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The effect of alkalis on the solubility of H2O and CO2 in alkali-rich silicate melts was investigated at 500 MPa and 1,250 °C in the systems with H2O/(H2O + CO2) ratio varying from 0 to 1. Using a synthetic analog of phonotephritic magma from Alban Hills (AH1) as a base composition, the Na/(Na + K) ratio was varied from 0.28 (AH1) to 0.60 (AH2) and 0.85 (AH3) at roughly constant total alkali content. The obtained results were compared with the data for shoshonitic and latitic melts having similar total alkali content but different structural characteristics, e.g., NBO/T parameter (the ratio of non-bridging oxygens over tetrahedrally coordinated cations), as those of the AH compositions. Little variation was observed in H2O solubility (melt equilibrated with pure H2O fluid) for the whole compositional range in this study with values ranging between 9.7 and 10.2 wt. As previously shown, the maximum CO2 content in melts equilibrated with CO2-rich fluids increases strongly with the NBO/T from 0.29 wt % for latite (NBO/T = 0.17) to 0.45 wt % for shoshonite (NBO/T = 0.38) to 0.90 wt % for AH2 (NBO/T = 0.55). The highest CO2 contents determined for AH3 and AH1 are 1.18 ± 0.05 wt % and 0.86 ± 0.12 wt %, respectively, indicating that Na is promoting carbonate incorporation stronger than potassium. At near constant NBO/T, CO2 solubility increases from 0.86 ± 0.12 wt % in AH1 [Na/(Na + K)] = 0.28, to 1.18 ± 0.05 wt % in AH3 [Na/(Na + K)] = 0.85, suggesting that Na favors CO2 solubility on an equimolar basis. An empirical equation is proposed to predict the maximum CO2 solubility at 500 MPa and 1,100–1,300 °C in various silicate melts as a function of the NBO/T, (Na + K)/∑cations and Na/(Na + K) parameters: \({\text{wt}}\% \;{\text{CO}}_{2} = - 0.246 + 0.014\exp \left( {6.995 \cdot \frac{\text{NBO}}{T}} \right) + 3.150 \cdot \frac{{{\text{Na}} + {\text{K}}}}{{\varSigma {\text{cations}}}} + 0.222 \cdot \frac{\text{Na}}{{{\text{Na}} + {\text{K}}}}.\) This model is valid for melt compositions with NBO/T between 0.0 and 0.6, (Na + K)/∑cation between 0.08 and 0.36 and Na/(Na + K) ratio from 0.25 to 0.95 at oxygen fugacities around the quartz–fayalite–magnetite buffer and above. 相似文献
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The discovery of Hadean to Paleoarchean zircons in a metaconglomerate from Jack Hills, Western Australia, has catalyzed intensive study of these zircons and their mineral inclusions, as they represent unique geochemical archives that can be used to unravel the geological evolution of early Earth. Here, we report the occurrence and physical properties of previously undetected CO2 inclusions that were identified in 3.36–3.47 Ga and 3.80–4.13 Ga zircon grains by confocal micro-Raman spectroscopy. Minimum P–T conditions of zircon formation were determined from the highest density of the inclusions, determined from the density-dependence of the Fermi diad splitting in the Raman spectrum and Ti-in-zircon thermometry. For both age periods, the CO2 densities and Ti-in-zircon temperatures correspond to high-grade metamorphic conditions (≥5 to ≥7 kbar/~670 to 770 °C) that are typical of mid-crustal regional metamorphism throughout Earth’s history. In addition, fully enclosed, highly disordered graphitic carbon inclusions were identified in two zircon grains from the older population that also contained CO2 inclusions. Transmission electron microscopy on one of these inclusions revealed that carbon forms a thin amorphous film on the inclusion wall, whereas the rest of the volume was probably occupied by CO2 prior to analysis. This indicates a close relationship between CO2 and the reduced carbon inclusions and, in particular that the carbon precipitated from a CO2-rich fluid, which is inconsistent with the recently proposed biogenic origin of carbon inclusions found in Hadean zircons from Jack Hills. 相似文献
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Jennifer L. Lewicki George E. Hilley Laura Dobeck Lee Spangler 《Environmental Earth Sciences》2010,60(2):285-297
A field facility located in Bozeman, Montana provides the opportunity to test methods to detect, locate, and quantify potential
CO2 leakage from geologic storage sites. From 9 July to 7 August 2008, 0.3 t CO2 day−1 were injected from a 100-m long, ~2.5-m deep horizontal well. Repeated measurements of soil CO2 fluxes on a grid characterized the spatio-temporal evolution of the surface leakage signal and quantified the surface leakage
rate. Infrared CO2 concentration sensors installed in the soil at 30 cm depth at 0–10 m from the well and at 4 cm above the ground at 0 and
