Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
A set of four reactive flow-through experiments at temperature T = 100 degrees C and total pressure P=12 MPa was performed in limestone reservoir samples. By using various ranging from 0.7 to 10 MPa, these experiments mimic mass transfers occurring (1) near the injection well, where the brine is almost saturated with CO2 (i.e. P-CO2 approximate to P), and (2) at increasing distances from the injection well, where the fluid displays lower values and higher divalent cation concentrations due rock dissolution along the fluid pathway. Results for P-CO2 = 10 MPa show non-uniform dissolution features associated with transport-controlled mass transfer, while reaction-controlled uniform dissolution is observed for P-CO2 = 2.5 MPa. The experiment with P-CO2 = 6 MPa allows investigating in detail the transition from transport-to reaction-controlled dissolution. Conversely, the experiment reproducing conditions far from the injection well (P-CO2 = 0.7 MPa), shows a decrease of porosity triggered by the precipitation of Mg-rich calcite. For all the dissolution experiments, the time-resolved porosity phi(t) can be modeled by a simple non-linear equation including parameters that characterise the dissolution regime triggered by the reactivity of the inlet fluid (measured by the Damkohler number, Da). Furthermore, all dissolution experiments display power scaling between permeability (k) and porosity (phi) with distinctly different scaling exponents characterising the reactivity of the fluid percolating the sample, independently from the decrease with time of the reactive surface area. It is shown also that dissolution at moderate positive values of Da seems the most efficient to increase permeability and promote a rapid spreading of the reaction front, while inducing minimal modification of the porosity in the vicinity of the CO2 injection well. These results can be used to parameterize the k-phi function for modeling the earliest dissolution processes occurring in the vicinity of the reaction front.
ISSN: 0009-2541

hal-00445277
https://hal.archives-ouvertes.fr/hal-00445277
DOI : 10.1016/j.chemgeo.2009.03.028

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
A reactive percolation experiment was conducted by injecting seawater into a permeable olivine aggregate at 190 °C and 19 MPa to explore the relationships between hydration reactions and hydrodynamic properties during the onset of serpentinization in the ultramafic lithosphere exposed at mid-ocean ridges. The experiment was stopped after 23 days when the sample became impermeable. The initial flow rate was 0.2 mL/h and then was decreased down to 0.06 mL/h after 8 days. Permeability decreased continuously throughout the experiment. The analyses of fluid chemistry time series and of the mineralogy and structure of the reacted sample showed olivine dissolution and precipitation of proto-serpentine, brucite and Fe-oxides. These reactions are controlled by coupled hydrodynamic and chemical processes interacting at different time and spatial scales. Their first characteristic is the production of silica rich outlet fluids in disequilibrium with the observed reacted mineral assemblages. These compositions are interpreted as resulting from a suite of coupled dissolution-precipitation reactions, controlled at the pore scale by surface kinetic processes, that rapidly reaches steady-state (constant fluid composition independent of fluid flux). Hence, the effective rate of serpentinization was controlled, to the first order, by the transport of reactants during the experiment. Mass balance calculations show that the rate of olivine conversion was fast (0.2-0.5 wt%/day), yet only ∼8 wt% of the olivine sample reacted, because the permeability drop limited fluid circulation. Porosity varied little during the experiment compared to permeability changes: the decrease of permeability was explained by the structure of the newly formed serpentine favouring the clogging of fluid paths. The rate at which permeability decreased was the fastest at low flux conditions. This suggests that permeability changes were not controlled simply by the kinetics of the serpentinization reactions, but mainly reflected the development of low Peclet pore scale zones forming micro-environments that control the serpentinization reaction-paths. These results outline the need to take into account the coupling of hydrodynamic and chemical processes when modelling the effects of reactive transport within the hydrating oceanic lithosphere.
ISSN: 0012-821X

hal-00855043
https://hal.archives-ouvertes.fr/hal-00855043
DOI : 10.1016/j.epsl.2013.03.052

Éditeur(s) : HAL CCSD American Association of Petroleum Geologists
Résumé : International audience
We describe the structure, microstructure, and petrophysical properties of fault rocks from two normal fault zones formed in low-porosity turbiditic arkosic sandstones, in deep diagenesis conditions similar to those of deeply buried reservoirs. These fault rocks are characterized by a foliated fabric and quartz-calcite sealed veins, which formation resulted from the combination of the (1) pressure solution of quartz, (2) intense fracturing sealed by quartz and calcite cements, and (3) neoformation of synkinematic white micas derived from the alteration of feldspars and chlorite. Fluid inclusion microthermometry in quartz and calcite cements demonstrates fault activity at temperatures of 195degC to 268degC. Permeability measurements on plugs oriented parallel with the principal axes of the finite strain ellipsoid show that the Y axis (parallel with the foliation and veins) is the direction of highest permeability in the foliated sandstone (10-2 md for Y against 10-3 md for X, Z, and the protolith, measured at a confining pressure of 20 bars). Microstructural observations document the localization of the preferential fluid path between the phyllosilicate particles forming the foliation. Hence, the direction of highest permeability in these fault rocks would be parallel with the fault and subhorizontal, that is, perpendicular to the slickenlines representing the local slip direction on the fault surface. We suggest that a similar relationship between kinematic markers and fault rock permeability anisotropy may be found in other fault zone types (reverse or strike-slip) affecting feldspar-rich lithologies in deep diagenesis conditions.
ISSN: 0149-1423

hal-00903428
https://hal.archives-ouvertes.fr/hal-00903428
DOI : 10.1306/03071312127

