No Arabic abstract
When carbon dioxide (CO2) is injected into an aquifer or a depleted geological reservoir, its dissolution into solution results in acidification of the pore waters. As a consequence, the pore waters become more reactive, which leads to enhanced dissolution-precipitation processes and a modification of the mechanical and hydrological properties of the rock. This effect is especially important for limestones given that the solubility and reactivity of carbonates is strongly dependent on pH and the partial pressure of CO2. The main mechanism that couples dissolution, precipitation and rock matrix deformation is commonly referred to as intergranular pressure solution creep (IPS) or pervasive pressure solution creep (PSC). This process involves dissolution at intergranular grain contacts subject to elevated stress, diffusion of dissolved material in an intergranular fluid, and precipitation in pore spaces subject to lower stress. This leads to an overall and pervasive reduction in porosity due to both grain indentation and precipitation in pore spaces. The percolation of CO2-rich fluids may influence on-going compaction due to pressure solution and can therefore potentially affect the reservoir and its long-term CO2 storage capacity. We aim at quantifying this effect by using a 2D numerical model to study the coupling between dissolution-precipitation processes, local mass transfer, and deformation of the rock over long time scales. We show that high partial pressures of dissolved CO2 (up to 30 MPa) significantly increase the rates of compaction by a factor of ~ 50 to ~ 75, and also result in a concomitant decrease in the viscosity of the rock matrix.
Pressure solution creep rates and interface structures have been measured by two methods on calcite single crystals. In the first kind of experiments, calcite monocrystals were indented at 40 degrees C for six weeks using ceramic indenters under stresses in the 50-200 MPa range in a saturated solution of calcite and in a calcite-saturated aqueous solution of NH4Cl. The deformation (depth of the hole below the indenter) is measured ex-situ at the end of the experiment. In the second type of experiment, calcite monocrystals were indented by spherical glass indenters for 200 hours under stresses in the 0-100 MPa range at room temperature in a saturated aqueous solution of calcite. The displacement of the indenter was continuously recorded using a specially constructed differential dilatometer. The experiments conducted in a calcite-saturated aqueous solution of NH4Cl show an enhanced indentation rate owing to the fairly high solubility of calcite in this solution. In contrast, the experiments conducted in a calcite-saturated aqueous solution show moderate indentation rate and the dry control experiments did not show any measurable deformation. The rate of calcite indentation is found to be inversely proportional to the indenter diameter, thus indicating that the process is diffusion-controlled. The microcracks in the dissolution region under the indenter dramatically enhance the rate of calcite indentation by a significant reduction of the distance of solute transport in the trapped fluid phase. This result indicates that care should be taken in extrapolating the kinetic data of pressure solution creep from one mineral to another.
Time-lapse seismic monitoring of carbon storage and sequestration is often challenging because the time-lapse signature of the growth of CO2 plumes is weak in amplitude and therefore difficult to detect seismically. This situation is compounded by the fact that the surveys are often coarsely sampled and not replicated to reduce costs. As a result, images obtained for different vintages (baseline and monitor surveys) often contain artifacts that may be attributed wrongly to time-lapse changes. To address these issues, we propose to invert the baseline and monitor surveys jointly. By using the joint recovery model, we exploit information shared between multiple time-lapse surveys. Contrary to other time-lapse methods, our approach does not rely on replicating the surveys to detect time-lapse changes. To illustrate this advantage, we present a numerical sensitivity study where CO2 is injected in a realistic synthetic model. This model is representative of the geology in the southeast of the North Sea, an area currently considered for carbon sequestration. Our example demonstrates that the joint recovery model improves the quality of time-lapse images allowing us to monitor the CO2 plume seismically.
Recent advances in the high sensitivity spectroscopy have made it possible, in combination with accurate theoretical predictions, to observe for the first time very weak electric quadrupole transitions in a polar polyatomic molecule of water. Here we present accurate theoretical predictions of the complete quadrupole ro-vibrational spectrum of a non-polar molecule CO$_2$, important in atmospheric and astrophysical applications. Our predictions are validated by recent cavity enhanced absorption spectroscopy measurements and are used to assign few weak features in the recent ExoMars ACS MIR spectroscopic observations of the martian atmosphere. Predicted quadrupole transitions appear in some of the mid-infrared CO$_2$ and water vapor transparency regions, making them important for detection and characterization of the minor absorbers in water- and CO$_2$-rich environments, such as present in the atmospheres of Earth, Venus and Mars.
We experimentally investigate laser-induced dissociative recombination of CO$_2$ in linearly polarized strong laser fields with coincidence measurements. Our results show laser-induced dissociation processes originate from an electron recombination process after laser-induced double ionization. After double ionization of CO$_2$, one electron is recaptured by the CO$_2^{2+}$ and localized to O$^+$ or CO$^+$ in the following dissociation process. We found that the probability of electron localization to O$^{+}$ is much higher than that to CO$^+$. Further, our measurements reveal that the recombination probability of the first ionized electron is three times as high as that of the second ionized electron. Our work may trigger further experimental and theoretical studies on involved nuclear and electron dynamics in laser-induced dissociative recombination of molecules and their applications in controlling molecular dissociation with ultrashort laser pulses.
Global Climate Models (GCMs) provide forecasts of future climate warming using a wide variety of highly sophisticated anthropogenic CO2 emissions models as input, each based on the evolution of four emissions drivers: population p, standard of living g, energy productivity (or efficiency) f and energy carbonization c. The range of scenarios considered is extremely broad, however, and this is a primary source of forecast uncertainty. Here, it is shown both theoretically and observationally how the evolution of the human system can be considered from a surprisingly simple thermodynamic perspective in which it is unnecessary to explicitly model two of the emissions drivers: population and standard of living. Specifically, the human system grows through a self-perpetuating feedback loop in which the consumption rate of primary energy resources stays tied to the historical accumulation of global economic production - or p times g - through a time-independent factor of 9.7 +/- 0.3 milliwatts per inflation-adjusted 1990 US dollar. This important constraint, and the fact that f and c have historically varied rather slowly, points towards substantially narrowed visions of future emissions scenarios for implementation in GCMs.