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1.
This study was aimed to test a new methodological approach to carry out measurements of gaseous elemental mercury (GEM) diffusively emitted from soils in hydrothermal-volcanic environments. This method was based on the use of a static closed-chamber (SCC) in combination with a Lumex® RA-915M analyzer that provides GEM measurements in a wide range of concentrations (from 2 to 50,000 ng m−3). Gas samples were collected at fixed time intervals from the SCC positioned on the ground (time-series samples). The Lumex® inlet port was equipped with a three-way Teflon valve allowing the free entrance of air through a carbon trap, in order to: (i) prevent disturbance to the Lumex® operative flow rate (10 L min−1) during the injection of the gas samples from the SCC and (ii) minimize the instability of the baseline signal induced by possible variations of GEM concentrations in air. In the lab, known amounts of GEM, pipetted from a vessel containing an Hg-saturated air in equilibrium with liquid mercury at 27 °C, were injected in the Lumex® via the modified inlet port to construct a calibration curve. The latter was used to calculate the amount of GEM in the SCC (KSCC) from the corresponding GEM concentrations measured by the Lumex® analyzer. The KSCC values of the time-series samples were proportionally increasing with the GEM fluxes (ϕGEM), thus ϕGEM values were computed according to the following equation: ϕGEM = (dKSCC/dt)/A, where A is the basal area of the SCC and dt is the time interval of the time-series sampling. Up to 214 ϕGEM measurements were carried out at Solfatara crater (Campi Flegrei, southern Italy), a hydrothermally altered tuff cone characterized by an anomalous diffuse soil emission of GEM-rich geogenic gases. The measured ϕGEM values varied up to 4 orders of magnitude, from 1,296, corresponding to the sensitivity of the method at the selected sampling time interval (1 min), to 1,957,500 ng m−2 day−1, and were consistent with those recently measured in this crater using a different method. In the field, 10 replicates were carried out in 5 selected sites, allowing to demonstrate that the proposed method has a high reproducibility (RDS < 4%). The ϕGEM and ϕCO2 values, the latter being measured in the same 214 sites by using the accumulation chamber method, showed a low correlation, although both gases were originated from the same deep source. This suggests that GEM and CO2 soil fluxes are differently affected by environmental parameters, such as soil humidity and temperature, which have a strong effect on the release of GEM from the soil, whereas they do not play a significant role in the diffuse degassing of CO2. The measured fluxes were used to compute the CO2 and GEM total outputs (402 and 5.41 × 10−6 t day−1, respectively) from the study area (92,000 m2) and to construct contour maps showing the spatial distribution of the ϕCO2 and ϕGEM values. By modifying the geometry of SCC and the time interval of the sampling series, the proposed method can be applied to the measurements of GEM soil fluxes in other geological systems and man-made environments.  相似文献   

2.
This study investigates the potential risks associated with high levels and long term exposure of carbon dioxide (CO2) on the mobility and speciation of exchangeable metals in soils. CO2 incubation batch experiments at high pressure and temperature coupled with geochemical modelling were carried out to elucidate the behaviour and mobilisation of metals and the response of soil chemical parameters as a result of long term CO2 exposure. A t-Student analysis was performed to ascertain whether differences in the mean concentration of exchangeable metals in soils before and after CO2-incubations are attributable to increase of metal molibilisation because of the long term CO2 exposure. The t-Student revealed the CO2 long term incubation was statistically significant (p < 0.05) for the exchangeable concentration of Ni, Zn, and Pb. The CO2-soil incubation induces the acidification of the pore water of soils via CO2 hydrolysis and as a consequence, it increases the exchangeable concentration of Ni, Zn, and Pb in the soils. As, Al, Cr, Cu, and Fe show a different mobilisation pattern depending on the moisture content in soils. Al3+, Fe2+, Cr3+, and Cu2+ as free cations, As as HAsO2, Pb2+and PbHCO3−, Zn2+ and ZnHCO3−, are predicted to be the predominant aqueous complexes in the pore water of the incubated soils.  相似文献   

