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1.
Cave air PCO2 at two Irish sites varied dramatically on daily to seasonal timescales, potentially affecting the timing of calcite deposition and consequently climate proxy records derived from stalagmites collected at the same sites. Temperature-dependent biochemical processes in the soil control CO2 production, resulting in high summer PCO2 values and low winter values at both sites. Large Large-amplitude, high-frequency variations superimposed on this seasonal cycle reflect cave air circulation. Here we model stalagmite growth rates, which are controlled partly by CO2 degassing rates from drip water, by considering both the seasonal and high-frequency cave air PCO2 variations. Modeled hourly growth rates for stalagmite CC-Bil from Crag Cave in SW Ireland reach maxima in late December (0.063 μm h− 1) and minima in late June/early July (0.033 μm h− 1). For well-mixed ‘diffuse flow’ cave drips such as those that feed CC-Bil, high summer cave air PCO2 depresses summer calcite deposition, while low winter PCO2 promotes degassing and enhances deposition rates. In stalagmites fed by well-mixed drips lacking seasonal variations in δ18O, integrated annual stalagmite calcite δ18O is unaffected; however, seasonality in cave air PCO2 may influence non-conservative geochemical climate proxies (e.g., δ13C, Sr/Ca). Stalagmites fed by ‘seasonal’ drips whose hydrochemical properties vary in response to seasonality may have higher growth rates in summer because soil air PCO2 may increase relative to cave air PCO2 due to higher soil temperatures. This in turn may bias stalagmite calcite δ18O records towards isotopically heavier summer drip water δ18O values, resulting in elevated calcite δ18O values compared to the ‘equilibrium’ values predicted by calcite–water isotope fractionation equations. Interpretations of stalagmite-based paleoclimate proxies should therefore consider the consequences of cave air PCO2 variability and the resulting intra-annual variability in calcite deposition rates.  相似文献   

2.
The temperatures induced in crystalline calcite (CaCO3) upon planar shock compression (95-160 GPa) are reported from two-stage light gas gun experiments. Temperatures of 3300-5400 K are obtained by fitting six-channel optical pyrometer radiances in the 450-900 nm range to the Planck gray-body radiation law. Thermodynamic calculations demonstrate that these temperatures are some 400-1350 K lower than expected for vibronic excitations of the lattice with a 3R/mole-atom specific heat (R is gas constant). The temperature deficit along the Hugoniot is larger than that expected from only melting. In addition to melting, it appears likely that shock-induced decomposition of calcite occurs behind the shock front. We modeled disproportionation of calcite into CaO (solid) plus CO2 (gas). For temperature calculations, specific heat at constant volume for 1 mole of CO2 is taken to be 6.7R as compared to 9R in the solid state; whereas a mole of calcite and a mole of CaO have their solid state values 15R and 6R, respectively. Calculations suggest that the calcite decomposes to CaO and CO2 at ∼110±10 GPa along the Hugoniot. Recent reanalysis of earlier VISAR measurements of particle velocity profiles [1] indicates that calcite shocked to 18 GPa undergoes disproportionation at much lower pressures upon isentropic expansion.  相似文献   

3.
Accurate modeling of storage of carbon dioxide (CO2) in heterogeneous aquifers requires experiments of the capillary pressure as function of temperature and pressure. We present a method with which static drainage and imbibition capillary pressures can be measured continuously as a function of saturation at various temperature (T) and pressure (P) conditions. The measurements are carried out at (T, P) conditions of practical interest. Static conditions can be assumed as small injection rates are applied. The capillary pressure curves are obtained for the unconsolidated sand–distilled water–CO2 system. The experimental results show a decrease of drainage and imbibition capillary pressure for increasing CO2 pressures and pronounced dissolution rate effects for gaseous CO2. Significant capillary pressure fluctuations and negative values during imbibition are observed at near critical conditions. The measurement procedure is validated by a numerical model that simulates the experiments.  相似文献   

