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1.
The objective of this study is to understand cement alteration processes with the evolution of porosity and hardness under geologic CO2 storage conditions. For this study, the cylindrical cement cores (class G) were reacted with CO2–saturated water in a vessel (40 °C and 8 MPa) for 10 and 100 days. After the experiment, the CO2 concentration and Vickers hardness were measured in the hydrated cement core to estimate the carbonation depth and to identify the change in hardness, respectively. Diffusive-reactive transport modeling was also performed to trace the alteration processes and subsequent porosity changes. The results show that cement alteration mainly results from carbonation. With alteration processes, four different reaction zones are developed: degradation zone, carbonation zone, portlandite depletion zone, and unreacted zone. In the degradation zone, the re-dissolution of calcite formed in the carbonation zone leads to the increase of porosity. In contrast, the carbonation zone is characterized by calcite formation resulting mainly from the dissolution of portlandite. The carbonation zone acts as a barrier to CO2 intrusion by consuming dissolved CO2. Especially in this zone, although the porosity decreases, the Vickers hardness increases. Our results show that cement alteration processes can affect the physical and hydrological properties of the hydrated cement under CO2-saturated conditions. Further long-term observation is required to confirm our results under in-situ fluid chemistry of a CO2 storage reservoir. Nonetheless, this study would be helpful to understand alteration processes of wellbore cements under CO2 storage conditions.  相似文献   

2.
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   

3.
Calcium carbonate scaling poses highly challenging tasks for its prediction and preventative action. Here an elemental, isotopic and modelling approach was used to decipher the evolution of alkaline tunnel drainage solutions and sinter formation mechanisms for 3 sites in Austria. Drainage solutions originate from local groundwater and form their characteristic chemical composition by interaction with shotcrete/concrete. This interaction is indicated by a positive correlation of dissolved K+ and pH (up to 12.3), and a decrease of aqueous Mg2+ by the formation of brucite (pH > 10.5). Variability in Ca2+ and DIC is strongly attributed to portlandite dissolution, calcite precipitation and CO2 exchange with the atmosphere, where the 13C/12C and 18O/16O signatures of calcite can be traced back to the source of carbonate. The internal PCO2 value is a reliable proxy to evaluate whether uptake of CO2 results in an increase or decrease of the degree of calcite saturation with a threshold value of 10−6.15 atm at 25 °C (pH ≈ 11). Precipitation rates of calcite are highest at pH ≈ 10. Mixing of groundwater-like solutions with strong alkaline drainage solutions has to be considered as a crucial factor for evaluating apparent composition of drainage solutions and calcite precipitation capacities.  相似文献   

4.
In laboratory experiments, the precipitation of dolomite at ambient temperature is virtually impossible due to strong solvation shells of magnesium ions in aqueous media and probably also due to the existence of a more intrinsic crystallization barrier that prevents the formation of long-range ordered crystallographic structures at ambient surface conditions. Conversely, dolomite can easily form at high temperature (>100 °C), but its precipitation and growth requires several days or weeks depending on experimental conditions. In the present study, experiments were performed to assess how a single heat-ageing step promotes the formation of dolomite under high-carbonate alkaline conditions via dissolution-precipitation reactions. This reaction pathway is relevant for the so-called hydrothermal dolomite frequently observed in carbonate platforms, but still ill-defined and understood. Our precipitation route is summarized by two main sequential reactions: (1) precipitation of Mg-calcite at low temperature (∼20 °C) by aqueous carbonation of synthetic portlandite (Ca(OH)2) in a highly alkaline medium (1 M of NaOH and 1 M of MgCl2), leading to precipitation of oriented nanoparticles of low- and high-Mg calcite (∼79 wt%) coexisting with aragonite (∼18 wt%) and brucite (∼3 wt%) after 24 h; (2) fast dolomitization process starting from 1 h of reaction by a single heat-ageing step from ∼20 to 200, 250 and 300 °C. Here, the Mg-calcite acts as a precursor that lowers the overall kinetics barrier for dolomite formation. Moreover, it is an important component in some bio-minerals (e.g. corals and seashells). Quantitative Rietveld refinements of XRD patterns, FESEM observations and FTIR measurements on the sequentially collected samples suggest fast dolomite precipitation coupled with dissolution of transient mineral phases such as low-Mg calcite (Mg < 4 mol%), high-Mg calcite (Mg > 4 mol%), proto-dolomite (or disordered dolomite; Mg > 40 mol%) and Ca-magnesite. In this case, the dolomite formation rate and the time-dependent mineral composition strongly depend on reaction temperature. For example, high-purity dolomitic material (87 wt% of dolomite mixed with 13 wt% of magnesite) was obtained at 300 °C after 48 h of reaction. Conversely, a lower proportion of dolomite (37 wt%), mixed with proto-dolomite (43 wt%), Ca-magnesite (16 wt%) and high-Mg calcite (4 wt%), was obtained at 200 °C after 72 h. The present experiments provide an additional mechanism for the massive dolomite formation in sedimentary environments (ex. deep sea organic-rich carbonate-sediments) if such sediments are subjected to significant temperature variations, for example by hot fluid circulations related to volcanic activity. In such systems, organic degradation increases the carbonate alkalinity (HCO3−) necessary to induce the dolomitization process at low and high temperature.  相似文献   