5 m from the well recorded surface breakthrough of CO2 leakage and migration of CO2 leakage through the soil. Temporal variations in CO2 concentrations were correlated with atmospheric and soil temperature, wind speed, atmospheric pressure, rainfall, and CO2 injection rate. 相似文献
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Priscille Lesne Bruno Scaillet Michel Pichavant Giada Iacono-Marziano Jean-Michel Beny 《Contributions to Mineralogy and Petrology》2011,162(1):133-151
Experiments were conducted to determine the water solubility of alkali basalts from Etna, Stromboli and Vesuvius volcanoes,
Italy. The basaltic melts were equilibrated at 1,200°C with pure water, under oxidized conditions, and at pressures ranging
from 163 to 3,842 bars. Our results show that at pressures above 1 kbar, alkali basalts dissolve more water than typical mid-ocean
ridge basalts (MORB). Combination of our data with those from previous studies allows the following simple empirical model
for the water solubility of basalts of varying alkalinity and fO2 to be derived:
\textH 2 \textO( \textwt% ) = \text H 2 \textO\textMORB ( \textwt% ) + ( 5.84 ×10 - 5 *\textP - 2.29 ×10 - 2 ) ×( \textNa2 \textO + \textK2 \textO )( \textwt% ) + 4.67 ×10 - 2 ×\Updelta \textNNO - 2.29 ×10 - 1 {\text{H}}_{ 2} {\text{O}}\left( {{\text{wt}}\% } \right) = {\text{ H}}_{ 2} {\text{O}}_{\text{MORB}} \left( {{\text{wt}}\% } \right) + \left( {5.84 \times 10^{ - 5} *{\text{P}} - 2.29 \times 10^{ - 2} } \right) \times \left( {{\text{Na}}_{2} {\text{O}} + {\text{K}}_{2} {\text{O}}} \right)\left( {{\text{wt}}\% } \right) + 4.67 \times 10^{ - 2} \times \Updelta {\text{NNO}} - 2.29 \times 10^{ - 1} where H2OMORB is the water solubility at the calculated P, using the model of Dixon et al. (1995). This equation reproduces the existing database on water solubilities in basaltic melts to within 5%. Interpretation of
the speciation data in the context of the glass transition theory shows that water speciation in basalt melts is severely
modified during quench. At magmatic temperatures, more than 90% of dissolved water forms hydroxyl groups at all water contents,
whilst in natural or synthetic glasses, the amount of molecular water is much larger. A regular solution model with an explicit
temperature dependence reproduces well-observed water species. Derivation of the partial molar volume of molecular water using
standard thermodynamic considerations yields values close to previous findings if room temperature water species are used.
When high temperature species proportions are used, a negative partial molar volume is obtained for molecular water. Calculation
of the partial molar volume of total water using H2O solubility data on basaltic melts at pressures above 1 kbar yields a value of 19 cm3/mol in reasonable agreement with estimates obtained from density measurements. 相似文献
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Fluid inclusions have recorded the history of degassing in basalt. Some fluid inclusions in olivine and pyroxene phenocrysts of basalt were analyzed by micro-thermometry and Raman spectroscopy in this paper. The experimental results showed that many inclusions are present almost in a pure CO2 system. The densities of some CO2 inclusions were computed in terms of Raman spectroscopic characteristics of CO2 Fermi resonance at room temperature. Their densities change over a wide range, but mainly between 0.044 g/cm3 and 0.289 g/cm3. Their micro-thermometric measurements showed that the CO2 inclusions examined reached homogenization between 1145.5℃ and 1265℃ . The mean value of homogenization temperatures of CO2 inclusions in basalts is near 1210℃. The trap pressures (depths) of inclusions were computed with the equation of state and computer program. Distribution of the trap depths makes it know that the degassing of magma can happen over a wide pressure (depth) range, but mainly at the depth of 0.48 km to 3.85 km. This implicates that basalt magma experienced intensive degassing and the CO2 gas reservoir from the basalt magma also may be formed in this range of depths. The results of this study showed that the depth of basalt magma degassing can be forecasted from CO2 fluid inclusions, and it is meaningful for understanding the process of magma degassing and constraining the inorganogenic CO2 gas reservoir. 相似文献
