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1.
This paper evaluates the expected environmental impact of several promising schemes for ocean carbon sequestration by direct injection of CO2, and serves as a major update to the assessment by Auerbach et al. (1997) and Caulfield et al. (1997) of water quality impacts and the induced mortality to zooplankton. Three discharge approaches are considered, each designed to maximize dilution over the water column: a point release of negatively buoyant CO2 hydrate particles from a moving ship; a stationary point release of CO2 hydrate particles forming a sinking plume; and a long, bottom-mounted diffuser discharging buoyant liquid CO2 droplets. Two of these scenarios take advantage of the enhanced dilution offered by CO2 hydrate particles, and are based on recent laboratory and field studies on the formation and behavior of such particles. Overall, results suggest that it is possible with present or near present technology to engineer discharge configurations that achieve sufficient dilution to largely avoid acute impacts. In particular, the moving ship hydrate discharge is identified as the most promising due to its operational flexibility. In addition to lethal effects, sub-lethal and ecosystem effects are discussed qualitatively, though not analyzed quantitatively. Our main conclusion is that ocean carbon sequestration by direct injection should not be dismissed as a climate change mitigation strategy on the basis of environmental impact alone. Rather, it can be considered as a viable option for further study, especially in regions where geologic sequestration proves impractical.  相似文献   

2.
A new apparatus employing a modular, mechanically agitated gas-inducing crystallizer is used to demonstrate the capture of CO2 via hydrate crystallization. The crystallizer enhances the contact of hydrate forming gases with water and thus the rate of hydrate crystallization increases. Flue gas (CO2/N2) and fuel gas (CO2/H2) mixtures were used to represent post- and precombustion capture. A comparison between the rates of hydrate formation in different crystallizers is presented by defining a metric called the normalized rate of hydrate formation. The gas uptake and the separation efficiency for the fuel and flue gas mixtures were found to be greater compared to the results obtained in a smaller scale stirred tank reactor (Kumar et al., 2009c, Linga et al., 2008). The gas uptake and CO2 recovery for flue gas mixture in the presence of THF obtained in this work was higher than that reported in the literature with tetra-n-butyl ammonium bromide and tetra-n-butyl ammonium fluoride (Fan et al., 2009, Li et al., 2009). Although hydrate crystallization is able to capture CO2, the power required for mechanical agitation was found to be very significant. If the hydrate process is to be used industrially then hydrate crystallization must be carried out without mechanical agitation.  相似文献   

3.
A numerical study was conducted to predict pCO2 change in the ocean on a continental shelf by the leakage of CO2, which is originally stored in the aquifer under the seabed, in the case that a large fault connects the CO2 reservoir and the seabed by an earthquake or other diastrophism. The leakage rate was set to be 6.025 × 10−4 kg/m2/sec from 2 m × 100 m fault band, which corresponds to 3800 t-CO2/year, referring to the monitored seepage rate from an existing EOR field. The target space in this study was limited to the ocean above the seabed, the depth of which was 200 or 500 m. The computational domain was idealistically rectangular with the seabed fault-band perpendicular to the uniform flow. The CO2 takes a form of bubbles or droplets, depending on the depth of water, and their behaviour and dissolution were numerically simulated during their rise in seawater flow. The advection–diffusion of dissolved CO2 was also simulated. As a result, it was suggested that the leaked CO2 droplets/bubbles all dissolve in the seawater before spouting up to the atmosphere, and that the increase in pCO2 in the seawater was smaller than 500 μ atm.  相似文献   

