共查询到20条相似文献,搜索用时 15 毫秒
1.
Janina Szaran 《Chemical Geology》1998,150(3-4):331-337
Fractionation of the stable carbon isotopes between dissolved and gaseous carbon dioxide has been measured at temperature 25°C by two methods. In the first method the open system conditions and different methods of CO2 sampling were arranged. In the second method—the closed system conditions and CO2 gas extraction were used. The results obtained by these methods are very consistent. Gaseous CO2 is enriched in heavy isotope
by 1.03±0.02 permil in comparison to dissolved carbon dioxide. 相似文献
2.
Joseph W Pardue Richard S Scalan Chase Van Baalen Patrick L Parker 《Geochimica et cosmochimica acta》1976,40(3):309-312
The maximum carbon isotope fractionation occurring in photosynthetic fixation of carbon dioxide in pure cultures of blue-green algae was ?23.9%. and for a green alga was ?22.6%., Maximum fractionations were obtained where cell densities were low and carbon dioxide concentrations were greater than 0.5%. Fractionation was reduced at higher temperatures using a thermophilic blue-green alga. For filamentous blue-green algae wherein clumping occurs and localized cell concentrations were high, fractionation was also lower. Fractionations reported in literature for Precambrian organic materials are comparable to the maximum fractionations reported here. This suggests that the early photosynthetic organisms developed under conditions of high carbon dioxide availability, i.e. slow growth rates and/or low population densities. 相似文献
3.
Experimental determination of the isotopic fractionation between gaseous CO2 and carbon dissolved in tholeiitic magma 总被引:1,自引:0,他引:1
Isotope fractionation of carbon between CO2 and carbon dissolved in a tholeiitic magma measured in the range 1120–1280 ° C, 7.0–8.4 Kb varies from 4.6 to 4 in favor of CO2. These results make possible to explain all deep seated 13C values from a restricted range of primary mantle 13C concentrations. They also suggest that carbon could be dissolved in basaltic magmas in a reduced form. 相似文献
4.
The partitioning of stable carbon isotopes between calcite, graphite and CO2 was experimentally determined at temperatures from 500 to 1200 °C and 1 to 15 kbar pressure. Attainment of carbon isotope equilibrium in CO2-calcite runs was proven by achieving the same fractionation from isotopically opposite directions. The resultant CO2-calcite fractionation curve for carbon differs from Bottinga's calculation by 1.2 and confirms recent experiments of Chacko et al. and Mattey et al. In CO2-graphite experiments equilibrium fractions were extrapolated by applying the partial-exchange technique of Northrop and Clayton and by optimizing the contribution of surface reaction in graphite. CO2-graphite fractionations at temperatures up to 800 °C are in fair agreement with Bottinga's calculation, but yield a surprisingly high fractionation of 5 at upper mantle temperatures. The combination of CO2-calcite (carbon) and CO2-graphite fractionation results in a new experimentally determined calcite-grapite fractionation curve, expressed by the equation:
相似文献
5.
Mario Trieloff Martina Falter Ekaterina V. Korochantseva Rainer Altherr 《Geochimica et cosmochimica acta》2005,69(5):1253-1264
Noble gas isotopes are widely used to elucidate the history of the rocks in which they have been trapped, either from distinct reservoirs or by accumulation following radioactive decay. To extract noble gases from their host rocks, stepwise heating is the most commonly used technique to deconvolve isotopically different components, e.g., atmospheric, in situ radiogenic, or excess radiogenic from mantle or crustal reservoirs. The accurate determination of the isotopic composition of these different components is of crucial importance, e.g., for ages obtained by 40Ar-39Ar stepheating plateaus. However, diffusion theory-based model calculations predict that the stepwise thermal extraction process from mineral phases induces isotope fractionation and, hence, adulterates the original composition. Such effects are largely unconsidered, as they are small and a compelling experimental observation is lacking. We report the first unequivocal evidence for significant mass fractionation of argon isotopes during thermal extraction, observed on shungite, a carbon-rich Precambrian sedimentary rock. The degree of fractionation, as monitored by 38Ar/36Ar and 40Ar/36Ar ratios, very well agrees with theoretical predictions assuming an inverse square root dependence of diffusion coefficient and atomic mass, resulting in easier extraction of lighter isotopes. Hence, subatmospheric 40Ar/36Ar ratios obtained for argon extracted at low temperatures may not represent paleoatmospheric argon. Shungite argon resembles modern atmospheric composition, but constraints on the timing of trapping appear difficult to obtain, as shungites are multicomponent systems.In 40Ar-39Ar stepwise heating, the isotope fractionation effect could cause systematic underestimations of plateau ages, between 0.15 and 0.4% depending on age, or considerably higher if samples contain appreciable atmospheric Ar. The magnitude of this effect is similar to the presently achieved uncertainties of this increasingly precise dating technique. Our results also indicate the importance of thermally activated diffusion as a possible fractionation mechanism, e.g., for hydrothermal gas exhalations, or for carbonaceous carrier phases such as “Q” in meteorites that have been suggested as carriers of highly fractionated noble gas residues from the early solar nebula. 相似文献
6.