4.
At 30 kbar, calcite melts congruently at 1615°C, and grossularite melts incongruently to liquid + gehlenite (tentative identification) at 1535°C. The assemblage calcite + grossularite melts at 1450°C to produce liquid + vapor, with piercing point at about 49 wt.% CaCO3. Vapor phase is present in all hypersolidus phase fields except for those with less than about 7% CaCO3 or 8% Ca3Al2Si3O12. These results, together with known liquidus data for CaO—SiO2—CO2 and inferred results for CaO—Al2O3—CO2 and Al2O3—SiO2—CO2, permit construction of the position of the CO2- saturated liquidus surface in the quaternary system, and estimation of the positions of liquidus field boundaries separating some of the primary crystallization fields on this surface. The field of calcite is separated from those for grossularite and quartz by a field boundary with about 50% dissolved CaCO3. Crystallization paths of silicate liquids in the range Ca2SiO4—Ca3Al2Si3O12—SiO2, with some dissolved CO2, will terminate at a quaternary eutectic on this field boundary, with the precipitation of calcite together with grossularite and quartz, at a temperature below 1450°C. Addition of Al2O3 to CaO—SiO2—CO2 in amounts sufficient to stabilize garnet thus causes little change in the general liquidus pattern as far as carbonates and silicates are concerned. With addition of MgO, we anticipate that silicate liquids with dissolved CO2 will also follow liquidus paths to fields for the precipitation of carbonates; we conclude that similar paths link kimberlite and some carnbonatite magmas.  相似文献   

5.
Surface partial pressure of CO2 (pCO2), temperature, salinity, nutrients, and chlorophyll a were measured in the East China Sea (ECS; 31°30′–34°00′N to 124°00′–127°30′E) in August 2003 (summer), May 2004 (spring), October 2004 (early fall), and November 2005 (fall). The warm and saline Tsushima Warm Current was observed in the eastern part of the survey area during four cruises, and relatively low salinity waters due to outflow from the Changjiang (Yangtze River) were observed over the western part of the survey area. Surface pCO2 ranged from 236 to 445 μatm in spring and summer, and from 326 to 517 μatm in fall. Large pCO2 (values >400 μatm) occurred in the western part of the study area in spring and fall, and in the eastern part in summer. A positive linear correlation existed between surface pCO2 and temperature in the eastern part of the study area, where the Tsushima Warm Current dominates; this correlation suggests that temperature is the major factor controlling surface pCO2 distribution in that area. In the western part of the study area, however, the main controlling factor is different and seasonally complex. There is large transport in this region of Changjiang Diluted Water in summer, causing low salinity and low pCO2 values. The relationship between surface pCO2 and water stability suggests that the amount of mixing and/or upwelling of CO2-rich water might be the important process controlling surface pCO2 levels during spring and fall in this shallow region. Sea–air CO2 flux, based on the application of a Wanninkhof [1992. Relationship between wind speed and gas exchange over the ocean. Journal of Geophysical Research 97, 7373–7382] formula for gas transfer velocity and a set of monthly averaged satellite wind data, were −5.04±1.59, −2.52±1.81, 1.71±2.87, and 0.39±0.18 mmol m−2 d−1 in spring, summer, early fall, and fall, respectively, in the northern ECS. The ocean in this study area is therefore a carbon sink in spring and summer, but a weak source or in equilibrium with the atmosphere in fall. If the winter flux value is assumed to have been the mean of autumnal and vernal values, then the northern ECS absorbs about 0.013 Pg C annually. That result suggests that the northern ECS is a net sink for atmospheric CO2, a result consistent with previous studies.  相似文献   

