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1.
《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   

2.
Geologic carbon sequestration is the capture of anthropogenic carbon dioxide (CO2) and its storage in deep geologic formations. The processes of CO2 seepage into surface water after migration through water-saturated sediments are reviewed. Natural CO2 and CH4 fluxes are pervasive in surface-water environments and are good analogues to potential leakage and seepage of CO2. Buoyancy-driven bubble rise in surface water reaches a maximum velocity of approximately 30 cm s−1. CO2 rise in saturated porous media tends to occur as channel flow rather than bubble flow. A comparison of ebullition versus dispersive gas transport for CO2 and CH4 shows that bubble flow will dominate over dispersion in surface water. Gaseous CO2 solubility in variable-salinity waters decreases as pressure decreases leading to greater likelihood of ebullition and bubble flow in surface water as CO2 migrates upward.  相似文献   

3.
A screening and ranking framework (SRF) has been developed to evaluate potential geologic carbon dioxide (CO2) storage sites on the basis of health, safety, and environmental (HSE) risk arising from CO2 leakage. The approach is based on the assumption that CO2 leakage risk is dependent on three basic characteristics of a geologic CO2 storage site: (1) the potential for primary containment by the target formation; (2) the potential for secondary containment if the primary formation leaks; and (3) the potential for attenuation and dispersion of leaking CO2 if the primary formation leaks and secondary containment fails. The framework is implemented in a spreadsheet in which users enter numerical scores representing expert opinions or published information along with estimates of uncertainty. Applications to three sites in California demonstrate the approach. Refinements and extensions are possible through the use of more detailed data or model results in place of property proxies.  相似文献   

4.
Instances of gas leakage from naturally occurring CO2 reservoirs and natural gas storage sites serve as analogues for the potential release of CO2 from geologic storage sites. This paper summarizes and compares the features, events, and processes that can be identified from these analogues, which include both naturally occurring releases and those associated with industrial processes. The following conclusions are drawn: (1) carbon dioxide can accumulate beneath, and be released from, primary and secondary shallower reservoirs with capping units located at a wide range of depths; (2) many natural releases of CO2 are correlated with a specific event that triggered the release; (3) unsealed fault and fracture zones may act as conduits for CO2 flow from depth to the surface; (4) improperly constructed or abandoned wells can rapidly release large quantities of CO2; (5) the types of CO2 release at the surface vary widely between and within different leakage sites; (6) the hazard to human health was small in most cases, possibly because of implementation of post-leakage public education and monitoring programs; (7) while changes in groundwater chemistry were related to CO2 leakage, waters often remained potable. Lessons learned for risk assessment associated with geologic carbon sequestration are discussed. Electronic supplementary material Supplementary material is available in the online version of this article at and is accessible for authorized users.  相似文献   

5.
Careful site characterization is critical for successful geologic storage of carbon dioxide (CO2) because of the many physical and chemical processes impacting CO2 movement and containment under field conditions. Traditional site characterization techniques such as geological mapping, geophysical imaging, well logging, core analyses, and hydraulic well testing provide the basis for judging whether or not a site is suitable for CO2 storage. However, only through the injection and monitoring of CO2 itself can the coupling between buoyancy flow, geologic heterogeneity, and history-dependent multi-phase flow effects be observed and quantified. CO2 injection and monitoring can therefore provide a valuable addition to the site-characterization process. Additionally, careful monitoring and verification of CO2 plume development during the early stages of commercial operation should be performed to assess storage potential and demonstrate permanence. The Frio brine pilot, a research project located in Dayton, Texas (USA) is used as a case study to illustrate the concept of an iterative sequence in which traditional site characterization is used to prepare for CO2 injection and then CO2 injection itself is used to further site-characterization efforts, constrain geologic storage potential, and validate understanding of geochemical and hydrological processes. At the Frio brine pilot, in addition to traditional site-characterization techniques, CO2 movement in the subsurface is monitored by sampling fluid at an observation well, running CO2-saturation-sensitive well logs periodically in both injection and observation wells, imaging with crosswell seismic in the plane between the injection and observation wells, and obtaining vertical seismic profiles to monitor the CO2 plume as it migrates beyond the immediate vicinity of the wells. Numerical modeling plays a central role in integrating geological, geophysical, and hydrological field observations.  相似文献   