The 13C/12C ratio of carbon compounds is used to identify sources and sinks in the global carbon cycle. However, the relatively enriched 13C content observed for marine organic carbon remains enigmatic. The majority of oceanic carbon is fixed by algae and cyanobacteria via the Calvin-Benson-Bassham cycle, yet isotopic discrimination by the CO2 fixation enzyme, RubisCO (ribulose 1,5-bisphosphate carboxylase/oxygenase), has only been measured for a single marine cyanobacterium. Different forms of RubisCO occur in different phytoplankton species (overall amino acid identity varying by as much as ∼75%) and thus may vary in the degree to which they fractionate carbon. Here we measured isotope discrimination by RubisCO from the coccolithophore Emiliania huxleyi, a cosmopolitan species used as a marine algal model.E. huxleyi RubisCO discriminated substantially less (ε = 11.1‰) against 13CO2 than other RubisCO enzymes (18-29‰), despite having Michaelis-Menten kinetic parameters (KCO2 = 72 μM; Vmax = 0.66 μmol min−1 mg−1 protein) similar to those measured for RubisCO enzymes from different organisms. If widespread, decreased isotope discrimination of 13C by phytoplankton RubisCO may be a major factor influencing the enriched 13C content of marine organic carbon. This finding emphasizes the necessity of (a) determining ε values for RubisCOs of other marine phytoplankton and (b) re-evaluation of δ13C values from physiological, environmental, and geological studies. 相似文献
7.
桂林漓江水体溶解无机碳迁移与水生光合碳固定研究 总被引:1,自引:0,他引:1
河流溶解无机碳含量昼夜变化主要受碳酸盐反向沉积、水生光合利用和脱气作用控制,被水生光合利用的溶解无机碳是岩溶碳汇的组成部分,脱气作用比例的大小是影响碳汇稳定性的决定因素。本文以漓江中游省里—冠岩之间15 km长河段为研究对象,开展昼夜高分辨率水化学自动化监测与高频取样,分析水生植物光合作用利用HCO3-1及相关钙沉降过程。结果表明,监测河段水生光合利用的无机碳转化通量为859 kgC?d-1,单位流程光合作用溶解无机碳转化量和钙沉降量分别为2.06 t?(d?km)-1和0.78 t?(d?km)-1。光合作用与钙沉降消耗DIC约占总转化量的70 %,以光合有机碳和CaCO3形式储存于河床,成为岩溶碳汇组成部分。无机碳转化量约占输入DIC总量的6.0 %(其中1.7%以CO2形式返回大气),说明夏季低水位期间强烈的水生植物光合利用溶解无机碳,可有效遏制白天水气界面CO2脱气过程发生,低脱气比例证实漓江水体的溶解无机碳还是比较稳定的。 相似文献
8.
The oxygen isotope fractionation factor of dissolved oxygen gas has been measured during inorganic reduction by aqueous FeSO4 at 10−54 °C under neutral (pH 7) and acidic (pH 2) conditions, with Fe(II) concentrations ranging up to 0.67 mol L−1, in order to better understand the geochemical behavior of oxygen in ferrous iron-rich groundwater and acidic mine pit lakes. The rate of oxygen reduction increased with increasing temperature and increasing Fe(II) concentration, with the pseudo-first-order rate constant k ranging from 2.3 to 82.9 × 10−6 s−1 under neutral conditions and 2.1 to 37.4 × 10−7 s−1 under acidic conditions. The activation energy of oxygen reduction was 30.9 ± 6.6 kJ mol−1 and 49.7 ± 13.0 kJ mol−1 under neutral and acidic conditions, respectively. Oxygen isotope enrichment factors (ε) become smaller with increasing temperature, increasing ferrous iron concentration, and increasing reaction rate under acidic conditions, with ε values ranging from −4.5‰ to −11.6‰. Under neutral conditions, ε does not show any systematic trends vs. temperature or ferrous iron concentration, with ε values ranging from −7.3 to −10.3‰. Characterization of the oxygen isotope fractionation factor associated with O2 reduction by Fe(II) will have application to elucidating the process or processes responsible for oxygen consumption in environments such as groundwater and acidic mine pit lakes, where a number of possible processes (e.g. biological respiration, reduction by reduced species) may have taken place. 相似文献
9.
