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1.
陨石原始型惰性气体的研究进展——Q气及其携带物特征 总被引：1，自引：1，他引：0
陨石中的原始型惰性气体是在陨石形成前或陨石形成期间,组成陨石的物质通过吸附、溶解等方式将原始太阳星云中的惰性气体保留在陨石中形成的。实验研究发现,球粒陨石中的原始型惰性气体浓集中一种称为Q相的物质中,因此在原始型惰性气体中占绝对优势的组分被称为Q气或P1气。介绍了陨石原型惰性气体概念的由来、Q相的发现经过、Q相的成分和在球粒陨石中的存在部位以及Q气的元素丰度和同位素组成。并根据不同类型损石中Q气的分配情况,对其成因意义进行了讨论。 相似文献
2.
To simulate trapping of noble gases by meteorites, we reacted 15 FeCr or FeCrNi alloy samples with CO, H2O or H2S at 350–720 K, in the presence of noble gases. The reaction products, including (Fe,Cr)2O3, FeCr2S4, FeS, C, and Fe3C, were analyzed by mass spectrometry, usually after chemical separation by selective solvents. Three carbon samples were prepared by catalytic decomposition of CO or by dehydration of carbohydrates with H2SO4.The spinel and carbon samples were similar to those of earlier studies (Yang et al., 1982 and Yang and Anders, 1982), with only minor effects attributable to the presence of Ni. All samples sorted substantial amounts of noble gases, with distribution coefficients of 10?1–10?2 cm3 STP/g atm for Xe. On the basis of release temperature three gas components were distinguished: a generally dominant physisorbed component (20–80% of total), and two more strongly bound, chemisorbed and trapped components. Judging from the elemental pattern, the adsorbed components were acquired at the highest noble gas partial pressure encountered by the sample—atmosphere or synthesis vessel.Sulfides, particularly daubréelite, showed three distinctive trends relative to chromite or magnetite: the high-T component was larger, 30–70% of the total; ratios were higher, by up to 102, possibly due to preferential diffusion of Ne during synthesis. In one synthesis, at relatively high P, the gases were sorbed with only minimal elemental fractionation, presumably by occlusion.Most of the features of primordial noble gases can be explained in terms of the data and concepts presented in the three papers of this series. The elemental fractionation pattern of Ar, Kr, Xe in meteorites, terrestrial rocks, and planets resembles the adsorption pattern on the solids studied: carbon, spinels, Sulfides, etc. The variation in ratio may be explained by preferential diffusion of Ne. The high release temperature of meteoritic noble gases may be explained by transformation of physisorbed to chemisorbed gas, as observed in some experiments. The ready loss of meteoritic heavy gases on surficial oxidation (“Phase Q”) is consistent with adsorption, as is the high abundance. Extrapolation of the limited laboratory data suggests that the observed amounts of noble gases could have been adsorbed from a solar gas at 160–170 K and 10?6–10?5 atm, i.e. in the early contraction stages of the solar nebula. The principal unsolved problem is the origin of isotopically anomalous, apparently mass-fractionated noble gases in the Earth's atmosphere and in meteoritic carbon and chromite. 相似文献
3.
《Chemie der Erde / Geochemistry》2014,74(4):519-544
Noble gases are not rare in the Universe, but they are rare in rocks. As a consequence, it has been possible to identify in detailed analyses a variety of components whose existence is barely visible in other elements: radiogenic and cosmogenic gases produced in situ, as well as a variety of “trapped” components – both of solar (solar wind) origin and the “planetary” noble gases. The latter are most abundant in the most primitive chondritic meteorites and are distinct in elemental and isotopic abundance patterns from planetary noble gases sensu strictu, e.g., those in the atmospheres of Earth and Mars, having in common only the strong relative depletion of light relative to heavy elements when compared to the solar abundance pattern. In themselves, the “planetary” noble gases in meteorites constitute again a complex mixture of components including such hosted by pre-solar stardust grains.The pre-solar components bear witness of the processes of nucleosynthesis in stars. In particular, krypton and xenon isotopes in pre-solar silicon carbide and graphite grains keep a record of physical conditions of the slow-neutron capture process (s-process) in asymptotic giant branch (AGB) stars. The more abundant Kr and Xe in the nanodiamonds, on the other hand, show a more enigmatic pattern, which, however, may be related to variants of the other two processes of heavy element nucleosynthesis, the rapid neutron capture process (r-process) and the p-process producing the proton-rich isotopes.