Éditeur(s) : HAL CCSD
Résumé : International audience
The injection of reactive mineral suspensions is a possible process to either reinforce or seal wells in geologic carbon sequestration sites. Among others, olivine slurries could be used as CO2-triggered cements, as they carbonate under the thermodynamic conditions of deep storage. However, injection of such slurries requires to control their initial fluidity and its evolution during the displacement. For this purpose, we have characterized the rheological evolution of olivine suspensions, of particle sizes 1−10 μm, sheared at 100 s−1, in the ranges of 10−40% for the volume fractions, 20−50 bars for the CO2 pressure, and 60-110°C for the temperature. The apparent viscosity, measured at 100 s−1, increases exponentially, with a characteristic time ranging from less than 1 h to more than 10 h, and decreasing with olivine concentration, CO2 pressure, and temperature. Moreover, a careful characterization of the slurry rheology carried out in the initial stages of slow evolution, shows that the slurry obeys a Bingham plastic law, with a yield stress ΣB, and a Bingham viscosity µB increasing from 1 to 20 Pa and from 4 to 110 mPa s, respectively, when the olivine volume fraction φ is increased from 10 to 30%. Such variations can be accounted by classical models (Wildemuth and Williams [1984]: Rheologica Acta, 23,627-635, Krieger [1972]: Advances in Colloid and Interface Science, 3, 111-136).
Environmental Progress & Sustainable Energy

hal-01054131
https://hal.archives-ouvertes.fr/hal-01054131
DOI : 10.1002/ep.11826

Éditeur(s) : HAL CCSD Elsevier
Résumé : We investigate experimentally the alteration of fractured class-G cement flowed by CO2-rich brine. The experiment mimics a mechanically damaged rough-walled fractured cement annulus at temperature 60 °C and pressure 10 MPa. The experiment consists of flowing a reservoir-equilibrated brine mixed with CO2 (partial pressure of 2.3 MPa) through the fracture of average aperture 14 μm at constant flow rate (100 μL min−1). This flow rate corresponds to pressure gradient representative of an average in situ hydrodynamic condition. Results indicate an intense alteration of the cement with a large removal of mass at the scale of the sample. However, the fracture alteration patterns are triggered by the initial heterogeneity of the fracture aperture; the aperture of the low aperture zones tends to decrease due to calcite precipitation whereas preferential paths develop in the zones of higher aperture associated. Nevertheless, the expected large permeability increase triggered by the mass removal is mitigated by the precipitation of a low density Si-rich amorphous material. The alteration rate will decrease with time because of the increasing distance of diffusion between the fracture where the reactants are actively renewed by advection and the portlandite and C-S-H dissolution fronts. The different zones of reaction can be adequately modeled by a simple 1D diffusion-reaction model using published kinetics coefficients and extrapolation to larger times than the experiment time can be drawn. Altogether, and in addition to the previous studies of the alteration of fractured well cement annulus, this study shows that the leakage potential is strongly controlled by the initial distribution of the aperture along the fracture: low aperture zones will tend to self-heal while localized flow in connected high aperture paths will be perennial.
ISSN: 1750-5836

hal-01346006
https://hal.archives-ouvertes.fr/hal-01346006
DOI : 10.1016/j.ijggc.2016.01.032

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
The main goal of the monitoring stage of Carbon Capture and Storage (CCS) is to obtain an accurate estimation of the subsurface CO2 accumulation and to detect any possible leakage. Laboratory experiments are necessary to investigate the small scale processes governing the CO2–brine–rock interaction. They also provide a means to calibrate the results coming from field scale geophysical methods. In this work we set up an experimental system which is able to perform Electrical Resistivity Tomography (ERT) measurements on centimeter-scale rock samples at various P–T conditions. We present the results of two new experiments related to CO2 monitoring, performed on a cylindrical (4 × 8 cm) Fontainebleau rock sample. In the first one, we have quantified the CO2 saturation at different volume fractions, representing zones from a deep saline aquifer with varying degrees of saturation. In the second one, we have monitored and quantified the effect of CO2 dissolution in the brine at a pressure of 40 bar during eight days, emulating the invasion of CO2 into a shallow aquifer. Results highlight the importance of accounting for the contribution of surface conductivity in highly CO2-saturated regions, even in clay-free rocks, and also for brine conductivity variation due to CO2 dissolution. Ignoring any of these effects will end up in a CO2 saturation underestimation. We present a modified CO2 saturation equation to account for these two influences.
ISSN: 0926-9851

hal-01356323
https://hal.archives-ouvertes.fr/hal-01356323
DOI : 10.1016/j.jappgeo.2016.03.039

