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1.
Chemical tracers have been used in various C capture and storage (CCS) projects worldwide primarily to provide information regarding subsurface migration of CO2 and to verify CO2 containment. Understanding the movement and interactions of CO2 in the subsurface is a challenging task considering the variety of states in which it exists (i.e. gas, liquid, supercritical, dissolved in water) and the range of possible storage mechanisms (i.e. residual or capillary trapping, dissolved in water, structural trapping or incorporation into minerals). This paper critically reviews several chemical tracer applications and case studies for CCS projects. In many instances, there are parallels (e.g. tracer classes and applications) between tracers in the oil and gas industry and in CCS. It has been shown that chemical tracers can complement geophysical measurements (e.g. seismic) in understanding the formation behaviour of CO2. Although tracers have been successfully used in many CCS projects, some fundamental information, for example partitioning and adsorption, about the behaviour of tracers is still lacking and this can be an issue when interpreting tracer data (e.g. determining leakage rates). In this paper the deployment and recovery of chemical tracers and their use on various CCS projects are described.  相似文献   

2.
Perfluorocarbon compounds (PFCs) have high chemical and thermal stability, low background levels in natural systems, and easy detectability. They are proposed as tracers for monitoring potential CO2 leakage associated with geological carbon sequestration (GCS). The fate of the PFCs in porous media, and in particular, the transport of these compounds relative to CO2 gas in geological formations, has not been thoroughly studied. We conducted column tests to study the transport of perfluoro-methylcyclo-pentane (PMCP), perfluoro-methylcyclo-hexane (PMCH), ortho-perfluoro-dimethylcyclo-hexane (ortho-PDCH), and perfluoro-trimethylcyclo-hexane (PTCH) gas tracers in a variety of porous media. The influence of water content and sediment minerals on the retardation of the tracers was tested. The transport of PFC tracers relative to 13CO2 and the conservative tracer sulfur hexafluoride (SF6) was also investigated. Results show that at high water content, the PFCs and SF6 transported together. In dry and low-water-content sediments, however, the PFCs were retarded relative to SF6 with the degree of retardation increasing with the molecular weight of the PFC. When water was present in the medium, the transport of CO2 was greatly retarded compared to SF6 and the PFC tracers. However, in dry laboratory sediments, the migration of CO2 was slightly faster than all the tracers. The type of minerals in the sediments also had a significant impact on the fate of the tracers. In order to use the PFC tracer data obtained from the ground surface or shallow subsurface in a GCS site to precisely interpret the extent and magnitude of CO2 leakage, the retardation of the tracers and the interaction of CO2 with the reservoir overlying formation water should be carefully quantified.  相似文献   

3.
A controlled release of CO2 was conducted at a field site in Bozeman, Montana, USA in July of 2008 in a multi-laboratory study of near surface transport and detection technologies. The development of a subsurface CO2 plume near the middle packer section of the horizontal release was studied using soil-gas and surface flux measurements of CO2. A perfluorocarbon tracer was added to the CO2 released from this section of the horizontal well, and the development of atmospheric plumes of the tracer was studied under various meteorological conditions using horizontal and vertical grids of monitors containing sorbent material to collect the tracer. This study demonstrated the feasibility of using remote sensing for the ultra low level detection of atmospheric plumes of tracers as means to monitor the near surface leakage of sequestered CO2.  相似文献   

4.
The effective site assessment is crucial to the successful remediation of the subsurface contaminated with light nonaqueous phase liquids (LNAPLs). Recent studies showed that large spatial volumes of the subsurface contaminated with LNAPLs could be investigated with the partitioning tracer method. This study investigated the applicability of the partitioning tracer method for detecting and quantifying refined petroleum products in a saturated aquifer containing alluvial soil or weathered granite soil. In the batch-partitioning experiments, the partition coefficients of alcohol tracers between the petroleum mixture and water were measured, and they were found to be increased in proportion to the boiling points of the alcohol tracers when the molecular weights of the alcohol tracers were similar. The sorption isotherm experiments indicated that a considerable amount of 4-methyl-2-pentanol was sorbed into Jumunjin sand (JS) or weathered granite soil (WGS). In the column experiments, it was confirmed that the partitioning tracer method could be used as a method for detecting the presence of the petroleum mixture in saturated soil, and the residual saturation of the petroleum mixture in the soil column prepared by firstly contaminating with the petroleum mixture and secondly saturating with water was measured higher than that in the soil column prepared by firstly saturating and secondly contaminating. The highest accuracy of estimation using the partitioning tracer method was found for 2-ethyl-1-butanol and the lowest accuracy was found for 4-methyl-2-pentanol.  相似文献   