6.
Fluid inclusion studies have been used to derive a model for fluid evolution in the Hohi geothermal area, Japan. Six types of fluid inclusions are found in quartz obtained from the drill core of DW-5 hole. They are: (I) primary liquid-rich with evidence of boiling; (II) primary liquid-rich without evidence of boiling; (III) primary vapor-rich (assumed to have been formed by boiling); (IV) secondary liquid-rich with evidence of boiling; (V) secondary liquid-rich without evidence of boiling; (VI) secondary vapor-rich (assumed to have been formed by boiling). Homogenization temperatures (Th) range between 196 and 347°C and the final melting point of ice (Tm) between −0.2 and −4.3°C. The CO2 content was estimated semiquantitatively to be between 0 and 0.39 wt. % based on the bubble behavior on crushing. NaCl equivalent solid solute salinity of fluid inclusions was determined as being between 0 and 6.8 wt. % after minor correction for CO2 content.Fluid inclusions in quartz provide a record of geothermal activity of early boiling and later cooling. The CO2 contents and homogenization temperatures of fluid inclusions with evidence of boiling generally increase with depth; these changes, and NaCl equivalent solid solute salinity of the fluid can be explained by an adiabatic boiling model for a CO2-bearing low-salinity fluid. Some high-salinity inclusions without CO2 are presumed to have formed by a local boiling process due to a temperature increase or a pressure decrease. The liquid-rich primary and secondary inclusions without evidence of boiling formed during the cooling process. The salinity and CO2 content of these inclusions are lower than those in the boiling fluid at the early stage, probably as a result of admixture with groundwater.  相似文献   

7.
Oxygen self diffusion rates were determined in quartz samples exchanged with18O-enriched CO2 between 745 and 900°C and various pressures, and the diffusion profiles were measured using an ion microprobe. The activation energy (Q) and preexponential factor (D0) at P(CO2) = P(tot) = 100 bar, for diffusion parallel to the c-axis are 159 ( ± 13) kJ/g atom and 2.10 (+0.75/ −0.55) × 10−8 cm2/s. This rate is approximately 100 times slower than that obtained from hydrothermal experiments and 100 times faster than a previous 1-bar quartz-O2 exchange experiment. The oxygen diffusion rate measured at 0.6 bar, 888°C, and at 900°C in vacuum is in agreement with the previous 1-bar exchange experiments with18O2. The effect of higher CO2 pressures is small. At 900°C, the diffusion rate exchanged with CO2 is = 2.35 × 10−15 cm2/s at 100 bar, 2.24 × 10−15 cm2/s at 3.45 kbar and 8.13 × 10−15 cm2/s at 7.2 kbar.There is probably a diffusing species, other than oxygen, that enhances the oxygen diffusion rate in these quartz-CO2 systems, relative to that occurring at very low pressures or in a vacuum. The effect of this diffusing species, however, is not as strong as that associated with H2O. Preserved oxygen isotope fractionations between coexisting minerals in a slowly cooled, high-grade metamorphic terrane will vary depending upon whether a water-rich phase was present or not. Closure temperatures will be approximately 100°C higher in rocks where no water-rich phase was present during cooling. The measured fractionations between coexisting minerals in metamorphic rocks may potentially be used as a sensor of water presence during retrogression.  相似文献   

8.
The use of regional attenuation in computing the local magnitude, ML, from strong motion data gathered at distances less than 100 km may lead to systematic underestimates approaching 0·5 magnitude units (Trifunac & Herak, Soil Dynamics and Earthquake Engineering, 1992, 18, 229-41). The use of the attenuation law Att(Δ), for example, with synthetic estimates of Wood-Anderson seismometer response, during the Loma Preita earthquake, leads to estimates of ML which agree with the surface wave and moment magnitudes, and which are essentially distance-independent.  相似文献   

9.
To improve understanding of Ca isotope transport during water-rock interaction on the continents, we measured dissolved δ44Ca values along a 236 km flow path in the Madison aquifer, South Dakota, where fluids have chemically evolved according to dolomite and anhydrite dissolution, calcite precipitation, and Ca-for-Na ion-exchange over a timescale spanning ~ 15 kyr. We used a reactive transport model employing rate data constrained from major ion mass-balances to evaluate the extent to which calcite precipitation and ion-exchange fractionate Ca isotopes. Elevated δ44Ca values during the initial and final stages of water transport possibly result from calcite precipitation under supersaturated conditions and Ca-for-Na ion-exchange, respectively. However, for the bulk of the flow path, δ44Ca values evolve by mixing between anhydrite and dolomite dissolution, with no fractionation during calcite precipitation under saturated conditions. We attribute the absence of Ca isotope fractionation to the long timescale of water-rock interaction and slow rate of calcite precipitation, which have enabled fluids to chemically and isotopically equilibrate with calcite. We therefore conclude that the equilibrium Ca isotope fractionation factor between calcite and water (Δcal–w) is very close to zero. To the extent that the Madison aquifer typifies other groundwater systems where calcite slowly precipitates from solutions at or near chemical equilibrium, this study suggests that groundwater contributions to δ44Ca variability on the continents can be modeled according to simple mixing theory without invoking isotope discrimination.  相似文献   