4.
Ultrasonic experiments were undertaken on CO2 flooded sandstone core samples, both synthetic sandstones and core plugs from the CRC1 CO2 injection well in the Otway Basin, Victoria, South Eastern. Australia. The aim of these laboratory tests was to investigate the effects of CO2 as a pore fluid on the seismo-acoustic response of the sandstone and ultimately to provide an indication of the sensitivity of time-lapse seismic imaging of the eventual CO2/CH4 plume in the Otway, Waarre C formation.The synthetic sandstones were manufactured using both a proprietary calcium in situ precipitation (CIPS) process and a silica cementing technique. Samples were tested in a computer controlled triaxial pressure cell where pore pressures can be controlled independently of the confining pressures. The pressure cell is equipped with ultrasonic transducers housed in the loading platens. Consequently, effective pressures equivalent to those expected in the reservoir can be applied while ultrasonic testing is undertaken. Both compressional, P and shear waves, S were recorded via a digital oscilloscope at a range of effective pressure steps. Pore pressures were varied from 4 MPa to 17 MPa to represent both the gaseous and liquid phase regions of the CO2 phase diagram. Similar experiments were conducted on core plugs from the Waarre C reservoir horizon obtained from the CRC1 injection well, but with an intervening brine-saturated step and in some cases with a CO2/CH4 mix of 80%/20% molar fraction which is representative of the field situation. However, the pore pressure in these experiments was held at 4 MPa. Finally, acoustic impedances and reflection coefficients were calculated for the reservoir using Gassmann theory and the implications for imaging the CO2 plume is discussed.  相似文献   

5.
Carbon dioxide sequestration in deep saline aquifers is a means of reducing anthropogenic atmospheric emissions of CO2. Among various mechanisms, CO2 can be trapped in saline aquifers by dissolution in the formation water. Vaporization of water occurs along with the dissolution of CO2. Vaporization can cause salt precipitation, which reduces porosity and impairs permeability of the reservoir in the vicinity of the wellbore, and can lead to reduction in injectivity. The amount of salt precipitation and the region in which it occurs may be important in CO2 storage operations if salt precipitation significantly reduces injectivity. Here we develop an analytical model, as a simple and efficient tool to predict the amount of salt precipitation over time and space. This model is particularly useful at high injection velocities, when viscous forces dominate.First, we develop a model which treats the vaporization of water and dissolution of CO2 in radial geometry. Next, the model is used to predict salt precipitation. The combined model is then extended to evaluate the effect of salt precipitation on permeability in terms of a time-dependent skin factor. Finally, the analytical model is corroborated by application to a specific problem with an available numerical solution, where a close agreement between the solutions is observed. We use the results to examine the effect of assumptions and approximations made in the development of the analytical solution. For cases studied, salt saturation was a few percent. The loss in injectivity depends on the degree of reduction of formation permeability with increased salt saturation. For permeability-reduction models considered in this work, the loss in injectivity was not severe. However, one limitation of the model is that it neglects capillary and gravity forces, and these forces might increase salt precipitation at the bottom of formation particularly when injection rate is low.  相似文献   

6.
In the carbon capture and storage (CCS) chain, transport and storage set different requirements for the composition of the gas stream mainly containing carbon dioxide (CO2). Currently, there is a lack of standards to define the required quality for CO2 pipelines. This study investigates and recommends likely maximum allowable concentrations of impurities in the CO2 for safe transportation in pipelines. The focus is on CO2 streams from pre-combustion processes. Among the issues addressed are safety and toxicity limits, compression work, hydrate formation, corrosion and free water formation, including the cross-effect of H2S and H2O and of H2O and CH4.  相似文献   

7.
Large-scale storage of carbon dioxide in saline aquifers may cause considerable pressure perturbation and brine migration in deep rock formations, which may have a significant influence on the regional groundwater system. With the help of parallel computing techniques, we conducted a comprehensive, large-scale numerical simulation of CO2 geologic storage that predicts not only CO2 migration, but also its impact on regional groundwater flow. As a case study, a hypothetical industrial-scale CO2 injection in Tokyo Bay, which is surrounded by the most heavily industrialized area in Japan, was considered, and the impact of CO2 injection on near-surface aquifers was investigated, assuming relatively high seal-layer permeability (higher than 10 microdarcy). A regional hydrogeological model with an area of about 60 km × 70 km around Tokyo Bay was discretized into about 10 million gridblocks. To solve the high-resolution model efficiently, we used a parallelized multiphase flow simulator TOUGH2-MP/ECO2N on a world-class high performance supercomputer in Japan, the Earth Simulator. In this simulation, CO2 was injected into a storage aquifer at about 1 km depth under Tokyo Bay from 10 wells, at a total rate of 10 million tons/year for 100 years. Through the model, we can examine regional groundwater pressure buildup and groundwater migration to the land surface. The results suggest that even if containment of CO2 plume is ensured, pressure buildup on the order of a few bars can occur in the shallow confined aquifers over extensive regions, including urban inlands.  相似文献   

