首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 31 毫秒
1.
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   

2.
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   

3.
富CO_2流体-砂岩相互作用是砂岩储层次生孔隙的重要形成机制。苏北黄桥地区作为中国重要的CO_2气产区,富CO_2流体对上二叠统龙潭组砂岩储层的改造问题备受关注。为揭示富CO_2流体的作用特征及其对储层的影响,对黄桥地区典型钻井开展了系统的岩心描述和岩矿鉴定,并进行了微区原位观测和相关地球化学分析。结果表明,在靠近CO_2流体活动强烈的断裂带部位(特别是断层上盘),砂岩中碳酸盐胶结物基本溶蚀殆尽,仅存少量交代成因菱铁矿,同时钾长石类碎屑溶蚀非常强烈,并伴随高岭石等矿物沉淀,以及石英次生加大,还发育片钠铝石等指示高浓度CO_2作用的特征矿物,形成与CO_2流体作用相关的特征矿物组合(片钠铝石+高岭石+次生石英+菱铁矿);而在远离断裂的部位,受CO_2流体影响较弱,溶蚀作用也较弱,有较多的次生方解石沉淀,形成了以方解石+菱铁矿为主的自生矿物组合。前者次生孔隙发育,后者则更加致密。据此提出了深源断裂主控下与富CO_2流体作用相关的储层发育模式,为油气勘探和开发提供了新的思路。  相似文献   

4.
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   

5.
The most suitable candidates for subsurface storage of CO2 are depleted gas fields. Their ability to retain CO2 can however be influenced by the effect which impurities in the CO2 stream (e.g. H2S and SO2) have on the mineralogy of reservoir and seal. In order to investigate the effects of SO2 we carried out laboratory experiments on reservoir and cap rock core samples from gas fields in the northeast of the Netherlands. The rock samples were contained in reactor vessels for 30 days in contact with CO2 and 100 ppm SO2 under in-situ conditions (300 bar, 100 °C). The vessels also contained brine with the same composition as in the actual reservoir. Furthermore equilibrium modeling was carried out using PHREEQC software in order to model the experiments on caprock samples.After the experiments the permeability of the reservoir samples had increased by a factor of 1.2–2.2 as a result of dissolution of primary reservoir minerals. Analysis of the associated brine samples before and after the experiments showed that concentrations of K, Si and Al had increased, indicative of silicate mineral dissolution.In the caprock samples, composed of carbonate and anhydrite minerals, permeability changed by a factor of 0.79–23. The increase in permeability is proportional to the amount of carbonate in the caprock. With higher carbonate content in comparison with anhydrite the permeability increase is higher due to the additional carbonate dissolution. This dependency of permeability variations was verified by the modeling study. Hence, caprock with a higher anhydrite content in comparison with carbonate minerals has a lower risk of leakage after co-injection of 100 ppmv SO2 with CO2.  相似文献   

6.
海拉尔盆地乌尔逊凹陷下白垩统含片钠铝石砂岩部分记录了幔源CO_2-砂岩相互作用历史.为揭示幔源CO_2充注对储层质量的影响,通过偏光显微镜、扫描电镜观察和孔隙度、渗透率数据研究了海拉尔盆地乌尔逊凹陷含片钠铝石砂岩的岩石学和储层特征.幔源CO_2的充注导致了长石的部分溶解和片钠铝石及铁白云石的沉淀.长石的溶解形成了次生孔隙.片钠铝石以针状晶形为特征,其集合体呈束状、簇状、扇状和玫瑰花状.部分片钠铝石呈板状.片钠铝石以充填孔隙为主,少量交代长石和其他骨架碎屑颗粒.片钠铝石局部被铁白云石交代,说明铁白云石的形成晚于片钠铝石.片钠铝石的含量为1%～20%.相同深度段的含片钠铝石砂岩(n=597,h=1309.15～2140.71m)与普通砂岩(n=1550,h=1323.72～2141.3m)的孔隙度、渗透率数据统计表明,含片钠铝石砂岩的物性整体上低于普通砂岩,说明CO_2的充注导致了储层质量的改变.片钠铝石含量-孔隙度和片钠铝石含量-渗透率之间的关系,揭示片钠铝石含量是引起储层质量改变的主要因素.片钠铝石含量10%似乎是储层质量发生变化的界限,当片钠铝石含量＞10%,随片钠铝石含量增加,砂岩的孔隙度和渗透率降低;当片钠铝石含量＜10%,随片钠铝石含量增加,部分砂岩的孔隙度和渗透率表现出增加趋势.作者认为,片钠铝石含量高的砂岩长期处于高CO_2分压成岩环境,而片钠铝石含量低的砂岩则处于高CO_2分压成岩环境的时间相对较短.  相似文献   