3.
《Geochimica et cosmochimica acta》1999,63(19-20):3417-3427
In order to verify Fe control by solution - mineral equilibria, soil solutions were sampled in hydromorphic soils on granites and shales, where the occurrence of Green Rusts had been demonstrated by Mössbauer and Raman spectroscopies. Eh and pH were measured in situ, and Fe(II) analyzed by colorimetry. Ionic Activity Products were computed from aqueous Fe(II) rather than total Fe in an attempt to avoid overestimation by including colloidal particles. Solid phases considered are Fe(II) and Fe(III) hydroxides and oxides, and the Green Rusts whose general formula is [FeII1−xFeIIIx(OH)2]+x· [x/z A−z]−x, where compensating interlayer anions, A−, can be Cl−, SO42−, CO32− or OH−, and where x ranges a priori from 0 to 1. In large ranges of variation of pH, pe and Fe(II) concentration, soil solutions are (i) oversaturated with respect to Fe(III) oxides; (ii) undersaturated with respect to Fe(II) oxides, chloride-, sulphate- and carbonate-Green Rusts; (iii) in equilibrium with hydroxy-Green Rusts, i.e., Fe(II)-Fe(III) mixed hydroxides. The ratios, x = Fe(III)/Fet, derived from the best fits for equilibrium between minerals and soil solutions are 1/3, 1/2 and 2/3, depending on the sampling site, and are in every case identical to the same ratios directly measured by Mössbauer spectroscopy. This implies reversible equilibrium between Green Rust and solution. Solubility products are proposed for the various hydroxy-Green Rusts as follows: log Ksp = 28.2 ± 0.8 for the reaction Fe3(OH)7 + e− + 7 H+ = 3 Fe2+ + 7 H2O; log Ksp = 25.4 ± 0.7 for the reaction Fe2(OH)5 + e− + 5 H+ = 2 Fe2+ + 5 H2O; log Ksp = 45.8 ± 0.9 for the reaction Fe3(OH)8 + 2e− + 8 H+ = 3 Fe2+ + 8 H2O at an average temperature of 9 ± 1°C, and 1 atm. pressure. Tentative values for the Gibbs free energies of formation of hydroxy-Green Rusts obtained are: ΔfG° (Fe3(OH)7, cr, 282.15 K) = −1799.7 ± 6 kJ mol−1, ΔfG° (Fe2(OH)5, cr, 282.15 K) = −1244.1 ± 6 kJ mol−1 and ΔfG° (Fe3(OH)8, cr, 282.15 K) = −1944.3 ± 6 kJ mol−1.  相似文献   

4.
The speciation of CO2 in dacite, phonolite, basaltic andesite, and alkali silicate melt was studied by synchrotron infrared spectroscopy in diamond anvil cells to 1,000 °C and more than 200 kbar. Upon compression to 110 kbar at room temperature, a conversion of molecular CO2 into a metastable carbonate species was observed for dacite and phonolite glass. Upon heating under high pressure, molecular CO2 re-appeared. Infrared extinction coefficients of both carbonate and molecular CO2 decrease with temperature. This effect can be quantitatively modeled as the result of a reduced occupancy of the vibrational ground state. In alkali silicate (NBO/t = 0.98) and basaltic andesite (NBO/t = 0.42) melt, only carbonate was detected up to the highest temperatures studied. For dacite (NBO/t = 0.09) and phonolite melts (NBO/t = 0.14), the equilibrium CO2 + O2? = CO3 2? in the melt shifts toward CO2 with increasing temperature, with ln K = ?4.57 (±1.68) + 5.05 (±1.44) 103 T ?1 for dacite melt (ΔH = ?42 kJ mol?1) and ln K = ?6.13 (±2.41) + 7.82 (±2.41) 103 T ?1 for phonolite melt (ΔH = ?65 kJ mol?1), where K is the molar ratio of carbonate over molecular CO2 and T is temperature in Kelvin. Together with published data from annealing experiments, these results suggest that ΔS and ΔH are linear functions of NBO/t. Based on this relationship, a general model for CO2 speciation in silicate melts is developed, with ln K = a + b/T, where T is temperature in Kelvin and a = ?2.69 ? 21.38 (NBO/t), b = 1,480 + 38,810 (NBO/t). The model shows that at temperatures around 1,500 °C, even depolymerized melts such as basalt contain appreciable amounts of molecular CO2, and therefore, the diffusion coefficient of CO2 is only slightly dependent on composition at such high temperatures. However, at temperatures close to 1,000 °C, the model predicts a much stronger dependence of CO2 solubility and speciation on melt composition, in accordance with available solubility data.  相似文献   

