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1.
Rice fields are an important source for the greenhouse gas methane. In Italian rice field soil CH4 is produced either by hydrogenotrophic and acetoclastic methanogenesis, or by hydrogenotrophic methanogenesis and syntrophic acetate oxidation when temperatures are below and above about 40-45 °C, respectively. In order to see whether these acetate consumption pathways differently discriminate the stable carbon isotopes of acetate, we measured the δ13C of total acetate and acetate-methyl as well as the δ13C of CO2 and CH4 in rice field soil that had been pre-incubated at 45 °C and then shifted to different temperatures between 25 and 50 °C. Acetate transiently accumulated to about 6 mM, which is about one-third of the amount of CH4 produced, irrespective of the incubation temperature and the CH4 production pathway involved. However, the patterns of δ13C of the CH4 and CO2 produced were different at low (25, 30, 35 °C) versus high (40, 45, 50 °C) temperatures. These patterns were consistent with CH4 being exclusively formed by hydrogenotrophic methanogenesis at high temperatures, and by a combination of acetoclastic and hydrogenotrophic methanogenesis at low temperatures. The patterns of δ13C of total acetate and acetate-methyl were also different at high versus low temperatures, indicating the involvement of different pathways of production and consumption of acetate at the two temperature regimes. Isotope fractionation during consumption of the methyl group of acetate was more pronounced at low (α = 1.010-1.025) than at high (α = 1.0-1.01) temperatures indicating that acetoclastic methanogenesis exhibits a stronger isotope effect than syntrophic acetate oxidation. Small amounts of propionate also transiently accumulated and were analyzed for δ13C. The δ13C values slightly increased (by about 10‰) during production and consumption of propionate, but were not affected by incubation temperature. Collectively, our results showed distinct isotope discrimination for different paths of acetate (and propionate) production and consumption, albeit differences were only small, and discrimination between methanogenic and syntrophic acetate consumption in nature may be difficult to detect.  相似文献   

2.
Variation in the degree of aromatic condensation of chars   总被引：1，自引：0，他引：1  
Char is ubiquitous in the environment and contributes significantly to the inert soil organic carbon pool. Its roles as a carbon sink and a strong sorbent of organic contaminants have come under increasing attention. However, quantifying these roles is difficult because properties such as degradability and sorption affinity vary greatly amongst chars, especially those produced at different temperatures. Here we describe a simple method for gauging the degree of aromatic condensation of chars, a molecular-scale property that affects both their degradability and sorption affinity. The method involves adding 13C6 benzene directly to char. The 13C nuclear magnetic resonance (NMR) chemical shift of the sorbed benzene is affected by diamagnetic ring currents in the fused aromatic structures in the char. These ring currents increase in magnitude with increasing extent of aromatic condensation. Seventeen heat-treated materials were analysed in this way. Our results confirm that aromatic condensation increases with increasing heat treatment temperature (HTT) and that activated chars contain the most highly condensed aromatic structures, but also show the importance of starting material and heat treatment time on aromatic condensation. We also show for four of the materials that the ring current effect on chemical shift was similar for other 13C-labelled molecules, including MeOH, CH3CN and toluene.  相似文献   

3.
The solubility of cyclooctasulfur in water and sea water at various temperatures in the range between 4 and 80 °C was determined. Cyclooctasulfur in equilibrium with rhombic sulfur reacted with hot acidic aqueous potassium cyanide to form thiocyanate anion which was measured by anion chromatography. Sulfur solubility in pure water was found to increase with temperature by more than 78 times: from 6.1 nM S8 at 4 °C to 478 nM S8 at 80 °C. The following thermodynamic values for solubilisation of S8 in water were calculated from the experimental data: K° = 3.01 ± 1.04 × 10−8, ΔGr° = 42.93 ± 0.73 kJ mol−1, ΔHr° = 47.4 ± 3.6 kJmol−1, ΔSr° = 15.0 ± 11.7 J mol−1 K−1). Solubility of cyclooctasulfur in sea water was found to be 61 ± 13% of the solubility in pure water regardless of the temperature.  相似文献   