10.
The equilibrium distribution of CO2H2O fluids in synthetic rock samples (principally dunite and quartzite) has been characterized by measurements of the dihedral wetting angle, θ, resulting from 5-day annealing periods at 950–1150°C and 1 GPa. For fluids in equilibrium with polycrystalline quartz, θ varies systematically from 57° for pure H2O to 90° at XCO2 0.9. Similarly, for San Carlos olivine, θ varies from 65° for pure H2O to 90° at XCO2 0.9. The addition of solutes (NaCl, KCl, CaF2, Na2CO3) to H2O causes a major decrease in θ in the quartz/fluid system (to values as low as 40°), but has no effect on fluid wetting in dunite. Reconnaissance experiments on other mono- and polymineralic aggregates indicate universally high wetting angles (θ 60°) in upper mantle assemblages and for CO2 in felsic compositions. For diopside + H2O, θ 80°, with large variation due to crystalline anisotropy. In no case does θ approach 0°, the condition necessary for fluid to be present along all grain boundaries.Because a value of θ greater than 60° precludes the existence of an interconnected fluid phase in a rock, our results have important implications not only for fluid transport but also for the physical properties of the bulk fluid/rock system. Any static fluid present in the upper mantle must exist as isolated pores located primarily at grain corners, and transport can occur only by hydrofracture. In the continental crust, aqueous fluids (especially saline ones) are likely to form an interconnected network along grain edges, thus contributing to high electrical conductivity and allowing the possibility of fluid transport by porous flow or surface energy-driven infiltration.  相似文献   

11.
A theoretical model is derived in which isotopic fractionations can be calculated as a function of variations in dissolved carbonate species on CO2 degassing and calcite precipitation. This model is tested by application to a calcite-depositing spring system near Westerhof, Germany. In agreement with the model,13C of the dissolved carbonate species changes systematically along the flow path. The difference in δ values between the upper and lower part of the stream is about 1‰. The13C content of the precipitated calcite is different from that expected from the theoretical partitioning. The isotopic composition of the solid CaCO3 is similar to that of the dissolved carbonate, though in theory it should be isotopically heavier by about 2.4‰. The18O composition of dissolved carbonate and H2O is constant along the stream. Calculated calcite-water temperatures differ by about +5°C from the observed temperatures demonstrating isotopic disequilibrium between the water and precipitated solid. This is attributed to kinetic effects during CaCO3 deposition from a highly supersaturated solution, in which precipitation is faster than equilibration with respect to isotopes.Plant populations in the water have virtually no influence on CO2 degassing, calcite saturation and isotopic fractionation. Measurements of PCO2, SC and13C within a diurnal cycle demonstrate that metabolic effects are below the detection limit in a system with a high supply-rate of dissolved carbonate species. The observed variations are due to differences in CO2 degassing and calcite precipitation, caused by continuously changing hydrodynamic conditions and carbonate nucleation rates.  相似文献   