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The present analysis adjusts previous estimates of global ocean CaCO3 production rates substantially upward, to 133 × 1012 mol yr?1 plankton production and 42 × 1012 mol yr?1 shelf benthos production. The plankton adjustment is consistent with recent satellite-based estimates; the benthos adjustment includes primarily an upward adjustment of CaCO3 production on so-called carbonate-poor sedimentary shelves and secondarily pays greater attention to high CaCO3 mass (calcimass) and turnover of shelf communities on temperate and polar shelves. Estimated CaCO3 sediment accumulation rates remain about the same as they have been for some years: ~20 × 1012 mol yr?1 on shelves and 11 × 1012 mol yr?1 in the deep ocean. The differences between production and accumulation of calcareous materials call for dissolution of ~22 × 1012 mol yr?1 (~50 %) of shelf benthonic carbonate production and 122 × 1012 mol yr?1 (>90 %) of planktonic production. Most CaCO3 production, whether planktonic or benthonic, is assumed to take place in water depths of <100 m, while most dissolution is assumed to occur below this depth. The molar ratio of CO2 release to CaCO3 precipitation (CO2↑/CaCO3↓) is <1.0 and varies with depth. This ratio, Ψ, is presently about 0.66 in surface seawater and 0.85 in ocean waters deeper than about 1000 m. The net flux of CO2 associated with CaCO3 reactions in the global ocean in late preindustrial time is estimated to be an apparent influx from the atmosphere to the ocean, of +7 × 1012 mol C yr?1, at a time scale of 102–103 years. The CaCO3-mediated influx of CO2 is approximately offset by CO2 release from organic C oxidation in the water column. Continuing ocean acidification will have effects on CaCO3 and organic C metabolic responses to the oceanic inorganic C cycle, although those responses remain poorly quantified. 相似文献
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A. A. Borisov 《Petrology》2007,15(6):523-529
The solubility of cobalt and iron in silicate melts with variable SiO2 content was experimentally determined under controlled oxygen fugacity. It was shown that, independent of temperature and oxygen fugacity, the solubility of the two metals reaches a maximum (minimum of CoO and FeO activity coefficients) in melts of intermediate compositions. The analysis of available published data demonstrated that the γMeO values of at least four metals (Ni, Co, Fe, and Cr) dissolving in melts as divalent oxides show a minimum in melts with \(X_{SiO_2 } \) ≈ 57 ± 2 mol %. The position of the minimum is essentially independent of the element, melt temperature, and oxide concentration (from a few ppm to 13 wt%). The extremes of iron solubility (γFeO) in Fe-rich MgO-free melts may shift toward significantly lower \(X_{SiO_2 } \) values, although this inference requires additional experimental verification. Using a numerical example, some problems were discussed in the use of experimental data obtained in different laboratories for the development of a general model for the γMeO dependence on melt composition. 相似文献
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Liwei Zhang Robert Dilmore Argha Namhata Grant Bromhal 《Computational Geosciences》2018,22(3):909-923
A numerical model was developed to investigate the potential to detect fluid migration in a (homogeneous, isotropic, with constant pressure lateral boundaries) porous and permeable interval overlying an imperfect primary seal of a geologic CO2 storage formation. The seal imperfection was modeled as a single higher-permeability zone in an otherwise low-permeability seal, with the center of that zone offset from the CO2 injection well by 1400 m. Pressure response resulting from fluid migration through the high-permeability zone was detectable up to 1650 m from the centroid of that zone at the base of the monitored interval after 30 years of CO2 injection (detection limit = 0.1 MPa pressure increase); no pressure response was detectable at the top of the monitored interval at the same point in time. CO2 saturation response could be up to 774 m from the center of the high-permeability zone at the bottom of the monitored interval, and 1103 m at the top (saturation detection limit = 0.01). More than 6% of the injected CO2, by mass, migrated out of primary containment after 130 years of site performance (including 30 years of active injection) in the case where the zone of seal imperfection had a moderately high permeability (10??17 m2 or 0.01 mD). Free-phase CO2 saturation monitoring at the top of the overlying interval provides favorable spatial coverage for detecting fluid migration across the primary seal. Improved sensitivity of detection for pressure perturbation will benefit time of detection above an imperfect seal. 相似文献
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Erin Jing Male William L. Pickles Eli A. Silver Gary D. Hoffmann Jennifer Lewicki Martha Apple Kevin Repasky Elizabeth A. Burton 《Environmental Earth Sciences》2010,60(2):251-261
Hyperspectral plant signatures can be used as a short-term, as well as long-term (100-year timescale) monitoring technique