4.
Different analytical techniques were used to find the most reliable and economic method for determining the labile fraction of C in biochar. Biochar was produced from pine, poplar and willow (PI, PO and WI, respectively) at two temperatures (400 and 550 °C) and characterised using spectroscopic techniques [solid state 13C nuclear magnetic resonance spectroscopy (NMR)], molecular markers [pyrolysis-gas chromatography-mass spectrometry (Py-GC-MS)], thermogravimetry (TG), elemental composition and wet oxidation (potassium permanganate and potassium dichromate). Short term incubation (110 h) of an A horizon from an Umbrisol amended with the biochar samples at two doses (7.5 and 15 t ha−1) was also carried out to provide supplementary information on the influence of biochar-soil interaction on CO2 evolution. Spectroscopic analysis demonstrated that the degree of biochar carbonisation was influenced by the type of feedstock and heating conditions and followed the order WI-400 < PI-400 ∼ WI-550 ∼ PO-400 < PO-550 < PI-550. The thermo-labile fraction of the biochar samples, estimated from TG, ranged between 21% and 49%. The fraction of total C oxidised with potassium permanganate (Cper/Ctotal) was <50 g kg−1 in all cases, whereas potassium dichromate (Cdichro/Ctotal) oxidation efficiency ranged between 180 and 545 g kg−1. For each type of feedstock, the highest values of either chemically or thermally degradable C corresponded to the biochar produced at low temperature. Results indicate that low cost methodologies, such as dichromate oxidation and TG, reflected the degree of biochar carbonisation, and could therefore be used to estimate the labile fraction of C in biochar.  相似文献   

5.
To establish the increase in temperature and the time span of the transition between the Late Glacial Maximum (LGM) and the Holocene, the noble gas content, 18O, 2H, 13C δ values, 3H and 14C activity and chemistry were studied in a groundwater flow system in Quaternary sediments in Hungary. The study area is a sub-basin of the Pannonian Basin, where the C isotope ratios are not influenced by carbonate reactions along the flow path, because the only water-rock interaction is ion exchange. The δ18O and δ2H values indicate a cold infiltration period, followed by warming, and, finally, warm temperature conditions. The noble gas data show that the average infiltration temperature was 3.3 °C in the cold, 12.9 °C in the warm, and intermediate in the transitional stage. Using the noble gas temperatures, geochemical batch modelling was performed to simulate the chemical processes. Based on the geochemical model, δ13C and 14C0 (initial radiocarbon activity) in the recharging water were calculated. Transport modelling was used to simulate the distribution of chemical components, δ18O, δ2H and 14C0, along the flow path. It was found that the main processes determining the chemical composition of the groundwater were dissolution/precipitation of calcite and dolomite during infiltration near the surface, and ion exchange along the flow path. In the recharge area the δ13C and 14C0 were controlled by dissolution and precipitation of carbonate minerals, C speciation, and fractionation processes. All these processes were influenced by the recharge temperature. NGTs calculated from the dissolved noble gas concentrations showed an average of 3.3 °C for cold, and 12.9 °C for warm infiltration, i.e. for the LGM and for the Holocene. The temperature difference was thus 9.1 ± 0.8 °C, which is one of the largest degree of warming detected by noble gases so far. The alkalinity indicates that carbonate reactions were unimportant along the flow path. Owing to the temperature dependence of the equilibrium constants, temperature conditions during infiltration have to be taken into consideration in radiocarbon age calculation. Dispersive transport along the flow path modified the chemical and isotopic composition of infiltrated water. The contribution of the old pore water, which was free of the 14C isotope, resulted in uncertainties in radiocarbon age determination. It was concluded that determination of the radiocarbon age or mean residence time requires detailed knowledge of the hydraulic conditions of groundwater.  相似文献   