“Q-type” noble gases of probably “local” origin dominate the inventory of the heavy noble gases (Ar, Kr, Xe). They are hosted by “phase Q”, a still ill-characterized carbonaceous phase that is concentrated in the acid-insoluble residue left after digestion of the main meteorite minerals in HF and HCl acids. While negligible in planetary-gas-rich primitive meteorites, the fraction carried by “solubles” becomes more important in chondrites of higher petrologic type. While apparently isotopically similar to Q gas, the elemental abundances are somewhat less fractionated relative to the solar pattern, and they deserve further study. Similar “planetary” gases occur in high abundance in the ureilite achondrites, while small amounts of Q-type noble gases may be present in some other achondrites. A “subsolar” component, possibly a mixture of Q and solar noble gases, is found in enstatite chondrites. While no definite mechanism has been identified for the introduction of the planetary noble gases into their meteoritic host phases, there are strong indications that ion implantation has played a major role.The planetary noble gases are concentrated in the meteorite matrix. Ca-Al-rich inclusions (CAIs) are largely planetary-gas-free, however, some trapped gases have been found in chondrules. Micrometeorites (MMs) and interplanetary dust particles (IDPs) often contain abundant solar wind He and Ne, but they are challenging objects for the analysis of the heavier noble gases that are characteristic for the planetary component. The few existing data for Xe point to a Q-like isotopic composition. Isotopically Q-Kr and Q-Xe show a mass dependent fractionation relative to solar wind, with small radiogenic/nuclear additions. They may be closer to “bulk solar” Kr and Xe than Kr and Xe in the solar wind, but for a firm conclusion it is necessary to gain a better understanding of mass fractionation during solar wind acceleration. 相似文献
4.
Abundances and isotopic compositions of Ne (in bulk samples only), Ar, Kr, and Xe have been investigated in 6 monomict, 3 polymict, and the diamond-free ureilite ALH78019 and their acid-resistant, C-rich residues. Isotopic ratios of Kr and Xe are very uniform and agree with data for ureilites from the literature. The measured ratio 38Ar/36Ar showed large variations due to an experimental artifact. This is shown to be connected to the pressure dependence of the instrumental mass discrimination, which for ureilites with their low abundance of 40Ar is different from that of the usual air standard. This observation necessitates a reassessment for the recently reported 36Ar excesses due to possible decay of extinct 36Cl in the Efremovka meteorite.Trapped 22Ne in the range of (1.4-2.5) × 10−8 cc STP/g is present in bulk ureilites. A Ne three-isotope plot for polymict ureilites indicates the presence of solar Ne. 21Ne-based cosmic ray exposure ages for the 10 ureilites studied range from 0.1 Ma (for ALH78019) to 46.8 Ma (for EET83309)All ureilites may have started with nearly the same initial elemental ratio (132Xe/36Ar)0, established in the nebula during gas trapping into their carbon carrier phases (diamond, amorphous C) by ion implantation. Whereas diamonds are highly retentive, amorphous C has suffered gas loss due to parent body metamorphism. The correlation of the elemental ratios 132Xe/36Ar and 84Kr/36Ar along the mass fractionation line could be understood as a two-component mixture of the unaffected diamond gases and the fractionated (to varying degrees) gases from amorphous C. In this view, the initial ratio (132Xe/36Ar)0 is a measure of the plasma temperature in the nebula at the formation location of the carbon phases. Its lack of correlation with Δ17O (a signature of the silicate formation location) indicates that carbon phases and silicates formed independently in the nebula, and not from a carbon-rich magmaThe elemental ratios 132Xe/36Ar and 84Kr/36Ar in carbon-rich acid residues show a decreasing trend with depth (inferred from carbon consumption during combustion), which can be interpreted as a consequence of the ion implantation mechanism of gas trapping that leads to greater depth of implantation for lighter mass ionThe similarity between trapped gases in phase Q in primitive chondrites and the C phases in ureilites—for both elemental and isotopic compositions—strongly suggests that phase Q might also have received its noble gases by ion implantation from the nebula. The slight differences in the elemental ratios can be explained by a plasma temperature at the location of phase Q gas loading that was about 2000 K lower than for ureilite C phases. This inference is also consistent with the finding that the trapped ratio 129Xe/132Xe (1.042 ± 0.002) in phase Q is slightly higher, compared to that of ureilite C phases (1.035 ± 0.002), as a consequence of in situ decay of 129I, and becomes observable due to higher value of I/Xe in phase Q as a result of ion implantation at about 2000 K lower plasma temperature. 相似文献
5.