5.
Partitioning tracer tests, as an alternative to the core sampling method, were conducted to quantify the degree of saturation of water and nonaqueous phase liquids (NAPL) in the vadose zone. Hydrocarbon gases, which have less effect on global warming than conventional tracers, were used as partitioning tracers. Column tests using CH4, C3H5, and C4H10 as non-partitioning and partitioning tracers were performed to determine the retardation factor and partition coefficient of the tracer into water and NAPL. The retardation factors of these tracers were estimated to be in the range of 1.0–7.0 based on breakthrough curves of the tracers. The partition coefficient of C3H5 to water and diesel phase was calculated to be 0.57 and 8.45, respectively. For a heavier tracer, C4H10, the partition coefficient to the water and diesel phases was 1.2 and 40.5, respectively. The average value of water and diesel saturation estimated from column tests agreed well with known values in unsaturated soil. A residence time longer than 7.5 h within soil pores was found to provide local equilibrium partitioning of the tracer to the diesel phase. The concentration of tracer had no effect on the partitioning process.  相似文献   

6.
Carbon dioxide sequestration in deep aquifers and depleted oilfields is a potential technical solution for reducing green-house gas release to the atmosphere: the gas containment relies on several trapping mechanisms (supercritical CO2, CO2(sc), dissolution together with slow water flows, mineral trapping) and on a low permeability cap-rock to prevent CO2(sc), which is less dense than the formation water, from leaking upwards. A leakproof cap-rock is thus essential to ensure the sequestration efficiency. It is also crucial for safety assessment to identify and assess potential alteration processes that may damage the cap-rock properties: chemical alteration, fracture reactivation, degradation of injection borehole seals, etc. The reactivity of the host-rock minerals with the supercritical CO2 fluid is one of the potential mechanisms, but it is altogether unknown. Reactivity tests have been carried out under such conditions, consisting of batch reactions between pure minerals and anhydrous supercritical CO2, or a two-phase CO2/H2O fluid at 200?°C and 105/160 bar. After 45 to 60 days, evidence of appreciable mineral-fluid reactivity was identified, including in the water-free experiments. For the mixed H2O/CO2 experiments, portlandite was totally transformed into calcite; anorthite displayed many dissolution patterns associated with calcite, aragonite, tridymite and smectite precipitations. For the anhydrous CO2 experiments, portlandite was totally carbonated to form calcite and aragonite; anorthite also displayed surface alteration patterns with secondary precipitation of fibrous calcite. To cite this article: O. Regnault et al., C. R. Geoscience 337 (2005).  相似文献   

7.
《Applied Geochemistry》2005,20(8):1461-1472
Iodine is a biophilic element, with one stable isotope, 127I, and one long-lived radioisotope, 129I. Radioiodine originates in the surface environment almost entirely from anthropogenic activities such as nuclear fuel reprocessing in Europe and thus provides a unique point source tracer. Very few studies have evaluated the geochemical behavior of I isotopes in the subsurface. In this study, the concentrations of 129I and 127I were measured in wells fed by a series of artificial recharge ponds in the Forebay Area of the Orange County ground water basin (California, USA) to evaluate their potential use as hydrological tracers. To substantiate interpretation of 129I and 127I concentration data, the aquifer system was evaluated using the literature values of aquifer water mass age based on 3H/3He, Xe and δ18O tracer data. The aquifer data demonstrate the nearly conservative behavior of 129I with 129I/127I ratios likely reflecting variations in source functions as well as climatic conditions, and with inferred particle-water partition coefficients (Kd) of 0.1 cm3 g−1 or less.  相似文献   