6.
Raman analysis of the vapor phase formed after heating pure water to near critical (355-374 °C) temperatures in a hydrothermal diamond-anvil cell (HDAC) reveals the synthesis of abiogenic methane. This unexpected result demonstrates the chemical reactivity of diamond at relatively low temperatures. The rate of methane production from the reaction between water and diamond increases with increasing temperature and is enhanced by the presence of a metal gasket (Re, Ir, or Inconel) which is compressed between the diamond anvils to seal the aqueous sample. The minimum detection limit for methane using Raman spectroscopy was determined to be ca. 0.047 MPa, indicating that more than 1.4 nanograms (or 8.6 × 10−11 mol) of methane were produced in the HDAC at 355 °C and 30 MPa over a period of ten minutes. At temperatures of 650 °C and greater, hydrogen and carbon dioxide were detected in addition to methane. The production of abiogenic methane, observed in all HDAC experiments where a gasket was used, necessitates a reexamination of the assumed chemical systems and intensive parameters reported in previous hydrothermal investigations employing diamonds. The results also demonstrate the need to minimize or eliminate the production of methane and other carbonic species in experiments by containing the sample within a HDAC without using a metal gasket.  相似文献   

7.
Stable carbon isotopes of organic matter and fossilized plant remains can be used to effectively reconstruct local palaeoclimate changes, especially from plants using a single photosynthetic mode. The charred grains of foxtail and common millet are chemically stable in the environment and have been preserved widely and continuously throughout the Holocene in North China. The charred remains of these species are ideal materials for reconstructing the palaeoclimate based on δ13C of foxtail and common millets heated to temperatures up to around 250 °C. This study reports δ13C values of modern millets carbonized at different temperatures. The results indicate that there are no significant changes in δ13C of intact and charred samples of foxtail millet (?0.46‰) and common millet (?0.49‰) for temperatures below 300 °C. The δ13C of charred foxtail millet formed at 250 °C were 0.2‰ higher in δ13C than the source samples. In contrast, the δ13C of charred common millet formed at 250 °C were 0.2‰ lighter in δ13C than the source samples. The δ13C values of grains were determined in part by the carbon content (i.e., starches, lignins and lipids) and the variable thermal tolerances of these compounds to heating. However, the observed 13C carbonization associated with fractionation of only 0.2‰ in grains is much less than the natural variation typically found in wood. We therefore suggest that δ13C measured in carbonized grains can serve as an effective indicator for paleoenvironmental and archaeological reconstructions.  相似文献   

8.
Diffusive isotopic fractionation factors are important in order to understand natural processes and have practical application in radioactive waste storage and carbon dioxide sequestration. We determined the isotope fractionation factors and the effective diffusion coefficients of chloride and bromide ions during aqueous diffusion in polyacrylamide gel. Diffusion was determined as functions of temperature, time and concentration. The effect of temperature is relatively large on the diffusion coefficient (D) but only small on isotope fractionation. For chlorine, the ratio, D35Cl/D37Cl varied from 1.00128 ± 0.00017 (1σ) at 2 °C to 1.00192 ± 0.00015 at 80 °C. For bromine, D79Br/D81Br varied from 1.00098 ± 0.00009 at 2 °C to 1.0064 ± 0.00013 at 21 °C and 1.00078 ± 0.00018 (1σ) at 80 °C. There were no significant effects on the isotope fractionation due to concentration. The lack of sensitivity of the diffusive isotope fractionation to anything at the most common temperatures (0 to 30 °C) makes it particularly valuable for application to understanding processes in geological environments and an important natural tracer in order to understand fluid transport processes.  相似文献   

9.
The yields and stable C and H isotopic composition of gaseous products from the reactions of pure n-C24 with (1) MgSO4; and (2) elemental S in sealed Au-tubes at a series of temperatures over the range 220–600 °C were monitored to better resolve the reaction mechanisms. Hydrogen sulfide formation from thermochemical sulfate reduction (TSR) of n-C24 with MgSO4 was initiated at 431 °C, coincident with the evolution of C2–C5 hydrocarbons. Whereas the yields of H2S increased progressively with pyrolysis temperature, the hydrocarbon yields decreased sharply above 490 °C due to subsequent S consumption. Ethane and propane were initially very 13C depleted, but became progressively heavier with pyrolysis temperature and were more 13C enriched than the values of a control treatment conducted on just n-C24 above 475 °C. TSR of MgSO4 also led to progressively higher concentrations of CO2 showing relatively low δ13C values, possibly due to input of isotopically light CO2 derived from gaseous hydrocarbon oxidation (e.g., more depleted CH4).  相似文献   