7.
《China Geology》2022,5(3):359-371
To accelerate the achievement of China’s carbon neutrality goal and to study the factors affecting the geologic CO2 storage in the Ordos Basin, China’s National Key R&D Programs propose to select the Chang 6 oil reservoir of the Yanchang Formation in the Ordos Basin as the target reservoir to conduct the geologic carbon capture and storage (CCS) of 100000 t per year. By applying the basic theories of disciplines such as seepage mechanics, multiphase fluid mechanics, and computational fluid mechanics and quantifying the amounts of CO2 captured in gas and dissolved forms, this study investigated the effects of seven factors that influence the CO2 storage capacity of reservoirs, namely reservoir porosity, horizontal permeability, temperature, formation stress, the ratio of vertical to horizontal permeability, capillary pressure, and residual gas saturation. The results show that the sensitivity of the factors affecting the gas capture capacity of CO2 decreases in the order of formation stress, temperature, residual gas saturation, horizontal permeability, and porosity. Meanwhile, the sensitivity of the factors affecting the dissolution capture capacity of CO2 decreases in the order of formation stress, residual gas saturation, temperature, horizontal permeability, and porosity. The sensitivity of the influencing factors can serve as the basis for carrying out a reasonable assessment of sites for future CO2 storage areas and for optimizing the design of existing CO2 storage areas. The sensitivity analysis of the influencing factors will provide basic data and technical support for implementing geologic CO2 storage and will assist in improving geologic CO2 storage technologies to achieve China’s carbon neutralization goal.©2022 China Geology Editorial Office.  相似文献   

8.
We use a reactive diffusion model to investigate what happens to CO2 injected into a subsurface sandstone reservoir capped by a chlorite- and illite-containing shale seal. The calculations simulate reaction and transport of supercritical (SC) CO2 at 348.15 K and 30 MPa up to 20,000 a. Given the low shale porosity (5%), chemical reactions mostly occurred in the sandstone for the first 2000 a with some precipitation at the ss/sh interface. From 2000 to 4000 a, ankerite, dolomite and illite began replacing Mg–Fe chlorite at the sandstone/shale interface. Transformation of chlorite to ankerite is the dominant reaction occluding the shale porosity in most simulations: from 4000 to 7500 a, this carbonation seals the reservoir and terminates reaction. Overall, the carbonates (calcite, ankerite, dolomite), chlorite and goethite all remain close to local chemical equilibrium with brine. Quartz is almost inert from the point of its dissolution/precipitation. However, the rate of quartz reaction controls the long-term decline in aqueous silica activity and its evolution toward equilibrium. The reactions of feldspars and clays depend strongly on their reaction rate constants (microcline is closer to local equilibrium than albite). The timing of porosity occlusion mostly therefore depends on the kinetic constants of kaolinite and illite. For example, an increase in the kaolinite kinetic constant by 0.25 logarithmic units hastened porosity closure by 4300 a. The earliest simulated closure of porosity occurred at approximately 108 a for simulations designed as sensitivity tests for the rate constants.These simulations also emphasize that the rate of CO2 immobilization as aqueous bicarbonate (solubility trapping) or as carbonate minerals (mineral trapping) in sandstone reservoirs depends upon reaction kinetics – but the relative fraction of each trapped CO2 species only depends upon the initial chemical composition of the host sandstone. For example, at the point of porosity occlusion the fraction of bicarbonate remaining in solution depends upon the initial Na and K content in the host rock but the fraction of carbonate mineralization depends only on the Ca, Mg, Fe content. Since ankerite is the dominant mineral that occludes porosity, the dissolved concentration of ferrous iron is also an important parameter. Future efforts should focus on cross-comparisons and ground-truthing of simulations made for standard case studies as well as laboratory measurements of the reactivities of clay minerals.  相似文献   