8.
Co-injection of sulfur dioxide during geologic carbon sequestration can cause enhanced brine acidification. The magnitude and timescale of this acidification will depend, in part, on the reactions that control acid production and on the extent and rate of SO2 dissolution from the injected CO2 phase. Here, brine pH changes were predicted for three possible SO2 reactions: hydrolysis, oxidation, or disproportionation. Also, three different model scenarios were considered, including models that account for diffusion-limited release of SO2 from the CO2 phase. In order to predict the most extreme acidification potential, mineral buffering reactions were not modeled. Predictions were compared to the case of CO2 alone which would cause a brine pH of 4.6 under typical pressure, temperature, and alkalinity conditions in an injection formation. In the unrealistic model scenario of SO2 phase equilibrium between the CO2 and brine phases, co-injection of 1% SO2 is predicted to lead to a pH close to 1 with SO2 oxidation or disproportionation, and close to 2 with SO2 hydrolysis. For a scenario in which SO2 dissolution is diffusion-limited and SO2 is uniformly distributed in a slowly advecting brine phase, SO2 oxidation would lead to pH values near 2.5 but not until almost 400 years after injection. In this scenario, SO2 hydrolysis would lead to pH values only slightly less than those due to CO2 alone. When SO2 transport is limited by diffusion in both phases, enhanced brine acidification occurs in a zone extending only 5 m proximal to the CO2 plume, and the effect is even less if the only possible reaction is SO2 hydrolysis. In conclusion, the extent to which co-injected SO2 can impact brine acidity is limited by diffusion-limited dissolution from the CO2 phase, and may also be limited by the availability of oxidants to produce sulfuric acid.  相似文献   

9.
In this paper we describe the thermodynamic and kinetic basis for mineral storage of carbon dioxide in basaltic rock, and how this storage can be optimized. Mineral storage is facilitated by the dissolution of CO2 into the aqueous phase. The amount of water required for this dissolution decreases with decreased temperature, decreased salinity, and increased pressure. Experimental and field evidence suggest that the factor limiting the rate of mineral fixation of carbon in silicate rocks is the release rate of divalent cations from silicate minerals and glasses. Ultramafic rocks and basalts, in glassy state, are the most promising rock types for the mineral sequestration of CO2 because of their relatively fast dissolution rate, high concentration of divalent cations, and abundance at the Earth's surface. Admixture of flue gases, such as SO2 and HF, will enhance the dissolution rates of silicate minerals and glasses. Elevated temperature increases dissolution rates but porosity of reactive rock formations decreases rapidly with increasing temperature. Reduced conditions enhance mineral carbonation as reduced iron can precipitate in carbonate minerals. Elevated CO2 partial pressure increases the relative amount of carbonate minerals over other secondary minerals formed. The feasibility to fix CO2 by carbonation in basaltic rocks will be tested in the CarbFix project by: (1) injection of CO2 charged waters into basaltic rocks in SW Iceland, (2) laboratory experiments, (3) studies of natural analogues, and (4) geochemical modelling.  相似文献   

10.
Large-scale injections of CO2 into subsurface saline aquifers have been proposed to remediate climate change related to buildup of green house gases in the atmosphere. The pressure buildup caused by such injections may impact a volume of the basin significantly larger than the CO2 plume itself. In areas with hydrological settings similar to the Gulf Coast Basin, the perturbation of the flow-field in deep parts of the basin could result in brines or brackish water being pushed up-dip into unconfined sections of the same formations or into the capture zone of fresh-water wells. The premise of the current study is that the details of multiple-phase flow processes necessary to model the near field evolution of the CO2 plume are not necessary to describe the impact of the pressure anomaly on up-dip aquifers. This paper quantitatively explores conditions under which shallow groundwater would be impacted by up-dip displacement of brines, utilizing an existing carefully calibrated flow model. Modeling an injection of water, arguably equivalent to 50 million tons of CO2/year for 50 years resulted in an average water-table rise of 1 m, with minor increase in stream baseflow and larger increase in ground water evapotranspiration, but no significant change in salinity.  相似文献   