5.
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   

6.
The sequestration of CO2 occurs naturally in (ultra)‐mafic rocks by carbonation processes and is commonly noted in areas of the seafloor where mantle lithologies are exhumed. As well as carbonation, mantle exhumation is also responsible for rock brecciation. The relationship between carbonation and brecciation is not well constrained. A temporal evolution from syn‐ to post‐tectonic carbonation and brecciation is proposed in line with progressive mantle exhumation. Using a petrological study of brecciated material from IODP drill cores of the Iberia–Newfoundland conjugated margins, we relate crack–seal veins to tectonic brecciation, authigenic calcite with scalenohedral structure to hydraulic brecciation and reworked clasts within cement to (tectono)‐sedimentary processes. Oxygen isotope compositions reveal late‐staged < 50°C carbonate generation in the proximal part of the ocean–continent transition, which have followed an earlier phase of sub‐seafloor carbonate generation. The results are crucial to understand CO2 exchange within the reworked sub‐seafloor in passive margins and oceanic systems.  相似文献   

7.
The global rise in atmospheric greenhouse gas concentrations calls for practicable solutions to capture CO2. In this study, a mineral carbonation process was applied in which CO2 reacts with alkaline lignite ash and forms stable carbonate solids. In comparison to previous studies, the assays were conducted at low temperatures and pressures and under semi-dry reaction conditions in an 8 L laboratory mixing device. In order to find optimum process conditions the pCO2 (10-20%), stirring rate (500-3000 rpm) and the liquid to solid ratio (L/S = 0.03-0.36 L kg−1) were varied. In all experiments a considerable CO2 uptake from the gas phase was observed. Concurrently the solid phase contents of Ca and Mg (hydr)oxides decreased and CaCO3 and MgCO3 fractions increased throughout the experiments, showing that CO2 was stabilized as a solid carbonate. The carbonation reaction depends on three factors: Dissolution of CO2 in the liquid phase, mobilization of Ca and Mg from the mineral surface and precipitation of the carbonate solids. Those limitations were found to depend strongly on the variation of the process parameters. Optimum reaction conditions could be found for L/S ratios between 0.12 and 0.18, medium stirring velocities and pCO2 between 10% and 20%.Maximum CO2 uptake by the solid phase was 4.8 mmol g−1 after 120 min, corresponding to a carbonation efficiency for the alkaline material of 53% of the theoretical CO2 binding capacity. In comparison to previous studies both CO2 uptake and carbonation efficiencies were in a similar range, but the reaction times in the semi-dry process were considerably shorter. The proposed method additionally allows for a more simple carbonation setup due to low T and P, and produces an easier to handle product with low water content.  相似文献   

8.
A rotating disc system has been constructed to study calcite dissolution kinetics. The disc system is shown to obey the Levich theory and to satisfy the stringent chemical controls required by the calcite dissolution system at neutral to alkaline pH values. The errors involved in using a CO2-free atmosphere are shown to be insignificant. It is shown that the stirring dependence of systems which are not hydrodynamically well-defined is variable and dependent on the shape of the reaction vessel. Extrapolation of such results into natural systems involves very large uncertainties.  相似文献   