9.
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   

10.
Sequestration of CO2 into a deep geological reservoir causes a complex interaction of different processes such as multiphase flow, phase transition, multicomponent transport, and geochemical reactions between dissolved CO2 and the mineral matrix of the porous medium. A prognosis of the reservoir behaviour and the feedback from large-scale geochemical alterations require efficient process-based numerical models. For this purpose, the multiphase flow and multicomponent transport code OpenGeoSys-Eclipse have been coupled to the geochemical model ChemApp. The newly developed coupled simulator was successfully verified for correctness and accuracy of the implemented reaction module by benchmarking tests. The code was then applied to assess the impact of geochemical reactions during CO2 sequestration at a hypothetical but typical Bunter sandstone formation in the Northern German Basin. Injection and spreading of 1.48 × 107 t of CO2 in an anticline structure of the reservoir were simulated over a period of 20 years of injection plus 80 years of post-injection time. Equilibrium geochemical calculations performed by ChemApp show only a low reactivity to the geochemical system. The increased acidity of the aqueous solution results in dissolution of small amounts of calcite, anhydrite, and quartz. Geochemical alterations of the mineral phase composition result in slight increases in porosity and permeability, which locally may reach up to +0.02 and 0.1 %, respectively.  相似文献   

11.
The aim of this experimental study was to evaluate and compare the geochemical impact of pure and impure CO2 on rock forming minerals of possible CO2 storage reservoirs. This geochemical approach takes into account the incomplete purification of industrial captured CO2 and the related effects during injection, and provides relevant data for long-term storage simulations of this specific greenhouse gas. Batch experiments were conducted to investigate the interactions of supercritical CO2, brine and rock-forming mineral concentrates (albite, microcline, kaolinite, biotite, muscovite, calcite, dolomite and anhydrite) using a newly developed experimental setup. After up to 42 day (1000 h) experiments using pure and impure supercritical CO2 the dissolution and solution characteristics were examined by XRD, XRF, SEM and EDS for the solid, and ICP–MS and IC for the fluid reactants, respectively. Experiments with mixtures of supercritical CO2 (99.5 vol.%) and SO2 or NO2 impurities (0.5 vol.%) suggest the formation of H2SO4 and HNO3, reflected in pH values between 1 and 4 for experiments with silicates and anhydrite and between 5 and 6 for experiments with carbonates. These acids should be responsible for the general larger amount of cations dissolved from the mineral phases compared to experiments using pure CO2. For pure CO2 a pH of around 4 was obtained using silicates and anhydrite, and 7–8 for carbonates. Dissolution of carbonates was observed after both pure and impure CO2 experiments. Anhydrite was corroded by approximately 50 wt.% and gypsum precipitated during experiments with supercritical CO2 + NO2. Silicates do not exhibit visible alterations during all experiments but released an increasing amount of cations in the reaction fluid during experiments with impure CO2. Nonetheless, precipitated secondary carbonates could not be identified.  相似文献   

12.
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   

13.
《Applied Geochemistry》2005,20(6):1131-1157
The Weyburn Oil Field is a carbonate reservoir in south central Saskatchewan, Canada and is the site of a large CO2 injection project for purposes of enhanced oil recovery. The Weyburn Field, in the Mississippian Midale Formation, was discovered in 1954 and was under primary production until secondary recovery by water flood began in 1964. The reservoir comprises two units, the Vuggy and the Marly, and primary and secondary recovery are thought to only have significantly depleted the Vuggy zone, leaving the Marly with higher oil saturations. In 2000, PanCanadian Resources (now EnCana), the operator of the field, began tertiary recovery by injection of CO2 and water, primarily into the Marly. The advent of this project was an opportunity to study the potential for geological storage of CO2.Using 43 Baseline samples collected in August 2000, before CO2 injection at Weyburn, and 44 monitoring samples collected in March 2001, changes in the fluid chemistry and isotope composition have been tracked. The initial fluid distribution showed water from discovery through water flood in the Midale Formation with Cl ranging from 25,000 to 60,000 mg/L, from the NW to the SE across the Phase 1A area. By the time of Baseline sampling the produced water had been diluted to Cl of 25,000–50,000 mg/L as a result of the addition of make up water from the low TDS Blairmore Formation, but the pattern of distribution was still present. The Cl distribution is mimicked by the distribution of other dissolved ions and variables, with Ca (1250–1500 mg/L) and NH3 (aq) increasing from NW to SE, and alkalinity (700–300 mg/L), resistivity, and H2S (300–100 mg/L) decreasing. Based on chemical and isotopic data, the H2S is interpreted to result from bacterial SO4 reduction. After 6 months of injection of CO2, the general patterns are changed very little, except that the pH has decreased by 0.5 units and alkalinity has increased, with values over 1400 mg/L in the NW, decreasing to 500 mg/L in the SE. Calcium has increased to range from 1250 to 1750 mg/L, but the pattern of NW–SE distribution is altered. Chemical and isotopic data suggest this change in distribution is caused by the dissolution of calcite due to water–rock reactions driven by CO2. The Baseline samples varied from −22 to −12‰ δ13C (V-PDB) for CO2 gas. The injected CO2 has an isotope ratio of −20‰. The Monitor-1 samples of produced CO2 ranged from −18 to −13‰, requiring a heavy source of C, most easily attributed to dissolution of carbonate minerals. Field measured pH had increased and alkalinity had decreased by the second monitoring trip (July 2001) to near Baseline values, suggesting continued reaction with reservoir minerals.Addition of CO2 to water–rock mixtures comprising carbonate minerals causes dissolution of carbonates and production of alkalinity. Geochemical modeling suggests dissolution is taking place, however more detail on water–oil–gas ratios needs to be gathered to obtain more accurate estimates of pH at the formation level. Geological storage of CO2 relies on the potential that, over the longer term, silicate minerals will buffer the pH, causing any added CO2 to be precipitated as calcite. Some initial modeling of water–rock reactions suggests that silica sources are available to the water resident in the Midale Formation, and that clay minerals may well be capable of acting as pH buffers, allowing injected CO2 to be stored as carbonate minerals. Further work is underway to document the mineralogy of the Midale Formation and associated units so as to define more accurately the potential for geological storage.  相似文献   