Éditeur(s) : HAL CCSD
Résumé : In order to minimize CO2 atmospheric concentration, a solution consists in sequestrating CO2 in geological reservoirs. To estimate long term risks, it is necessary to quantify the couplings between reaction processes as well as structural and hydrodynamical modifications. We realised two experimental benches enabling injecting CO2-enriched-brine in conditions corresponding to in situ storage (T < 200 oC and P < 200 bar) and developed
an experimental protocol using X-Ray microtomography and fluid and rock analyses in order to measure the variations of physical and chemical parameters.
The study of carbonated reservoirs near the injection well, allows quantifying different k-phi relationships depending on the dissolution processes and triggered by the local fluid chemical composition and initials conditions. Away from the injection well, we observe carbonate precipitation decreasing the permeability. The study of fracturated caprock samples shows that alternative percolation of CO2-enriched-brine and CO2 gas increases the fracture permeability.
The study of silicated rocks indicates carbonate precipitation in zeolite sandstone and sintered dunite grains. Nevertheless, in zeolite sandstone we also observe the precipitation of clay particles located in the uid pathways which decrease strongly the permeability.
Afin de minimiser la concentration en CO2 dans l'atmosphère une solution consiste à le séquestrer dans les réservoirs géologiques. Pour évaluer les risques à long terme, il est nécessaire de quantifier les couplages entre les processus réactionnels et les modifications structurales et hydrodynamiques. Dans cette optique, nous avons construit deux dispositifs expérimentaux permettant d'injecter des saumures chargées en CO2 dans les conditions de stockage (T < 200 °C et P < 200 bar) et mis en oeuvre un protocole expérimental utilisant la microtomographie RX et l'analyse des roches et des fuides pour quantifier les variations des paramètres physiques et chimiques. Dans le cas des réservoirs carbonatés, on observe, près du puits d'injection, une forte variabilité des relations k-phi en fonction du régime de dissolution contrôlé par la chimie locale du fluide, ainsi que par les conditions initiales. A plus grande distance, on observe des processus de précipitation diminuant fortement la perméabilité. L'étude des roches de couverture fracturées (argilite) a montré qu'une percolation alternée d'une saumure chargée en CO2 et de CO2 gaz augmentait la perméabilité de fracture. Dans le cas des roches silicatées, la précipitation de carbonates est mise en évidence aussi bien dans les grès à zéolites que dans les frittés de dunite de San Carlos. Cependant, dans les grès à zéolites, la précipitation d'une phase argileuse est observée dans les chemins d'écoulement et engendre une forte diminution de la perméabilité.
https://tel.archives-ouvertes.fr/tel-00416408

tel-00416408
https://tel.archives-ouvertes.fr/tel-00416408
https://tel.archives-ouvertes.fr/tel-00416408/document
https://tel.archives-ouvertes.fr/tel-00416408/file/These_Luquot.pdf

Éditeur(s) : HAL CCSD
Résumé : International audience
RST 2008
Nancy, France

hal-00569242
https://hal-mines-paristech.archives-ouvertes.fr/hal-00569242

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Numerical programs for simulating flow and reactive transport in porous media are essential tools for predicting reservoir properties changes triggered by CO2 underground injection. At reservoir scale, meshed models in which equations are solved assuming that constant macroscopic properties can be defined in each cells, are widely used. However, the parameterization of the dissolution-precipitation problem and of the feedback effects of these processes on the flow field is still challenging. The problem arises from the mismatch between the scales at which averaged parameters are defined in the meshed model and the scale at which chemical reactions occur and modify the pore network geometry. In this paper we investigate the links between the dissolution mechanisms that control the porosity changes and the related changes of the reactive surface area and of the permeability. First, the reactive surface area is computed from X-ray microtomography data obtained before and after a set of dissolution experiments of pure calcite rock samples using distinctly different brine-CO2 mixtures characterizing homogeneous to heterogeneous dissolution regimes. The results are used to validate the power law empirical model relating the reactive surface area to porosity proposed by Luquot and Gauze (2009). Second, we investigate the spatial distribution of the effective hydraulic radius and of the tortuosity, two structural parameters that control permeability, in order to explain the different porosity-permeability relationships observed for heterogeneous and homogeneous dissolution regimes. It is shown that the increase of permeability is due to the decrease of the tortuosity for homogeneous dissolution, whereas it is due to the combination of tortuosity decrease and hydraulic radius increase for heterogeneous dissolution. For the intermediate dissolution regime, identified to be the optimal regime for increasing permeability with small changes in porosity, the increase of permeability results from a large increase in the mean effective hydraulic radius of the sample.
ISSN: 0169-7722

hal-00617671
https://hal.archives-ouvertes.fr/hal-00617671
DOI : 10.1016/j.jconhyd.2010.07.004