生物气CO2还原途径中碳同位素分馏作用研究及应用 总被引:2,自引:0,他引:2
地质历史中,CO2/H2还原产甲烷作用对生物气的形成具有十分重要的意义。中国柴达木盆地第四系生物气主要为CO2/H2还原型生物气。笔者以CO2/H2还原生气理论为指导,进行不同初始碳同位素值和不同赋存状态碳源的生物模拟实验,研究CO2/H2还原产气过程中发生的碳同位素分馏作用。实验结果表明,产物中δ13CH4值与底物的δ13C值呈很好的正相关关系;在反应母质过量的情况下,碳源的赋存状态可以影响产物甲烷的碳同位素组成。以游离形式CO2还原产生的甲烷δ13C值,相对于以HCO3-、CO23-离子形式产生的甲烷δ13C值轻。通过柴达木盆地东部第四系生物气田实例分析,探讨了该区生物气的主要底物CO2的来源及赋存状态,对评价盆地生物气资源和有利勘探区预测有重要的参考价值。 相似文献
10.
11.
Richard E. Zeebe 《Geochimica et cosmochimica acta》2010,74(3):818-7445
Although the stable oxygen isotope fractionation between dissolved sulfate ion and H2O (hereafter ) is of physico-chemical and biogeochemical significance, no experimental value has been established until present. The primary reason being that uncatalyzed oxygen exchange between and H2O is extremely slow, taking ∼105 years at room temperature. For lack of a better approach, values of 16‰ and 31‰ at 25 °C have been assumed in the past, based on theoretical ‘gas-phase’ calculations and extrapolation of laboratory results obtained at temperatures >75 °C that actually pertain to the bisulfate system. Here I use novel quantum-chemistry calculations, which take into account detailed solute-water interactions to establish a new value for of 23‰ at 25 °C. The results of the corresponding calculations for the bisulfate ion are in agreement with observations. The new theoretical values show that sediment -data, which reflect oxygen isotope equilibration between sulfate and ambient water during microbial sulfate reduction, are consistent with the abiotic equilibrium between and water. 相似文献
12.
Chemolithotrophic homoacetogenic bacteria apparently express a characteristic stable carbon isotope fractionation and may contribute significantly to acetate production in anoxic environments. However, fractionation factors (ε) in bacterial cultures have rarely been determined and the effect of substrate availability has not been assessed. We therefore studied the kinetic carbon isotope effect in cultures of Thermoanaerobacter kivui grown at 55 °C. The fractionation factor in HCO3− buffered medium was ca. 15‰ more negative than that in PO43− buffered medium. To test whether the difference was caused by the initial substrate ratio of H2 and total inorganic carbon (TIC; 0.5 in HCO3− vs. 4.0 in PO43− buffered medium), T. kivui was grown in either [3-(N-morpholino) propanesulfonic acid, MOPS] buffered or PO43− buffered media with different HCO3− concentration. Indeed, the fractionation factor became more negative with increasing HCO3− concentration and decreasing H2/TIC ratio. While pH had only a small effect, the fractionation was generally more negative in MOPS buffered than in phosphate buffered media, indicating that the buffer system also affected fractionation. Collectively, the results show that substrate availability and other environmental factors affect the magnitude of isotope fractionation during acetate production by chemolithotrophic homoacetogenesis. 相似文献
13.