8.
Carbon dioxide capture and geological storage (CCGS) is an emerging technology that is increasingly being considered for reducing greenhouse gas emissions to the atmosphere. Deep saline aquifers provide a very large capacity for CO2 storage and, unlike hydrocarbon reservoirs and coal beds, are immediately accessible and are found in all sedimentary basins. Proper understanding of the displacement character of CO2-brine systems at in-situ conditions is essential in ascertaining CO2 injectivity, migration and trapping in the pore space as a residual gas or supercritical fluid, and in assessing the suitability and safety of prospective CO2 storage sites. Because of lack of published data, the authors conducted a program of measuring the relative permeability and other displacement characteristics of CO2-brine systems for sandstone, carbonate and shale formations in central Alberta in western Canada. The tested formations are representative of the in-situ characteristics of deep saline aquifers in compacted on-shore North American sedimentary basins. The results show that the capillary pressure, interfacial tension, relative permeability and other displacements characteristics of CO2-brine systems depend on the in-situ conditions of pressure, temperature and water salinity, and on the pore size distribution of the sedimentary rock. This paper presents a synthesis and interpretation of the results.  相似文献   

9.
The chalcogenes (S, Se, Te), semimetals (As, Sb) and the metal Bi are important ligands for noble metals and form a wide range of compositionally diverse minerals with the platinum-group elements (PGE). With the exception of S, few experimental data exist to quantify the behavior of these elements in magmatic sulfide systems. Here we report experimental partition coefficients for Se, Te, As, Sb, and Bi between monosulfide solid solution (mss) and sulfide melt, determined at 950 °C at a range of sulfur fugacities (fS2) bracketed by the Fe-FeS (metal-troilite) and the Fe1−×S-Sx (mss-sulfur) equilibria. Selenium is shown to partition in mss-saturated sulfide melt as an anion replacing S2−. Arsenic changes its oxidation state with fS2 from predominantly anionic speciation at low fS2, to cationic speciation at high fS2. The elements Sb, Te, and Bi are so highly incompatible with mss that they can only be present in sulfide melt as cations and/or as neutral metallic species. The partition coefficients derived fall with increasing atomic radius of the element. They also reflect the positions of the respective elements in the Periodic Table: within a group (e.g., As, Sb, Bi) the partition coefficients fall with increasing atomic radius, and within a period the elements of the 15th group are more incompatible with mss than the neighboring elements of the 16th group.  相似文献   

10.
Deep saline aquifers in sedimentary basins are considered to have the greatest potential for CO2 geological storage in order to reduce carbon emissions. CO2 injected into a saline sandstone aquifer tends to migrate upwards toward the caprock because the density of the supercritical CO2 phase is lower than that of formation water. The accumulated CO2 in the upper portions of the reservoir gradually dissolves into brine, lowers pH and changes the aqueous complexation, whereby induces mineral alteration. In turn, the mineralogical composition could impose significant effects on the evolution of solution, further on the mineralized CO2. The high density of aqueous phase will then move downward due to gravity, give rise to “convective mixing,” which facilitate the transformation of CO2 from the supercritical phase to the aqueous phase and then to the solid phase. In order to determine the impacts of mineralogical compositions on trapping amounts in different mechanisms for CO2 geological storage, a 2D radial model was developed. The mineralogical composition for the base case was taken from a deep saline formation of the Ordos Basin, China. Three additional models with varying mineralogical compositions were carried out. Results indicate that the mineralogical composition had very obvious effects on different CO2 trapping mechanisms. Specific to our cases, the dissolution of chlorite provided Mg2+ and Fe2+ for the formation of secondary carbonate minerals (ankerite, siderite and magnesite). When chlorite was absent in the saline aquifer, the dominant secondary carbon sequestration mineral was dawsonite, and the amount of CO2 mineral trapping increased with an increase in the concentration of chlorite. After 3000 years, 69.08, 76.93, 83.52 and 87.24 % of the injected CO2 can be trapped in the solid (mineral) phase, 16.05, 11.86, 8.82 and 6.99 % in the aqueous phase, and 14.87, 11.21, 7.66 and 5.77 % in the gas phase for Case 1 through 4, respectively.  相似文献   