10.
The speciation of cobalt (II) in Cl− and H2S-bearing solutions was investigated spectrophotometrically at temperatures of 200, 250, and 300 °C and a pressure of 100 bars, and by measuring the solubility of cobaltpentlandite at temperatures of 120-300 °C and variable pressures of H2S. From the results of these experiments, it is evident that CoHS+ and predominate in the solutions except at 150 °C, for which the dominant chloride complex is CoCl3−. The logarithms of the stability constant for CoHS+ show moderate variation with temperature, decreasing from 6.24 at 120 °C to 5.84 at 200 °C, and increasing to 6.52 at 300 °C. Formation constants for chloride species increase smoothly with temperature and at 300°C their logarithms reach 8.33 for , 6.44 for CoCl3−, 4.94 to 5.36 for , and 2.42 for CoCl+. Calculations based on the composition of a model hydrothermal fluid (Ksp-Mu-Qz, KCl = 0.25 m, NaCl = 0.75 m, ΣS = 0.3 m) suggest that at temperatures ?200 °C, cobalt occurs dominantly as CoHS+, whereas at higher temperatures the dominant species is .  相似文献   

11.
We investigated alkenones recorded in suspended particles and a settling particle time series collected at three stations, 40N (40°N, 165°E), KNOT (44°N, 155°E), and 50N (50°N, 165°E), in the northwestern North Pacific from December 1997 to May 1999. Emiliania huxleyi, the most abundant alkenone producer in this area, is present in surface to subsurface (to ∼50 m depth) waters. The alkenone concentrations recorded in the suspended particles indicated that the seasonal alkenone particle distribution differed significantly interannually. Alkenone export fluxes at the three sediment-trap stations ranged from 0.16 to 49.3 μg m−2 day−1, and the maximum export flux, which occurred in summer to fall (July-November), was associated with a high organic carbon export flux. The amount of alkenone produced during the maximum export season accounted for 60-80% of the total annual amount of alkenone, and the alkenones accumulated in the sediment below the traps had characteristics corresponding to subsurface waters during the summer-autumn season. Alkenone-derived temperatures recorded in suspended particles corresponded to the in situ temperature within ∼2 °C. Although alkenone-derived temperatures corresponded approximately to the temperatures observed in the stratified subsurface waters at the three trap stations during the high-export season, large differences were observed during the low-export (winter-spring) period. For example, the alkenone-derived temperatures observed at stations KNOT and 50N were much higher than the in situ subsurface temperatures reported in the World Ocean Atlas 2001. Relatively large differences between alkenone-derived temperatures and in situ temperatures in the subarctic might be due to (1) a low-light limitation or (2) contributions of allochthonous alkenones in particulate material transported from subtropical areas within a warm-core ring.  相似文献   

12.
Authigenic sedimentary low-temperature K-feldspar separated from Albian-Turonian carbonates in Israel was dated by the step-heating 40Ar-39Ar method. In contrast to high-temperature K-feldspars, ca. 90% of the radiogenic Ar was released at temperatures lower than 600 °C and fusion mostly occurred below 750 °C. Though formed under low temperature, Ar loss in all but one sample is estimated to be less than 2%. Nevertheless, the effect of 39Ar recoil is evident in some separates, probably due to their very fine size (4-10 μm). The plateau age of one sample with the highest content of authigenic K-feldspar (93%, 96 Ma) is slightly younger than the assumed stratigraphic age and thus defines the timing of an early diagenetic event within a few million years after deposition. Other samples where a plateau age could be determined yield ages slightly older. Strong acid etching (7 N HNO3, 85 °C) of the K-feldspar-enriched fraction may have improved the 39Ar-40Ar spectra but did not eliminate the presence of minute quantities of detrital K-bearing minerals. Though the present set of data is insufficient for a clear-cut conclusion, the activation energy of the authigenic K-feldspar is in the range of 14-26 kcal mol− 1 s− 1, much lower than that of magmatic and hydrothermal K-feldspars and can probably be attributed to the heating schedule and the small crystal size. It is not clear whether the formation at low temperatures (< 50 °C) has any effect on the activation energy.  相似文献   