12.
In a series of experiments at 0.5–1.3 GPa and 1050–1200°C we have monitored the transport, via crack propagation, of CO2 into well-annealed olivine and quartz aggregates. The objectives were to determine (1) the extent and rate of fluid penetration; (2) the effect of varying both P-T conditions and microstructure; and (3) the fluid penetration pathways. Experiments on CO2 penetration into dunite annealed in the absence of MgO indicate rapid and pervasive fluid transport on a grain-dimension scale, but a limited penetration distance ( 1 mm). Additional experiments on dunite annealed in the presence of MgO (either dispersed or present at both ends), however, resulted in CO2 penetration that was both pervasive on the scale of individual grains and almost always completely through the 5 mm long samples. The abundance of fine (10 μm) grains in the MgO-free dunite, in contrast to the much larger grain sizes of the samples annealed with MgO present, suggests the difference in fluid penetration behavior may arise because the strength variation in dunite scales with the grain size. Effects arising from changes in olivine point defect chemistry, however, are an additional possibility. The response of synthetic quartzite to CO2 overpressure is distinct from that of dunite: Quartzite experiences rapid and complete penetration of CO2, via a macroscopically visible system of transgranular fractures, over the range of P-T conditions investigated.The small amount of porosity ( 2–3%) present in most rock samples fabricated for this study, lacks three-dimensional connectivity, thus precluding any enhanced fluid penetration via porous flow. Pores could possibly enhance fluid penetration as the result of a small reduction in resistance to fracture, but the probable abundance of strength-controlling flaws in natural rocks is likely to produce similar behavior.The results of our experiments on olivine and olivine + MgO suggest that the transport of pressurized CO2 in very olivine-rich mantle environments will be pervasive on the scale of individual grains and its extent may be dependent on rock microstructure and/or crystal chemical effects. Such pervasive fluid transport, perhaps associated with magma decarbonation, may have interesting implications for both magma transport and local LREE enrichment of adjacent mantle wall-rock. The ease with which quartzite is penetrated by CO2 at the conditions of our experiments underscores the possible role of decarbonation reactions in crustal permeability-enhancement processes.  相似文献   

13.
The Bay of Biscay is part of the North Atlantic Ocean, the most important sink of CO2, and a subduction zone of mode waters that favours the entry of carbon to the ocean interior. To investigate the seasonal and interannual variability of CO2 uptake, continuous underway measurements of the partial pressure of CO2 at sea surface were performed along a commercial route between Vigo (Spain) and St. Nazaire (France). An unattended measuring system of CO2 fugacity (fCO2), with meteorological station, and temperature, salinity, oxygen and fluorescence sensors, was installed on board of ships of opportunity (RO-RO L’Audace and RO-RO Surprise).  相似文献   

14.
The carbon isotopic composition of diagenetic dolomite and calcite in some sediments of the Gulf of Mexico varies between “normal-marine” (δ13C ca. 0‰) and −14.6‰ which suggests that biogenic CO2 contributed to the carbonate formation. The δ13O values of dolomite and coexisting calcite are very similar but variable down-core.Dolomite and calcite precipitated early from pore water where SO42− was not reduced. However, during (and after?) SO42− reduction dolomite and calcite still formed and there are at least two generations of carbonate minerals present.  相似文献   

15.
The elastic moduli of single-crystal CaF2, SrF2 and BaF2 have been determined by the ultrasonic pulse superposition technique as a function of temperature from T = 298 to T = 650°K. These new data are consistent with other data obtained by ultrasonic pulse techniques in the region of room temperature and are superior to previous high-temperature data from resonance experiments. The elastic moduli (c) are represented by quadratic functions in T over the experimental temperature range with the curvature in the same sense for all the moduli. Evaluation of the temperature derivatives of the elastic moduli at constant volume indicates that the dominant temperature effect is extrinsic for (?KS/?T)P and intrinsic for (?μ/?T)P, where KS and μ are the isotropic bulk and shear moduli, respectively. For the series CaF2SrF2BaF2, |(?c/?T)p| decreases with increasing molar volume for all moduli; however there are no theoretical or empirical grounds on which to derive a simple relationship between (?c/?T)P and crystallographic parameters.  相似文献   