9.
A laboratory geochemical study was conducted using a drill core sample of cap rock from the Surat Basin, Australia, to investigate the effect of NO2 contained in the CO2 gas exhausted from the oxyfuel combustion process (oxyfuel combustion CO2) on the cap rock. A gas (CO2 containing NO2) was prepared to simulate the exhaust gas produced from the oxyfuel combustion process. Two types of gases (pure CO2 and CO2 containing SO2) were also prepared as reference gases. The effect of NO2 on cap rock was studied experimentally using these gases. No differences in the amounts of leached ions and pH changes for CO2 containing NO2 (36 ppmv), pure CO2, and CO2 containing SO2 (35 ppmv) existed. The pH values decreased immediately after CO2 gas injection but increased with time as a result of mineral buffering. Leaching of Fe, Mg, Ca, and K was suggested to have occurred as the result of dissolution of Fe-chlorite, prehnite and illite-smectite mixed layer clay in the shale sample. The amounts of Ca, Fe, and Mg leached with CO2 containing NO2 (318 ppmv) were higher than those for pure CO2. For the mixture containing 318 ppmv NO2, the pH increased more than that for the other gas conditions immediately after the pH fall at the start of the experiment, because oxidation-reduction reactions occurred between Fe2+ and NO3−. Moreover, the results indicated that some of the leached Ca and Fe were deposited on the shale sample because of the pH increase. Therefore, we concluded that the effects of NO2 on mineral dissolution and pH changes of formation water are negligible when oxyfuel combustion CO2 containing about 30 ppmv of NO2 is injected into an underground aquifer. In addition, even if about 300 ppmv NO2 is accidentally injected into the underground aquifer, mineral dissolution is suppressed due to the buffering of pH decrease after gas injection.  相似文献   

10.
Far from equilibrium enstatite dissolution rates both open to atmospheric CO2 and CO2 purged were measured as a function of solution pH from 8 to 13 in batch reactors at room temperature. Congruent dissolution was observed after an initial period of incongruent dissolution with preferential Si release from the enstatite. Steady-state dissolution rates in open to atmospheric CO2 conditions decrease with increase in solution pH from 8 to 12 similar to the behavior reported by other investigators. Judging from the pH 13 dissolution rate, rates increase with pH above pH 12. This is thought to occur because of the increase in overall negative surface charges on enstatite as Mg surface sites become negative above pH 12.4, the pH of zero surface charge of MgO.Steady-state dissolution rates of enstatite increase above pH 10 when CO2 was purged by performing the experiments in a N2 atmosphere. This suggests inhibition of dissolution rates above pH 10 when experiments were open to the atmosphere. The dissolved carbonate in these solutions becomes dominantly CO32− above pH 10.33. It is argued that CO32− forms a >Mg2-CO3 complex at positively charged Mg surface sites on enstatite, resulting in stabilization of the surface Si-O bonds. Therefore, removal of solution carbonate results in an increase in dissolution rates of enstatite above pH 10. The log rate of CO2-purged enstatite dissolution in moles per cm2 per s as a function of increasing pH above pH 10 is equal to 0.35. This is consistent with the model of silicate mineral dissolution in the absence of surface carbonation in alkaline solutions proposed earlier in the literature.  相似文献   

11.

De Beers kimberlite mine operations in South Africa (Venetia and Voorspoed) and Canada (Gahcho Kué, Victor, and Snap Lake) have the potential to sequester carbon dioxide (CO2) through weathering of kimberlite mine tailings, which can store carbon in secondary carbonate minerals (mineral carbonation). Carbonation of ca. 4.7 to 24.0 wt% (average = 13.8 wt%) of annual processed kimberlite production could offset 100% of each mine site’s carbon dioxide equivalent (CO2e) emissions. Minerals of particular interest for reactivity with atmospheric or waste CO2 from energy production include serpentine minerals, olivine (forsterite), brucite, and smectite. The most abundant minerals, such as serpentine polymorphs, provide the bulk of the carbonation potential. However, the detection of minor amounts of highly reactive brucite in tailings from Victor, as well as the likely presence of brucite at Venetia, Gahcho Kué, and Snap Lake, is also important for the mineral carbonation potential of the mine sites.

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12.
Capture and geological sequestration of CO2 from energy production is proposed to help mitigate climate change caused by anthropogenic emissions of CO2 and other greenhouse gases. Performance goals set by the US Department of Energy for CO2 storage permanence include retention of at least 99% of injected CO2 which requires detailed assessments of each potential storage site’s geologic system, including reservoir(s) and seal(s). The objective of this study was to review relevant basin-wide physical and chemical characteristics of geological seals considered for saline reservoir CO2 sequestration in the United States. Results showed that the seal strata can exhibit substantial heterogeneity in the composition, structural, and fluid transport characteristics on a basin scale. Analysis of available field and wellbore core data reveal several common inter-basin features of the seals, including the occurrence of quartz, dolomite, illite, calcite, and glauconite minerals along with structural features containing fractures, faults, and salt structures. In certain localities within the examined basins, some seal strata also serve as source rock for oil and gas production and can be subject to salt intrusions. The regional features identified in this study can help guide modeling, laboratory, and field studies needed to assess local seal performances within the examined basins.  相似文献   

