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1.
Geological heterogeneities affect the dynamics of carbon dioxide (CO2) plumes in subsurface environments in important ways. Previously, we showed how the dynamics of CO2 plumes are influenced by the multiscaled sedimentary architecture in deep brine fluvial-type reservoirs. The results confirm that representing small-scale features and the corresponding heterogeneity in saturation functions, along with hysteresis in saturation functions, are all critical to understanding capillary trapping processes. Here, we show that when heterogeneity and hysteresis are represented, the two conventional approaches for defining saturation functions, Brooks-Corey and van Genuchten, represent fundamentally different physical systems. The Brooks-Corey approach represents heterogeneity in entry pressures, and leads to trapping by capillary pinning. The van Genuchten approach represents a network of pores transporting the nonwetting fluid, across rock types, with negligible capillary entry pressure, and leads to capillary retardation. These differences significantly affect the large-scale characteristics of CO2 plumes (i.e., their mass, shape, and position).  相似文献   

2.
The entrainment dynamics in the D″-layer are influenced by multitudinous factors, such as thermal and compositional buoyancy, and temperature- and composition-dependent viscosity. Here, we are focusing on the effect of compositionally dependent viscosity on the mixing dynamics of the D″-layer, arising from the less viscous but denser D″-material. The marker method, with one million markers, is used for portraying the fine scale features of the compositional components, D″-layer and lower-mantle. The D″-layer has a higher density but a lower viscosity than the ambient lower-mantle, as suggested by melting point systematics. Results from a two-dimensional finite-difference numerical model including the extended Boussinesq approximation with dissipation number Di=0.3, show that a D″-layer, less viscous than the ambient mantle by 1.5 orders of magnitude, cannot efficiently mix with the lower-mantle, even though the buoyancy parameter is as low as Rρ=0.6. However, very small-scale schlieren structures of D″-layer material are entrained into the lower-mantle. These small-scale lower-mantle heterogeneities have been imaged with one-dimensional wavelets in order to delineate quantitatively the multiscale features. They may offer an explanation for small-scale seismic heterogeneity inferred by seismic scattering in the lower-mantle.  相似文献   

3.
Tracking the migration of the CO2 plume is essential in order to better manage the operation of geologic sequestration of CO2. However, the large cost of most monitoring technologies, such as time-lapse seismic, limits their application. We investigated the application of a probabilistic history matching methodology using routine measurements of injection data, which are affected by the presence of large-scale heterogeneities, as an inexpensive alternative to track the migration of CO2 plume in an aquifer. The approach is demonstrated first through a synthetic example in which the ability to detect the presence of flow barriers was tested. In a second example, we applied our method to the In Salah field, one of the largest geological sequestration projects in the world, where the main direction of high permeability features was inferred. The accuracy and reproducibility of the results show that our approach for assisted history matching is an economic and viable option for plume monitoring during geologic CO2 sequestration.  相似文献   

4.
Contact angle is a principal control of the flow of multiple fluid phases through porous media; however its measurement on other than flat surfaces remains a challenge. A new method is presented for the measurement of the contact angle between immiscible fluids at the pore scale at reservoir conditions (10 MPa and 50 °C) inside a quarry limestone through the use of X-ray microtomography. It is applied to a super-critical CO2–brine–carbonate system by resampling the micro-CT data onto planes orthogonal to the contact lines, allowing for vectors to be traced along the grain surface and the CO2–brine interface. A distribution of contact angles ranging from 35° to 55° is observed, indicating that the CO2–brine–carbonate system is weakly water-wet. This range of contact angles can be understood as the result of contact angle hysteresis and surface heterogeneity on a range of length scales. Surface heterogeneity is examined by comparison of micro-CT results with optical thin sections and SEM images.  相似文献   

5.
Geologic carbon sequestration (GCS) is being considered as a climate change mitigation option in many future energy scenarios. Mathematical modeling is routinely used to predict subsurface CO2 and resident brine migration for the design of injection operations, to demonstrate the permanence of CO2 storage, and to show that other subsurface resources will not be degraded. Many processes impact the migration of CO2 and brine, including multiphase flow dynamics, geochemistry, and geomechanics, along with the spatial distribution of parameters such as porosity and permeability. In this article, we review a set of multiphase modeling approaches with different levels of conceptual complexity that have been used to model GCS. Model complexity ranges from coupled multiprocess models to simplified vertical equilibrium (VE) models and macroscopic invasion percolation models. The goal of this article is to give a framework of conceptual model complexity, and to show the types of modeling approaches that have been used to address specific GCS questions. Application of the modeling approaches is shown using five ongoing or proposed CO2 injection sites. For the selected sites, the majority of GCS models follow a simplified multiphase approach, especially for questions related to injection and local‐scale heterogeneity. Coupled multiprocess models are only applied in one case where geomechanics have a strong impact on the flow. Owing to their computational efficiency, VE models tend to be applied at large scales. A macroscopic invasion percolation approach was used to predict the CO2 migration at one site to examine details of CO2 migration under the caprock.  相似文献   