5.
Annually laminated carbonates, known as tufas, commonly develop in limestone areas and typically record seasonal patterns of oxygen- and carbon-isotope compositions. δ18O values are principally controlled by seasonal changes of water temperature, whereas δ13C values are the result of complex reactions among the gaseous, liquid, and solid sources of carbon in the system. We examined the processes that cause the seasonal patterns of δ13C in groundwater systems at three tufa-depositing sites in southwestern Japan by applying model calculations to geochemical data. Underground inorganic carbon species are exchanged with gaseous CO2, which is mainly introduced to the underground hydrological system by natural atmospheric ventilation and by diffusion of soil air. These processes control the seasonal pattern of δ13C, which is low in summer and high in winter. Among the three sites we investigated, we identified two extreme cases of the degree of carbon exchange between liquid and gaseous phases. For the case with high radiocarbon composition (Δ14C) and low pCO2, there was substantial carbon exchange because of a large contribution of atmospheric CO2 and a small water mass. For the other extreme case, which was characterized by low Δ14C and high pCO2, the contribution of atmospheric CO2 was small and the water mass was relatively large. Our results suggest that at two of the three sites water residence time within the soil profile was longer than 1 year. Our results also suggested a short residence time (less than 1 year) of water in the soil profile at the site with the smallest water mass, which is consistent with large seasonal amplitude of the springwater temperature variations. The Δ14C value of tufas is closely related to the hydrological conditions in which they are deposited. If the initial Δ14C value of a tufa-depositing system is stable, 14C-chronology can be used to date paleo-tufas.  相似文献   

6.
《Geochimica et cosmochimica acta》1999,63(13-14):1969-1980
The solubility of ettringite (Ca6[Al(OH)6]2(SO4)3 · 26H2O) was measured in a series of dissolution and precipitation experiments at 5–75°C and at pH between 10.5 and 13.0 using synthesized material. Equilibrium was established within 4 to 6 days, with samples collected between 10 and 36 days. The log KSP for the reaction Ca6[Al(OH)6]2(SO4)3 · 26H2O ⇌ 6Ca2+ + 2Al(OH)4− + 3SO42− + 4OH− + 26H2O at 25°C calculated for dissolution experiments (−45.0 ± 0.2) is not significantly different from the log KSP calculated for precipitation experiments (−44.8 ± 0.4) at the 95% confidence level. There is no apparent trend in log KSP with pH and the mean log KSP,298 is −44.9 ± 0.3. The solubility product decreased linearly with the inverse of temperature indicating a constant enthalpy of reaction from 5 to 75°C. The enthalpy and entropy of reaction ΔH°r and ΔS°r, were determined from the linear regression to be 204.6 ± 0.6 kJ mol−1 and 170 ± 38 J mol−1 K−1. Using our values for log KSP, ΔH°r, and ΔS°r and published partial molal quantities for the constituent ions, we calculated the free energy of formation ΔG°f,298, the enthalpy of formation ΔH°f,298, and the entropy of formation ΔS°f,298 to be −15211 ± 20, −17550 ± 16 kJ mol−1, and 1867 ± 59 J mol−1 K−1. Assuming ΔCP,r is zero, the heat capacity of ettringite is 590 ± 140 J mol−1 K−1.  相似文献   