to verify that CO2 sequestration fields have not been compromised. An influx of CO2 gas into the soil can stress vegetation, which causes changes in the visible to near-infrared reflectance spectral signature
of the vegetation. For 29 days, beginning on July 9, 2008, pure carbon dioxide gas was released through a 100-m long horizontal
injection well, at a flow rate of 300 kg day−1. Spectral signatures were recorded almost daily from an unmown patch of plants over the injection with a “FieldSpec Pro”
spectrometer by Analytical Spectral Devices, Inc. Measurements were taken both inside and outside of the CO2 leak zone to normalize observations for other environmental factors affecting the plants. Four to five days after the injection
began, stress was observed in the spectral signatures of plants within 1 m of the well. After approximately 10 days, moderate
to high amounts of stress were measured out to 2.5 m from the well. This spatial distribution corresponded to areas of high
CO2 flux from the injection. Airborne hyperspectral imagery, acquired by Resonon, Inc. of Bozeman, MT using their hyperspectral
camera, also showed the same pattern of plant stress. Spectral signatures of the plants were also compared to the CO2 concentrations in the soil, which indicated that the lower limit of soil CO2 needed to stress vegetation is between 4 and 8% by volume. 相似文献
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CH4 and CO2 fluxes from a high-cold swamp meadow and an alpine meadow on the Qinghai-Tibetan Plateau, subject to different degrees of
degradation, were measured over a 12-month period. Air temperature, soil temperature and moisture, and the depths of the water
table and thawing-freezing layer were determined. For swamp meadows, the greater the degradation, the lesser the carbon efflux.
CH4 emissions at the nondegraded swamp meadow site were 1.09–3.5 and 2.5–11.27 times greater, and CO2 emissions 1.08–1.69 and 1.41–4.43 times greater, respectively, than those from moderately and severely degraded sites. For
alpine meadows, the greater the degradation, the greater the CH4 consumption and CO2 emissions. CH4 consumption at the severely degraded alpine meadow site was 6.6–21 and 1.1–5.25 times greater, and CO2 emissions 1.05–78.5 and 1.04–6.28 times greater, respectively, than those from the nondegraded and moderately degraded sites.
The CH4 and CO2 fluxes at both sites were significantly correlated (R
2 > 0.59, P < 0.05) with air temperature, soil temperature, and topsoil (0–5 cm depth) moisture, indicating these to be the main environmental
factors affecting such fluxes. 相似文献
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After more than a decade of multidisciplinary studies of the Central American subduction zone mainly in the framework of two large research programmes, the US MARGINS program and the German Collaborative Research Center SFB 574, we here review and interpret the data pertinent to quantify the cycling of mineral-bound volatiles (H2O, CO2, Cl, S) through this subduction system. For input-flux calculations, we divide the Middle America Trench into four segments differing in convergence rate and slab lithological profiles, use the latest evidence for mantle serpentinization of the Cocos slab approaching the trench, and for the first time explicitly include subduction erosion of forearc basement. Resulting input fluxes are 40–62 (53) Tg/Ma/m H2O, 7.8–11.4 (9.3) Tg/Ma/m CO2, 1.3–1.9 (1.6) Tg/Ma/m Cl, and 1.3–2.1 (1.6) Tg/Ma/m S (bracketed are mean values for entire trench length). Output by cold seeps on the forearc amounts to 0.625–1.25 Tg/Ma/m H2O partly derived from the slab sediments as determined by geochemical analyses of fluids and carbonates. The major volatile output occurs at the Central American volcanic arc that is divided into ten arc segments by dextral strike-slip tectonics. Based on volcanic edifice and widespread tephra volumes as well as calculated parental magma masses needed to form observed evolved compositions, we determine long-term (105 years) average magma and K2O fluxes for each of the ten segments as 32–242 (106) Tg/Ma/m magma and 0.28–2.91 (1.38) Tg/Ma/m K2O (bracketed are mean values for entire Central American volcanic arc length). Volatile/K2O concentration ratios derived from melt inclusion analyses and petrologic modelling then allow to calculate volatile fluxes as 1.02–14.3 (6.2) Tg/Ma/m H2O, 0.02–0.45 (0.17) Tg/Ma/m CO2, and 0.07–0.34 (0.22) Tg/Ma/m Cl. The same approach yields long-term sulfur fluxes of 0.12–1.08 (0.54) Tg/Ma/m while present-day open-vent SO2-flux monitoring yields 0.06–2.37 (0.83) Tg/Ma/m S. Input–output comparisons show that the arc water fluxes only account for up to 40 % of the input even if we include an “invisible” plutonic component constrained by crustal growth. With 20–30 % of the H2O input transferred into the deeper mantle as suggested by petrologic modeling, there remains a deficiency of, say, 30–40 % in the water budget. At least some of this water is transferred into two upper-plate regions of low seismic velocity and electrical resistivity whose sizes vary along arc: one region widely envelopes the melt ascent paths from slab top to arc and the other extends obliquely from the slab below the forearc to below the arc. Whether these reservoirs are transient or steady remains unknown. 相似文献