6.
During geologic storage of carbon dioxide (CO2), trapping of the buoyant CO2 after injection is essential in order to minimize the risk of leakage into shallower formations through a fracture or abandoned well. Models for the subsurface behavior of the CO2 are useful for the design, implementation, and long-term monitoring of injection sites, but traditional reservoir-simulation tools are currently unable to resolve the impact of small-scale trapping processes on fluid flow at the scale of a geologic basin. Here, we study the impact of solubility trapping from convective dissolution on the up-dip migration of a buoyant gravity current in a sloping aquifer. To do so, we conduct high-resolution numerical simulations of the gravity current that forms from a pair of miscible analogue fluids. Our simulations fully resolve the dense, sinking fingers that drive the convective dissolution process. We analyze the dynamics of the dissolution flux along the moving CO2–brine interface, including its decay as dissolved buoyant fluid accumulates beneath the buoyant current. We show that the dynamics of the dissolution flux and the macroscopic features of the migrating current can be captured with an upscaled sharp-interface model.  相似文献   

7.
We used the 3D continuum-scale reactive transport models to simulate eight core flood experiments for two different carbonate rocks. In these experiments the core samples were reacted with brines equilibrated with pCO2 = 3, 2, 1, 0.5 MPa (Smith et al., 2013 [27]). The carbonate rocks were from specific Marly dolostone and Vuggy limestone flow units at the IEAGHG Weyburn-Midale CO2 Monitoring and Storage Project in south-eastern Saskatchewan, Canada. Initial model porosity, permeability, mineral, and surface area distributions were constructed from micro tomography and microscopy characterization data. We constrained model reaction kinetics and porosity–permeability equations with the experimental data. The experimental data included time-dependent solution chemistry and differential pressure measured across the core, and the initial and final pore space and mineral distribution. Calibration of the model with the experimental data allowed investigation of effects of carbonate reactivity, flow velocity, effective permeability, and time on the development and consequences of stable and unstable dissolution fronts.The continuum scale model captured the evolution of distinct dissolution fronts that developed as a consequence of carbonate mineral dissolution and pore scale transport properties. The results show that initial heterogeneity and porosity contrast control the development of the dissolution fronts in these highly reactive systems. This finding is consistent with linear stability analysis and the known positive feedback between mineral dissolution and fluid flow in carbonate formations. Differences in the carbonate kinetic drivers resulting from the range of pCO2 used in the experiments and the different proportions of more reactive calcite and less reactive dolomite contributed to the development of new pore space, but not to the type of dissolution fronts observed for the two different rock types. The development of the dissolution front was much more dependent on the physical heterogeneity of the carbonate rock. The observed stable dissolution fronts with small but visible dissolution fingers were a consequence of the clustering of a small percentage of larger pores in an otherwise homogeneous Marly dolostone. The observed wormholes in the heterogeneous Vuggy limestone initiated and developed in areas of greater porosity and permeability contrast, following pre-existing preferential flow paths.Model calibration of core flood experiments is one way to specifically constrain parameter input used for specific sites for larger scale simulations. Calibration of the governing rate equations and constants for Vuggy limestones showed that dissolution rate constants reasonably agree with published values. However the calcite dissolution rate constants fitted to the Marly dolostone experiments are much lower than those suggested by literature. The differences in fitted calcite rate constants between the two rock types reflect uncertainty associated with measured reactive surface area and appropriately scaling heterogeneous distribution of less abundant reactive minerals. Calibration of the power-law based porosity–permeability equations was sensitive to the overall heterogeneity of the cores. Stable dissolution fronts of the more homogeneous Marly dolostone could be fit with the exponent n = 3 consistent with the traditional Kozeny–Carman equation developed for porous sandstones. More impermeable and heterogeneous cores required larger n values (n = 6–8).  相似文献   