Éditeur(s) : HAL CCSD
Résumé : The coastal intrusion of brine threatens populations. This is particularly prejudicial in carbonate environments. We have studied the Miocene coral reef of S-E Majorca for better understanding the relation between geological structure and intrusion. For that purpose, we have used multi-scalar and multi-disciplinary methods. The measurements in 25 boreholes over the whole coral platform have allowed defining the stratigraphic structure and some elements of the regional tectonic. The reef progrades in the NE-SW direction, starting from the Aquitanian to terminates at the Messinian. The Messinian Salinity Crisis involves a disappearance of the Mediterranean corals and results in a Terminal Carbonate Complex which overlays a great part of the previously living corals of Majorca. At the experimental site scale, the study of the mineral composition, the texture, and the diagenesis have allowed characterization of the carbonate sequence heterogeneity. Layers of mineralization accompanied by dolomitization and low porosity correspond to postdepositional eustatic levels. The causes for the existence and the orientation of fractures are studied. The permeability to porosity relation is approached. The porosity structure is studied by comparison between primary and secondary porosity. This study contributes to the knowledge of the world best documented site for the evolution of carbonate reef reservoirs, with applications for brine intrusion and for hydrocarbon extraction.
Les intrusions d'eau salée en zone côtière constituent une menace pour la population. Celles-ci sont particulièrement dommageables en contexte carbonaté. Nous avons étudié le récif corallien Miocène du sud-est de Majorque afin de comprendre la relation entre structure géologique et intrusion. Pour cela nous avons utilisé des méthodes multi-scalaires et multi-disciplinaires. Les mesures dans 25 forages sur l'ensemble de la plateforme corallienne ont permis de préciser la structure stratigraphique et certains éléments de la tectonique régionale. Le récif prograde dans la direction NE-SO, en partant de l'Aquitanien pour aboutir au Messinien. La Crise de Salinité Messinienne entraîne une disparition des coraux méditerranéens et se traduit par un Complexe Carbonaté Terminal qui s'étend sur une grande partie des coraux autrefois vivants de Majorque. A l'échelle du site expérimental, l'étude de la composition minérale, de la texture et de la diagenèse ont permis de caractériser l'hétérogénéité de la séquence carbonatée. Des couches de minéralisation accompagnées de dolomitisation et de faible porosité correspondent à différents niveaux eustatiques post-dépositionnels. Les causes de l'existence et de l'orientation des fractures sont étudiées. La relation de perméabilité à porosité est précisée. La structure de porosité est étudiée par comparaison entre la porosité primaire et la porosité secondaire. Cette étude contribue à la connaissance du site le mieux documenté au monde pour l'évolution des réservoirs carbonatés récifaux, avec applications pour les intrusions d'eau salée et l'extraction des hydrocarbures.
https://tel.archives-ouvertes.fr/tel-00440019

tel-00440019
https://tel.archives-ouvertes.fr/tel-00440019
https://tel.archives-ouvertes.fr/tel-00440019/document
https://tel.archives-ouvertes.fr/tel-00440019/file/thesemariasube.pdf

Éditeur(s) : HAL CCSD American Geophysical Union
Résumé : International audience
The brittle to ductile transition (BDT) in rocks may strongly influence their transport properties (i.e., permeability, porosity topology ...) and the maximum depth and temperature where hydrothermal fluids may circulate. To examine this transition in the context of Icelandic crust, we conducted deformation experiments on a glassy basalt (GB) and a glass-free basalt (GFB) under oceanic crust conditions. Mechanical and micro-structural observations at a constant strain rate of 10(-5) s(-1) and at confining pressure of 100-300 MPa indicate that the rocks are brittle and dilatant up to 700-800 degrees C. At higher temperatures and effective pressures the deformation mode becomes macroscopically ductile, i.e., deformation is distributed throughout the sample and no localized shear rupture plane develops. The presence of glass is a key component reducing the sample strength and lowering the pressure of the BDT. In the brittle field, strength is consistent with a Mohr-Coulomb failure criterion with an internal coefficient of friction of 0.42 for both samples. In the ductile field, strength is strain rate-and temperature-dependent and both samples were characterized by the same stress exponent in the range 3 < n < 4.2 but by very different activation energy Q(GB) = 59 +/- 15 KJ/mol and Q(GFB) = 456 +/- 4 KJ/mol. Extrapolation of these results to the Iceland oceanic crust conditions predicts a BDT at similar to 100 degrees C for a glassy basalt, whereas the BDT might occur in non-glassy basalts at deeper conditions, i.e., temperatures higher than 550 +/- 100 degrees C, in agreement with the Icelandic seismogenic zone.
ISSN: 0148-0227

hal-00760905
https://hal.archives-ouvertes.fr/hal-00760905
DOI : 10.1029/2011JB008884