11.
Partitioning of Ni in calcite, CaCO3, was evaluated with the aim of collecting data on partition and distribution coefficients and to enhance understanding about the interaction of Ni with the calcite surface and further incorporation into the bulk. This information will aid in the interpretation of geological processes for safety assessment of waste repositories and contamination of groundwater. Coprecipitation experiments were carried out by the constant addition method at 25 °C and pCO2 = 1 and 10−3.5 atm. Ni was moderately partitioned from solution into calcite. For dilute solid solutions (XNi < 0.001), Ni partition coefficients were estimated to be ∼1 and found to be weakly dependent on calcite precipitation rate in the range of 3-230 nmol m−2 s−1. Ni molar fraction in the solid is directly proportional to Ni concentration in the solution. The fit of the data to such a model is good evidence that Ni is taken up as a true solid solution, not simply by physical trapping.  相似文献   

12.
The intensity of biogenic sediment mixing is often expressed as a “biodiffusion coefficient” (Db), quantified by fitting a diffusive model of bioturbation to vertical profiles of particle-bound radioisotopes. The biodiffusion coefficient often exhibits a dependence on tracer half-life: short-lived radioisotopes (e.g. 234Th) tend to yield notably larger Db values than longer-lived radioisotopes (e.g. 210Pb). It has been hypothesized that this is a result of differential mixing of tracers by particle-selective benthos. This study employs a lattice-automaton model of bioturbation to explore how steady-state tracers with different half-lives are mixed in typical marine settings. Every particle in the model is tagged with the same array of radioisotopes, so that all tracers experienced exactly the same degree of mixing. Two different estimates of the mixing intensity are calculated: a tracer-derived Db, obtained in the standard way by fitting the biodiffusion model to resulting tracer profiles, and a particle-tracking Db, derived from the statistics of particle movements. The latter provides a tracer-independent measure of mixing for use as a reference. Our simulations demonstrate that an apparent Db tracer-dependence results from violating the underlying assumptions of the biodiffusion model. Breakdown of the model is rarely apparent from tracer profiles, emphasizing the need to evaluate the model’s criteria from biological and ecological parameters, rather than relying on obvious indications of model breakdown, e.g., subsurface maxima. Simulations of various marine environments (coastal, slope, abyssal) suggest that the time scales of short-lived radioisotopes, such as 234Th and 7Be, are insufficient for the tracers to be used with the biodiffusion model. 210Pb appears an appropriate tracer for abyssal sediments, while 210Pb and 228Th are suitable for slope and coastal sediments.  相似文献   

13.
This study examined the impacts of reservoir properties on carbon dioxide (CO2) migration after subsurface injection and evaluated the possibility of characterizing reservoir properties using CO2 monitoring data such as spatial–temporal distributions of gas pressure, which can be reasonably monitored in practice. The injection reservoir was assumed to be located 1,400–1,500 m below the ground surface such that CO2 remained in the supercritical state. The reservoir was assumed to contain layers with alternating conductive and resistive properties, which is analogous to actual geological formations such as the Mount Simon Sandstone unit. The CO2 injection simulation used a cylindrical grid setting in which the injection well was situated at the center of the domain, which extended out 8,000 m from the injection well. The CO2 migration was simulated using the latest version of the simulator, subsurface transport over multiple phases (the water–salt–CO2–energy module), developed by Pacific Northwest National Laboratory. A nonlinear parameter estimation and optimization modeling software package, Parameter ESTimation (PEST), is adopted for automated reservoir parameter estimation. The effects of data quality, data worth, and data redundancy were explored regarding the detectability of reservoir parameters using gas pressure monitoring data, by comparing PEST inversion results using data with different levels of noises, various numbers of monitoring wells and locations, and different data collection spacing and temporal sampling intervals. This study yielded insight into the use of CO2 monitoring data for reservoir characterization and how to design the monitoring system to optimize data worth and reduce data redundancy. The feasibility of using CO2 saturation data for improving reservoir characterization was also discussed.  相似文献   