13.
The response to CO2 exposure of a variety of carbonate cemented rocks has been investigated using pressurised batch experiments conducted under simulated reservoir conditions, 70 °C and 20 MPa, and with a durations of up to14 months. Calcite, dolomite, ankerite and siderite cement were present in the unreacted reservoir rocks and caprocks. Core plugs of the reservoir rocks were used in order to investigate the alterations in situ. Crushing of the caprock samples was necessary to maximise reactions within the relatively short duration of the laboratory experiments. Synthetic brines were constructed for each batch experiment to match the specific formation water composition known from the reservoir and caprock formations in each well. Chemical matched synthetic brines proved crucial in order to avoid reactions due to non-equilibra of the fluids with the rock samples, for example observations of the dissolution of anhydrite, which were not associated with the CO2 injection, but rather caused by mismatched brines.Carbonate dissolution as a response to CO2 injection was confirmed in all batch experiments by both petrographical observations and geochemical changes in the brines. Increased Ca and Mg concentrations after 1 month reaction with CO2 and crushed caprocks are ascribed to calcite and dolomite dissolution, respectively, though not verified petrographically. Ankerite and possible siderite dissolution in the sandstone plugs are observed petrographically after 7 months reaction with CO2; and are accompanied by increased Fe and Mn contents in the reacted fluids. Clear evidence for calcite dissolution in sandstone plugs is observed petrographically after 14 months of reaction with CO2, and is associated with increased amounts of Ca (and Mg) in the reacted fluid. Dolomite in sandstones shows only minor dissolution features, which are not clearly supported by increased Mg content in the reacted fluid.Silicate dissolution cannot be demonstrated, either by chemical changes in the fluids, as Si and Al concentrations remain below the analytical detection limits, nor by petrographical changes, as partly dissolved feldspar grains and authigenic analcime are present in the sediments prior to the experiments. It is noteworthy, that authigenic K-feldspar and authigenic albite in sandstones show no signs of dissolution and consequently seem to be stable under the experimental conditions.  相似文献   

14.
中国大陆新生代典型火山区温室气体释放的规模及其成因   总被引：5，自引：5，他引：0  
火山活动能够将地球深部的碳输送到大气圈,是地质碳排放和深部碳循环的重要形式.火山作用不仅在喷发期能够释放大量温室气体,而且在休眠期也能释放巨量的温室气体.在全球变暖的背景下,定量化地研究火山活动对大气圈温室气体含量增加的贡献具有至关重要的意义.本文利用密闭气室法等该领域国际先进的测试技术,测量并计算了长白山、腾冲、五大连池及青藏高原南部的羊八井等典型火山区的温室气体释放规模.结果显示,我国大陆新生代典型火山区向大气圈输送的温室气体总通量约为8.13×106t·a-1,接近107t·a-1级别,相当于全球火山活动导致的温室气体(主要为CO2)释放总量的6%左右.太平洋构造域火山区的温室气体在释放通量与总量方面均低于特提斯构造域,并且太平洋构造域火山气体的地壳混染程度较低,显示出大洋俯冲带与大陆俯冲带火山区温室气体释放的成因差异.  相似文献   

15.
Zou  Lin  Dong  Lin  Ning  Meng  Huang  Kangjun  Peng  Yongbo  Qin  Shujian  Yuan  Honglin  Shen  Bing 《中国地球化学学报》2019,38(4):481-496

The continent is the second largest carbon sink on Earth’s surface. With the diversification of vascular land plants in the late Paleozoic, terrestrial organic carbon burial is represented by massive coal formation, while the development of soil profiles would account for both organic and inorganic carbon burial. As compared with soil organic carbon, inorganic carbon burial, collectively known as the soil carbonate, would have a greater impact on the long-term carbon cycle. Soil carbonate would have multiple carbon sources, including dissolution of host calcareous rocks, dissolved inorganic carbon from freshwater, and oxidation of organic matter, but the host calcareous rock dissolution would not cause atmospheric CO2 drawdown. Thus, to evaluate the potential effect of soil carbonate formation on the atmospheric pCO2 level, different carbon sources of soil carbonate should be quantitatively differentiated. In this study, we analyzed the carbon and magnesium isotopes of pedogenic calcite veins developed in a heavily weathered outcrop, consisting of limestone of the early Paleogene Guanzhuang Group in North China. Based on the C and Mg isotope data, we developed a numerical model to quantify the carbon source of calcite veins. The modeling results indicate that 4–37 wt% of carbon in these calcite veins was derived from atmospheric CO2. The low contribution from atmospheric CO2 might be attributed to the host limestone that might have diluted the atmospheric CO2 sink. Nevertheless, taking this value into consideration, it is estimated that soil carbonate formation would lower 1 ppm atmospheric CO2 within 2000 years, i.e., soil carbonate alone would sequester all atmospheric CO2 within 1 million years. Finally, our study suggests the C–Mg isotope system might be a better tool in quantifying the carbon source of soil carbonate.