11.
Stable carbon isotopes are important tools to assess potential storage sites for CO2, as they allow the quantification of ionic trapping via isotope mass balances. In deep geological formations high p/T conditions need to be considered, because CO2 dissolution, equilibrium constants and isotope fractionation of dissolved inorganic carbon (DIC) depend on temperature, pressure and solute composition. After reviewing different approaches to account for these dependencies, an expanded scheme is presented for speciation and carbon isotope fractionation of DIC and dissolution of CaCO3 for pCO2 up to 100 bar, pH down to 3 and temperatures of up to 200 °C. The scheme evaluates the influence of respective parameters on isotope ratios during CO2 sequestration. The pCO2 and pH are the dominant controlling factors in the DIC/δ13C/pH system. The fugacity of CO2 has major impact on DIC concentrations at temperatures below 100 °C at high pCO2. Temperature dependency of activities and equilibrium dominates at temperatures above 100 °C. Isotope ratios of DIC are expected to be about 1–2‰ more depleted in 13C compared to the free CO2 at pCO2 values above 10 bar. This depletion is controlled by carbon isotope fractionation between CO2 and H2CO3* which is the dominant species of DIC at the resulting pH below 5.  相似文献   

12.
Carbon dioxide (CO2) injection into saline aquifers is one of the promising options to sequester large amounts of CO2 in geological formations. During as well as after injection of CO2 into an aquifer, CO2 migrates towards the top of the formation due to density differences between the formation brine and the injected CO2. The time scales of CO2 migration towards the top of an aquifer and the fraction of CO2 that is trapped as residual gas depends strongly on the driving forces that are acting on the injected CO2.When CO2 migrates to the top of an aquifer, brine may be displaced downwards in a counter-current flow setting particularly during the injection period. A majority of the published work on counter-current flow settings have reported significant reductions in the associated relative permeability functions as compared to co-current measurements. However, this phenomenon has not yet been considered in the simulation of CO2 storage into saline aquifers.In this paper we study the impact of changes in mobility for the two-phase brine/CO2 system as a result of transitions between co- and counter-current flow settings. We have included this effect in a simulator and studied the impact of the related mobility reduction on the saturation distribution and residual saturation of CO2 in aquifers over relevant time scales. We demonstrate that the reduction in relative permeability in the vertical direction changes the plume migration pattern and has an impact on the amount of gas that is trapped as a function of time. This is to our best knowledge the first attempt to integrate counter-current relative permeability into the simulation of injection and subsequent migration of CO2 in aquifers. The results and analysis presented in this paper are directly relevant to all ongoing activities related to the design of large-scale CO2 storage in saline aquifers.  相似文献   

13.
This work is motivated by the growing interest in injecting carbon dioxide into deep geological formations as a means of avoiding its atmospheric emissions and consequent global warming. Ideally, the injected greenhouse gas stays in the injection zone for a geologic time, eventually dissolves in the formation brine and remains trapped by mineralization. However, one of the potential problems associated with the geologic method of sequestration is that naturally present or inadvertently created conduits in the cap rock may result in a gas leakage from primary storage. Even in supercritical state, the carbon dioxide viscosity and density are lower than those of the formation brine. Buoyancy tends to drive the leaked CO2plume upward. Theoretical and experimental studies of buoyancy-driven supercritical CO2 flow, including estimation of time scales associated with plume evolution and migration, are critical for developing technology, monitoring policy, and regulations for safe carbon dioxide geologic sequestration.In this study, we obtain simple estimates of vertical plume propagation velocity taking into account the density and viscosity contrast between CO2 and brine. We describe buoyancy-driven countercurrent flow of two immiscible phases by a Buckley–Leverett type model. The model predicts that a plume of supercritical carbon dioxide in a homogeneous water-saturated porous medium does not migrate upward like a bubble in bulk water. Rather, it spreads upward until it reaches a seal or until it becomes immobile. A simple formula requiring no complex numerical calculations describes the velocity of plume propagation. This solution is a simplification of a more comprehensive theory of countercurrent plume migration [Silin, D., Patzek, T.W., Benson, S.M., 2007. A Model of Buoyancy-driven Two-phase Countercurrent Fluid Flow. Laboratory Report LBNL-62607. Lawrence Berkeley National Laboratory, Berkeley, CA]. In a layered reservoir, the simplified solution predicts a slower plume front propagation relative to a homogeneous formation with the same harmonic mean permeability. In contrast, the model yields much higher plume propagation estimates in a high-permeability conduit like a vertical fracture.  相似文献   

