Éditeur(s) : HAL CCSD Elsevier
Résumé : International audience
A shallow field experimental site for CO2 injection was established at Maguelone (Languedoc, France), in order to test in an integrated manner a suite of surface and downhole hydrogeophysical monitoring methods. The objective is to improve monitoring of gas transport in the shallow subsurface and to determine the sensitivity of CO2 monitoring systems for leakage detection. The site offers a natural laboratory to study the processes associated with CO2 injection in a clastic and clay-rich context saturated with saline fluids. Prior to CO2 injection, three nitrogen (N2) injections were undertaken in 2012 to measure the site response to neutral gas injection. In 2013, a volume of 111 m3 (mass of 220 kg) of CO2 was injected during 3.5 h at 15 m depth. During each experiment, the gas plumes were successfully detected from pressure monitoring, time-lapse induction logging and downhole resistivity monitoring with dipole–dipole array. Increases in resistivity are attributed to free gas propagation (either N2 or CO2) whereas decreases in resistivity correlate with CO2 dissolution in the pore fluid. Chemical analyses confirm this hypothesis with a decrease in pH and an increase in the concentration of dissolved species in the latter case.
ISSN: 1750-5836

hal-01355943
https://hal.archives-ouvertes.fr/hal-01355943
DOI : 10.1016/j.ijggc.2015.12.005

Éditeur(s) : HAL CCSD Mineralogical Society of America
Résumé : International audience
In situ mineralization of CO2 in ultramafic rock-hosted aquifers is one of the promising solutions for decreasing CO2 concentrations in the atmosphere. Naturally altered ultramafic rocks suggest that carbonation processes are controlled by local heterogeneities in the structure of the rock and fluid transport at the water-rock interfaces. We studied the role of rock crystallographic anisotropy relative to the global fluid flow direction on the mineralization of CO2 by means of electron microscope analyses from the macro- to the micrometer scale (EBSD-FIB). The sample used for the measurements was a hot pressed olivine core percolated by water enriched in CO2 (pCO2 = 10 MPa) at 180 °C. During the percolation experiment, olivine was dissolved and two types of carbonates, dolomite, and magnesite, were precipitated on olivine surfaces. The results showed that the dissolution of olivine is controlled by its crystallographic properties as shown by the development of etch-pits only on the (010)ol planes and with elongated shapes parallel to the [010]ol axes. In contrast, the precipitation of carbonates is governed by hydrodynamic properties. Carbonates are heterogeneously distributed in the percolated rock. They are mainly located along the moderate (for dolomite) and the minor (for magnesite) flow paths, both oriented parallel to the principal fluid flow direction, which allow carbonates to be supplied with divalent cations (e.g., Ca2+, Mg2+, and Fe2+). In these flow paths, carbonate growth is systematically oriented normal to the flow that facilitates the development of chemical gradients with cationic supersaturation conditions for carbonate precipitation near the walls.In natural systems, the (010)ol planes are parallel to the Moho and the (100)ol planes are vertical; our study suggests that flow of CO2-rich fluids will induce precipitation of carbonates localized along, and preferentially clogging, vertical flow paths while favoring olivine dissolution along horizontal fluid pathways. This dual control of structure and fluid flow on carbonation mechanisms could be an important parameter allowing sustainable CO2 storage in peridotites, while limiting the risks of leakage toward the surface.
ISSN: 0003-004X

hal-01143393
https://hal.archives-ouvertes.fr/hal-01143393
DOI : 10.2138/am-2015-4913

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 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 American Chemical Society
Résumé : Experiments were conducted to assess the potential impact of fractured well-cement degradation on leakage rate. Permeability was monitored while CO2-enriched reservoir-equilibrated brine was flowed at constant rate through a single fracture in a class G cement core under conditions mimicking geologic sequestration environments (temperature 60 °C, pressure 10 MPa). The results demonstrate that, at least for the conditions used in the experiment, an initial leakage in a 42 μm aperture fracture (permeability = 1.5 × 10-10 m2) can be self-mitigated due to the decrease of the fracture hydraulic aperture after about 15 h. This decrease results from the development of continuous highly hydrated amorphous Si-rich alteration products at the edge of the fracture and the dense carbonation of the bulk cement that mitigate the penetration of the alteration front.
ISSN: 0013-936X

hal-00950088
https://hal.archives-ouvertes.fr/hal-00950088
DOI : 10.1021/es401317c

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