14.
Hydrated Portland cement was reacted with CO2 in supercritical, gaseous and aqueous phases to understand the potential cement alteration processes along the length of a wellbore, extending from a deep CO2 storage reservoir to the shallow subsurface during geologic carbon sequestration. The 3-D X-ray microtomography (XMT) images showed that the cement alteration was significantly more extensive with CO2-saturated synthetic groundwater than dry or wet supercritical CO2 at high P (10 MPa)-T (50 °C) conditions. Scanning electron microscopy with energy dispersive spectroscopy (SEM–EDS) analysis also exhibited a systematic Ca depletion and C enrichment in cement matrix exposed to CO2-saturated groundwater. Integrated XMT, XRD and SEM–EDS analyses identified the formation of an extensive carbonated zone filled with CaCO3(s), as well as a porous degradation front and an outermost silica-rich zone in cement after exposure to CO2-saturated groundwater. Cement alteration by CO2-saturated groundwater for 2–8 months overall decreased the porosity from 31% to 22% and the permeability by an order of magnitude. Cement alteration by dry or wet supercritical CO2 was slow and minor compared to CO2-saturated groundwater. A thin single carbonation zone was formed in cement after exposure to wet supercritical CO2 for 8 months or dry supercritical CO2 for 15 months. An extensive calcite coating was formed on the outside surface of a cement sample after exposure to wet gaseous CO2 for 1–3 months. The chemical–physical characterization of hydrated Portland cement after exposure to various phases of CO2 indicates that the extent of cement carbonation can be significantly heterogeneous depending on the CO2 phase present in the wellbore environment. Both experimental and geochemical modeling results suggest that wellbore cement exposure to supercritical, gaseous and aqueous phases of CO2 during geologic C sequestration is unlikely to damage the wellbore integrity because cement alteration by all phases of CO2 is dominated by carbonation reactions. This is consistent with previous field studies of wellbore cement with extensive carbonation after exposure to CO2 for three decades. However, XMT imaging indicates that preferential cement alteration by supercritical CO2 or CO2-saturated groundwater can occur along the cement–steel or cement–rock interfaces. This highlights the importance of further investigation of cement degradation along the interfaces of wellbore materials to ensure permanent geologic carbon storage.  相似文献   

15.
Carbon sequestration in shallow aquifers can be facilitated by water withdrawal. The factors that optimize the injection/withdrawal balance to minimize potential environmental impacts have been studied, including reservoir size, well pattern, injection rate, reservoir heterogeneity, anisotropy ratio, and permeability sequence. The effects of these factors on CO2 storage capacity and efficiency were studied using a compositional simulator Computer Modeling Group-General Equation of State Model, which modeled features including residual gas trapping, CO2 solubility, and mineralization reactions. Two terms, storage efficiency and CO2 relative breakthrough time, were introduced to better describe the problem. The simulation results show that simultaneous water withdrawal during CO2 injection greatly improves CO2 storage capacity and efficiency. A certain degree of heterogeneity or anisotropy benefits CO2 storage. A high injection rate favors storage capacity, but reduces the storage efficiency and CO2 breakthrough time, which in turn limits the total amount of CO2 injected.  相似文献   

16.
Modeling geological carbon storage represents a new and substantial challenge for the subsurface geosciences. To increase understanding and make good engineering decisions, containment processes and large-scale storage operations must be simulated in a thousand-year perspective. Large differences in spatial and temporal scales make it prohibitively expensive to compute the fate of injected CO2 using traditional 3D simulators. Instead, accurate forecast can be computed using simplified models that are adapted to the specific setting of the bouyancy-driven migration of the light fluid phase. This paper presents a family of vertically integrated models for studying the combined large-scale and long-term effects of structural, residual, and solubility trapping of CO2. The models are based on an assumption of a sharp interface separating CO2 and brine and can provide a detailed inventory of the injected CO2 volumes over periods of thousands of years within reasonable computational time. To be compatible with simulation tools used in industry, the models are formulated in a black-oil framework. The models are implemented in MRST-co2lab, which is an open community software developed especially to study and optimize large-scale, long-term geological storage of CO2. The resulting simulators are fully implicit and handle input from standard geomodeling tools.  相似文献   