6.
Carbon Capture and Storage (CCS) is one of the effective means to deal with global warming, and saline aquifer storage is considered to be the most promising storage method. Junggar Basin, located in the northern part of Xinjiang and with a large distribution area of saline aquifer, is an effective carbon storage site. Based on well logging data and 2D seismic data, a 3D heterogeneous geological model of the Cretaceous Donggou Formation reservoir near D7 well was constructed, and dynamic simulations under two scenarios of single-well injection and multi-well injection were carried out to explore the storage potential and CO2 storage mechanism of deep saline aquifer with real geological conditions in this study. The results show that within 100 km2 of the saline aquifer of Donggou Formation in the vicinity of D7 well, the theoretical static CO2 storage is 71.967 × 106 tons (P50)①, and the maximum dynamic CO2 storage is 145.295 × 106 tons (Case2). The heterogeneity of saline aquifer has a great influence on the spatial distribution of CO2 in the reservoir. The multi-well injection scenario is conducive to the efficient utilization of reservoir space and safer for storage. Based on the results from theoretical static calculation and the dynamic simulation, the effective coefficient of CO2 storage in deep saline aquifer in the eastern part of Xinjiang is recommended to be 4.9%. This study can be applied to the engineering practice of CO2 sequestration in the deep saline aquifer in Xinjiang.  相似文献   

7.
Dissolution of CO2 into deep subsurface brines for carbon sequestration is regarded as one of the few viable means of reducing the amount of CO2 entering the atmosphere. Ions in solution partially control the amount of CO2 that dissolves, but the mechanisms of the ion's influence are not clearly understood and thus CO2 solubility is difficult to predict. In this study, CO2 solubility was experimentally determined in water, NaCl, CaCl2, Na2SO4, and NaHCO3 solutions and a mixed brine similar to the Bravo Dome natural CO2 reservoir; ionic strengths ranged up to 3.4 molal, temperatures to 140 °C, and CO2 pressures to 35.5 MPa. Increasing ionic strength decreased CO2 solubility for all solutions when the salt type remained unchanged, but ionic strength was a poor predictor of CO2 solubility in solutions with different salts. A new equation was developed to use ion hydration number to calculate the concentration of electrostricted water molecules in solution. Dissolved CO2 was strongly correlated (R2 = 0.96) to electrostricted water concentration. Strong correlations were also identified between CO2 solubility and hydration enthalpy and hydration entropy. These linear correlation equations predicted CO2 solubility within 1% of the Bravo Dome brine and within 10% of two mixed brines from literature (a 10 wt % NaCl + KCl + CaCl2 brine and a natural Na+, Ca2+, Cl− type brine with minor amounts of Mg2+, K+, Sr2+ and Br−).  相似文献   