7.
《Applied Geochemistry》2000,15(8):1203-1218
Ca6[Al(OH)6]2(CrO4)3·26H2O, the chromate analog of the sulfate mineral ettringite, was synthesized and characterized by X-ray diffraction, Fourier transform infra-red spectroscopy, thermogravimetric analyses, energy dispersive X-ray spectrometry, and bulk chemical analyses. The solubility of the synthesized solid was measured in a series of dissolution and precipitation experiments conducted at 5–75°C and at initial pH values between 10.5 and 12.5. The ion activity product (IAP) for the reaction Ca6[Al(OH)6]2(CrO4)3·26H2O⇌6Ca2++2Al(OH)−4+3CrO2−4+4OH−+26H2O varies with pH unless a CaCrO4(aq) complex is included in the speciation model. The log K for the formation of this complex by the reaction Ca2++CrO2−4=CaCrO4(aq) was obtained by minimizing the variance in the IAP for Ca6[Al(OH)6]2(CrO4)3·26H2O. There is no significant trend in the formation constant with temperature and the average log K is 2.77±0.16 over the temperature range 5–75°C. The log solubility product (log KSP) of Ca6[Al(OH)6]2(CrO4)3·26H2O at 25°C is −41.46±0.30. The temperature dependence of the log KSP is log KSP=A−B/T+D log(T) where A=498.94±48.99, B=27,499±2257, and D=−181.11±16.74. The values of ΔG0r,298 and ΔH0r,298 for the dissolution reaction are 236.6±3.9 and 77.5±2.4 kJ mol−1. the values of ΔC0P,r,298 and ΔS0r,298 are −1506±140 and −534±83 J mol−1 K−1. Using these values and published standard state partial molal quantities for constituent ions, ΔG0f,298=−15,131±19 kJ mol−1, ΔH0f,298=−17,330±8.6 kJ mol−1, ΔS0298=2.19±0.10 kJ mol−1 K−1, and ΔC0Pf,298=2.12±0.53 kJ mol−1 K−1, were calculated.  相似文献   

8.
The capture and geological storage of CO2 can be used to reduce anthropogenic greenhouse gas emissions. To assess the environmental impact of potential CO2 leakage from deep storage reservoirs on the abundance and functional diversity of microorganisms in near-surface terrestrial environments, a natural CO2 vent (>90% CO2 in the soil gas) was studied as an analogue. The microbial communities were investigated using lipid biomarkers combined with compound-specific stable carbon isotope analyses, the determination of microbial activities, and the use of quantitative polymerase chain reactions (Q-PCR). With this complementary set of methods, significant differences between the CO2-rich vent and a reference site with a normal CO2 concentration were detected. The δ13C values of the plant and microbial lipids within the CO2 vent demonstrate that substantial amounts of geothermal CO2 were incorporated into the microbial, plant, and soil carbon pools. Moreover, the numbers of Archaea and Bacteria were highest at the reference site and substantially lower at the CO2 vent. Lipid biomarker analyses, Q-PCR, and the determination of microbial activities showed the presence of CO2-utilising methanogenic Archaea, Geobacteraceae, and sulphate-reducing Bacteria (SRB) mainly at the CO2 vent, only minor quantities were found at the reference site. Stable carbon isotopic analyses revealed that the methanogenic Archaea and SRB utilised the vent-derived CO2 for assimilatory biosynthesis. Our results show a shift in the microbial community towards anaerobic and acidophilic microorganisms as a consequence of the long-term exposure of the soil environment to high CO2 concentrations.  相似文献   