Éditeur(s) : HAL CCSD
Résumé : International audience
The porosity (from values of <1% up to more than 50%, with a mean value of 36.5%) and permeability (from very low values to 20.4 D, with a mean value around 800 mD) of 38 plugs, with a diameter 40 mm, have been measured. These plugs were taken approximately every 1.5 m along a 100 m-long core, sampling a series of reefal carbonate platform lithofacies. A non-unique relationship between porosity and permeability is obtained. In addition, the porosity was measured from processing X-ray micro-tomography images with resolutions ranging from 0.42 to 190.0 µm and sampling volumes ranging from less than 1 µm3 to few cm3. Depending on the structure of the pore network, the computed porosity is, in some cases, controlled by the X-ray image resolution and the sampled volume. While high resolution is required to image micro-porous material, large samples with lower resolution images are necessary for identifying distributed vugs and millimetre-scale structures. This study shows that multi-resolution X-ray micro-tomography is an effective tool for characterizing the multi-scale pore structure of carbonate rocks and understanding how it may control key petrophysical parameters such as porosity and permeability.
Geological Society Special Publication

hal-01174157
https://hal.archives-ouvertes.fr/hal-01174157
DOI : 10.1144/SP406.12

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
The interplay between fault zone cataclasis and cementation is important since both processes can drastically reduce the permeability of faults in porous sandstones. Yet the prediction of fault cementation in high-porosity sandstone reservoirs remains elusive. Nevertheless, this process has rarely been investigated in shallowly buried faults (<2 km; T°<80 °C) where its sealing capacity could be acquired early in the geological history of a reservoir. In this paper, the macro- and microscopic analysis of a fault zone in the porous Cenomanian quartz arenite sands of Provence (France) shows that silica diagenesis occurs in the most intensely-deformed cataclastic parts of the fault zone. This fault zone shows 19–48% of its total thickness occupied by low-porosity quartz-cemented cataclastic shear bands whose porosities range from 0 – ca. 5%. The analysis of the weathering profile around the fault zone reveals the presence of groundwater silcretes in the form of tabular, tightly silicified concretions cross-cut by the fault. Detailed transmitted light, cold-cathodoluminescence and scanning electron microscopy analyses of the silica cements (from the fault and the silcrete) reveal that all the silica cements originate from groundwater diagenetic processes. This study therefore shows that silica cementation can occur specifically in fault zones and as groundwater silcrete in the shallow context of a groundwater system, generated at the vicinity of an erosional unconformity.
ISSN: 0191-8141

hal-01278286
https://hal.archives-ouvertes.fr/hal-01278286
DOI : 10.1016/j.jsg.2015.10.001

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Underground CO2 sequestration is highly recommended as an effective means of significantly decreasing CO2 concentration in the atmosphere. Mineral storage is the more secure technology, but requires the presence of high concentration of divalent cations in the pore-fluid. Results from CO2 percolation experiments through chlorite/zeolite-rich sandstone samples from the Pretty Hill Formation (Otway Basin, Australia) are presented. The dissolution of the laumontite (7 wt.%) and chamosite (7 wt.%) are the potential sources of calcium, iron and magnesium required for carbonate precipitation. The percolation experiment was setup to reproduce, at laboratory scale, the in situ temperature and pressure conditions (T = 95 degrees C and P = 10 MPa). The fluid injected at constant flow rate is a rock-equilibrated brine subsequently enriched in CO2 up to partial pressure of 6 MPa. We observe feldspars, laumontite and chamosite dissolution, kaolinite and silica precipitation and a noticeable sink of CO2 in the sample which is attributed to the precipitation of both amorphous carbon due to the reduction of CO2 and Fe-rich carbonate. Permeability decreases of about one order of magnitude due to the localization of the kaolinite precipitation in the main flow paths, while porosity increases. The high reactivity of this sandstone makes this reservoir a valuable target for CO2 mineralization, but the associated permeability decrease may limit the injection rate and the spreading of the CO2 in the reservoir.
ISSN: 0009-2541

hal-00712829
https://hal.archives-ouvertes.fr/hal-00712829
DOI : 10.1016/j.chemgeo.2011.11.018

Éditeur(s) : HAL CCSD American Chemical Society
Résumé : International audience
Carbonation of ultramafic rocks in geological reservoirs is, in theory, the most efficient way to trap CO2 irreversibly; however, possible feedback effects between carbonation reactions and changes in the reservoir permeability must be considered to realistically assess the efficiency and sustainability of this process. We investigated changes in the hydrodynamic properties of sintered dunite samples by means of percolation experiments, under conditions analogous to that of in situ carbonation. Our results show that carbonation efficiency is controlled by the local renewal of the reactants and the heterogeneity of the pore structure. Preferential flow zones are characterized by the formation of magnetite and of a silica-rich layer at the olivine surfaces, which eventually inhibits olivine dissolution. Conversely, sustainable olivine dissolution together with coprecipitation of magnesite, siderite, and minor Mg-TOT-phyllosilicates, occur in reduced-flow zones. Thus carbonate precipitation only decreases porosity in zones where diffusion-controlled transport is dominant. Consequently, while high flow rates will decrease the carbonation efficiency of the reservoir and low flow rates may reduce the permeability irreversibly close to the injection point, moderate injection rates will ensure a partial carbonation of the rock and maintain the reservoir permeability.
ISSN: 0013-936X

hal-00424540
https://hal.archives-ouvertes.fr/hal-00424540
DOI : 10.1021/es8018429