以中国南方亚热带地区典型的地下水补给型水库——大龙洞水库为对象,于2018年1月、4月、7月、10月、12月分别在上、中、下游三个监测点进行采样,探究水库热结构变化对于水体无机碳及其同位素的影响过程及机理。结果表明:(1)大龙洞水库水体在一个水文年中呈现周期性的混合期—分层期—混合期的热结构变化,4月热分层开始显现,7月逐渐显著呈现完整的热分层,10月以后热分层逐渐消失,水体逐渐实现混合;(2)水体热分层是溶解无机碳(DIC)浓度与碳稳定同位素(δ13CDIC)值变化的主要驱动力。表水层中DIC主要受水—气界面二氧化碳脱气、水生生物光合作用控制,其DIC浓度与δ13CDIC值分别为3.22 mmol·L−1和−9.15‰;温跃层中DIC主要受有机质降解过程影响,其DIC浓度与δ13CDIC值分别为3.43 mmol·L−1和−9.70‰;底水层中DIC主要受碳酸盐沉淀过程影响,其DIC浓度与δ13CDIC值分别为4.32 mmol·L−1和−11.89‰;(3)三种过程伴随水库热结构的变化而变化,驱动DIC浓度及其同位素的变化梯度 G (DIC)与 G (δ13CDIC)的变化,表现为底水层<表水层<温跃层。热分层结束进入混合期后,DIC浓度与δ13CDIC值的时空差异均逐渐消失,最终表现出DIC浓度与δ13CDIC值的均一化。 相似文献
14.
Bruce D LaZerte 《Geochimica et cosmochimica acta》1981,45(5):647-656
A model is constructed to predict the stable carbon isotope ratio of the total dissolved CO2 in aquatic sediments and laboratory reactors. The major parameters of the model are the fractionation between CO2 and CH4 as well as the intra-molecular fractionation of acetate, the relative production of CH4 from CO2 reduction versus acetate fermentation, the net production ratio of CO2 to CH4 and the stable carbon isotope ratio of the source organic carbon. The model is fitted to published data and to date from the littoral sediments of Lake Memphremagog, Quebec, Canada. The inclusion of the intra-molecular fractionation factor of acetate in the model provides a good fit to the data; without this factor, the values of the other parameters necessary for a good fit appear unreasonable. 相似文献
15.
电气石和水之间的氢同位素分馏 总被引:1,自引:0,他引:1
作者对电气-水体系氢同位素平衡分馏和动力学分馏和动力学分馏开展了实验研究,丰富了羟基矿物氢同位素分馏资料。本文对该研究的实验技术、分析方法作了介绍,并对实验结果进行讨论与国外已有的该方面的资料作了对比。在800-650℃时电气石和水之间氢同位素平衡分馏系数与温度间线性关系为103lna电气石-水=-28.24(106/T2)+2.60;交换速率常数与温度间关系为lnk2=-0.19-6.70(103/T) 相似文献
16.
Oxygen isotope fractionation between rutile and water 总被引:1,自引:0,他引:1
Synthetic rutile-water fractionations (1000 ln α) at 775, 675, and 575° C were found to be ?2.8, ?3.5, and ?4.8, respectively. Partial exchange experiments with natural rutile at 575° C and with synthetic rutile at 475° C failed to yield reliable fractionations. Isotopic fractionation within the range 575–775° C may be expressed as follows:
17.
Alan Matthews Julian R. Goldsmith Robert N. Clayton 《Geochimica et cosmochimica acta》1983,47(3):645-654
Oxygen isotope fractionations between zoisite and water have been studied at 400–700°C, PH2O = 13.4 kbar, using the three-isotope method described by Matsuhisaet al. (1978) and Matthewset al. (1983a). The zoisite-waier exchange reaction takes place extremely slowly and consequently direct-exchange calibration of equilibrium fractionation factors was possible only at 600 and 700°C. Fractionation factors at 400–600°C were determined from samples hydrothermally crystallized from a glass of the anhydrous zoisite composition. At 600°C, both exchange procedures gave identical fractionations within experimental error. Scanning electron microscope studies showed that the zoisite-water exchange reaction occurs largely by solution-precipitation mass-transfer mechanisms. The slow kinetics of zoisite-water exchange may be typical of hydrous silicates, since additional experiments on tremolite-water and chlorite-water exchange also showed very low rates. When the zoisite-water fractionation factors determined in this study are combined with the quartz and albite-water data of Matsuhisaet al. (1979) and the calcite-water data of O'Nellet al. (1969), mineral-pair fractionations are obtained for which the coefficients “A” in the equation 1000 In α = A × 106T?2 are:
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