9.
Evidence from laboratory experiments indicates that fractionation against the heavy stable isotope of carbon (Δ13C) by bryophytes (liverworts and mosses) is strongly dependent on atmospheric CO2. This physiological response may therefore provide the basis for developing a new terrestrial CO2 proxy [Fletcher, B.J., Beerling, D.J., Brentnall, S.J., Royer, D.L., 2005. Fossil bryophytes as recorders of ancient CO2 levels: experimental evidence and a Cretaceous case study. Global Biogeochem. Cycles19, GB3012]. Here, we establish a theoretical basis for the proxy by developing an extended model of bryophyte carbon isotope fractionation (BRYOCARB) that integrates the biochemical theory of photosynthetic CO2 assimilation with controls on CO2 supply by diffusion from the atmosphere. The BRYOCARB model is evaluated against measurements of the response of liverwort photosynthesis and Δ13C to variations in atmospheric O2, temperature and irradiance at different CO2 concentrations. We show that the bryophyte proxy is at least as sensitive to variations in atmosphere CO2 as the two other leading carbon isotope-based approaches to estimating palaeo-CO2 levels (δ13C of phytoplankton and of paleosols). Mathematical inversion of BRYOCARB provides a mechanistic means of estimating atmospheric CO2 levels from fossil bryophyte carbon that can explicitly account for the effects of past differences in O2 and climate.  相似文献   

10.
We have performed experiments to determine the effects of pressure, temperature and oxygen fugacity on the CO2 contents in nominally anhydrous andesitic melts at graphite saturation. The andesite composition was specifically chosen to match a low-degree partial melt composition that is generated from MORB-like eclogite in the convective, oceanic upper mantle. Experiments were performed at 1–3 GPa, 1375–1550?°C, and fO2 of FMQ ?3.2 to FMQ ?2.3 and the resulting experimental glasses were analyzed for CO2 and H2O contents using FTIR and SIMS. Experimental results were used to develop a thermodynamic model to predict CO2 content of nominally anhydrous andesitic melts at graphite saturation. Fitting of experimental data returned thermodynamic parameters for dissolution of CO2 as molecular CO2: ln(K 0) = ?21.79?±?0.04, ΔV 0?=?32.91?±?0.65 cm3mol?1, ΔH 0?=?107?±?21 kJ mol?1, and dissolution of CO2 as CO3 2?: ln(K 0 ) = ?21.38?±?0.08, ΔV 0?=?30.66?±?1.33 cm3 mol?1, ΔH 0?=?42?±?37 kJ mol?1, where K 0 is the equilibrium constant at some reference pressure and temperature, ΔV 0 is the volume change of reaction, and ΔH 0 is the enthalpy change of reaction. The thermodynamic model was used along with trace element partition coefficients to calculate the CO2 contents and CO2/Nb ratios resulting from the mixing of a depleted MORB and the partial melt of a graphite-saturated eclogite. Comparison with natural MORB and OIB data suggests that the CO2 contents and CO2/Nb ratios of CO2-enriched oceanic basalts cannot be produced by mixing with partial melts of graphite-saturated eclogite. Instead, they must be produced by melting of a source containing carbonate. This result places a lower bound on the oxygen fugacity for the source region of these CO2-enriched basalts, and suggests that fO2 measurements made on cratonic xenoliths may not be applicable to the convecting upper mantle. CO2-depleted basalts, on the other hand, are consistent with mixing between depleted MORB and partial melts of a graphite-saturated eclogite. Furthermore, calculations suggest that eclogite can remain saturated in graphite in the convecting upper mantle, acting as a reservoir for C.  相似文献   

11.
Crystal field stabilization (CFS) plays a significant role in determining equilibrium phase boundaries in olivine→spinel transformations involving transition-metal cations, including Fe2+ which is a major constituent of the upper mantle. Previous calculations for Fe2SiO4 ignored pressure and temperature dependencies of crystal field stabilization enthalpies (CFSE) and the electronic configurational entropy (S CFS). We have calculated free energy changes (ΔG CFS) due to differences of crystal field splittings between Fe2SiO4 spinel and fayalite from: ΔG CFS=?ΔCFSE?TΔS CFS, as functions of P and T, for different energy splittings of t 2g orbital levels of Fe2+ in spinel. The results indicate that ΔG CFS is always negative, suggesting that CFS always promotes the olivine→spinel transition in Fe2SiO4, and expands the stability field of spinel at the expense of olivine. Because of crystal field effects, transition pressures for olivine→spinel transformations in compositions (Mg1?x Fe x )2SiO4 are lowered by approximately 50x kbar, which is equivalent to having raised the olivine→spinel boundary in the upper mantle by about 15 km.  相似文献   