17.
For the utilization of deep saline aquifers in the frame of geotechnical use, such as geological sequestration of CO2, H2 or energy storage, a baseline characterization of pristine reservoir rock cores is required to monitor changes in the indigenous microbial communities and pore fluids, and to study alterations in rock characteristics resulting from interaction with geological storage technologies. However, drilling procedures and technical fluids, particularly drill mud, are sources of core contamination. To measure the penetration of drill mud into the cores, three tracers (fluorescein, microspheres, and 4′,6-diamidino-2-phenylindole stained bacteria) were tested under laboratory conditions. The flow of drill mud into core samples was induced by applying uniaxial pressure differentials to the core, and the penetration depth was microscopically determined for each tracer. Fluorescein was extracted from the rock samples and quantified fluorometrically. The results indicate that all tested tracers are suitable for tracking drill-mud penetration. The actual penetration depth seems to be related to differences in mineral composition and texture as well as microfractures. Among all tested tracers, fluorescein labelling is the simplest, cheapest and most accurate method for analyzing the contamination of rock cores by technical fluids. The application of this tracer was successfully applied during two deep drilling campaigns at the CO2 storage pilot site in Ketzin, Germany. The results highlight that the use of tracers is indispensable to ensure the quality of core samples for microbiological and biogeochemical analysis.  相似文献   

18.
Hydrothermal volatile-solubility and partitioning experiments were conducted with fluid-saturated haplogranitic melt, H2O, CO2, and S in an internally heated pressure vessel at 900°C and 200?MPa; three additional experiments were conducted with iron-bearing melt. The run-product glasses were analyzed by electron microprobe, FTIR, and SIMS; and they contain ??0.12 wt% S, ??0.097 wt% CO2, and ??6.4 wt% H2O. Apparent values of log f O2 for the experiments at run conditions were computed from the [(S6+)/(S6++S2?)] ratio of the glasses, and they range from NNO ?0.4 to NNO?+?1.4. The C?CO?CH?CS fluid compositions at run conditions were computed by mass balance, and they contained 22?C99?mol% H2O, 0?C78?mol% CO2, 0?C12?mol% S, and <3 wt% alkalis. Eight S-free experiments were conducted to determine the H2O and CO2 concentrations of melt and fluid compositions and to compare them with prior experimental results for C?CO?CH fluid-saturated rhyolite melt, and the agreement is excellent. Sulfur partitions very strongly in favor of fluid in all experiments, and the presence of S modifies the fluid compositions, and hence, the CO2 solubilities in coexisting felsic melt. The square of the mole fraction of H2O in melt increases in a linear fashion, from 0.05 to 0.25, with the H2O concentration of the fluid. The mole fraction of CO2 in melt increases linearly, from 0.0003 to 0.0045, with the CO2 concentration of C?CO?CH?CS fluids. Interestingly, the CO2 concentration in melts, involving relatively reduced runs (log f O2????NNO?+?0.3) that contain 2.5?C7?mol% S in the fluid, decreases significantly with increasing S in the system. This response to the changing fluid composition causes the H2O and CO2 solubility curve for C?CO?CH?CS fluid-saturated haplogranitic melts at 200?MPa to shift to values near that modeled for C?CO?CH fluid-saturated, S-free rhyolite melt at 150?MPa. The concentration of S in haplogranitic melt increases in a linear fashion with increasing S in C?CO?CH?CS fluids, but these data show significant dispersion that likely reflects the strong influence of f O2 on S speciation in melt and fluid. Importantly, the partitioning of S between fluid and melt does not vary with the (H2O/H2O?+?CO2) ratio of the fluid. The fluid-melt partition coefficients for H2O, CO2, and S and the atomic (C/S) ratios of the run-product fluids are virtually identical to thermodynamic constraints on volatile partitioning and the H, S, and C contents of pre-eruptive magmatic fluids and volcanic gases for subduction-related magmatic systems thus confirming our experiments are relevant to natural eruptive systems.  相似文献   