8.
We suggest that different equations of state (EOS) algorithms can and frequently will provide very different predictions of CO2 migration following injection for sequestration. Rather than carry out an exhaustive examination of all EOS algorithms available, we elected to evaluate this general hypothesis by making detailed comparisons of simulation results of two very common EOS algorithms. We simulated and compared CO2 migration patterns using two fundamentally different EOS algorithms – Modified Redlich-Kwong EOS (MRKEOS) and Span and Wagner EOS (SWEOS). In general, the predictions of thermophysical properties for both algorithms are close, except for a contrast in the predicted fugacity coefficient of CO2, which subsequently propagates to a contrast in predicted solubility in water/brine. Typically, MRKEOS underestimates solubility of CO2 compared to both SWEOS and experimental solubility data. In simulations of CO2 migration, dissolution rates of separate-phase CO2 predicted from the two EOS algorithms were significantly different, even for small contrasts in predicted fluid properties from EOS algorithms, resulting in markedly different migration patterns.  相似文献   

9.
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10.
基于随机介质模型的储层非均质性分析   总被引：10，自引：5，他引：5       下载免费PDF全文
本文利用随机介质模型对复杂岩性储层进行了非均质性描述.利用模型特征量即非均质纵横比、纵向谱指数、横向谱指数以及扰动标准差等来模拟不同的随机介质.在前人工作的基础上,由某油气田的两口井资料估计储层非均质性能谱,从能谱曲线上提取储层纵向大小尺度非均质谱指数.通过将二维随机介质模拟的合成井记录互相关系数与实际井记录互相关系数进行分析比较,分别得到大小尺度非均质情况下最佳拟合时的横向谱指数和非均质性纵横比.以上求得的各种特征量从不同角度定量分析了储层非均质性的纵横向变化,为储层横向预测提供了依据.  相似文献   

11.
Scattering attenuation in short wavelengths has long been interesting to geophysicists. Ultrasonic coda waves, observed as the tail portion of ultrasonic wavetrains in laboratory ultrasonic measurements, are important for such studies where ultrasonic waves interact with small-scale random heterogeneities on a scale of micrometers, but often ignored as noises because of the contamination of boundary reflections from the side ends of a sample core. Numerical simulations with accurate absorbing boundary can provide insight into the effect of boundary reflections on coda waves in laboratory experiments. The simulation of wave propagation in digital and heterogeneous porous cores really challenges numerical techniques by digital image of poroelastic properties, numerical dispersion at high frequency and strong heterogeneity, and accurate absorbing boundary schemes at grazing incidence. To overcome these difficulties, we present a staggered-grid high-order finite-difference (FD) method of Biot’s poroelastic equations, with an arbitrary even-order (2L) accuracy to simulate ultrasonic wave propagation in digital porous cores with strong heterogeneity. An unsplit convolutional perfectly matched layer (CPML) absorbing boundary, which improves conventional PML methods at grazing incidence with less memory and better computational efficiency, is employed in the simulation to investigate the influence of boundary reflections on ultrasonic coda waves. Numerical experiments with saturated poroelastic media demonstrate that the 2L FD scheme with the CPML for ultrasonic wave propagation significantly improves stability conditions at strong heterogeneity and absorbing performance at grazing incidence. The boundary reflections from the artificial boundary surrounding the digital core decay fast with the increase of CPML thicknesses, almost disappearing at the CPML thickness of 15 grids. Comparisons of the resulting ultrasonic coda Q sc values between the numerical and experimental ultrasonic S waveforms for a cylindrical rock sample demonstrate that the boundary reflection may contribute around one-third of the ultrasonic coda attenuation observed in laboratory experiments.  相似文献   

12.
The typical shape of a capillary-pressure curve is either convex (e.g., Brooks–Corey model) or S-shaped (e.g., van Genuchten model). It is not universally agreed which model reflects natural rocks better. The difference between the two models lies in the representation of the capillary entry pressure. This difference does not lead to significantly different simulation results for modeling CO2 sequestration in aquifers without considering CO2 dissolution. However, we observe that the van-Genuchten-type capillary-pressure model accelerates CO2 solubility trapping significantly compared with the Brooks–Corey-type model. We also show that the simulation results are very sensitive to the slope of the van-Genuchten-type curve around the entry-pressure region. For the representative examples we study, the differences can be so large as to have complete dissolution of the CO2 plume versus persistence of over 50% of the plume over a 5000-year period.The cause of such sensitivity to the capillary-pressure model is studied. Particularly, we focus on how the entry pressure is represented in each model. We examine the mass-transfer processes under gravity-capillary equilibrium, molecular diffusion, convective mixing, and in the presence of small-scale heterogeneities. Laboratory measurement of capillary-pressure curves and some important implementation issues of capillary-pressure models in numerical simulators are also discussed. Most CO2 sequestration simulations in the literature employ one of the two capillary-pressure models. It is important to recognize that these two representations lead to very different predictions of long-term CO2 sequestration.  相似文献   