14.
There is a strong political will to decrease CO2 emissions. Although the steel industry only accounts for some 5% of worldwide CO2 emissions (which totalled 1,200 million tonnes per annum in the late 1990s), it will be strongly affected by this. The EU, for example, is putting up strong economic incentives for reductions. This is taking place at a time when demand for steel products is greater than ever. To radically change existing processes and production routes to decrease the CO2 emissions would be extremely expensive, even if it were possible. Nevertheless, many of the solutions which have been discussed seem to go in this direction. The other alternative discussed seems to be the creation of process solutions and alterations that lead to a focusing of CO2 streams, i.e., much higher CO2 concentrations in flue gases than today, for entrapment of the CO2 so that it is not discharged into the atmosphere. These solutions are feasible, but expensive.

However, there exists today a number of solutions and technologies which, if fully implemented, could substantially decrease CO2 emissions without seriously altering current methods of operation; they are short-term viable solutions. The present paper reviews and discusses such technologies, throughout the steel production paths. If these solutions are fully implemented, the combined impact on CO2 emissions from the steel industry worldwide is estimated to be a reduction of 100–150 million tonnes of CO2 per annum, i.e., current emissions can be reduced by some 8–10% within a relatively short time span.  相似文献   

15.
Injection and movement/saturation of carbon dioxide (CO2) in a geological formation will cause changes in seismic velocities. We investigate the capability of coda-wave interferometry technique for estimating CO2-induced seismic velocity changes using time-lapse synthetic vertical seismic profiling (VSP) data and the field VSP datasets acquired for monitoring injected CO2 in a brine aquifer in Texas, USA. Synthetic VSP data are calculated using a finite-difference elastic-wave equation scheme and a layered model based on the elastic Marmousi model. A possible leakage scenario is simulated by introducing seismic velocity changes in a layer above the CO2 injection layer. We find that the leakage can be detected by the detection of a difference in seismograms recorded after the injection compared to those recorded before the injection at an earlier time in the seismogram than would be expected if there was no leakage. The absolute values of estimated mean velocity changes, from both synthetic and field VSP data, increase significantly for receiver positions approaching the top of a CO2 reservoir. Our results from field data suggest that the velocity changes caused by CO2 injection could be more than 10% and are consistent with results from a crosswell tomogram study. This study demonstrates that time-lapse VSP with coda-wave interferometry analysis can reliably and effectively monitor geological carbon sequestration.  相似文献   

16.
Climate change is being caused by greenhouse gases such as carbon dioxide (CO2). Carbon capture and storage (CCS) is of interest to the scientific community as one way of achieving significant global reductions of atmospheric CO2 emissions in the medium term. CO2 would be captured from large stationary sources such as power plants and transported via pipelines under high pressure conditions to underground storage. If a downward leakage from a surface transportation system module occurs, the CO2 would undergo a large temperature reduction and form a bank of “dry ice” on the ground surface; the sublimation of the gas from this bank represents an area source term for subsequent atmospheric dispersion, with an emission rate dependent on the energy balance at the bank surface. Gaseous CO2 is denser than air and tends to remain close to the surface; it is an asphyxiant, a cerebral vasodilator and at high concentrations causes rapid circulatory insufficiency leading to coma and death. Hence a subliming bank of dry ice represents safety hazard. A model is presented for evaluating the energy balance and sublimation rate at the surface of a solid frozen CO2 bank under different environmental conditions. The results suggest that subliming gas behaves as a proper dense gas (i.e. it remains close to the ground surface) only for low ambient wind speeds.  相似文献   