Two examined fragments of the Kaidun meteorite principally differ in the concentrations of isotopes of noble gases and are very heterogeneous in terms of the isotopic composition of the gases. Because these fragments belong to two basically different types of meteoritic material (EL and CR chondrites), these characteristics of noble gases could be caused by differences in the cosmochemical histories of the fragments before their incorporation into the parent asteroid. As follows from the escape kinetics of all gases, atoms of trapped and cosmogenic noble gases are contained mostly in the structures of two carrier minerals in the samples. The concentrations and proportions of the concentrations of various primary noble gases in the examined fragments of Kaidun are obviously unusual compared to data on most currently known EL and CR meteorites. In contrast to EL and CR meteorites, which contain the primary component of mostly solar provenance, the elemental ratios and isotopic composition of Ne and He in the fragments of Kaidun correspond to those typical of the primary components of A and Q planetary gases. This testifies to the unique conditions under which the bulk of the noble gases were trapped from the early protoplanetary nebula. The apparent cosmic-ray age of both of the Kaidun fragments calculated based on cosmogenic isotopes from 3He to 126Xe varies from 0.027 to 246 Ma as a result of the escape of much cosmogenic isotopes at relatively low temperatures. The extrapolated cosmic-ray age of the Kaidun meteorite, calculated from the concentrations of cosmogenic isotopes of noble gases, is as old as a few billion years, which suggests that the material of the Kaidun meteorite could be irradiated for billions of years when residing in an unusual parent body. 相似文献
6.
Noble gases were measured both in bulk samples (stepped pyrolysis and total extraction) and in a HF/HCl residue (stepped pyrolysis and combustion) from the Klein Glacier (KLE) 98300 EH3 chondrite. Like the bulk meteorite and as seen in previous studies of bulk type 3 E chondrites (“sub-Q”), the acid residue contains elementally fractionated primordial noble gases. As we show here, isotopically these are like those in phase-Q of primitive meteorites, but elementally they are heavily fractionated relative to these. The observed noble gases are different from “normal” Q noble gases also with respect to release patterns, which are similar to those of Ar-rich noble gases in anhydrous carbonaceous chondrites and unequilibrated ordinary chondrites (with also similar isotopic compositions). While we cannot completely rule out a role for parent body processes such as thermal and shock metamorphism (including a later thermal event) in creating the fractionated elemental compositions, parent body processes in general seem not be able to account for the distinct release patterns from those of normal Q noble gases. The fractionated gases may have originated from ion implantation from a nebular plasma as has been suggested for other types of primordial noble gases, including Q, Ar-rich, and ureilite noble gases. With solar starting composition, the corresponding effective electron temperature is about 5000 K. This is lower than inferred for other primordial noble gases (10,000-6000 K). Thus, if ion implantation from a solar composition reservoir was a common process for the acquisition of primordial gas, electron temperatures in the early solar system must have varied spatially or temporally between 10,000 and 5000 K.Neon and xenon isotopic ratios of the residue suggest the presence of presolar silicon carbide and diamond in abundances lower than in the Qingzhen EH3 and Indarch EH4 chondrites. Parent body processes including thermal and shock metamorphism and a late thermal event also cannot be responsible for the low abundances of presolar grains. KLE 98300 may have started out with smaller amounts of presolar grains than Qingzhen and Indarch. 相似文献
7.
As- and Mo- bearing secondary mineral phases formed during the neutralization of uranium mill wastes require characterization. Previous studies indicate that arsenate and molybdate adsorbed to ferrihydrite are the dominant controls in the tailings materials. A lab-scale plant was employed to characterize secondary precipitates from a variety of ore blends. Through total elemental analysis of precipitates and As and Mo K-edge X-ray absorption spectroscopy, different ratios of contributing phases were determined for each pH stage (4.2, 6.5, and 9.2) of the neutralization process. Overall, arsenate adsorbed to ferrihydrite was the dominant As mineral phase regardless of pH or sample blend (53–77%), with fractional contribution from ferric arsenates, and adsorption to aluminum phases. Molybdate adsorbed to ferrihydrite was the dominant Mo mineral phase, with fractional contribution decreasing with increasing pH (100–69%). The characterization of these phases in the secondary precipitates provides further understanding of the contributing mineral species in tailing facilities. 相似文献
8.