13.
Generally, the intensity and magnitude of explosive volcanic activity increase in parallel with SiO2 content. Pyroclastic-flow-forming eruptions in the Colli Albani ultrapotassic volcanic district (Italy) represent the most striking exception on a global scale, with volumes on the order of tens of cubic kilometres and K-foiditic compositions (SiO2 even <42 wt.%). Here, we reconstruct the pre-eruptive scenario and event dynamics of the ~456 ka Pozzolane Rosse (PR) eruption, the largest mafic explosive event of the Colli Albani district. In particular, we focus on the driving mechanisms for the unusually explosive eruption of a low-viscosity, mafic magma. Geologic, petrographic and geochemical data with mass balance calculations, supported by experimental data for Colli Albani magma compositions, provide evidence for significant ingestion of carbonate wall rocks by the Pozzolane Rosse K-foiditic magma. Moreover, the scattered occurrence of cored bombs in Pozzolane Rosse pyroclastic-flow deposits records carbonate entrainment even at the eruptive time scale, as also tested quantitatively by thermal modelling of magma–carbonate interaction and carbonate assimilation experiments. We suggest that the addition of free CO2 from decarbonation of country rocks was the major factor controlling magma explosivity. High CO2 activity in the volatile component, coupled with magma depressurisation, produced extensive leucite crystallisation at short time scales, resulting in a dramatic increase in magma viscosity and volatile pressurisation, which was manifested a change of eruptive dynamics from early effusion to the Pozzolane Rosse's highly explosive eruption climax.  相似文献   

14.
Geochemical reaction rate laws are often measured using crushed minerals in well-mixed laboratory systems that are designed to eliminate mass transport limitations. Such rate laws are often used directly in reactive transport models to predict the reaction and transport of chemical species in consolidated porous media found in subsurface environments. Due to the inherent heterogeneities of porous media, such use of lab-measured rate laws may introduce errors, leading to a need to develop methods for upscaling reaction rates. In this work, we present a methodology for using pore-scale network modeling to investigate scaling effects in geochemical reaction rates. The reactive transport processes are simulated at the pore scale, accounting for heterogeneities of both physical and mineral properties. Mass balance principles are then used to calculate reaction rates at the continuum scale. To examine the scaling behavior of reaction kinetics, these continuum-scale rates from the network model are compared to the rates calculated by directly using laboratory-measured reaction rate laws and ignoring pore-scale heterogeneities. In this work, this methodology is demonstrated by upscaling anorthite and kaolinite reaction rates under simulation conditions relevant to geological CO2 sequestration. Simulation results show that under conditions with CO2 present at high concentrations, pore-scale concentrations of reactive species and reaction rates vary spatially by orders of magnitude, and the scaling effect is significant. With a much smaller CO2 concentration, the scaling effect is relatively small. These results indicate that the increased acidity associated with geological sequestration can generate conditions for which proper scaling tools are yet to be developed. This work demonstrates the use of pore-scale network modeling as a valuable research tool for examining upscaling of geochemical kinetics. The pore-scale model allows the effects of pore-scale heterogeneities to be integrated into system behavior at multiple scales, thereby identifying important factors that contribute to the scaling effect.  相似文献   

15.
Hydroelectric reservoirs generate energy without significant combustion of fossil fuels. However, these systems can, potentially, emit greenhouse gases (GHG’s) at a rate which may be significant at the global scale, and, possible, co-equal, per kilowatt-hour, to that from conventional coal or oil-fired systems. Although much of the new construction of hydroelectric reservoirs is in the tropics, most of the data on GHG emissions comes from temperate regions. Further, much of the existing data on reservoir gas emissions comes from single sites, usually near the terminal dams. Large tropical reservoirs often involve the impoundments of river systems with complex morphology which in turn can cause spatial heterogeneity in gas flux. We evaluated spatial and seasonal variability in CO2 concentrations and gas flux for five large (50–1,400 km2) reservoirs in the Cerrado region of Brazil. Most of data set (87% of all measurements) showed CO2 supersaturation and net efflux to the atmosphere. There was as much or more variation in pCO2 over space and among seasons. The large studied reservoirs showed different zones in terms of CO2 emission because those fluxes are dependent on flooded biomass, watershed input of organic matter and dam operation regime. Here we demonstrate that the reservoirs in the Brazilian Cerrado have low rates of CO2 emissions compared to existing global comparisons. Our results suggest that ignoring the spatial variability can lead to more than 25% error in total system gas flux.  相似文献   