17.
Public concern over the possibility of migration of stored CO2 to the surface with resulting damage to vegetation or hazard to humans and animals is a matter which will need to be addressed to be able to satisfy likely regulatory requirements for onshore CO2 storage in a number of jurisdictions. While soil CO2 concentration is readily measured continuously and in situ with current technology, the measurement of CO2 flux at depths below the soil A horizon may be a more sensitive and meaningful technique for early detection of a near surface CO2 plume. We describe a system for the continuous measurement of soil CO2 flux at a depth of approximately 1.3 m and present results from three instruments deployed at the Otway Basin Pilot Project in Victoria, Australia and one development system deployed at Sutton, near the Australian Capital Canberra.  相似文献   

18.
Reservoirs of clathrate hydrates of natural gases (hydrates), found worldwide and containing huge amounts of bound natural gases (mostly methane), represent potentially vast and yet untapped energy resources. Since CO2-containing hydrates are considerably more stable thermodynamically than methane hydrates, if we find a way to replace the original hydrate-bound hydrocarbons by the CO2, two goals can be accomplished at the same time: safe storage of carbon dioxide in hydrate reservoirs, and in situ release of hydrocarbon gas. We have applied the techniques of Magnetic Resonance Imaging (MRI) as a tool to visualize the conversion of CH4 hydrate within Bentheim sandstone matrix into the CO2 hydrate. Corresponding model systems have been simulated using the Phase Field Theory approach. Our theoretical studies indicate that the kinetic behaviour of the systems closely resembles that of CO2 transport through an aqueous solution. We have interpreted this to mean that the hydrate and the matrix mineral surfaces are separated by liquid-containing channels. These channels will serve as escape routes for released natural gas, as well as distribution channels for injected CO2.  相似文献   

19.
A column of silica gel was employed to contact water with flue gas (CO2/N2) mixture to assess if CO2 can be separated by hydrate crystallization. Three different silica gels were used. One with a pore size of 30 nm (particle size 40–75 μm) and two with a pore size of 100 nm and particle sizes of 40–75 and 75–200 μm respectively. The observed trends indicate that larger pores and particle size increase the gas consumption, CO2 recovery, separation factor and water conversion to hydrate. Thus, the gel (gel #3) with the larger particle size and larger pore size was chosen to carry out experiments with concentrated CO2 mixtures and for experiments in the presence of tetrahydrofuran (THF), which itself is a hydrate forming substance. Addition of THF reduces the operating pressure in the crystallizer but it also reduces the gas uptake. Gel #3 was also used in experiments with a fuel gas (CO2/H2) mixture in order to recover CO2 and H2. It was found that the gel column performs as well as a stirred reactor in separating the gas components from both flue gas and fuel gas mixtures. However, the crystallization rate and hydrate yield are considerably enhanced in the former. Finally the need for stirring is eliminated with the gel column which is enormously beneficial economically.  相似文献   

20.
In order to evaluate the risk of hydrate formation in CO2 transport one has to be able to predict the water content in the fluid phase in equilibrium with the CO2-hydrate. A literature review has identified some knowledge gaps, for example, there are no results available at temperatures lower than 243.15 K (?30 °C); and none of the models found in literature predicts the water content with high accuracy. A model based on equality of water fugacity in fluid and hydrate phase is presented here and used for the predictions of water content in equilibrium with hydrates. Although this model gives better accuracy in the overall temperature and pressure ranges of measurements than the models found in the literature, it is not accurate enough to satisfy the requirements of CO2 transport. The simulation results also show that it is possible to form hydrate at low water content, such as xw = 50 vppm, if temperature is low enough. In order to verify the results and improve the model accuracy further, more experimental data in a larger temperature and pressure region are required.  相似文献   

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