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1.
Carbon dioxide enhanced oil recovery (CO 2-EOR) has been widely applied to the process of carbon capture, utilization, and storage (CCUS). Here, we investigate CO 2–oil–water–rock interactions under reservoir conditions (100 °C and 24 MPa) in order to understand the fluid–rock interactions following termination of a CO 2-EOR project. Our experimental results show that CO 2-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 CO 2-EOR projects. 相似文献
2.
We define and calibrate a new model of molar volume as a function of pressure, temperature, ordering state, and composition for spinels in the supersystem (Mg, Fe 2+)(Al, Cr, Fe 3+) 2O 4 ? (Mg, Fe 2+) 2TiO 4. We use 832 X-ray and neutron diffraction measurements performed on spinels at ambient and in situ high- P, T conditions to calibrate end-member equations of state and an excess volume model for this system. The effect on molar volume of cation ordering over the octahedral and tetrahedral sites is captured with linear dependence on Mg 2+, Al 3+, and Fe 3+ site occupancy terms. We allow standard-state volumes and coefficients of thermal expansion of the end members to vary within their uncertainties during extraction of the mixing properties, in order to achieve the best fit. Published equations of state of the various spinel end members are analyzed to obtain optimal values of the bulk modulus and its pressure derivative, for each explicit end member. For any spinel composition in the supersystem, the model molar volume is obtained by adding excess volume and cation order-dependent terms to a linear combination of the five end-member volumes, estimated at pressure and temperature using the high- T Vinet equation of state. The preferred model has a total of 9 excess volume and order-dependent parameters and fits nearly all experiments to within 0.02 J/bar/mol, or better than 0.5 % in volume. The model is compared to the current MELTS spinel model with a demonstration of the impact of the model difference on the estimated spinel-garnet lherzolite transition pressure. 相似文献
3.
Saturation index with respect to calcite (SIc) and equilibrium CO 2 partial pressure are important parameters to study groundwater in limestone aquifers. Aside from their use in time series, CO 2 and SIc are used to estimate the baseline of CO 2 in the vadose zone. The objective of this paper is to present conceptual examples on the use of the CO 2–SIc relationship to have new information from usual parameters. Case study was considered as an example of use from Cussac site, a limestone aquifer in southwest of France. The result showed that CO 2 baseline in unsaturated zone is found close to 25,000 ± 1,000 ppm. 相似文献
4.
The type and kinetics of metamorphic CO 2-producing processes in metacarbonate rocks is of importance to understand the nature and magnitude of orogenic CO 2 cycle. This paper focuses on CO 2 production by garnet-forming reactions occurring in calc-silicate rocks. Phase equilibria in the CaO–FeO–Al 2O 3–SiO 2–CO 2–H 2O (CFAS–CO 2–H 2O) system are investigated using P– T phase diagrams at fixed fluid composition, isobaric T– X(CO 2) phase diagram sections and phase diagram projections in which fluid composition is unconstrained. The relevance of the CFAS–CO 2–H 2O garnet-bearing equilibria during metamorphic evolution of calc-silicate rocks is discussed in the light of the observed microstructures and measured mineral compositions in two representative samples of calc-silicate rocks from eastern Nepal Himalaya. The results of this study demonstrate that calc-silicate rocks may act as a significant CO 2 source during prograde heating and/or early decompression. However, if the system remains closed, fluid–rock interactions may induce hydration of the calc-silicate assemblages and the in situ precipitation of graphite. The interplay between these two contrasting processes (production of CO 2-rich fluids vs. carbon sequestration through graphite precipitation) must be considered when dealing with a global estimate of the role exerted by decarbonation processes on the orogenic CO 2 cycle. 相似文献
5.
We present the results of a series of density experiments in the system O–S–Fe–Ni–Cu. These experiments were designed to extend
our understanding of the physical properties of sulfide liquids, and to extend one-bar thermochemical models for sulfide liquids
to apply to low to moderate pressures. Density measurements indicate both positive and negative deviations from linear mixing
of partial molar volumes across this five-dimensional composition space. In terms of the homogeneous speciation model of Kress
(in Contrib Mineral Petrol 154:191–204, 2007), the best fit to experimental data can be achieved by starting with a model
where the volume of formation reaction for associated species initially is set to zero. Further refinement of this first-order
fit yields a volume mixing model which reproduces experimental data to within nearly the estimated experimental uncertainty.
Experimental ultrasonic and X-ray absorption data from the literature, along with the bulk modulus–volume relation of Anderson
and Nafe (J Geophys Res 16:3951–3963, 1965), allow the estimation of the pressure dependence of partial molar volumes for
sulfide liquid species. The resulting combined thermochemical model should be valid to about 2,000 K and 3 GPa. Application
of this thermochemical model in a simple adiabatic magma ascent scenario confirms earlier work suggesting that the pressure
dependence of sulfur solubility in sulfide-saturated magma will decrease with increasing pressure along geologically reasonable
paths in P– T–– space. 相似文献
6.