13.
Goethite (Ax-2) from Axel Heiberg Island (∼80°N) on the margin of the Arctic Ocean is the dominant mineral in a sample of “petrified” Eocene wood, but U, Th, and He measurements suggest that the goethite (α-FeOOH) crystallized in the latest Miocene/Pliocene (ca. 5.5 to 2.8 Ma). Measured δD and δ18O values of Ax-2 are −221 (±6)‰ and −9.6 (±0.5)‰, respectively. The inferred δD and δ18O values of the ancient water were about −139‰ and −18.6‰, respectively, with a calculated temperature of crystallization of 3 (±5)°C, which compares with the modern summer (J-J-A) temperature of 3 °C and contrasts with a modern MAT of −19 °C. Published results from various biological proxies on nearby Ellesmere Island indicate a Pliocene (∼4 Ma) MAT of either −6 or −0.4 °C and corresponding seasonal amplitudes of about 18 or 13 °C. A conductive heat flow model suggests that a temperature of 3 °C could represent goethite crystallization at depths of ∼100-200 cm (for MAT = −6 °C) or ∼250-450 cm (for MAT = −0.4 °C) over seasonally restricted intervals of time.The δ18O value of the Ax-2 water (−18.6‰) is more positive than the modern J-J-A precipitation (−22‰). In combination, the paleotemperatures and δ18O values of ancient waters (from Ax-2 and published results from three Eocene or Pliocene proxy sites on Axel Heiberg and Ellesmere Islands) are consistent with a warm season bias in those isotopic proxies. The results are also consistent with higher proportions of J-J-A precipitation in the annual total. If so, this emphasizes the importance of seasonality at high latitudes even in times of warmer global climates, and suggests that the Arctic hydrologic cycle, as expressed in the seasonal distribution and isotopic composition of precipitation (perhaps modified by a warmer Arctic Ocean), differed from modern.The δ13C value of the Fe(CO3)OH component in the Ax-2 goethite is +6.6‰, which is much more positive than expected if crystallizing goethite incorporated CO2 derived primarily from oxidation of relict Eocene wood with δ13C values of about −24‰. This apparent paradox may be resolved if the goethite is a product of oxidation of 13C-rich siderite, which had previously replaced wood in an Eocene methanogenic burial environment. Thus, the goethite retains a carbon isotope “memory” of a diagenetic Eocene event, but a δD and δ18O record of the latest Miocene/Pliocene Arctic climate.  相似文献   

14.
The TEX86 (TetraEther indeX of tetraethers consisting of 86 carbon atoms) paleothermometer is based on the relative distribution of archaeal lipids, i.e. isoprenoid glycerol dibiphytanyl glycerol tetraethers (GDGTs), and is increasingly used to reconstruct past sea water temperatures. To establish a more extensive, global calibration of the TEX86 paleothermometer, we analyzed GDGTs in 287 (in comparison with 44 in currently used calibration) core-top sediments distributed over the world oceans and deposited at different depths. Comparisons of TEX86 data with (depth-weighted) annual mean temperatures of the overlying waters between 0 m and 4000 m as well as with different seasonal mean temperatures at 0 m water depth showed that the TEX86 proxy reflects mostly annual mean temperatures of the upper mixed layer. The relationship between TEX86 values and sea-surface temperatures (SSTs) was non-linear mainly because below 5 °C the change in TEX86 values was minor with temperature. This suggests that the TEX86 proxy might not be directly applicable for the Polar Oceans. Nevertheless, between 5 °C and 30 °C, the TEX86 proxy has a strong linear relationship with SSTs. Here, we, therefore, propose a new linear calibration model (T = −10.78 + 56.2 ∗ TEX86, r2 = 0.935, n = 223) for past SST reconstructions using the TEX86 palaeothermometer.  相似文献   

