Experimental evaluation of interactions in supercritical CO2/water/rock minerals system under geologic CO2 sequestration conditions

Lin, Hua; Fujii, Takashi; Takisawa, Reisuke; Takahashi, Toru; Hashida, Toshiyuki

doi:10.1007/s10853-007-2029-4

Cited by 131 publications

(78 citation statements)

References 13 publications

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“…There are four principal mechanisms by which scCO 2 might be immobilized in the subsurface: stratigraphic, solubility, mineral and residual trapping. Stratigraphic trapping is where CO 2 is held underneath impermeable seal rocks; solubility trapping is where CO 2 dissolves into the resident brine surrounding the injected CO 2 [2][3][4] ; mineral trapping is where carbonate mineral phases are precipitated into the rock 5 ; and residual or capillary trapping is where CO 2 is held by surface forces as tiny droplets (ganglia) in the pore-space of the rock 6 . This can occur either naturally, by the migration of the CO 2 plume [7][8][9] , or can be induced by the injection of chase brines 10 .…”

Section: Introductionmentioning

confidence: 99%

Reservoir Condition Pore-scale Imaging of Multiple Fluid Phases Using X-ray Microtomography

Andrew

Bijeljic

Blunt

2015

JoVE

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X-ray microtomography was used to image, at a resolution of 6.6 µm, the pore-scale arrangement of residual carbon dioxide ganglia in the pore-space of a carbonate rock at pressures and temperatures representative of typical formations used for CO 2 storage. Chemical equilibrium between the CO 2 , brine and rock phases was maintained using a high pressure high temperature reactor, replicating conditions far away from the injection site. Fluid flow was controlled using high pressure high temperature syringe pumps. To maintain representative in-situ conditions within the micro-CT scanner a carbon fiber high pressure micro-CT coreholder was used. Diffusive CO 2 exchange across the confining sleeve from the pore-space of the rock to the confining fluid was prevented by surrounding the core with a triple wrap of aluminum foil. Reconstructed brine contrast was modeled using a polychromatic x-ray source, and brine composition was chosen to maximize the three phase contrast between the two fluids and the rock. Flexible flow lines were used to reduce forces on the sample during image acquisition, potentially causing unwanted sample motion, a major shortcoming in previous techniques. An internal thermocouple, placed directly adjacent to the rock core, coupled with an external flexible heating wrap and a PID controller was used to maintain a constant temperature within the flow cell. Substantial amounts of CO 2 were trapped, with a residual saturation of 0.203 ± 0.013, and the sizes of larger volume ganglia obey power law distributions, consistent with percolation theory.

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Section: Introductionmentioning

confidence: 99%

Reservoir Condition Pore-scale Imaging of Multiple Fluid Phases Using X-ray Microtomography

Andrew

Bijeljic

Blunt

2015

JoVE

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“…Capillary condensation of water from scCO 2 and coalescence of water films will also occur; however, little is known about water film behavior, or even thickness, in scCO 2 . Moreover, recent studies [7][8][9][10][11] have shown that the development of a water layer controls the chemical reactivity at the scCO 2 -mineral interface, may be critical to mineral dissolution reactions in scCO 2 .…”

Section: Introductionmentioning

confidence: 99%

Fundamental study of CO2-H2O-mineral interactions for carbon sequestration, with emphasis on the nature of the supercritical fluid-mineral interface.