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Improving the prediction of sub-seismic structures and their petrophysical properties is essential for realistic characterization of deformed sandstone reservoirs. In the present paper, we describe permeability contrasts induced by cataclastic deformation bands and faults in porous sandstones (766 data synthesized from field examples and the literature). We also discuss the influence of several factors, including tectonic regime, presence of a fault, burial depth, host sandstone porosity, and grain size and sorting for their initiation and permeability. This analysis confirms that permeability decrease is as a function of grain-crushing intensity in bands. Permeability reduction ranges from very limited in crush-microbreccia of compaction bands to high permeability reduction in cataclasites and ultracataclasites of shear-dominated bands, band clusters and faults. Tectonic regime, and especially normal-fault regime, with its tendency to localize strain and generate faults, is identified as the most important factor, leading to the formation of cataclastic bands with high permeability contrasts. Moreover, moderate burial depth (1–3 km) favors cataclastic bands with high permeability contrasts with respect to the host sandstone. High porosity, coarse-grain size and good grain sorting can slightly amplify the permeability reductions recorded in bands.
ISSN: 0191-8141

hal-01218408
https://hal.archives-ouvertes.fr/hal-01218408
DOI : 10.1016/j.jsg.2015.03.013

Éditeur(s) : HAL CCSD Springer Verlag (Germany) Springer Verlag
Résumé : International audience
The dissolution of carbonate rocks usually leads to both porosity (ϕ) and permeability (k) increase. We present experimental evidences and physical-based models of positive and anti-correlated dynamics of k and ϕ observed during dissolution experiments of carbonate rocks. We study the way the rate of change of ϕ and k is controlled by the degree of undersaturation of the percolating solution for two different types of carbonate rocks. We document the occurrence of an anti-correlated k−ϕ trend when the flowing fluid (deionized water) has a weak capacity of dissolution. A positive correlation is found when CO2 is added to the deionized water to increase the potential dissolution rate. Detailed analyses of the microstructures of the rock performed by X-ray microtomography reveal that low dissolution rate favors detachment of solid particles and their subsequent accumulation at the pore-throat inlet. Particles are detached from the rock matrix due to the differential dissolution rate of the indurated grains and the microporous cement. We then propose a simple phenomenological model to interpret the effect of the pore-throat clogging by the accumulation of partially dissolved carbonate particles. We conjecture that permeability is controlled by the decrease of the effective hydraulic radius and the increase of the tortuosity due to partial and localized obstruction of the pore network. Conversely, increasing the level of undersaturation of the flowing solution leads to an augmented potential of dissolving most of the transported particles before they reach the throats. In this case, both k and ϕ increase and display power-law correlations.
ISSN: 0169-3913

hal-01174145
https://hal.archives-ouvertes.fr/hal-01174145
DOI : 10.1007/s11242-015-0456-2