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16.
《Applied Geochemistry》2004,19(6):917-936
Carbon dioxide disposal into deep aquifers is a potential means whereby atmospheric emissions of greenhouse gases may be reduced. However, our knowledge of the geohydrology, geochemistry, geophysics, and geomechanics of CO2 disposal must be refined if this technology is to be implemented safely, efficiently, and predictably. As a prelude to a fully coupled treatment of physical and chemical effects of CO2 injection, the authors have analyzed the impact of CO2 immobilization through carbonate mineral precipitation. Batch reaction modeling of the geochemical evolution of 3 different aquifer mineral compositions in the presence of CO2 at high pressure were performed. The modeling considered the following important factors affecting CO2 sequestration: (1) the kinetics of chemical interactions between the host rock minerals and the aqueous phase, (2) CO2 solubility dependence on pressure, temperature and salinity of the system, and (3) redox processes that could be important in deep subsurface environments. The geochemical evolution under CO2 injection conditions was evaluated. In addition, changes in porosity were monitored during the simulations. Results indicate that CO2 sequestration by matrix minerals varies considerably with rock type. Under favorable conditions the amount of CO2 that may be sequestered by precipitation of secondary carbonates is comparable with and can be larger than the effect of CO2 dissolution in pore waters. The precipitation of ankerite and siderite is sensitive to the rate of reduction of Fe(III) mineral precursors such as goethite or glauconite. The accumulation of carbonates in the rock matrix leads to a considerable decrease in porosity. This in turn adversely affects permeability and fluid flow in the aquifer. The numerical experiments described here provide useful insight into sequestration mechanisms, and their controlling geochemical conditions and parameters.  相似文献   

17.
《Applied Geochemistry》2002,17(4):455-474
In a recent survey of the spring waters of the Genova province, many neutral Mg–HCO3 waters and some high-pH, Ca–OH waters were found in association with serpentinites. All the springs are of meteoric origin as indicated by the stable isotopes of water and dissolved N2 and Ar. Interaction of these meteoric waters with serpentinites determines a progressive evolution in the chemistry of the aqueous phase from an immature Mg-rich, SO4–Cl facies of low salinity to an intermediate Mg–HCO3 facies (pH 7.0–8.5, PCO210−3.5–10−2.5 bar, Eh 150–250 mV), and to a mature Ca–OH facies (pH 10–12, PCO2 10−9.4−10−10.6 bar, Eh-390 to-516 mV). The irreversible water–rock mass transfer leading to these chemical changes in the aqueous phase was simulated through reaction path modeling, assuming bulk dissolution of a local serpentinite, and the precipitation of gibbsite, goethite, calcite, hydromagnesite, kaolinite, a montmorillonite solid mixture, a saponite solid mixture, sepiolite, and serpentine. The simulation was carried out in two steps, under open-system and closed-system conditions with respect to CO2, respectively. The calculated concentrations agree with analytical data, indicating that the computed water-rock mass transfer is a realistic simulation of the natural process. Moreover, the simulation elucidates the role of calcite precipitation during closed-system serpentinite dissolution in depleting the aqueous solution of C species, allowing the concurrent increment in Ca and the acquisition of a Ca–OH composition. Calcium–OH waters, due to their high pH, tend to absorb CO2, precipitating calcite. Therefore, these waters might be used to sequester anthropogenic CO2, locally preventing environmental impact to the atmosphere.  相似文献   