12.
This contribution considers the critical time increment (Δtcrit) to achieve stable simulations using particulate discrete element method (DEM) codes that adopt a Verlet-type time integration scheme. The Δtcrit is determined by considering the maximum vibration frequency of the system. Based on a series of parametric studies, Δtcrit is shown to depend on the particle mass (m), the maximum contact stiffness (Kmax), and the maximum particle coordination number (CN,max). Empirical expressions relating Δtcrit to m, Kmax, and CN,max are presented; while strictly only valid within the range of simulation scenarios considered here, these can inform DEM analysts selecting appropriate Δtcrit values.  相似文献   

13.
The budget of atmospheric CO2 is widely studied using records of temporal and spatial variations of concentrations, δ13C and δ18O values. However, the number and diversity of sources and sinks prevents these alone from fully constraining the budget. Molecules containing two rare isotopes can serve as additional tracers and potentially provide additional, independent, constraints. We present data documenting seasonal and diurnal variations of CO2 having a mass of 47 u (mostly 13C18O16O) in air from Pasadena, CA. We report these data using the ‘mass 47 anomaly’ (Δ47), which is defined as the deviation of R47(=[47]/[44]) from that expected for a random distribution of isotopologues. Between February 2004 and December 2005, Δ47 showed a seasonal pattern that differed significantly from that expected based on thermodynamic equilibrium. During the year 2004 Δ47 was 0.76‰ in winter, increased to 0.87‰ in summer and gradually decreased through the autumn to 0.81‰ at the end of the year. Δ47 then increased again through the winter and spring of 2005 to 0.97‰ in summer followed by a decrease to 0.88‰ at the end of 2005. The seasonal variations cannot be accounted for by variations in the relative contribution of local fossil fuel sources. Diurnal variations were the combined effect of both fuel combustion and respiration having Δ47 values of 0.41‰ and ca. 0.77‰, respectively. The seasonal cycle may be interpreted as a competition between low Δ47 values in respiration and higher Δ47 values resulting from CO2-water exchange in photosynthesis.  相似文献   

14.
Atmospheric carbon dioxide is widely studied using records of CO2 mixing ratio, δ13C and δ18O. However, the number and variability of sources and sinks prevents these alone from uniquely defining the budget. Carbon dioxide having a mass of 47 u (principally 13C18O16O) provides an additional constraint. In particular, the mass 47 anomaly (Δ47) can distinguish between CO2 produced by high temperature combustion processes vs. low temperature respiratory processes. Δ47 is defined as the abundance of mass 47 isotopologues in excess of that expected for a random distribution of isotopes, where random distribution means that the abundance of an isotopologue is the product of abundances of the isotopes it is composed of and is calculated based on the measured 13C and 18O values. In this study, we estimate the δ13C (vs. VPDB), δ18O (vs. VSMOW), δ47, and Δ47 values of CO2 from car exhaust and from human breath, by constructing ‘Keeling plots’ using samples that are mixtures of ambient air and CO2 from these sources. δ47 is defined as , where is the R47 value for a hypothetical CO2 whose δ13CVPDB = 0, δ18OVSMOW = 0, and Δ47 = 0. Ambient air in Pasadena, CA, where this study was conducted, varied in [CO2] from 383 to 404 μmol mol−1, in δ13C and δ18O from −9.2 to −10.2‰ and from 40.6 to 41.9‰, respectively, in δ47 from 32.5 to 33.9‰, and in Δ47 from 0.73 to 0.96‰. Air sampled at varying distances from a car exhaust pipe was enriched in a combustion source having a composition, as determined by a ‘Keeling plot’ intercept, of −24.4 ± 0.2‰ for δ13C (similar to the δ13C of local gasoline), δ18O of 29.9 ± 0.4‰, δ47 of 6.6 ± 0.6‰, and Δ47 of 0.41 ± 0.03‰. Both δ18O and Δ47 values of the car exhaust end-member are consistent with that expected for thermodynamic equilibrium at∼200 °C between CO2 and water generated by combustion of gasoline-air mixtures. Samples of CO2 from human breath were found to have δ13C and δ18O values broadly similar to those of car exhaust-air mixtures, −22.3 ± 0.2 and 34.3 ± 0.3‰, respectively, and δ47 of 13.4 ± 0.4‰. Δ47 in human breath was 0.76  ± 0.03‰, similar to that of ambient Pasadena air and higher than that of the car exhaust signature.  相似文献   