Éditeur(s) : HAL CCSD
Résumé : Fault zones are major discontinuities in sedimentary basins. Understanding their role on fluid migrations is an essential issue to (i) characterize the mechanisms and kinematics of deformation and (ii) to determine the parameters which control the distribution of energetic or mineral resources. This work applies to faulting under a temperature range of 200-250°C, corresponding to that of deeply buried reservoirs as well as potentially seismogenic fault zones. The studied faults are normal faults affecting the “Grès d’Annot” Formation, a Priabonian-Rupelian siliclastic turbidite succession of the Alpine foreland basin. They are located in two distinct areas: the Moutière-Restefond area in the eastern part of the basin and the Estrop area in the western part. Vitrinite reflectance outside fault zones indicates maximal temperatures of 240-260°C at Moutière-Restefond and 170-200°C at Estrop, i.e. burial depths around 8 km and 6 km, respectively, assuming a mean geothermal gradient of 30°C/km. Burial was due to underthrusting below the Embrunais-Ubaye Alpine nappes, the difference in burial between the two areas traducing the westward taper of the nappe front.The studied faults affect alternating arkosic sandstone beds and pelite layers with offsets from centimeters to decameters. Two types of core zones are recognized: (1) the foliated core zones of the Moutière-Restefond area, where deformation dominated by pressure solution and synkinematic phyllosilicate neoformation resulted in a foliated fabric, and (2) the core zones of the Estrop area, characterized by dilatant quartz-mineralized veins and breccia. Fault and host rock petrophysical properties were measured on drill plugs, using the water porosity technique and nitrogen permeability technique under 2 Mpa of confining pressure. In the Moutière-Restefond fault zones, plug axes were oriented in three orthogonal directions corresponding to the main deformation axes (X, Y, Z) of the foliated arkose to characterize the effect of structural anisotropy. In the Estrop fault zones, where deformation does not show equivalent anisotropy, the plug axes were oriented according to the main fault plane orientation (i.e., parallel to azimuth, parallel to dip and normal). In each fault zone, the porosity of fault rocks is equivalent to that of host rocks. In the Moutière-Restefond fault zones, the plugs parallel to the X and Z axes of deformation have a permeability similar to that of the host rocks, whereas permeability parallel to the Y axis (i.e. parallel to the foliation and the main fault plane) is one order of magnitude higher. By contrast, the permeability values in the Estrop fault zones are isotropic and equivalent to the host rock values. This study highlights the importance of various types of deformation mechanisms and related fluid-rock interactions in determining different fault rock types within a similar protolith, ultimately controlling distinct petrophysical properties of fault zones.
Les zones de failles constituent des discontinuités majeures dans la croûte supérieure. Ce mémoire s’intéresse aux failles actives à des profondeurs de 5-8 km, i.e. dans des conditions pouvant jouer un rôle important (i) sur le comportement mécanique de de la croûte, en particulier sur son potentiel sismogénique et (ii) sur la compartimentation des réservoirs géologiques profondément enfouis.Les failles étudiées sont des failles normales (rejet jusqu’à 50 mètres) affectant des alternances de bancs de grès arkosiques et de pélites dans les Grès d’Annot, une formation turbiditique d’âge priabonien-rupélien du bassin d’avant-chaine alpin. Les Grès d’Annot ont été enfouis sous les nappes de l’Embrunais-Ubaye peu de temps après leur dépôt et exhumés au Miocène moyen-supérieur. L’étude a été réalisée dans deux secteurs des Alpes de Haute-Provence, (1) le secteur de l’Estrop (chaine des Trois Evéchés, dans la partie occidentale du bassin) et (2) le secteur de Point Vert-Restefond (alentours du col de la Bonette, dans la partie orientale du bassin). La réflectance de la vitrinite dans les Grès d’Annot indique des températures maximales de 160-190°C dans le secteur (1) et de 240-260 °C dans le secteur (2) , soit des profondeurs d’enfouissement de 5-6 km et 8-10 km, respectivement, dans l’hypothèse d’un gradient géothermique moyen de 25-30°C/km. A partir des observations microstructurales, de données d’inclusions de fluides, de modélisations thermodynamiques sur chlorites syncinématiques et des indices de cristallinité de l’illite, on a établi que les failles du secteur (1) ont fonctionné à une température d’environ 200°C pour une pression de 0.6Kbar et celles du secteur (2) dans une gamme de température de 200-220°C et de pression comprise entre 0.6 et 1.1 Kba. L’activité de la faille de Point-Vert a été datée par la méthode 40Ar/39Ar au Miocène inférieur (21 Ma). Ces failles sont interprétées comme associées aux premiers stades du soulèvement résultant de l’activité des chevauchements dans le socle sous-jacent.Deux types principaux de roches de failles caractérisent les failles étudiées. Les brèches dilatantes sont majoritaires dans les zones de failles du secteur (1) alors que les arkoses foliées sont majoritaires dans les zones de failles du secteur (2). Les brèches dilatantes témoignent de mécanismes de déformation dominés par la fracturation transgranulaire et la pression-solution des silicates. Ce dernier mécanisme se manifeste principalement par d’abondantes précipitations cycliques de quartz, les stylolites restant peu développés. Les géométries structurales sont associées à l’activation de plans T de Riedel déterminant l’ouverture de relais extensifs et un régime localement dilatant. Nous associons ce type de roche de faille à une faible pression effective au cours de la déformation.La déformation cisaillante exprimée dans les arkoses foliées témoigne de mécanismes de déformation dominés par (i) la fracturation intragranulaire et transgranulaire, (ii) la pressionsolution/ précipitation des silicates, principalement le quartz, (iii) la néoformation de micas blancs liée à l’altération des feldspaths et (iv) la précipitation de chlorite. Ce travail montre également que les transformations minéralogiques liées aux interactions fluide-roche dans la zone de faille (forte augmentation de la proportion des phyllosilicates au dépend des feldspaths) changent radicalementla composition minéralogique de la roche. Nous associons ce type de roche de faille à une forte pression effective au cours de la déformation.La pétrophysique montre que les brèches de failles (secteur 1) ont une perméabilité isotrope et équivalente à celle du protolithe (10-3mD sous 2 MPa de confinement) tandis que les roches foliées (secteur 2) montrent une augmentation de perméabilité (10-2mD) selon l’axe Y de la déformation, d’un ordre de grandeur supérieure aux perméabilités suivant les axes X et Z et dans la roche hôte (10-3mD). Ce drain préférentiel potentiel est associé à l’orientation des phyllosilicates dans la foliation.
https://hal.archives-ouvertes.fr/tel-01310382

tel-01310382
https://hal.archives-ouvertes.fr/tel-01310382
https://hal.archives-ouvertes.fr/tel-01310382/document
https://hal.archives-ouvertes.fr/tel-01310382/file/Th%C3%A8seCAVAILHES2012.pdf