16.
Determining consistent sets of vent conditions for next expected eruptions at Vesuvius is crucial for the simulation of the sub-aerial processes originating the volcanic hazard and the eruption impact. Here we refer to the expected eruptive scales and conditions defined in the frame of the EC Exploris project, and simulate the dynamics of magma ascent along the volcanic conduit for sub-steady phases of next eruptions characterized by intensities of the Violent Strombolian (VS), Sub-Plinian 2 (SP2), and Sub-Plinian 1 (SP1) scale. Sets of conditions for the simulations are determined on the basis of the bulk of knowledge on the past history of Vesuvius [Cioni, R., Bertagnini, A., Santacroce, R., Andronico, D., Explosive activity and eruption scenarios at Somma–Vesuvius (Italy): towards a new classification scheme. Journal of Volcanology and Geothermal Research, this issue.]. Volatile contents (H2O and CO2) are parameterized in order to account for the uncertainty in their expected amounts for a next eruption. In all cases the flow in the conduit is found to be choked, with velocities at the conduit exit or vent corresponding to the sonic velocity in the two-phase non-equilibrium magmatic mixture. Conduit diameters and vent mixture densities are found to display minimum overlapping between the different eruptive scales, while exit gas and particle velocities, as well as vent pressures, largely overlap. Vent diameters vary from as low as about 5 m for VS eruptions, to 35–55 m for the most violent SP1 eruption scale. Vent pressures can be as low as less than 1 MPa for the lowest volatile content employed of 2 wt.% H2O and no CO2, to 7–8 MPa for highest volatile contents of 5 wt.% H2O and 2 wt.% CO2 and large eruptive scales. Gas and particle velocities at the vent range from 100–250 m/s, with a tendency to decrease, and to increase the mechanical decoupling between the phases, with increasing eruptive scale. Except for velocities, all relevant vent quantities are more sensitive to the volatile content of the discharged magma for the highest eruptive scales considered.  相似文献   

17.
 An estimated average CO2 output from Etna's summit craters in the range of 13±3 Mt/a has recently been determined from the measured SO2 output and measured CO2/SO2 molar ratios. To this amount the CO2 output emitted diffusely from the soil (≈ 1 Mt/a) and the amount of CO2 dissolved in Etna's aquifers (≈ 0.25 Mt/a) must be added. Data on the solubility of CO2 in Etnean magmas at high temperature and pressure allow the volume of magma involved in the release of such an amount of this gas to be estimated. This volume of magma (≈ 0.7 km3/a) is approximately 20 times greater than the volume of magma erupted annually during the period 1971–1995. On the basis of C-isotopic data of CO2 collected in the Etna area and of new hypotheses on the source of Mediterranean magmas, significant contributions of CO2 from non-magmatic sources to the total output from Etna are unlikely. Such large outputs of CO2 and also of SO2 from Etna could be due to an anomalously shallow asthenosphere beneath the volcano that allows a continuous escape of gases toward the surface, even without migration of magma. Received: 7 August 1996 / Accepted: 9 November 1996  相似文献   

18.
We characterize and quantify volatile emissions at Hot Spring Basin (HSB), a large acid-sulfate region that lies just outside the northeastern edge of the 640 ka Yellowstone Caldera. Relative to other thermal areas in Yellowstone, HSB gases are rich in He and H2, and mildly enriched in CH4 and H2S. Gas compositions are consistent with boiling directly off a deep geothermal liquid at depth as it migrates toward the surface. This fluid, and the gases evolved from it, carries geochemical signatures of magmatic volatiles and water–rock reactions with multiple crustal sources, including limestones or quartz-rich sediments with low K/U (or 40?Ar/4?He). Variations in gas chemistry across the region reflect reservoir heterogeneity and variable degrees of boiling. Gas-geothermometer temperatures approach 300 °C and suggest that the reservoir feeding HSB is one of the hottest at Yellowstone. Diffuse CO2 flux in the western basin of HSB, as measured by accumulation-chamber methods, is similar in magnitude to other acid-sulfate areas of Yellowstone and is well correlated to shallow soil temperatures. The extrapolation of diffuse CO2 fluxes across all the thermal/altered area suggests that 410 ± 140 t d− 1 CO2 are emitted at HSB (vent emissions not included). Diffuse fluxes of H2S were measured in Yellowstone for the first time and likely exceed 2.4 t d− 1 at HSB. Comparing estimates of the total estimated diffuse H2S emission to the amount of sulfur as SO42− in streams indicates ~ 50% of the original H2S in the gas emission is lost into shallow groundwater, precipitated as native sulfur, or vented through fumaroles. We estimate the heat output of HSB as ~ 140–370 MW using CO2 as a tracer for steam condensate, but not including the contribution from fumaroles and hydrothermal vents. Overall, the diffuse heat and volatile fluxes of HSB are as great as some active volcanoes, but they are a small fraction (1–3% for CO2, 2–8% for heat) of that estimated for the entire Yellowstone system.  相似文献   