18.
Capturing CO2 from point sources and storing it in geologic formations is a potential option for allaying the CO2 level in the atmosphere. In order to evaluate the effect of geological storage of CO2 on rock-water interaction, batch experiments were performed on sandstone samples taken from the Altmark reservoir, Germany, under in situ conditions of 125 °C and 50 bar CO2 partial pressure. Two sets of experiments were performed on pulverized sample material placed inside a closed batch reactor in (a) CO2 saturated and (b) CO2 free environment for 5, 9 and 14 days. A 3M NaCl brine was used in both cases to mimic the reservoir formation water. For the “CO2 free” environment, Ar was used as a pressure medium. The sandstone was mainly composed of quartz, feldspars, anhydrite, calcite, illite and chlorite minerals. Chemical analyses of the liquid phase suggested dissolution of both calcite and anhydrite in both cases. However, dissolution of calcite was more pronounced in the presence of CO2. In addition, the presence of CO2 enhanced dissolution of feldspar minerals. Solid phase analysis by X-ray diffraction and Mössbauer spectroscopy did not show any secondary mineral precipitation. Moreover, Mössbauer analysis did not show any evidence of significant changes in redox conditions. Calculations of total dissolved solids’ concentrations indicated that the extent of mineral dissolution was enhanced by a factor of approximately 1.5 during the injection of CO2, which might improve the injectivity and storage capacity of the targeted reservoir. The experimental data provide a basis for numerical simulations to evaluate the effect of injected CO2 on long-term geochemical alteration at reservoir scale.  相似文献   

19.
Geological sequestration of anthropogenic CO2 appears to be a promising method for reducing the amount of greenhouse gases released to the atmosphere. Geochemical modelling of the storage capacity for CO2 in saline aquifers, sandstones and/or carbonates should be based on natural analogues both in situ and in the laboratory. The main focus of this paper has been to study natural gas emissions representing extremely attractive surrogates for the study and prediction of the possible consequences of leakage from geological sequestration sites of anthropogenic CO2 (i.e., the return to surface, potentially causing localised environmental problems). These include a comparison among three different Italian case histories: (i) the Solfatara crater (Phlegraean Fields caldera, southern Italy) is an ancient Roman spa. The area is characterised by intense and diffuse hydrothermal activity, testified by hot acidic mud pools, thermal springs and a large fumarolic field. Soil gas flux measurements show that the entire area discharges between 1200 and 1500 tons of CO2 per day; (ii) the Panarea Island (Aeolian Islands, southern Italy) where a huge submarine volcanic-hydrothermal gas burst occurred in November, 2002. The submarine gas emissions chemically modified seawater causing a strong modification of the marine ecosystem. All of the collected gases are CO2-dominant (maximum value: 98.43 vol.%); (iii) the Tor Caldara area (Central Italy), located in a peripheral sector of the quiescent Alban Hills volcano, along the faults of the Ardea Basin transfer structure. The area is characterised by huge CO2 degassing both from water and soil. Although the above mentioned areas do not represent a storage scenario, these sites do provide many opportunities to study near-surface processes and to test monitoring methodologies.  相似文献   

20.
This paper reviews various coal seam gas (CSG) models that have been developed for the Sydney Basin, and provides an alternative interpretation for gas composition layering and deep-seated CO2 origins. Open file CSG wells, supplemented by mine-scale information, were used to examine trends in gas content and composition at locations from the margin to the centre of the basin. Regionally available hydrochemistry data and interpretations of hydrodynamics were incorporated with conventional petroleum well data on porosity and permeability. The synthesised gas and groundwater model presented in this paper suggests that meteoric water flow under hydrostatic pressure transports methanogenic consortia into the subsurface and that water chemistry evolves during migration from calcium-rich freshwaters in inland recharge areas towards sodium-rich brackish water down-gradient and with depth. Groundwater chemistry changes result in the dissolution and precipitation of minerals as well as affecting the behaviour of dissolved gases such as CO2. Mixing of carbonate-rich waters with waters of significantly different chemistries at depth causes the liberation of CO2 gas from the solution that is adsorbed into the coal matrix in hydrodynamically closed terrains. In more open systems, excess CO2 in the groundwater (carried as bicarbonate) may lead to precipitation of calcite in the host strata. As a result, areas in the central and eastern parts of the basin do not host spatially extensive CO2 gas accumulations but experience more widespread calcite mineralisation, with gas compositions dominated by hydrocarbons, including wet gases. Basin boundary areas (commonly topographic and/or structural highs) in the northern, western and southern parts of the basin commonly contain CO2-rich gases at depth. This deep-seated CO2-rich gas is generally thought to derive from local to continental scale magmatic intrusions, but could also be the product of carbonate dissolution or acetate fermentation.  相似文献   

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