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Carbonation of peridotite is a widespread process in nature, with emerging societal and environmental implications through geological storage of CO2. We studied the micro- and nano-scale structures associated with the carbonation of peridotite pervaded by a CO2-rich water and the induced changes of its hydrodynamic properties. Focused ion beam (FIB) nanotomography was coupled with scanning electron microscopy (SEM) and transmission electron microscopy (TEM) observations. An experimental sample of dunite core percolated by a CO2-rich fluid (pCO2 = 11 MPa) at 160 °C was compared with a naturally carbonated sample from the Atlantic Ridge (Exp. IODP 304). Results of the 8-days percolation experiment show continuous alteration of olivine into magnesite locally associated with a poorly crystalline serpentine-type mineral referred to as proto-serpentine. The experiment is also characterized by an overall decrease in rock porosity (from 7.7 to 6.4%) and permeability (from 8.5 × 10− 16 to 1.7 × 10− 16 m2). The primary inter-granular porosity (1 to 10 μm) is progressively filled with magnesite, leading to the overall decrease of permeability. At the same time, a secondary small-scale porosity (10 nm to 1 μm) is created at the tip of the dissolution features along the (010) cleavage planes of olivine grains. Carbonate crystals grow within these etch-pit structures behind the dissolution front. Dissolution and precipitation occur at a relative rate that maintains the secondary porosity over the timescale of the experiment (i.e. carbonate growth has to be the slowest one). This process is interpreted as an interface coupled dissolution-precipitation mechanism of olivine carbonation. Proto-serpentine is only formed in highly reduced flow areas, such as small olivine etch-pits (10 to 500 nm wide), which are more isolated from CO2 input. SEM-FIB analyses show the 3D preferential orientation of the dissolution-precipitation planes within a given olivine grain. It suggests the formation of lateral connections between the etch-pits (infra-micrometric “channels”) providing access to reactants and removing reaction products at the reaction sites. The experimental results show that olivine dissolution and magnesite precipitation converge to a quasi-steady state resulting in a constant carbonation rate controlled by reaction kinetics and not by mass transfer for this flow regime. The system self-regulates, independently of the porosity change at least during this incipient stage of olivine carbonation. Similar textures are observed in natural samples collected at 170 m-depth in the vicinity of veinlets driving late fluids down into the cooling oceanic lithosphere. This suggests that similar mechanisms are active in nature and can play an important role in the late, low temperature alteration stages of fractured peridotite. These results also highlight the critical role of nm-scale spatial arrangement of dissolution and precipitation features on mass transfers and on the sustainability of olivine carbonation through coupled dissolution-precipitation processes.
ISSN: 0009-2541

hal-01684733
https://hal.archives-ouvertes.fr/hal-01684733
DOI : 10.1016/j.chemgeo.2017.11.013

Éditeur(s) : HAL CCSD American Geophysical Union
Résumé : International audience
A CO2-rich brine core-flood experiment in calcite limestone for conditions representative of underground storage (P = 12 MPa and T = 100°C) was performed in order to explore the dissolution mechanisms arising at moderate CO2 partial pressure (0.3 MPa). An increase of the total porosity (φT) accompanied by a persistent permeability (k) decrease was measured. The mechanisms controlling this atypical anticorrelated k − φT relationship were investigated from the analysis of high-resolution X-ray microtomography images of the sample acquired before and after the experiment. All the evidences converge to the conclusion that the ubiquitous decrease of permeability measured during the 44 h of dissolution is due to the clogging of a fraction of the macroporosity by microporous material triggered by the rearrangement of the detached undissolved particles. This mechanism results in the development of low permeability zones bridging the macroporosity.
ISSN: 0094-8276

hal-00903585
https://hal.archives-ouvertes.fr/hal-00903585
DOI : 10.1002/grl.50595

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
From outcrops located in Provence (South-East France), we describe the distribution, the microstructures, and the petrophysical properties of deformation band networks related to both contractional and extensional tectonic events. In contraction, pervasively distributed networks of reverse-sense compactional shear bands are observed in all folded sand units of the foreland, whereas localized networks of clustered reverse-sense shear bands are only observed close to a large-scale thrust. In extensional setting, networks of clustered normal-sense shear bands are generally observed adjacent to map-scale faults (100 m–10 km scale), although some randomly distributed bands are also observed between these faults. Normal-sense cataclastic faults, i.e. zone of deformation bands containing a localized slip-surface, are also observed to be restricted to sand units, suggesting that faults initiated in the sands during extension, but not during contraction. Shear bands and faults show cataclastic microstructures with high-permeability reduction whereas compactional shear bands show crush microbreccia or protocataclastic microstructures with moderate permeability reduction. This basin-scale analysis underlines the major role of tectonic settings (thrust-fault versus normal-fault andersonian-stress regime) and the influence of inherited large-scale faults on the formation/localization of low-permeability shear bands. We also provide a geometrical analysis of the band network properties (spacing, thickness, shear/compaction ratio, degree of cataclasis, petrophysical properties) with respect to the median grain size, porosity and grain sorting of host sand. This analysis suggests that grain size, although less important than stress-state conditions and the presence of large-scale faults, has a non-negligible effect on band network geometry. No correlations are observed between the grain sorting, porosity and band network geometry.
ISSN: 0264-8172

hal-01116421
https://hal.archives-ouvertes.fr/hal-01116421
DOI : 10.1016/j.marpetgeo.2013.12.020

Éditeur(s) : HAL CCSD Elsevier
Résumé : Deficient sealing in the well cement plugs and annulus due to mechanical fracturing is an important risk of CO2 leakage from the reservoir to others permeable layers and the surface. Such situation was reproduced at laboratory scale in order to determine the hydro-chemical control on the fracture permeability. Specifically, we investigated the effect of CO2 rich-brine flowing through fractured Portland cements at T = 60 °C and P = 10 MPa and variable flow rates. We showed that carbonation process is dominant and induces permeability decrease and leakage mitigation for extremely low flow rate whereas for high flow rate injection the permeability remains constant due to the precipitation of a low density secondary Si-rich phase which maintains the initial fracture aperture. At intermediate flow rate the hydraulic aperture can increase due to the densification of the material triggered by the net precipitation of low porosity calcite. These results emphasize that more complex behaviors than those considered from batch experiments may take place in the vicinity of flowing fractures. Specifically, the redissolution of the neoformed calcite as well as the development of amorphous phases, both controlled by the CO2-rich brine renewing rate in the fracture may prevent the healing fracture.
ISSN: 1750-5836

hal-00857555
https://hal.archives-ouvertes.fr/hal-00857555
DOI : 10.1016/j.ijggc.2013.04.002