15.
The solubility of baddeleyite (ZrO2) and the speciation of zirconium have been investigated in HF-bearing aqueous solutions at temperatures up to 400 °C and pressures up to 700 bar. The data obtained suggest that in HF-bearing solutions zirconium is transported mainly in the form of the hydroxyfluoride species ZrF(OH)3° and ZrF2(OH)2°. Formation constants determined for these species (Zr4+ + nF− + mOH− = ZrFn(OH)m°) range from 43.7 at 100 °C to 46.41 at 400 °C for ZrF(OH)3°, and from 37.25 at 100 °C to 43.88 at 400 °C for ZrF2(OH)2°.Although the solubility of ZrO2 is retrograde with respect to temperature, the measured concentrations of Zr are orders of magnitude higher than those predicted from theoretical extrapolations based on simple fluoride species (ZrF3+-ZrF62−). Model calculations performed for zircon show that zirconium can be transported by aqueous fluids in concentrations sufficient to account for the concentration of this metal at conditions commonly encountered in fluoride-rich natural hydrothermal systems.  相似文献   

16.
We have used advanced and quantitative solid-state nuclear magnetic resonance (NMR) techniques to investigate structural changes in a series of type II kerogen samples from the New Albany Shale across a range of maturity (vitrinite reflectance R0 from 0.29% to 1.27%). Specific functional groups such as CH3, CH2, alkyl CH, aromatic CH, aromatic C-O, and other nonprotonated aromatics, as well as “oil prone” and “gas prone” carbons, have been quantified by 13C NMR; atomic H/C and O/C ratios calculated from the NMR data agree with elemental analysis. Relationships between NMR structural parameters and vitrinite reflectance, a proxy for thermal maturity, were evaluated. The aromatic cluster size is probed in terms of the fraction of aromatic carbons that are protonated (∼30%) and the average distance of aromatic C from the nearest protons in long-range H-C dephasing, both of which do not increase much with maturation, in spite of a great increase in aromaticity. The aromatic clusters in the most mature sample consist of ∼30 carbons, and of ∼20 carbons in the least mature samples. Proof of many links between alkyl chains and aromatic rings is provided by short-range and long-range 1H-13C correlation NMR. The alkyl segments provide most H in the samples; even at a carbon aromaticity of 83%, the fraction of aromatic H is only 38%. While aromaticity increases with thermal maturity, most other NMR structural parameters, including the aromatic C-O fractions, decrease. Aromaticity is confirmed as an excellent NMR structural parameter for assessing thermal maturity. In this series of samples, thermal maturation mostly increases aromaticity by reducing the length of the alkyl chains attached to the aromatic cores, not by pronounced growth of the size of the fused aromatic ring clusters.  相似文献   

17.
Sandstone dissolution is a common water–rock reaction in the Earth’s crust, but a thorough understanding of this phenomenon is constrained by poorly determined kinetic data. To this end, kinetic data were determined for the dissolution of arkosic sandstone powders in deionised water (pH was about 7.0–7.3 and electrical conductivity was between 0.95 and 1.00 μS/cm). Release rates of dissolved elements were determined over the range 50–350 °C at 20, 15, and 10 MPa using a column flow-through pressure vessel reactor. The conductivity of the outlet solution, measured at room temperature, is dependent on the charge of major cations such as Na+, K+, Ca2+ and Mg2+ at these conditions. The conductivity of the outlet solution was used to determine the steady state of the dissolution of sandstone powders. The pH values of the outlet solutions at the steady state, measured ex situ at room temperature, were about 7.7, 8.3, 8.4, 8.4 and 7.6 at 75, 100, 150, 200 and 250 °C, respectively, at 10 MPa. Silicon, Na, K, Ca, Al and Mg are the major ions found in the solution at low temperatures, but Si is the only major ion retained at higher temperatures (>150 °C). Compared with static experiments, the flowing dissolution experiments occurred at conditions far from equilibrium. The relationship between temperature and dissolution rates of arkosic sandstone powders was described as log R = 0.005469t − 10.50 where R is the dissolution rates of sandstone powders in kg/(m2 s), t is temperature in °C which ranged from 100 to 350 °C at 20 and 15 MPa, and the dissolution rates of sandstone powders were measured only for the major dissolved elements without oxygen in the outlet solutions.  相似文献   