8.
Release of CO2 from surface ocean water owing to precipitation of CaCO3 and the imbalance between biological production of organic matter and its respiration, and their net removal from surface water to sedimentary storage was studied by means of a quotient θ = (CO2 flux to the atmosphere)/(CaCO3 precipitated). θ depends not only on water temperature and atmospheric CO2 concentration but also on the CaCO3 and organic carbon masses formed. In CO2 generation by CaCO3 precipitation, θ varies from a fraction of 0.44 to 0.79, increasing with decreasing temperature (25 to 5°C), increasing atmospheric CO2 concentration (195–375 ppmv), and increasing CaCO3 precipitated mass (up to 45% of the initial DIC concentration in surface water). Primary production and net storage of organic carbon counteracts the CO2 production by carbonate precipitation and it results in lower CO2 emissions from the surface layer. When atmospheric CO2 increases due to the ocean-to-atmosphere flux rather than remaining constant, the amount of CO2 transferred is a non-linear function of the surface layer thickness because of the back-pressure of the rising atmospheric CO2. For a surface ocean layer approximated by a 50-m-thick euphotic zone that receives input of inorganic and organic carbon from land, the calculated CO2 flux to the atmosphere is a function of the CaCO3 and Corg net storage rates. In general, the carbonate storage rate has been greater than that of organic carbon. The CO2 flux near the Last Glacial Maximum is 17 to 7×1012 mol/yr (0.2–0.08 Gt C/yr), reflecting the range of organic carbon storage rates in sediments, and for pre-industrial time it is 38–42×1012 mol/yr (0.46–0.50 Gt C/yr). Within the imbalanced global carbon cycle, our estimates indicate that prior to anthropogenic emissions of CO2 to the atmosphere the land organic reservoir was gaining carbon and the surface ocean was losing carbon, calcium, and total alkalinity owing to the CaCO3 storage and consequent emission of CO2. These results are in agreement with the conclusions of a number of other investigators. As the CO2 uptake in mineral weathering is a major flux in the global carbon cycle, the CO2 weathering pathway that originates in the CO2 produced by remineralization of soil humus rather than by direct uptake from the atmosphere may reduce the relatively large imbalances of the atmosphere and land organic reservoir at 102–104-year time scales.  相似文献   

9.
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   

10.
Assessing the influence of CO2 on soil and aquifer geochemistry is a task of increasing interest when considering risk assessment for geologic carbon sequestration. Leakage and CO2 ascent can lead to soil acidification and mobilization of potentially toxic metals and metalloids due to desorption or dissolution reactions. We studied the CO2 influence on an Fe(III) (oxyhydr)oxide rich, gleyic Fluvisol sampled in close vicinity to a Czech mofette site and compared the short-term CO2 influence in laboratory experiments with observations on long-term influence at the natural site. Six week batch experiments with/without CO2 gas flow at 3 different temperatures and monitoring of liquid phase metal(loid) concentrations revealed two main short-term mobilization processes. Within 1 h to 1 d after CO2 addition, mobilization of weakly adsorbed metal cations occurred due to surface protonation, most pronounced for Mn (2.5–3.3 fold concentration increase, mobilization rates up to 278 ± 18 μg Mn kgsoil−1 d−1) and strongest at low temperatures. However, total metal(loid) mobilization by abiotic desorption was low. After 1–3 d significant Fe mobilization due to microbially-triggered Fe(III) (oxyhydr)oxide dissolution began and continued throughout the experiment (up to 111 ± 24 fold increase or up to 1.9 ± 0.6 mg Fe kgsoil−1 d−1). Rates increased at higher temperature and with a higher content of organic matter. The Fe(III) mineral dissolution was coupled to co-release of incorporated metal(loid)s, shown for As (up to 16 ± 7 fold, 11 ± 8 μg As kgsoil−1 d−1). At high organic matter content, re-immobilization due to resorption reactions could be observed for Cu. The already low pH (4.5–5.0) did not change significantly during Fe(III) reduction due to buffering from sorption and dissolution reactions, but a drop in redox potential (from > +500 mV to minimum +340 ± 20 mV) occurred due to oxygen depletion. We conclude that microbial processes following CO2 induction into a soil can contribute significantly to metal(loid) mobilization, especially at optimal microbial growth conditions (moderate temperature, high organic carbon content) and should be considered for carbon sequestration monitoring and risk assessment.  相似文献   

11.

Background

Reactive-transport simulation is a tool that is being used to estimate long-term trapping of CO2, and wellbore and cap rock integrity for geologic CO2 storage. We reacted end member components of a heterolithic sandstone and shale unit that forms the upper section of the In Salah Gas Project carbon storage reservoir in Krechba, Algeria with supercritical CO2, brine, and with/without cement at reservoir conditions to develop experimentally constrained geochemical models for use in reactive transport simulations.

