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Register a new userDirect observation of coupled geochemical and geomechanical impacts on chalk microstructural evolution under elevated CO2 pressure. Part I
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Y. Yang
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The dissolution of porous media in a geologic formation induced by the injection of massive amounts of CO2 can undermine the mechanical stability of the formation structure before carbon mineralization takes place. The geomechanical impact of geologic carbon storage is therefore closely related to the structural sustainability of the chosen reservoir as well as the probability of buoyancy driven CO2 leakage through caprocks. Here we show, with a combination of ex situ nanotomography and in situ microtomography, that the presence of dissolved CO2 in water produces a homogeneous dissolution pattern in natural chalk microstructure. This pattern stems from a greater apparent solubility of chalk and therefore a greater reactive subvolume in a sample. When a porous medium dissolves homogeneously in an imposed flow field, three geomechanical effects were observed: material compaction, fracturing and grain relocation. These phenomena demonstrated distinct feedbacks to the migration of the dissolution front and severely complicated the infiltration instability problem. We conclude that the presence of dissolved CO2 makes the dissolution front less susceptible to spatial and temporal perturbations in the strongly coupled geochemical and geomechanical processes.
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When reactive fluids flow through a dissolving porous medium, conductive channels form, leading to fluid breakthrough. This phenomenon is important in geologic carbon storage, where the dissolution of CO2 in water increases the acidity and produce microstructures significantly different from those in an intact reservoir. We demonstrate the controlling mechanism for the dissolution patterns in natural porous materials. This was done using numerical simulations based on high resolution digital models of North Sea chalk. We tested three model scenarios, and found that aqueous CO2 dissolve porous media homogeneously, leading to large breakthrough porosity. In contrast, CO2-free solution develops elongated convective channels in porous media, known as wormholes, and resulting in small breakthrough porosity. We further show that a homogeneous dissolution pattern appears because the sample size is smaller than the theoretical size of a developing wormhole. The result indicates that the presence of dissolved CO2 expands the reactive subvolume of a porous medium, and thus enhances the geochemical alteration of reservoir structures and might undermine the sealing integrity of caprocks when minerals dissolve.
The formation of solid calcium carbonate (CaCO3) from aqueous solutions or slurries containing calcium and carbon dioxide (CO2) is a complex process of considerable importance in the ecological, geochemical and biological areas. Moreover, the demand for powdered CaCO3 has increased considerably recently in various fields of industry. The aim of this study was therefore to synthesize fine particles of calcite with controlled morphology by hydrothermal carbonation of calcium hydroxide at high CO2 pressure (initial PCO2=55 bar) and at moderate and high temperature (30 and 90 degrees C). The morphology of precipitated particles was identified by transmission electron microscopy (TEM/EDS) and scanning electron microscopy (SEM/EDS). In addition, an X-ray diffraction analysis was performed to investigate the carbonation efficiency and purity of the solid product. Carbonation of dispersed calcium hydroxide in the presence of supercritical (PT=90 bar, T=90 degrees C) or gaseous (PT=55 bar, T=30 degrees C) CO2 led to the precipitation of sub-micrometric isolated particles (<1$mu$m) and micrometric agglomerates (<5$mu$m) of calcite. For this study, the carbonation efficiency (Ca(OH)2-CaCO3 conversion) was not significantly affected by PT conditions after 24 h of reaction. In contrast, the initial rate of calcium carbonate precipitation increased from 4.3 mol/h in the 90bar-90 degrees C system to 15.9 mol/h in the 55bar-30 degrees C system. The use of high CO2 pressure may therefore be desirable for increasing the production rate of CaCO3, carbonation efficiency and purity, to approximately 48 kg/m3h, 95% and 96.3%, respectively in this study. The dissipated heat for this exothermic reaction was estimated by calorimetry to be -32 kJ/mol in the 90bar-90 degrees C system and -42 kJ/mol in the 55bar-30 degrees C system.
Stalagmites are an extraordinarily powerful resource for the reconstruction of climatological palaeoseasonality. Here, we provide a comprehensive review of different types of seasonality preserved by stalagmites and methods for extracting this information. A new drip classification scheme is introduced, which facilitates the identification of stalagmites fed by seasonally responsive drips and which highlights the wide variability in drip types feeding stalagmites. This hydrological variability, combined with seasonality in Earth atmospheric processes, meteoric precipitation, biological processes within the soil, and cave atmosphere composition means that every stalagmite retains a different and distinct (but correct) record of environmental conditions. Replication of a record is extremely useful but should not be expected unless comparing stalagmites affected by the same processes in the same proportion. A short overview of common microanalytical techniques is presented, and suggested best practice discussed. In addition to geochemical methods, a new modelling technique for extracting meteoric precipitation and temperature palaeoseasonality from stalagmite d18O data is discussed and tested with both synthetic and real-world datasets. Finally, world maps of temperature, meteoric precipitation amount, and meteoric precipitation oxygen isotope ratio seasonality are presented and discussed, with an aim of helping to identify regions most sensitive to shifts in seasonality.
The crystal structure of CO2 filled pure SiO2 LTA zeolite has been studied at high pressures and temperatures using synchrotron based x ray powder diffraction. Its structure consists of 13 CO2 guest molecules, 12 of them accommodated in the large alpha cages and 1 in the beta cages, giving a SiO2:CO2 stoichiometric ratio smaller than 2. The structure remains stable under pressure up to 20 GPa with a slight pressure dependent rhombohedral distortion, indicating that pressure induced amorphization is prevented by the insertion of guest species in this open framework. The ambient-temperature lattice compressibility has been determined. In situ high pressure resistive heating experiments up to 750 K allow us to estimate the thermal expansivity at 5 GPa. Our data confirm that the insertion of CO2 reverses the negative thermal expansion of the empty zeolite structure. No evidence of any chemical reaction was observed. The possibility of synthesizing a silicon carbonate at high temperatures and higher pressures is discussed in terms of the evolution of C-O and Si-O distances between molecular and framework atoms.
The Mantanza-Riachuelo basin recovery is one of the most ambitious environmental projects under construction in Argentina. In this context, the sanitary bureau of the metropolitan area of Buenos Aires (AySA) is building a sewage collection network to transport the waste water of the population in the southern area of the city, composed by almost five million people. The most complex tunnel in this big project is named textit{Lot 3}, an outfall EPB-TBM tunnel starting at a shaft located at the textit{Rio de la Plata} margin and running under the river 12 km to a discharge area. The tunnel runs through soft clay belonging to the textit{post-pampeano} formation and dense sands of the textit{Puelchese} formation. In operation, it will be pressurized by a pumping station which will produce a piezometer head that, in the first 2000 m, might be eventually higher than the confining pressure around the tunnel. This paper presents the numerical analysis of the structural forces acting on the tunnel rings using a risk-oriented approach that considers the stochastic nature of materials, stratigraphy and tunnel-ground interaction. The compression of the lining is evaluated and compared with field measurements in order to predict the structural forces and the risk of the rings going into tension beyond the structural capacity of the system.
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