Éditeur(s) : HAL CCSD
Résumé : Geological storage of CO2 is one of diverse technologies being explored to reduce atmospheric carbon fromindustrial processes (i.e. fossil fuel combustion). One of the specific features of CO2 injection is the possibility ofgeochemical reactions (dissolution – precipitation) between mobile reactive brine (e.g. formation water enrichedin CO2) and the host rock during the spatial and temporal evolution of CO2. That leads to modifications in thepore structure, which in turn change the flow dynamics of the reservoir (e.g. the permeability k). Then, thesesstructural modifications can largely control the injectivity, so that the pressure field in the reservoir and also theCO2 propagation. Accordingly, it is crucial to explore the changes in the reservoir properties (e.g. structural andhydrodynamic) induced during a CO2 injection and specially the relationships between them (e.g. k or reactivesurface-Sr versus porosity-φ , k versus rock heterogeneity), for developing predictive modelling tools of thetransport and reaction processes occurring during a CO2 injection and reliable risk assessment. In the case ofcarbonate rocks, the application of the predictive models of transport and reaction is still challenging, because oftheir high heterogeneity so that the incertitude in the reaction kinetics of carbonate minerals.From this perspective, we realized brine-enriched in CO2 percolation experiments through carbonate rocksamples in thermodynamic conditions expected during CO2 injection in deep reservoirs (T = 100°C et P =12MPa). The permeability changes k(t) is monitored during the experiments and the porosity variationφ (t) iscalculated from chemical analyses of the sampled outlet fluids, using ICP-EAS. The pore structure modificationsare investigated from high resolution X ray micro tomography images acquired from the synchrotron ofGrenoble (ESRF). Depending to the dissolution regime, controlled by the reservoir rock fabric and the chemicalcomposition of the brine (e.g. PCO2), we observed that a modification of pore structure can either improve(atypical result in dissolution context) or impair the value of the permeability k.
Le stockage géologique du CO2 est l’une des diverses technologies étant explorées afin deréduire les émissions de carbone atmosphérique des processus industriels (i.e. combustion del’énergie fossile). L’une des spécifiques caractéristiques de l’injection du CO2 en profondeurreste la possibilité de réactions géochimiques (dissolution-précipitation) entre la saumureréactive mobile (e.g. eau de formation enrichie en CO2) et la roche encaissante durantl’évolution spatiale et temporelle du CO2, conduisant à des modifications dans la structure despores et par conséquent dans les propriétés d’écoulement du réservoir (e.g. la perméabilité k).Donc, ces changements structuraux peuvent largement contrôler l’injectivité, ainsi que lechamp de pression dans le réservoir et aussi la propagation du CO2. Il demeure ainsi cruciald’explorer les changement dans les propriétés de réservoirs (e.g. structurales ethydrodynamiques) induits durant une injection de CO2 et explicitement les relations existantesentre eux (e.g. k ou surface réactive-Sr versus porosité-φ , k versus hétérogénéité de la roche),afin de développer des outils de modélisation prédictive des processus de transport etréactionnels se produisant durant une injection de CO2 et d’évaluer de façon fiable les risques.Dans le cas des réservoirs carbonatés, l’application des modèles prédictifs de transport réactifdemeure toujours un enjeu, car contrainte par la forte hétérogénéité en leur sein ainsi que parl’incertitude dans la cinétique de réactions des minéraux carbonatés dans ce contexte. Danscette optique, nous avons réalisé des expériences de percolation à travers des échantillons deroches carbonatées dans les conditions thermodynamiques de stockage en profondeur (T =100°C et P =12 MPa). L’évolution de la perméabilité k(t) est suivie au cours desexpériences ; et la variation de la porosité φ (t) est calculée à partir des résultats d’analyseschimiques au ICP-AES des fluides de sortie échantillonnés. L’investigation des modificationsapportées à la structure des pores est réalisée par le biais de la Micro-Tomographie hauterésolution à rayon X, acquise au synchrotron de Grenoble (e.g. ESRF).Dépendant du régime de dissolution, contrôlé par la fabrique de la roche réservoir et lacomposition chimique de la saumuré chargée en CO2 (e.g. PCO2 engagée), on a observéqu’une modification de la structure de la roche peut soit améliorer soit détériorer (résultatatypique en contexte de dissolution) la valeur de la perméabilité k.
https://hal.archives-ouvertes.fr/tel-01142136

tel-01142136
https://hal.archives-ouvertes.fr/tel-01142136
https://hal.archives-ouvertes.fr/tel-01142136/document
https://hal.archives-ouvertes.fr/tel-01142136/file/thesemangane2013.pdf