18.
The fractionation of sulfur isotopes by the thermophilic chemolithoautotrophic Thermodesulfatator indicus was explored during sulfate reduction under excess and reduced hydrogen supply, and the full temperature range of growth (40-80 °C). Fractionation of sulfur isotopes measured under reduced H2 conditions in a fed-batch culture revealed high fractionations (24-37‰) compared to fractionations produced under excess H2 supply (1-6‰). Higher fractionations correlated with lower sulfate reduction rates. Such high fractionations have never been reported for growth on H2. For temperature-dependant fractionation experiments cell-specific rates of sulfate reduction increased with increasing temperatures to 70 °C after which sulfate-reduction rates rapidly decreased. Fractionations were relatively high at 40 °C and decreased with increasing temperature from 40-60 °C. Above 60 °C, fractionation trends switched and increased again with increasing temperatures. These temperature-dependant fractionation trends have not previously been reported for growth on H2 and are not predicted by a generally accepted fractionation model for sulfate reduction, where fractionations are controlled as a function of temperature, by the balance of the exchange of sulfate across the cell membrane, and enzymatic reduction rates of sulfate. Our results are reproduced with a model where fractionation is controlled by differences in the temperature response of enzyme reaction rates and the exchange of sulfate in and out of the cell.  相似文献   

19.
Over the last decade, sea surface temperature (SST) reconstructed from the Mg/Ca ratio of foraminiferal calcite has increasingly been used, in combination with the δ18O signal measured on the same material, to calculate the δ18Ow, a proxy for sea surface salinity (SSS). A number of studies, however, have shown that the Mg/Ca ratio is also sensitive to other parameters, such as pH or , and salinity. To increase the reliability of foraminiferal Mg/Ca ratios as temperature proxies, these effects should be quantified in isolation. Individuals of the benthic foraminifera Ammonia tepida were cultured at three different salinities (20, 33 and 40 psu) and two temperatures (10-15 °C). The Mg/Ca and Sr/Ca ratios of newly formed calcite were analyzed by Laser Ablation ICP-MS and demonstrate that the Mg concentration in A. tepida is overall relatively low (mean value per experimental condition between 0.5 and 1.3 mmol/mol) when compared to other foraminiferal species, Sr being similar to other foraminiferal species. The Mg and Sr incorporation are both enhanced with increasing temperatures. However, the temperature dependency for Sr disappears when the distribution factor DSr is plotted as a function of calcite saturation state (Ω). This suggests that a kinetic process related to Ω is responsible for the observed dependency of Sr incorporation on sea water temperature. The inferred relative increase in DMg per unit salinity is 2.8% at 10 °C and 3.3% at 15 °C, for the salinity interval 20-40 psu. This implies that a salinity increase of 2 psu results in enhanced Mg incorporation equivalent to 1 °C temperature increase. The DSr increase per unit salinity is 0.8% at 10 °C and 1.3% at 15 °C, for the salinity interval 20-40 psu.  相似文献   

20.
A 13-step alkaline permanganate degradation of Bulgarian oil shale kerogen concentrate at ambient temperature was carried out. A high yield of oxidation products (90.1%) and a low yield of gaseous products (2.79%) were obtained. IR and 1H NMR spectroscopic studies have shown that two significantly different types of high molecular products are present in kerogen. Further oxidation of these structures leads to the formation of low molecular aliphatic and aromatic acids, proven by gas chromotography (GC) and gas chromatography-mass spectrometry (GC-MS). The data obtained at these mild conditions allow us to acquire detailed information about the aromatic structures and polymethylene chain lengths in kerogen.The 5-step oxidation of the kerogen at 90 °C provides information about stable aromatic structures. Soluble and insoluble polyfunctional acids in acid medium have close molecular masses and spectral characteristics. The amount of benzene and naphthalene carboxylic acids is 11.3% of the organic matter of the oil shale.  相似文献   

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