15.
Raman spectroscopy is a powerful method for the determination of CO2 densities in fluid inclusions, especially for those with small size and/or low fluid density. The relationship between CO2 Fermi diad split (Δ, cm−1) and CO2 density (ρ, g/cm3) has been documented by several previous studies. However, significant discrepancies exist among these studies mainly because of inconsistent calibration procedures and lack of measurements for CO2 fluids having densities between 0.21 and 0.75 g/cm3, where liquid and vapor phases coexist near room temperature.In this study, a high-pressure optical cell and fused silica capillary capsules were used to prepare pure CO2 samples with densities between 0.0472 and 1.0060 g/cm3. The measured CO2 Fermi diad splits were calibrated with two well established Raman bands of benzonitrile at 1192.6 and 1598.9 cm−1. The relationship between the CO2 Fermi diad split and density can be represented by: ρ = 47513.64243 − 1374.824414 × Δ + 13.25586152 × Δ2 − 0.04258891551 × Δ3 (r2 = 0.99835, σ = 0.0253 g/cm3), and this relationship was tested by synthetic fluid inclusions and natural CO2-rich fluid inclusions. The effects of temperature and the presence of H2O and CH4 on this relationship were also examined.  相似文献   

16.
《Applied Geochemistry》2001,16(7-8):883-894
Total CO2 output from fumaroles, bubbling and water dissolved gases and soil gases was investigated at Pantelleria Island volcano, Italy. The preliminary results indicate an overall output of 0.39 Mt a−1 of CO2 from the island. The main contribution to the total output was from diffuse soil degassing (about 0.32 Mt a−1), followed by dissolved CO2 (0.034 Mt a−1), focussed soil degassing (0.028 Mt a−1) and bubbling CO2 (0.013 Mt a−1). The contribution of CO2 from fumarole gases was found to be negligible (1.4×10−6 Mt a−1). Carbon-13 values for CO2 coupled with those for associated He in gases from fumaroles and sites of focussed soil degassing clearly rule out any significant organic CO2 component and suggest a common mantle origin for these gas species. The inferred mantle source beneath Pantelleria would seem to have peculiar geochemical characteristics, quite distinct from those of mantle producing MORB but compatible with those of magmatic sources of central Mediterranean and central European volcanoes. These findings indicate that the Pantelleria volcanic complex is a site of active mantle degassing that is worthy of attention for future geochemical surveillance of the island.  相似文献   

17.
In 2001, a special issue of the Bulletin of the Seismological Society of America (BSSA) featured seismological research for the 1999 Chi–Chi Taiwan earthquake. This study uses source parameters suggested by the first author in this special issue to estimate static stress drop associated with the Chi–Chi earthquake. The waveform simulation method was used to carefully examine these source parameters. The simulation results indicate that source parameters, inferred from near-fault observations, are well determined. According to the rupture area and slip, the static stress drops (Δσs) obtained were distributed between a small value of 47 bars near the epicentral region and a much larger value (>200 bars) to the north. Similar trends in dynamic stress drop (Δσd) were also recognized by the first author in his paper published in 2001 BSSA special issue. Comparing the Δσs with Δσd, satisfies the relation Δσs/Δσd ≈ 1. This relation suggests that fault motion is mostly spent releasing seismic wave energy during the rupture process of the Chi–Chi earthquake. The consistency between static and dynamic stress drops thus provides a measure of energy-moment (Es/M0) ratios, which range from 9.0 × 10−5 to 6.5 × 10−4. The average Es/M0 ratio estimated for the northern portions of the fault is 3.4 × 10−4, which is about 3 times that of the south. Such a high Es/M0 ratio can be interpreted as having low strength in the rupture for the northern portions of the fault, where the fault would release less energy per unit rupture surface to create the new rupture.  相似文献   