Éditeur(s) : HAL CCSD
Résumé : Geothermal energy is considered as a green and infinite energy source at human scale. Currently, the yield of geothermal power plants is limited to temperatures of the operating fluid which 350 °C. From tectonic and volcanic activity at mid-ocean ridges, Iceland is a location where supercritical fluid extraction (T> 375 °C) can considered for the near future. Exploiting such fluids could theoretically multiply by a factor of ten the electrical power delivered by geothermal wells. Can such fluids circulate at the base of brittle oceanic crust? This work investigates the petrophysical properties of basalts in order to constrain geophysical observations in Iceland and predict the behavior of very high temperature geo-hydrothermal reservoirs. The first approach consisted in studying the physical properties of rocks that have hosted deep hydrothermal circulations at oceanic ridges. The study of these rocks at ODP Site 1256 shows that the porosity measured both in the field and in the lab is associated with amphibolite facies alteration minerals (T> 500 ° C). The second approach was to recreate in the laboratory the conditions of pressure, temperature and pore fluid pressure of high temperature to supercritical hydrothermal systems to predict the mechanical and electrical properties of basalts under these conditions. The mechanical results indicate that the brittle/ductile transition occurs at a temperature of about 550° C, where a strong permeability decrease is expected. The implementation and calibration of a new cell for measuring electrical conductivity at high temperature provide the first results for the interpretation of geophysical data. When applied to basaltic crustal conditions in Iceland, these results indicate that hydrothermal fluids could circulate, at least temporarily, in a supercritical state up to 5 km depth.
La géothermie est considérée comme une source d'énergie propre et inépuisable à échelle humaine. Actuellement, le rendement des centrales géothermiques est limité à l'exploitation de fluides de températures inférieures à 350 °C. L'association de l'activité tectonique et volcanique aux dorsales océaniques fait de l'Islande un lieu où l'extraction de fluides supercritiques (T> 375 °C) peut être envisagée. Cette exploitation pourrait multiplier par dix la puissance électrique délivrée par le système géothermal. Ces fluides peuvent-ils circuler dans la croûte océanique ? Ce travail propose de contraindre les observations géophysiques et de prédire le fonctionnement des réservoirs géo-hydrothermaux de très haute température par l'étude des propriétés physiques des basaltes. La première approche est focalisée sur l'étude de roches ayant accueilli une circulation hydrothermale par le passé. L'étude de ces roches au site ODP 1256, montre que leur porosité est associée à la présence de minéraux d'altération hydrothermale du facies amphibolite (T> 500 °C). La seconde approche a consisté à recréer, en laboratoire, les conditions des systèmes hydrothermaux, à très haute température, afin de prédire les propriétés mécaniques et électriques des basaltes dans ces conditions. Les résultats mécaniques indiquent que la transition fragile/ductile, souvent associée à une forte décroissance de perméabilité, intervient à une température d'environ 550 °C. La mise en place d'une cellule de mesure de la conductivité électrique de haute température a fourni les premiers résultats utiles à l'analyse des données géophysiques. Appliqués aux conditions de la croûte basaltique Islandaise, ces résultats indiquent que des fluides hydrothermaux pourraient circuler au moins transitoirement à l'état supercritique jusqu'à ~ 5 km de profondeur.
https://tel.archives-ouvertes.fr/tel-00591798

tel-00591798
https://tel.archives-ouvertes.fr/tel-00591798
https://tel.archives-ouvertes.fr/tel-00591798/document
https://tel.archives-ouvertes.fr/tel-00591798/file/THESE_MV_pro.pdf

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Coastal aquifers often display seawater intrusion resulting in the formation of a salty water wedge progressing inland. This study investigates the mass transfers in the mixing zone at the freshwater-seawater interface where the water is out of equilibrium with the rock-forming carbonates. Investigations were conducted in two boreholes, separated by 5 m, at the Ses Sitjoles test site (Mallorca Island, Spain) where repeated electrical conductivity logs of the formation and the saturating fluid, as well as regular pore-water sampling and permanent downhole multi-parameter monitoring of the water were performed over a period of 9 a. In the mixing zone, the significant acidification, the calcite saturation index profile and the Ca concentration profile cannot be explained by conservative mixing nor by dissolution-precipitation reactions only. Conversely, the analysis of organic C content and of the distinctly different time-resolved pH profiles measured in the two boreholes suggests the development of perennial biomass that triggers calcite dissolution. Moreover, the presence of biomass seems to be correlated with the permeability and vertical connectivity at the meter-scale. It is speculated that the mechanism could be self-activated because the microbiological activity induces calcite dissolution and tends to increase porosity and permeability that favors biomass development.
ISSN: 0883-2927

hal-00937665
https://hal.archives-ouvertes.fr/hal-00937665
DOI : 10.1016/j.apgeochem.2013.09.011

Éditeur(s) : HAL CCSD American Association of Petroleum Geologists
Résumé : In reservoir engineering, hydrodynamic properties can be estimated from downhole electrical data using heuristic models (e.g., Archie and Kozeny-Carman's equations) relating electrical conductivity to porosity and permeability. Although proven to be predictive for many sandstone reservoirs, the models mostly fail when applied to carbonate reservoirs that generally display extremely complex pore network structures. In this article, we investigate the control of the three-dimensional (3-D) geometry and morphology of the pore network on the electrical and flow properties, comparing core-scale laboratory measurements and 3-D x-ray microtomography image analysis of samples from a Miocene reefal carbonate platform located in Mallorca (Spain). The results show that micrometer- to centimeter-scale heterogeneities strongly influence the measured macroscopic physical parameters that are then used to evaluate the hydrodynamic properties of the rock, and therefore, existing models might not provide accurate descriptions because these heterogeneities occur at scales smaller than those of the integration volume of the borehole geophysical methods. However, associated with specific data processing, 3-D imagery techniques are a useful and probably unique mean to characterize the rock heterogeneity and, thus, the properties variability.
ISSN: 0149-1423

hal-00950066
https://hal.archives-ouvertes.fr/hal-00950066
DOI : 10.1306/05221312134