19.
Integrated modeling of basin- and plume-scale processes induced by full-scale deployment of CO2 storage was applied to the Mt. Simon Aquifer in the Illinois Basin. A three-dimensional mesh was generated with local refinement around 20 injection sites, with approximately 30 km spacing. A total annual injection rate of 100 Mt CO2 over 50 years was used. The CO2-brine flow at the plume scale and the single-phase flow at the basin scale were simulated. Simulation results show the overall shape of a CO2 plume consisting of a typical gravity-override subplume in the bottom injection zone of high injectivity and a pyramid-shaped subplume in the overlying multilayered Mt. Simon, indicating the important role of a secondary seal with relatively low-permeability and high-entry capillary pressure. The secondary-seal effect is manifested by retarded upward CO2 migration as a result of multiple secondary seals, coupled with lateral preferential CO2 viscous fingering through high-permeability layers. The plume width varies from 9.0 to 13.5 km at 200 years, indicating the slow CO2 migration and no plume interference between storage sites. On the basin scale, pressure perturbations propagate quickly away from injection centers, interfere after less than 1 year, and eventually reach basin margins. The simulated pressure buildup of 35 bar in the injection area is not expected to affect caprock geomechanical integrity. Moderate pressure buildup is observed in Mt. Simon in northern Illinois. However, its impact on groundwater resources is less than the hydraulic drawdown induced by long-term extensive pumping from overlying freshwater aquifers.  相似文献   

20.
Cook Inlet volcanoes that experienced an eruption between 1989 and 2006 had mean gas emission rates that were roughly an order of magnitude higher than at volcanoes where unrest stalled. For the six events studied, mean emission rates for eruptions were ∼13,000 t/d CO2 and 5200 t/d SO2, but only ∼1200 t/d CO2 and 500 t/d SO2 for non-eruptive events (‘failed eruptions’). Statistical analysis suggests degassing thresholds for eruption on the order of 1500 and 1000 t/d for CO2 and SO2, respectively. Emission rates greater than 4000 and 2000 t/d for CO2 and SO2, respectively, almost exclusively resulted during eruptive events (the only exception being two measurements at Fourpeaked). While this analysis could suggest that unerupted magmas have lower pre-eruptive volatile contents, we favor the explanations that either the amount of magma feeding actual eruptions is larger than that driving failed eruptions, or that magmas from failed eruptions experience less decompression such that the majority of H2O remains dissolved and thus insufficient permeability is produced to release the trapped volatile phase (or both). In the majority of unrest and eruption sequences, increases in CO2 emission relative to SO2 emission were observed early in the sequence. With time, all events converged to a common molar value of C/S between 0.5 and 2. These geochemical trends argue for roughly similar decompression histories until shallow levels are reached beneath the edifice (i.e., from 20–35 to ∼4–6 km) and perhaps roughly similar initial volatile contents in all cases. Early elevated CO2 levels that we find at these high-latitude, andesitic arc volcanoes have also been observed at mid-latitude, relatively snow-free, basaltic volcanoes such as Stromboli and Etna. Typically such patterns are attributed to injection and decompression of deep (CO2-rich) magma into a shallower chamber and open system degassing prior to eruption. Here we argue that the C/S trends probably represent tapping of vapor-saturated regions with high C/S, and then gradual degassing of remaining dissolved volatiles as the magma progresses toward the surface. At these volcanoes, however, C/S is often accentuated due to early preferential scrubbing of sulfur gases. The range of equilibrium degassing is consistent with the bulk degassing of a magma with initial CO2 and S of 0.6 and 0.2 wt.%, respectively, similar to what has been suggested for primitive Redoubt magmas.  相似文献   

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