18.
The application of chemical and isotopic geothermometry to geothermal systems is reviewed, pointing out the uses and limitations of specific reactions in estimating deep temperatures from well, hot-spring and fumarole discharges.At present the most reliable indicators are: the silica-water equilibria; the Na/K ratio; the isotopic distributions Δ2H(H2“H2O), Δ2H(H2“CH4), Δ18O(H2O“HSO?4); and the gas reactions CO2 + 4H2 ? CH4 + 2H2O, and 2NH3 ? N2 + 3H2. Many other qualitative chemical indicators exist.  相似文献   

19.
The instability of transition metal dolomites [CaR2+(CO3)2 where R2+ is Fe, Co, Ni, Cu, or Zn] and the limited substitution of transition metal cations for Mg in the dolomite structure can be accounted for by the effect of octahedral distortion. For example, trigonal elongation of the Fe octahedron, due to the Jahn-Teller effect, observed in siderite and ankerite, results in elongation of the Ca octahedron which is sensitive to distortion because the radius of Ca2+ is close to the upper limit for octahedral coordination. Co, Ni, Cu, Zn octahedra are also thought to be deformed, relative to Mg octahedra, in carbonates.The free energy of formation (ΔGof) of R2+CO3 becomes more positive with increasing octahedral distortion. Estimated ΔGof(dolomite) as well as stabilities and solubility limits of R2+ in natural and synthetic dolomites suggest a series in order of decreasing stability: Mg >Mn >Zn >Fe >Co >Ni >Cu.ΔGof(est.) for the terminal Fe-dolomite solid solution [72 mol% CaFe(CO3)2] in the system CaCO3-MgCO3-FeCO3 may represent an empirical threshold value for dolomite stability which lies between ΔGof for Mn- and Zn-dolomites. While Zn-dolomite is probably not a stable phase, very extensive solid solution toward CaZn(CO3)2 is to be expected in the system CaCO3-MgCO3-ZnCO3. The tendency for transition metal dolomites to contain excess CaCO3 can also be accounted for in terms of octahedral distortion and AGof.  相似文献   

20.
The stable carbon isotope compositions and the stomatal parameters (stomatal density and stomatal index) of four Cheirolepidiaceae species, Brachyphyllum ningxiaensis, Brachyphyllum obtusum, Pseudofrenelopsis dalatzensis and Pseudofrenelopsis gansuensis, were analyzed to recover the late Early Cretaceous atmospheric CO2 levels. The fossil plants were collected from 5 consecutive sedimentary members of the uppermost Zhonggou Formation. Based on the stomatal data, the estimated palaeo-atmospheric CO2 concentrations in the Jiuquan Basin during the late Early Cretaceous were 1060–882 ppmv based on the carboniferous standardization and were 641–531 ppmv based on the recent standardization; the pCO2 values present at first a decreasing and then an increasing trend within the sedimentary time of the five members. The δ13Cp values based on the 21 Brachyphyllum specimens showed a large variation, which ranged from −20.98‰ to −25.69‰, with an average of −24.2‰. The values also identified a C3 photosynthetic pathway for the Brachyphyllum specimens. The predicted δ13Ca values varied from −2.1‰ to −6.38‰, with an average of −5.03‰. These two proxies were irregular within the different members; therefore, the correlation with the change in atmospheric CO2 concentrations was not significant. Moreover, a water-stressed environment was proposed based on the δ13C values of the present fossil plants, a proposal that was also supported by the previous palaeobotanical, palynological and stratigraphical evidence. In the present study, an inconsistent relationship between the stable carbon isotope and the stomata values was apparent, which most likely indicated that the stomata numbers of the plant were more sensitive to the variation in the concentration of the atmospheric CO2, whereas the δ13C values were sensitive to the moisture conditions.  相似文献   

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