19.
Seal or cap-rock integrity is a safety issue during geological carbon dioxide capture and storage (CCS). Industrial impurities such as SO2, O2, and NOx, may be present in CO2 streams from coal combustion sources. SO2 and O2 have been shown recently to influence rock reactivity when dissolved in formation water. Buoyant water-saturated supercritical CO2 fluid may also come into contact with the base of cap-rock after CO2 injection. Supercritical fluid-rock reactions have the potential to result in corrosion of reactive minerals in rock, with impurity gases additionally present there is the potential for enhanced reactivity but also favourable mineral precipitation.The first observation of mineral dissolution and precipitation on phyllosilicates and CO2 storage cap-rock (siliciclastic reservoir) core during water-saturated supercritical CO2 reactions with industrial impurities SO2 and O2 at simulated reservoir conditions is presented. Phyllosilicates (biotite, phlogopite and muscovite) were reacted in contact with a water-saturated supercritical CO2 containing SO2, or SO2 and O2, and were also immersed in the gas-saturated bulk water. Secondary precipitated sulfate minerals were formed on mineral surfaces concentrated at sheet edges. SO2 dissolution and oxidation resulted in solution pH decreasing to 0.74 through sulfuric acid formation. Phyllosilicate dissolution released elements to solution with ∼50% Fe mobilized. Geochemical modelling was in good agreement with experimental water chemistry. New minerals nontronite (smectite), hematite, jarosite and goethite were saturated in models. A cap-rock core siltstone sample from the Surat Basin, Australia, was also reacted in water-saturated supercritical CO2 containing SO2 or in pure supercritical CO2. In the presence of SO2, siderite and ankerite were corroded, and Fe-chlorite altered by the leaching of mainly Fe and Al. Corrosion of micas in the cap-rock was however not observed as the pH was buffered by carbonate dissolution. Ca-sulfate, and Fe-bearing precipitates were observed post SO2-CO2 reaction, mainly centered on surface cracks and an illite rich illite-smectite precipitate quantified. Water saturated impure supercritical CO2 was observed to have reactivity to rock-forming biotite, muscovite and phlogopite mineral separates. In the cap-rock core however carbonates and chlorite were the main reacting minerals showing the importance of assessing actual whole core.  相似文献   

20.
Partitioning of Eu(III) in calcite, CaCO3, was evaluated with the aim of collecting data on partition coefficients and to enhance understanding of the incorporation mechanisms. This information will aid in the interpretation of geological processes from rare Earth element (REE) data and in the use of Eu(III) as a chemical analogue for the trivalent actinides, particularly Am(III) and Cm(III). Coprecipitation experiments were carried out by the constant addition method at 25°C and PCO2 = 1 atm. Eu(III) was strongly partitioned from the solution into calcite. For dilute solid solutions (XEu < 0.001), Eu partition coefficients were estimated to be 770 ± 290 and found to be independent of calcite precipitation rate in the range of 0.02 to 2.7 nmol mg−1 min−1. This could be explained by the approximately equal values of the Eu partition and adsorption coefficients. Several solid solution models were tested. A vacancy model for Eu2(CO3)3-CaCO3 is consistent with the experimental results and constraints on geometry for Eu fit in the calcite lattice. For low Eu content, vacancy density is independent of Eu concentration in the solid so logarithm of the ion activity product, log (Eu)2(CO32−)3, depends linearly on log XEu2. The fit of the data to such a model is good evidence that Eu(III) is taken up as a true solid solution, not simply by physical trapping. A model using EuOHCO3-CaCO3 is also consistent with the uptake stoichiometry, but EuOH2+ substitution for Ca2+ would be expected to distort the calcite structure more than is compatible with such a high KD. Several other models, including EuNa(CO3)2-CaCO3, were abandoned because their stoichiometric relationships did not fit the experimental data.  相似文献   

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