Bryan¹,

Dewers²,

Heath³

et al. 2013

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In the supercritical CO 2 -water-mineral systems relevant to subsurface CO 2 sequestration, interfacial processes at the supercritical fluid-mineral interface will strongly affect core-and reservoir-scale hydrologic properties. Experimental and theoretical studies have shown that water films will form on mineral surfaces in supercritical CO 2 , but will be thinner than those that form in vadose zone environments at any given matric potential. The theoretical model presented here allows assessment of water saturation as a function of matric potential, a critical step for evaluating relative permeabilities the CO 2 sequestration environment. The experimental water adsorption studies, using Quartz Crystal Microbalance and Fourier Transform Infrared Spectroscopy methods, confirm the major conclusions of the adsorption/condensation model. Additional data provided by the FTIR study is that CO 2 intercalation into clays, if it occurs, does not involve carbonate or bicarbonate formation, or significant restriction of CO 2 mobility.We have shown that the water film that forms in supercritical CO 2 is reactive with common rock-forming minerals, including albite, orthoclase, labradorite, and muscovite. The experimental data indicate that reactivity is a function of water film thickness; at an activity of water of 0.9, the greatest extent of reaction in scCO 2 occurred in areas (step edges, surface pits) where capillary condensation thickened the water films. This suggests that dissolution/precipitation reactions may occur preferentially in small pores and pore throats, where it may have a disproportionately large effect on rock hydrologic properties.Finally, a theoretical model is presented here that describes the formation and movement of CO 2 ganglia in porous media, allowing assessment of the effect of pore size and structural heterogeneity on capillary trapping efficiency. The model results also suggest possible engineering approaches for optimizing trapping capacity and for monitoring ganglion formation in the subsurface. 6 ACKNOWLEDGMENTS

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“…The solubility of water into CO 2 is also of importance, because it affects the reactivity of CO 2 with surrounding rocks (e.g., Regnault et al 2005;Rimmelé et al 2008;Lin et al 2008;Suto et al 2007) and determines the capacity of injected CO 2 to dry the rock formations adjacent to injection wells (Giorgis et al 2007;Hurter et al 2007;Pruess and Müller 2009). In the case of a CO 2 -based EGS, the partitioning of water into CO 2 would also determine the time required for the removal of water from the (central portion of the) EGS, and the type of chemical interactions that may take place between the CO 2 plume, reservoir rocks, and engineered systems.…”

Section: Introductionmentioning

confidence: 99%

A Phase-Partitioning Model for CO2–Brine Mixtures at Elevated Temperatures and Pressures: Application to CO2-Enhanced Geothermal Systems

2009

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Correlations are presented to compute the mutual solubilities of CO 2 and chloride brines at temperatures 12-300 • C, pressures 1-600 bar (0.1-60 MPa), and salinities 0-6 m NaCl. The formulation is computationally efficient and primarily intended for numerical simulations of CO 2 -water flow in carbon sequestration and geothermal studies. The phase-partitioning model relies on experimental data from literature for phase partitioning between CO 2 and NaCl brines, and extends the previously published correlations to higher temperatures. The model relies on activity coefficients for the H 2 O-rich (aqueous) phase and fugacity coefficients for the CO 2 -rich phase. Activity coefficients are treated using a Margules expression for CO 2 in pure water, and a Pitzer expression for salting-out effects. Fugacity coefficients are computed using a modified Redlich-Kwong equation of state and mixing rules that incorporate asymmetric binary interaction parameters. Parameters for the calculation of activity and fugacity coefficients were fitted to published solubility data over the P-T range of interest. In doing so, mutual solubilities and gas-phase volumetric data are typically reproduced within the scatter of the available data. An example of multiphase flow simulation implementing the mutual solubility model is presented for the case of a hypothetical, enhanced geothermal system where CO 2 is used as the heat extraction fluid. In this simulation, dry supercritical CO 2 at 20 • C is injected into a 200 • C hot-water reservoir. Results show that the injected CO 2 displaces the formation water relatively quickly, but that the produced CO 2 contains significant water for long periods of time. The amount of water in the CO 2 could have implications for reactivity with reservoir rocks and engineered materials.

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Experimental evaluation of interactions in supercritical CO2/water/rock minerals system under geologic CO2 sequestration conditions

Cited by 131 publications

References 13 publications

Reservoir Condition Pore-scale Imaging of Multiple Fluid Phases Using X-ray Microtomography

Reservoir Condition Pore-scale Imaging of Multiple Fluid Phases Using X-ray Microtomography

Fundamental study of CO2-H2O-mineral interactions for carbon sequestration, with emphasis on the nature of the supercritical fluid-mineral interface.

A Phase-Partitioning Model for CO2–Brine Mixtures at Elevated Temperatures and Pressures: Application to CO2-Enhanced Geothermal Systems

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