Results

We observe marked changes in solution composition when CO2 reacted with cement, sandstone, and shale components at reservoir conditions. The geochemical model for the reaction of sandstone and shale with CO2 and brine is a simple one in which albite, chlorite, illite and carbonate minerals partially dissolve and boehmite, smectite, and amorphous silica precipitate. The geochemical model for the wellbore environment is also fairly simple, in which alkaline cements and rock react with CO2-rich brines to form an Fe containing calcite, amorphous silica, smectite and boehmite or amorphous Al(OH)3.

Conclusions

Our research shows that relatively simple geochemical models can describe the dominant reactions that are likely to occur when CO2 is stored in deep saline aquifers sealed with overlying shale cap rocks, as well as the dominant reactions for cement carbonation at the wellbore interface.  相似文献   

12.
Arctic soils contain a large fraction of Earth’s stored carbon. Temperature increases in the Arctic may enhance decomposition of this stored carbon, shifting the role of Arctic soils from a net sink to a new source of atmospheric CO2. Predicting the impact of Arctic warming on soil carbon reserves requires knowledge of the composition of the stored organic matter. Here, we employ solid state 13C nuclear magnetic resonance (NMR) spectroscopy and Fourier transform infrared-photoacoustic spectroscopy (FTIR-PAS) to investigate the chemical composition of soil organic matter collected from drained thaw-lake basins ranging in age from 0 to 5500 years before present (y BP). The 13C NMR and FTIR-PAS data were largely congruent. Surface horizons contain relatively large amounts of O-alkyl carbon, suggesting that the soil organic matter is rich in labile constituents. Soil organic matter decreases with depth with the relative amounts of O-alkyl carbon decreasing and aromatic carbon increasing. These data indicate that lower horizons are in a more advanced stage of decomposition than upper horizons. Nonetheless, a substantial fraction of carbon in lower horizons, even for ancient thaw-lake basins (2000-5500 y BP), is present as O-alkyl carbon reflecting the preservation of intrinsically labile organic matter constituents. Climate change-induced increases in the depth of the soil active layer are expected to accelerate the depletion of this carbon.  相似文献   

13.
The capture and geological storage of CO2 can be used to reduce anthropogenic greenhouse gas emissions. To assess the environmental impact of potential CO2 leakage from deep storage reservoirs on the abundance and functional diversity of microorganisms in near-surface terrestrial environments, a natural CO2 vent (>90% CO2 in the soil gas) was studied as an analogue. The microbial communities were investigated using lipid biomarkers combined with compound-specific stable carbon isotope analyses, the determination of microbial activities, and the use of quantitative polymerase chain reactions (Q-PCR). With this complementary set of methods, significant differences between the CO2-rich vent and a reference site with a normal CO2 concentration were detected. The δ13C values of the plant and microbial lipids within the CO2 vent demonstrate that substantial amounts of geothermal CO2 were incorporated into the microbial, plant, and soil carbon pools. Moreover, the numbers of Archaea and Bacteria were highest at the reference site and substantially lower at the CO2 vent. Lipid biomarker analyses, Q-PCR, and the determination of microbial activities showed the presence of CO2-utilising methanogenic Archaea, Geobacteraceae, and sulphate-reducing Bacteria (SRB) mainly at the CO2 vent, only minor quantities were found at the reference site. Stable carbon isotopic analyses revealed that the methanogenic Archaea and SRB utilised the vent-derived CO2 for assimilatory biosynthesis. Our results show a shift in the microbial community towards anaerobic and acidophilic microorganisms as a consequence of the long-term exposure of the soil environment to high CO2 concentrations.  相似文献   