14.
Geochemical interactions of brine–rock–gas have a significant impact on the stability and integrity of the caprock for long-term CO2 geological storage. Invasion of CO2 into the caprock from the storage reservoir by (1) molecular diffusion of dissolved CO2, (2) CO2-water two-phase flow after capillary breakthrough, and (3) CO2 flow through existing open fractures may alter the mineralogy, porosity, and mechanical strength of the caprock due to the mineral dissolution or precipitation. This determines the self-enhancement or self-sealing efficiency of the caprock. In this paper, two types of caprock, a clay-rich shale and a mudstone, are considered for the modeling analyses of the self-sealing and self-enhancement phenomena. The clay-rich shale taken from the Jianghan Basin of China is used as the base-case model. The results are compared with a mudstone caprock which is compositionally very different than the clay-rich shale. We focus on mineral alterations induced by the invasion of CO2, feedback on medium properties such as porosity, and the self-sealing efficiency of the caprock. A number of sensitivity simulations are performed using the multiphase reactive transport code TOUGHREACT to identify the major minerals that have an impact on the caprock’s self-sealing efficiency. Our model results indicate that under the same hydrogeological conditions, the mudstone is more suitable to be used as a caprock. The sealing distances are barely different in the two types of caprock, both being about 0.6 m far from the interface between the reservoir and caprock. However, the times of occurrence of sealing are considerably different. For the mudstone model, the self-sealing occurs at the beginning of simulation, while for the clay-rich shale model, the porosity begins to decline only after 100 years. At the bottom of the clay-rich shale column, the porosity declines to 0.034, while that of mudstone declines to 0.02. The sensitive minerals in the clay-rich shale model are calcite, magnesite, and smectite-Ca. Anhydrite and illite provide Ca2+ and Mg2+ to the sensitive minerals for their precipitation. The mudstone model simulation is divided into three stages. There are different governing minerals in different stages, and the effect of the reservoir formation water on the alteration of sensitive minerals is significant.  相似文献   

15.
A detailed study of the chemical composition of the groundwater surrounding the Mt. Hekla volcano in south Iceland was performed to assess fluid evolution and toxic metal mobility during CO2-rich fluid basalt interaction. These fluids provide a natural analogue for evaluating the consequences of CO2 sequestration in basalt. The concentration of dissolved inorganic C in these groundwaters decreases from 3.88 to 0.746 mmol/kg with increasing basalt dissolution while the pH increases from 6.9 to 9.2. This observation provides direct evidence of the potential for basalt dissolution to sequester CO2. Reaction path calculations suggest that dolomite and calcite precipitation is largely responsible for this drop in groundwater dissolved C concentration. The concentrations of toxic metal(loid)s in the waters are low, for example the maximum measured concentrations of Cd, As and Pb were 0.09, 22.8 and 0.06 nmol/kg, respectively. Reaction path modelling indicates that although many toxic metals may be initially liberated by the dissolution of basalt by acidic CO2-rich solutions, these metals are reincorporated into solid phases as the groundwaters are neutralized by continued basalt dissolution. The identity of the secondary toxic metal bearing phases depends on the metal. For example, calculations suggest that Sr and Ba are incorporated into carbonates, while Pb, Zn and Cd are incorporated into Fe (oxy)hydroxide phases.  相似文献   

