible dans différentes formations, et permet un suivi à la fois des flux des espèces chimiques et des propriétés d'écoulement. / Over the last decade, an international will to reduce the emissions of greenhouse gases in the atmosphere developed, in order to limit their atmospheric concentration. Thus, to deal with the large amounts of CO₂ produced by human activities, this gas is to be injected under supercritical state in the underground. Outside the CO₂ plume, this gas dissolves within brine and acidifies it. Two phenomena occurs then. They are the main subject of this work: (i) the fate of chemical species mobilized by mineral dissolution, and (ii) the evolution of flooding properties induced by mineral reactivity. To study those phenomena, experiments were carried out on the Lavoux and the Saint-Emilion carbonates. Those two natural samples were selected because their mineralogical composition ensures a high reactivity and limits the complexity of the geochemical system, as they contain neither clays nor organic matter. Two types of experiments were carried out. Competition between dissolution and sorption was studied in batch reactors, from conditions similar to those of the surface (20°C – 1 atm) to those of a storage site (40°C – 90 bar of CO₂), passing by intermediate pressures (30 and 60 bar). The parameters investigated are salinity, initial concentration of divalent cations, and the state of solid samples (powder, core). On the other hand, an experimental setting was developed during the thesis project. It allows the study of trace elements diffusion through a core in CO₂ geological storage conditions. The experimental results evidence the impact of dissolution on chemical species mobilization, competition between those species regarding sorption and consequences of this selectivity on transport and availability of those chemical species. The petrophysical study of reacted samples evidence a porosity increase and the homogenization of the porous network. The data resulting from the batch experiments are used as input data for simulations, in order to estimate sorption parameters of trace elements in the systems investigated. Thanks to those results, the monitoring of CO₂ geological storage sites is possible within several different geological formations, and allows to track both flux of chemical species and flooding properties evolution.

Une solution prometteuse pour diminuer les émissions anthropogéniques de gaz à effet de serre consiste à injecter une partie des rejets industriels de CO2 dans des formations souterraines. Celles-ci comportent un réservoir entouré de roches de couverture, qui constituent la première barrière à la migration des fluides. La caractérisation de leurs propriétés de confinement et de leur évolution en présence de CO2 est donc un élément clé de la sécurité d’un site de stockage. Le travail présenté propose une méthodologie, appliquée ici à des roches carbonatées du bassin parisien, permettant de mesurer les paramètres de transport de roches de couverture et les conséquences d’un vieillissement en conditions représentatives de celles d’un stockage en aquifère profond. La pression de percée, le coefficient de diffusion des produits de dissolution du CO2, et la perméabilité, paramètres contrôlant les principaux mécanismes de fuite, ont été mesurés avant et après altération des matériaux par réaction avec une saumure saturée en CO2 dans des conditions thermodynamiques typiques d’un réservoir (environ 80°C et 100 bar). Les résultats obtenus ont révélé un bon comportement global des roches, mais également une forte diminution du potentiel de confinement en présence de défauts structurels initiaux (fractures rebouchées, pores de grand diamètre...). Une simulation numérique décrivant les évolutions de la formation rocheuse non-fissurée sur une durée de 1000 ans a été réalisée en s’appuyant sur des paramètres mesurés directement ou obtenus par modélisation des essais d’altération. Elle a montré que les transformations engendrées par le stockage de CO2 sous une roche de couverture homogène restent très limitées spatialement / A promising solution to reduce anthropogenic emissions of greenhouse effect gases consists in the injection and long-term storage of a part of the industrial carbon dioxide discharges in underground formations. These formations must be composed of a reservoir surrounded by tight caprocks, which represent the first barrier preventing fluids migration. The characterization of their confining properties and of their evolution in presence of CO2 is thus a key element regarding a storage site security. This work presents a methodology allowing the measurement of caprocks transport parameters and the consequences of an alteration under representative conditions of deep aquifers storage. This methodology was applied to carbonate rocks from the Paris basin. The breakthrough pressure, the diffusion coefficient of CO2 dissolution products, and the permeability, controlling parameters of leakage mechanisms, were measured before and after alteration of the materials by reaction with a CO2-saturated brine under reservoir thermodynamic conditions (about 80°C and 100 bar). Results revealed a satisfactory global behaviour under these aggressive conditions, but also a strong diminution of the confinement potential in presence of initial structural faults (sealed fractures, large-diameter pores…) forming higher-permeability zones. A numeric simulation describing the evolution of a homogeneous rock formation during 1000 years was also realized based on parameters directly measured or obtained by modelling of the alteration experiments. It showed that the transformations brought by the CO2 storage under a rock formation with no initial faults remain very localized spatially