Experiments on water solubility in forsterite in the systems Mg 2SiO 4–K 2Mg(CO 3) 2–H 2O and Mg 2SiO 4–H 2O–C were conducted at 7.5–14.0 GPa and 1200–1600 °C. The resulting crystals contain 448 to 1480 ppm water, which is 40–70% less than in the forsterite–water system under the same conditions. This can be attributed to lower water activity in the carbonate-bearing melt. The water content of forsterite was found to vary systematically with temperature and pressure. For instance, at 14 GPa in the system forsterite–carbonate–H 2O the H 2O content of forsterite drops from 1140 ppm at 1200 °C to 450 ppm at 1600 °C, and at 8 GPa it remains constant or increases from 550 to 870 ppm at 1300–1600 °C. Preliminary data for D-H-bearing forsterite are reported. Considerable differences were found between IR spectra of D-H- and H-bearing forsterite. The results suggest that CO 2 can significantly affect the width of the olivine-wadsleyite transition, i.e., the 410-km seismic discontinuity, which is a function of the water content of olivine and wadsleyite. 相似文献
7.
The configurational heat capacity, shear modulus and shear viscosity of a series of Na 2O–Fe 2O 3–Al 2O 3–SiO 2 melts have been determined as a function of composition. A change in composition dependence of each of the physical properties
is observed as Na 2O/(Na 2O + Al 2O 3) is decreased, and the peralkaline melts become peraluminous and a new charge-balanced Al-structure appears in the melts.
Of special interest are the frequency dependent (1 mHz–1 Hz) measurements of the shear modulus. These forced oscillation measurements
determine the lifetimes of Si–O bonds and Na–O bonds in the melt. The lifetime of the Al–O bonds could not, however, be resolved
from the mechanical spectrum. Therefore, it appears that the lifetime of Al–O bonds in these melts is similar to that of Si–O
bonds with the Al–O relaxation peak being subsumed by the Si–O relaxation peak. The appearance of a new Al-structure in the
peraluminous melts also cannot be resolved from the mechanical spectra, although a change in elastic shear modulus is determined
as a function of composition. The structural shear-relaxation time of some of these melts is not that which is predicted by
the Maxwell equation, but up to 1.5 orders of magnitude faster. Although the configurational heat capacity, density and shear
modulus of the melts show a change in trend as a function of composition at the boundary between peralkaline and peraluminous,
the deviation in relaxation time from the Maxwell equation occurs in the peralkaline regime. The measured relaxation times
for both the very peralkaline melts and the peraluminous melts are identical with the calculated Maxwell relaxation time.
As the Maxwell equation was created to describe the timescale of flow of a mono-structure material, a deviation from the prediction
would indicate that the structure of the melt is too complex to be described by this simple flow equation. One possibility
is that Al-rich channels form and then disappear with decreasing Si/Al, and that the flow is dominated by the lifetime of
Si–O bonds in the Al-poor peralkaline melts, and by the lifetime of Al–O bonds in the relatively Si-poor peralkaline and peraluminous
melts with a complex flow mechanism occurring in the mid-compositions. This anomalous deviation from the calculated relaxation
time appears to be independent of the change in structure expected to occur at the peralkaline/peraluminous boundary due to
the lack of charge-balancing cations for the Al-tetrahedra. 相似文献
8.
The thermodynamic properties of the copper carbonates malachite and azurite have been studied by adiabatic calorimetry, by heat-flux Calvet Calorimetry, by differential thermal analysis (DTA) and by thermogravimetrie (TGA) analysis. The heat capacities, C p 0 of natural malachite and azurite have been measured between 3.8 and 300 K by low-temperature adiabatic calorimetry. The heat capacity of azurite exhibits anomalous behavior at low temperatures. At 298.15 K the molar heat capacities C p 0 and the third law entropies S 298.15 0 are 228.5±1.4 and 254.4±3.8 J mol ?1 K ?1 for azurite and 154.3±0.93 and 166.3±2.5 J mol ?1 K ?1 for malachite. Enthalpies of solution at 973 K in lead borate 2PbO·B 2O 3 have been measured for heat treated malachite and azurite. The enthalpies of decomposition are 105.1±5.8 for azurite and 66.1±5.0 kJ mol ? for malachite. The enthalpies of formation from oxides of azurite and malachite determined by oxide melt solution calorimetry, are ?84.7±7.4 and ?52.5±5.9 kJ mol ?1, respectively. On the basis of the thermodynamic data obtained, phase relations of azurite and malachite in the system Cu 2+-H 2O-CO 2 at 25 and 75 °C have been studied. 相似文献
10.