16.
Geological sequestration of CO2 into depleted hydrocarbon reserviors or saline aquifers presents the enormous potential to reduce greenhouse gas emission from fossil fuels. However, it may give rise to a complicated coupling physical and chemical process. One of the processes is the hydro-mechanical impact of CO2 injection. During the injection project, the increase of pore pressures of storing formations can induce the instability, which finally results in a catastrophic failure of disposal sites. This paper focuses mainly on the role of CO2-saturated water in the fracturing behavior of rocks. To investigate how much the dissolved CO2 can influence the pore pressure change of rocks, acoustic emission (AE) experiments were performed on sandstone and granite samples under triaxial conditions. The main innovation of this paper is to propose a time dependent porosity method to simulate the abrupt failure process, which is observed in the laboratory and induced by the pore pressure change due to the volume dilatancy of rocks, using a finite element scheme associated with two-phase characteristics. The results successfully explained the phenomena obtained in the physical experiments.  相似文献   

17.
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   

18.
To assess CO2 underground sequestration from a geochemical viewpoint, the anorthite dissolution rate, which is an important parameter of risk analysis, was measured in a CO2–water system. The authors sought to obtain precise dissolution rate data in a short time observing a crystal surface on a nanoscale. For this purpose, phase-shift interferometry was applied. Using this method, uncertainty of the reactive surface area that is imparted on calculation of the dissolution rate constant can also be avoided. The time-course profile of vertical retreat of the surface revealed that the anorthite dissolution process changes from the initial transient state to a later steady state, which is consistent with results of numerous precedent studies. The transient dissolution rate depends strongly on local features (e.g., density of defects, variation of chemical compositions) of the crystal surface, rather than on temperature. Therefore, it is very important to determine the original properties of the anorthite surface for the examination of subsequent dissolution process. Contrary to general expectations, the anorthite dissolution can alter the physical properties of reservoir rock immediately after CO2 injection. The simple estimation using the anorthite dissolution rate obtained in this study, which was done as a test case for the CO2 underground sequestration project conducted by RITE, revealed that porosity of reservoir rock increased about 2% (23–23.4%) of initial values during 60 a. That change in physical property in such a short time might enhance the diffusion of injected CO2 and formation water, and therefore accelerate further geochemical reactions. Results of this study demonstrate that the geochemical water–rock interaction, which is generally regarded as a longer-term phenomenon than various physical processes, can also affect the reservoir system from the initial stage.  相似文献   

19.
Safety assessment of geosequestration of CO2 into deep saline aquifers requires a precise understanding of the study of hydro‐chemo‐mechanical couplings occurring in the rocks and the cement well. To this aim, a coupled chemo‐poromechanical model has been developed and implemented into a research code well‐suited to the resolution of fully coupled problems. This code is based on the finite volume methods. In a 1D axisymmetrical configuration, this study aims to simulate the chemo‐poromechanical behaviour of a system composed by the cement well and the caprock during CO2 injection. Major chemical reactions of carbonation occurring into cement paste and rocks are considered in order to evaluate the consequences of the presence of CO2 on the amount of dissolved matrix and precipitated calcium carbonates. The dissolution of the solid matrix is taken into account through the use of a chemical porosity. Matrix leaching and carbonation lead, as expected, to important variations of porosity, permeability and to alterations of transport properties and mechanical stiffness. These results justify the importance of considering a coupled analysis accounting for the main chemical reactions. It is worth noting that the modelling framework proposed in the present study could be extended to model the chemo‐poromechanical behaviour of the reservoir rock and the caprock when subjected to the presence of an acidic pore fluid (CO2‐rich brine). Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   

20.
Carbon dioxide enhanced oil recovery (CO2-EOR) has been widely applied to the process of carbon capture, utilization, and storage (CCUS). Here, we investigate CO2–oil–water–rock interactions under reservoir conditions (100 °C and 24 MPa) in order to understand the fluid–rock interactions following termination of a CO2-EOR project. Our experimental results show that CO2-rich fluid remained the active fluid controlling the dissolution–precipitation processes in an oil-undersaturated sandstone reservoir; e.g., the dissolution of feldspar and calcite, and the precipitation of kaolinite as well as solid phases comprising O, Si, Al, Na, C, and Ti. Mineral dissolution rates were reduced in the case that mineral surfaces were coated by oil. Mineral wettability and composition, and oil saturation were the main controls on the exposed surface area of grains, and mineral wettability in particular led to selective dissolution. In addition, the permeability of the reservoir decreased substantially due to the precipitation of kaolinite and solid-phase particles, and due to the clogging of less soluble mineral particles released by the dissolution of K-feldspar and carbonate cement, whereas porosity increased. The results provide insight into potential formation damage resulting from CO2-EOR projects.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号