16.
The oxygen minimum zones (OMZs) are recognized as intense sources of N2O greenhouse gas (GHG) and could also be potential sources of CO2, the most important GHG for the present climate change. This study evaluates, for one of the most intense and shallow OMZ, the Chilean East South Pacific OMZ, the simultaneous N2O and CO2 fluxes at the air–sea interface. Four cruises (2000–2002) and 1 year of monitoring (21°–30°–36°S) off Chile allowed the determination of the CO2 and N2O concentrations at the sea surface and the analysis of fluxes variations associated with different OMZ configurations. The Chilean OMZ area can be an intense GHG oceanic local source of both N2O and CO2. The mean N2O fluxes are 5–10 times higher than the maximal previous historical source in an OMZ open area as in the Pacific and Indian Oceans. For CO2, the mean fluxes are also positive and correspond to very high oceanic sources. Even if different coupling and decoupling between N2O and CO2 are observed along the Chilean OMZ, 65% of the situations represent high CO2 and/or N2O sources. The high GHG sources are associated with coastal upwelling transport of OMZ waters rich in N2O and probably also in CO2, located at a shallow depth. The integrated OMZ role on GHG should be better considered to improve our understanding of the past and future atmospheric CO2 and N2O evolutions.  相似文献   

17.
The effectiveness of CO2 storage in deep saline aquifers and hydrocarbon reservoirs is governed, among other factors, by the interfacial tension between the injected CO2 and formation water (brine). Experimental data on CO2/water and CO2/NaCl solution have revealed that the interfacial tension depends on the pressure, temperature and water salinity. However, there is still a lack of data for other salts (such as MgCl2 and CaCl2) which are also present in aquifers and carbonate reservoirs.  相似文献   

18.
13C and ΣCO2 data from the North and South Atlantic, the Antarctic, and the North and South Pacific are given. The δ13C of the ΣCO2 in the deep water (～3000m) decreases from 1.7‰ in the North Atlantic to ?0.10‰ in the North Pacific. This change is attributed to the addition of about 158 μmoles of CO2 per kg of seawater. The in-situ oxidation of organic matter accounts for 83% of this increase in ΣCO2, while the remainder is attributed to dissolution of calcium carbonate.The δ13C of the dissolved CO2 in mid-latitude surface water samples is controlled by a quasi-steady-state equilibrium with atmospheric CO2 at a mean temperature of 16°C. The δ13C and ΣCO2 values of Antarctic surface water samples suggest that these waters are derived from a mixture of North Atlantic deep water and equilibrated surface water.  相似文献   

19.
Some planktonic groups suffer negative effects from ocean acidification (OA), although copepods might be less sensitive. We investigated the effect of predicted CO2 levels (range 480–750 ppm), on egg production and hatching success of two copepod species, Centropages typicus and Temora longicornis. In these short-term incubations there was no significant effect of high CO2 on these parameters. Additionally a very high CO2 treatment, (CO2 = 9830 ppm), representative of carbon capture and storage scenarios, resulted in a reduction of egg production rate and hatching success of C. typicus, but not T. longicornis. In conclusion, reproduction of C. typicus was more sensitive to acute elevated seawater CO2 than that of T. longicornis, but neither species was affected by exposure to CO2 levels predicted for the year 2100. The duration and seasonal timing of exposures to high pCO2, however, might have a significant effect on the reproduction success of calanoid copepods.  相似文献   

20.
In the join CaCO3-CaSiO3 at 30 kbars, calcite melts at 1615°C, wollastonite II at 1600°C, and a binary eutectic occurs at 1365°C with liquid composition 43 wt.% CaCO3, 57 wt.% CaSiO3. The eutectic liquid quenches to a glass with few quench crystals. In the join MgCO3-MgSiO3 at 30 kbars, magnesite melts at 1590°C, enstatite at 1837°C, and the fields for the primary crystallization of magnesite and enstatite are separated by a thermal barrier near 1900°C for the melting of forsterite in the presence of CO2. Only about 10 wt.% MgSiO3 dissolves in the carbonate liquid. These data, are considered together with incomplete results for joins CaMgSi2O6-CaMg(CO3)2, CaMgSi2O6-MgCO3, CaMgSi2O6-CaCO3, and other published data in the system CaO-MgO-SiO2-CO2. A thermal barrier separates the silicate and carbonate liquids in MgO-SiO2-CO2 but, in the quaternary system, silicate liquids with dissolved CO2 can follow fractionation paths around the forsterite field to the fields for the primary crystallization of carbonates. This suggests that fractional crystallization of CO2-bearing ultrabasic magma at 100 km depth can produce residual carbonatite magma.  相似文献   

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