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We designed and carried out experiments to investigate the effect of H2O on the liquidus temperature of olivine-saturated primitive melts. The effect of H2O was isolated from other influences by experimentally determining the liquidus temperatures of the same melt composition
with various amounts of H2O added. Experimental data indicate that the effect of H2O does not depend on pressure or melt composition in the basaltic compositional range. The influence of H2O on melting point lowering can be described as a polynomial function
This expression can be used to account for the effect of H2O on olivine-melt thermometers, and can be incorporated into fractionation models for primitive basalts. The non-linear effect
of H2O indicates that incorporation of H2O in silicate melts is non-ideal, and involves interaction between H2O and other melt components. The simple speciation approach that seems to account for the influence of H2O in simple systems (albite-H2O, diopside-H2O) fails to describe the mixing behavior of H2O in multi-component silicate melts. However, a non-ideal solution model that treats the effect of H2O addition as a positive excess free energy can be fitted to describe the effect of melting point lowering. 相似文献
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Assessing potential repositories for geologic sequestration of carbon dioxide using numerical models can be complicated, costly,
and time-consuming, especially when faced with the challenge of selecting a repository from a multitude of potential repositories.
This paper presents a set of simple analytical equations (model), based on the work of previous researchers, that could be
used to evaluate the suitability of candidate repositories for subsurface sequestration of carbon dioxide. We considered the
injection of carbon dioxide at a constant rate into a confined saline aquifer via a fully perforated vertical injection well.
The validity of the analytical model was assessed via comparison with the TOUGH2 numerical model. The metrics used in comparing
the two models include (1) spatial variations in formation pressure and (2) vertically integrated brine saturation profile.
The analytical model and TOUGH2 show excellent agreement in their results when similar input conditions and assumptions are
applied in both. The analytical model neglects capillary pressure and the pressure dependence of fluid properties. However,
simulations in TOUGH2 indicate that little error is introduced by these simplifications. Sensitivity studies indicate that
the agreement between the analytical model and TOUGH2 depends strongly on (1) the residual brine saturation, (2) the difference
in density between carbon dioxide and resident brine (buoyancy), and (3) the relationship between relative permeability and
brine saturation. The results achieved suggest that the analytical model is valid when the relationship between relative permeability
and brine saturation is linear or quasi-linear and when the irreducible saturation of brine is zero or very small. 相似文献
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Theodore C. Labotka Lawrence M. Anovitz James G. Blencoe 《Contributions to Mineralogy and Petrology》2002,144(3):305-313
The molar volume of mixtures of CO2 and H2O is a strong function of the fluid composition. Both CO2 and H2O participate in the metamorphism of carbonate rocks, resulting in a change in the fluid composition during reaction. One of the effects of the change in composition is the increase in pore-fluid pressure with only small increases in extent of reaction, ;. Pressure calculated from the volumetric properties of CO2-H2O mixtures at 400 °C increases greatly with small increases of ; but drops at greater values because of the increase in pore volume as a result of (Vsolid. The pore pressure increase at small values of ;, though, readily exceeds the reported tensile strength of carbonate rocks, and the rock cannot sustain significant reaction without fracturing. The result of a small amount of reaction is a fractured rock with increased permeability, which promotes fluid transport. 相似文献