An equation of state (EOS) explicit in Helmholtz free energy has been improved to calculate the PVTx and vapor–liquid phase equilibrium properties of CH 4–CO 2 fluid mixture. This EOS, where four mixing parameters are used, is based on highly accurate EOSs recommended by NIST for pure components (CH 4 and CO 2) and contains a simple generalized departure function presented by Lemmon and Jacobsen (1999). Comparison with experimental data available indicates that the EOS can calculate both vapor–liquid phase equilibrium and volumetric properties of this binary fluid system with accuracy close to that of experimental data up to high temperature and pressure within full range of composition. The EOS of CH 4–CO 2 fluid, together with the updated Gibbs free energy model of solid CO 2 (dry ice), is applied to calculate the CH 4 content ( xCH4) and molar volume ( Vm) of the CH 4–CO 2 fluid inclusion based on the assumption that the volume of an inclusion keeps constant during heating and cooling. diagrams are presented, which describe phase transitions involving vapor, liquid and CO 2 solid phases of CH 4–CO 2 fluid inclusions. Isochores of CH 4–CO 2 inclusions at given and Vm can be easily calculated from the improved EOS. 相似文献
12.
Here, we present the first analytical technique (the quartz tube system technique—QTS) to directly analyze H 2O and CO 2 contents in liquids following high-pressure, high-temperature experiments in capsules containing mantle minerals and a diamond layer serving as a fluid/melt trap. In this technique, the capsule is frozen prior to opening; the diamond trap is cut out of the capsule and placed inside a N 2-filled quartz tube. The diamond trap is heated up to 900 °C to release the gases to an Infrared Gas Analyzer, which determines the CO 2 and H 2O contents. Three sets of experiments containing SiO 2 and CaCO 3 powders were performed at 6 GPa and 1,000 °C in order to calibrate and validate the technique. These experiments demonstrated that when samples are prepared in a N 2 environment, CO 2 and H 2O can be directly measured with an accuracy and precision of 2–3 and 3–4 %, respectively. The QTS technique (for H 2O and CO 2 determination) together with the cryogenic technique (total dissolved solids content) can be applied to diamond-trap capsules following HP–HT experiments in order to provide direct and complete liquid compositions coexisting with mantle material. The principal advantage of the QTS technique of direct analysis of volatile content in liquids over the indirect approach of mass balance calculations is the possibility of studying carbonated and hydrous liquid compositions in equilibrium with mantle material regardless of chemistry and pressure–temperature experimental conditions. 相似文献
14.
The sound velocity ( V P) of liquid Fe–10 wt% Ni and Fe–10 wt% Ni–4 wt% C up to 6.6 GPa was studied using the ultrasonic pulse-echo method combined with synchrotron X-ray techniques. The obtained V P of liquid Fe–Ni is insensitive to temperature, whereas that of liquid Fe–Ni–C tends to decrease with increasing temperature. The V P values of both liquid Fe–Ni and Fe–Ni–C increase with pressure. Alloying with 10 wt% of Ni slightly reduces the V P of liquid Fe, whereas alloying with C is likely to increase the V P. However, a difference in V P between liquid Fe–Ni and Fe–Ni–C becomes to be smaller at higher temperature. By fitting the measured V P data with the Murnaghan equation of state, the adiabatic bulk modulus ( K S0) and its pressure derivative ( K S ′ ) were obtained to be K S0 = 103 GPa and K S ′ = 5.7 for liquid Fe–Ni and K S0 = 110 GPa and K S ′ = 7.6 for liquid Fe–Ni–C. The calculated density of liquid Fe–Ni–C using the obtained elastic parameters was consistent with the density values measured directly using the X-ray computed tomography technique. In the relation between the density ( ρ) and sound velocity ( V P) at 5 GPa (the lunar core condition), it was found that the effect of alloying Fe with Ni was that ρ increased mildly and V P decreased, whereas the effect of C dissolution was to decrease ρ but increase V P. In contrast, alloying with S significantly reduces both ρ and V P. Therefore, the effects of light elements (C and S) and Ni on the ρ and V P of liquid Fe are quite different under the lunar core conditions, providing a clue to constrain the light element in the lunar core by comparing with lunar seismic data. 相似文献
15.