14.
The carbon isotopic composition of CO2 inclusions trapped in minerals reflects the origin and evolution of CO2-bearing fluids and melts, and records the multiple-stages carbon geodynamic cycle, as CO2 took part in various geological processes widely. However, the practical method for determination isotope composition of individual CO2 inclusion is still lacking. Developing a microanalytical technique with spatial resolution in micrometers to precisely determinate the δ13C value of individual CO2 inclusion, will make it possible to analyze a tiny portion of a zoning mineral crystal, distinguish the differences in micro-scale, and possible to find many useful information that could not be obtained with the bulk extraction and analysis techniques. In this study, we systematically collected Raman spectra of CO2 standards with different δ13C values (?34.9 ‰ to 3.58 ‰) at 32.0 °C and from ～7.0 MPa to 120.0 MPa, and developed a new procedure to precisely determinate the δ13C value of individual CO2 inclusion. We investigated the relationship among the Raman peak intensity ratio, δ13C value, and CO2 density, and established a calibration model with high accuracy (0.5 ‰?1.5 ‰), sufficient for geological application to distinguish different source of CO2 with varying δ13CO2. As a demonstration, we measured the δ13C values and the density of CO2 inclusions in the growth zones of alkali basalt-hosted corundum megacrysts from Changle, Shandong Province. We found the significant differences of density and δ13C between the CO2 inclusions in the core of corundum and those inclusions in the outer growth zones, the δ13C value decreases from core to rim with decreasing density: δ13C values are from ?7.5 ‰ to ?9.2 ‰ for the inclusions in the core, indicating the corundum core was crystallized from mantle-derived magmas; from ?13.5 ‰ to ?18.5 ‰ for CO2 inclusions in zone 1 and from ?16.5 ‰ to –22.0 ‰ for inclusions in zone 2, indicating the outer zones of corundum grew in a low δ13C value environment, resulted from an infilling of low δ13C value fluid and/or degassing of the ascending basaltic magma.  相似文献   

15.
Structural traps like anticline structures are preferred for carbon dioxide sequestration as they limit lateral spreading of CO2 and thus provide localized storage. This study, therefore, assesses strategies for maximizing storage of CO2 using as hypothetical but realistic storage site a typical anticline structure in the North German sedimentary basin. Scenario simulations are performed to investigate the effects of well number, location, spacing and alignment, using fracture pressure and containment of CO2 within the anticline as constraining factors. Scenarios are ranked by stored CO2 mass, pressure increase due to injection and CO2 immobilized by dissolution or residual trapping. It is found that pressure overlap from different injectors influences CO2 migration considerably, limiting the storable amount to about 150 Mt, which represents half of the static capacity estimate.  相似文献   

16.
Subsurface sequestration of CO2 in oil and gas provinces where permanence of hydrocarbon accumulations has proven the reliability of potential traps is rightly seen as a solid option for containment of CO2 atmospheric concentrations. However, one of the most promising provinces for carbon storage in North America, the Texas Gulf Coast, has also been heavily drilled for more than a century, puncturing many otherwise perfectly sound seals (>125,000 wells over ~50,000 km2). As a result, boreholes and, in particular, older abandoned wells could be major leakage pathways for sequestered CO2. This article presents statistics on well spatial and depth distribution that have been drawn from public domain sources and relates these data to historical plugging and abandonment regulations in the Texas Gulf Coast. Surface-well density averages of 2.4 wells/km2 can be locally much higher—but also much lower in larger areas. Average well penetration density drops to 0.27 and 0.05 well/km2 below a depth of 2,440 and 3,660 m, respectively. Natural mitigating factors such as thief zones and heaving “shales” could also play a role in limiting the impact of these direct conduits to the shallow subsurface and surface.  相似文献   

17.
Soils act as sources and sinks for greenhouse gases (GHG) such as carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O). Since both storage and emission capacities may be large, precise quantifications are needed to obtain reliable global budgets that are necessary for land-use management (agriculture, forestry), global change and for climate research. This paper discusses exclusively the soil emission-related processes and their influencing parameters. It reviews soil emission studies involving the most important land-cover types and climate zones and introduces important measuring systems for soil emissions. It addresses current shortcomings and the obvious bias towards northern hemispheric data.When using a conservative average of 300 mg CO2e m−2 h−1 (based on our literature review), this leads to global annual net soil emissions of ≥350 Pg CO2e (CO2e = CO2 equivalents = total effect of all GHG normalized to CO2). This corresponds to roughly 21% of the global soil C and N pools. For comparison, 33.4 Pg CO2 are being emitted annually by fossil fuel combustion and the cement industry.  相似文献   

18.
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   

19.
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   

20.
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   

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