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 : 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 Elsevier
Résumé : International audience
To evaluate the performance of downhole and surface geophysical monitoring methods, a series of shallow gas injection-monitoring experiments has been performed in a coastal saline aquifer at Maguelone, France. The recorded data include pressure measurements with a Westbay multilevel completion and CO2 saturation at an observation well derived from electrical resistivity with a modified Waxman-Smits (MWS) model. In this work, the aim is to develop a simulation model capturing the gas transport behavior and consistent with field data. For this purpose, the simulation of the CO2 injection experiment is carried out with two conceptual models, a homogeneous model and a heterogeneous model treated with multiple realization Monte Carlo simulations. Numerical simulator TOUGH2 with the equation of state module EOS7C is used for the simulations. Comparison of the model results with field data suggests that the pressure responses are captured with relatively good accuracy. Similarly, the model also provides an overall reasonable agreement and correct order of magnitude for predicted gas saturation values. However, as the heterogeneity pattern in the field data remains largely unknown, the model predictions can only be used to capture the mean behavior as well as to provide insights into how heterogeneity can influence the system behavior, by means of sensitivity analyses of the influence of heterogeneities on individual realizations.
ISSN: 1750-5836

hal-01467240
https://hal.archives-ouvertes.fr/hal-01467240
DOI : 10.1016/j.ijggc.2016.09.006

Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
Numerical programs for simulating flow and reactive transport in porous media is essential for predicting reservoir properties related to CO2 sequestration performance, subsurface storage and risk assessment. In this paper we solve the Navier Stokes' equation using finite difference method, on a simulated porous rock structure, to study the velocity distribution of fluid flowing through it under a constant pressure gradient. A reactive solute carried through the fluid is allowed to interact with the minerals in the rock. This chemical reaction dissolves the mineral which changes the rock structure thus affecting its flow properties. These changes of flow properties are studied with variation in reactive solute concentration and pressure field. The different mechanisms of dissolution responsible for the variation of flow properties for the different parameters is predicted. Before the onset of homogeneous dissolution, variation in porosity follows a power-law behaviour with change in permeability when the latter is scaled by the concentration of the reactive species. The simulation results are compared with available experimental data and found to give a reasonable match.
ISSN: 0022-1694

hal-00757760
https://hal.archives-ouvertes.fr/hal-00757760
DOI : 10.1016/j.jhydrol.2012.05.024

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