在熔融的2PbO.B2O3中(974K),用滴溶量热法测定了298K下由组分K2CO3和CaCO3形成的复碳酸盐K2Ca(CO3)2(它有胶方解石和碳钾钙石两种多型)和K2Ca2(CO3)3为-7.2±5.8kJ/mol。同时推算出了复碳酸盐生砀熵变ΔSt。假定具有序结构的胶方解石的ΔSt=0,则碳钾钙石的生成熵为40.9±5.1J/mol.K,K2Ca2(CO3)3为39.4±7.3J/mol. 相似文献
17.
To characterize the influence of alkaline metal chlorides on the phase ratios under melting of upper mantle eclogites, the eclogite–CaCO3–NaCl–KCl system with Н2О + СО2-fluid was studied in the experiments under 4 GPa and 1200–1300°C. A low difference in temperatures (<100°C) was registered between the eclogite solidus and liquidus (>1200 and <1300°C, respectively), which is characteristic for the near-eutectic compositions. The phase proportions were peculiar for the absence of any silicate melt over the entire temperature range considered. The carbonate melt coexisted with clinopyroxene and garnet within 1200–1250°C, whereas a carbonate melt exclusively occurred under above-liquidus conditions at 1300°C. The melt quenching resulted in the formation of a multiphase fine-grained mixture of Ca, Na, and K carbonates and chlorides containing microinclusions of clinopyroxene and garnet. The occurrence of a high-calcium carbonate melt in Cl-containing eclogite systems might play a significant role in the mantle metasomatism of subduction zones characterized by the water–alkaline–chloride type of fluids. 相似文献
18.
水体吸收的CO2转变为HCO3-,构成了碳酸盐水化学系统对CO2气体的缓冲,通常用Revelle因子(R)表征。陆地淡水系统释放的CO2是全球碳循环的重要组成部分,一方面,湖泊水体释放的CO2是来源于流域碳酸盐风化产物的输入,另一方面,碳酸盐的缓冲作用也是调节内陆水体CO2释放的重要因素,这两个结论看似是矛盾的。为了揭示碳酸盐循环对水体CO2的影响与缓冲机制,本研究选取一个碳酸盐岩地区的季节性分层湖泊(百花湖),分析Revelle因子变化,并与非碳酸盐湖泊进行比较。结果发现,碳酸盐岩湖泊Revell因子平均为20.1±8.1(8.0~50.0),大于表层海水的10.0(8.0~15.0),也远大于非碳酸盐地区湖泊的3.9±3.9,较高的Revelle因子意味着对CO2的缓冲能力更弱。Revelle因子最大值46.4出现在夏季分层期的中部斜温层,对应的无机碳浓度为2.1 mmol?L-1、pH为8.38、总无机碳与碱度比接近1.0、CO2/CO32-等于1.0。实际观测与理论分析结果完全吻合,表明碳酸盐化学平衡是控制湖泊Revelle因子变化的主要因素。低pH的非碳酸盐岩系统可以溶解碳酸盐矿物,使pH升高,碱度增加,导致Revelle因子升高,在碳酸盐溶解达到平衡时Revelle因子升至最大。其后,无论是光合作用导致的碳酸盐沉淀还是呼吸作用导致的碳酸盐溶解,Revelle因子都会降低,新陈代谢导致碳酸盐系统的CO2缓冲能力增强。 相似文献
19.
A comprehensive low-temperature thermodynamic model for the geochemically important Na 2CO 3−MgCO 3−CaCO 3−H 2O system is presented. The model is based on calorimetrically determined Δ fH° 298 values, S° 298 values and C° p( T) functions taken from the literature as well as on μ° 298 values of solids derived in this work from solubility measurements obtained in our laboratories or by others. When these thermodynamic quantities were combined with temperature-dependent Pitzer parameters taken from the literature, solubilities calculated for a wide range of conditions agree well with experimental data. The results for several subsystems were summarized by depicting the respective phase diagrams. For the MgO−CO 2−H 2O subsystem, it was found that the commonly believed stability relations must be revised, i.e., in the temperature range covered, nesquehonite never becomes more stable than hydromagnesite at pCO2 ≤ 1 atm. Although the recommended set of thermodynamic data on sparingly soluble solids was derived from experimental results on mainly NaClO 4 systems, it can be incorporated in databanks containing additional Pitzer parameters for modeling more complex fresh- or seawater systems. 相似文献
20.
减少CO2向大气排放的一个主要的方法是将其隔离在地下深部,即CO2地质处置。CO2地质处置的方法主要包括:含水层处置,海洋处置,利用CO2开采油气以及煤层甲烷气体等。含水层处置有三种机制:(1)水力学方法;(2)溶解的方法;(3)矿物处置。CO2地质处置是可行的技术方法,在实际中已有了应用。在难以获得复杂的深部含水层环境的情况下,地球化学数值模拟方法在评价地质处置CO2可行性上具有重要的作用。 相似文献
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