A. B. Verchovsky 《Geochemistry International》2017,55(11):957-970
Bulk meteorite samples of various chemical classes and petrologic types (mainly carbonaceous chondrites) were systematically investigated by the stepped combustion method with the simultaneous isotopic analysis of carbon, nitrogen, and noble gases. A correlation was revealed between planetary noble gases associating with the Q phase and isotopically light nitrogen (δ15N up to –150‰). The analysis of this correlation showed that the isotopically light nitrogen (ILN) is carried by Q. In most meteorites, isotopically heavy nitrogen (IHN) of organic compounds (macromolecular material) is dominant. The ILN of presolar grains (diamond and SiC) and Q can be detected after separation from dominant IHN. Such a separation of nitrogen from Q and macromolecular material occurs under natural conditions and during laboratory stepped combustion owing to Q shielding from direct contact with oxygen, which results in Q oxidation at temperatures higher than the temperatures of the release of most IHN. There are arguments that ILN released at high temperature cannot be related to nanodiamond and SiC. The separation effect allowed us to constrain the contents of noble gases in Q, assuming that this phase is carbon-dominated. The directly measured 36Ar/C and 132Xe/C ratios in ILN-rich temperature fractions are up to 0.1 and 1 × 10–4 cm3/g, respectively. These are only lower constraints on the contents. The analysis of the obtained data on the three-isotope diagram δ15N–36Ar/14N showed that Q noble gases were lost to a large extent from most meteorites during the metamorphism of their parent bodies. Hence, the initial contents of noble gases in Q could be more than an order of magnitude higher than those directly measured. Compared with other carbon phases, Q was predominantly transformed to diamond in ureilites affected by shock metamorphism. The analysis of their Ar–N systematics showed that, similar to carbonaceous chondrites, noble gases were lost from Q probably before its transformation to diamond. 相似文献
9.
10.
Reductive dissolution of arsenic-bearing ferrihydrite 总被引：2，自引：0，他引：2
Jasmine J. Erbs Brian C. Reinsch Gregory V. Lowry Subir K. Banerjee 《Geochimica et cosmochimica acta》2010,74(12):3382-8833
Ferrihydrites were prepared by coprecipitation (COP) or adsorption (ADS) of arsenate, and the products were characterized using solid-state methods. In addition, the kinetics of reductive dissolution by hydroquinone of these well-characterized materials were quantified. Characterization and magnetism results indicate that the 10 wt% As COP ferrihydrite is less crystalline and possibly has smaller crystallite size than the other ferrihydrites, which all have similar crystallinity and particle size. The results from reductive dissolution experiments show similar reaction rates, reaction mechanism, and activation energy for ferrihydrite precipitated with or without added arsenate. However, a marked decrease in reactivity was observed for 10 wt% As ADS ferrihydrite. The decrease is not attributed to differences in activation energy but rather the preferential blocking of active sites on the ferrihydrite surface. Results demonstrate that arsenic may be released by the reductive dissolution of arsenic-bearing ferrihydrite regardless of whether the arsenic is coprecipitated with or adsorbed onto the ferrihydrite. However, under these reaction conditions, release from materials with adsorbed arsenate greatly exceeds that from materials with coprecipitated arsenate. In fact, a considerable amount of arsenic was released from the 10 wt% ADS ferrihydrite before reductive dissolution was initiated. Therefore, the characterization of arsenate-bearing iron oxide materials to determine the method of arsenate incorporation into structures—perhaps by quantification of Fe-Fe coordination with EXAFS spectroscopy—may lead to improved predictions of the large-scale release of arsenic within aquifer systems under reducing conditions. 相似文献
11.
Jun-ichi Matsuda Kazuhiko Morishita Chie Miyakawa Sachiko Amari Seiji Takeda 《Geochimica et cosmochimica acta》2010,74(18):5398-5409
We have prepared a HF-HCl residue and its oxidized residue of the Allende meteorite and have measured the elemental concentrations and the isotopic compositions of noble gases. In the HF-HCl reside, noble gases are enriched in colloidal fraction compared to the non-colloidal fraction by a factor of 2-4. The heavy noble gases were evidently lost after the oxidization, indicating that phase Q (carrier of planetary heavy noble gases) was removed by the oxidation. The Raman spectroscopic parameters show that the colloidal fraction of the HF-HCl residue is more amorphous compared to the non-colloidal fraction. As the ion irradiation converts carbon into a more amorphous form, our result indicates that the “plasma model” is more plausible than the “labyrinth model” as the origin of phase Q. TEM (Transmission Electron Microscope) observations also show such a trace of ion irradiation. While the TEM observations did not show any large difference between the HF-HCl residue and its oxidized residue, the Raman spectroscopic parameters changed discretely resulting from the oxidization. This observation indicates that the oxidization not only dissolved and removed oxidized carbon, but also changed the carbon structure itself to a more amorphous (disordered) state. The Raman spectroscopic results indicate the possibility that release of Q-gas during oxidation is not accompanied by mass loss and that the release of Q-gas simply resulted from rearrangement of carbon structure during oxidation. 相似文献
12.
Pyrolysis experiments were carried out on Monterey formation kerogen and bitumen and Green River formation kerogen (Type II and I, respectively), in the presence and absence of montmorillonite, illite and calcite at 200 and 300°C for 2–2000 hours. The pyrolysis products were identified and quantified and the results of the measurements on the gas and condensate range are reported here.A significant catalytic effect was observed for the pyrolysis of kerogen with montmorillonite, whereas small or no effects were observed with illite and calcite, respectively. Catalytic activity was evident by the production of up to five times higher C1–C6 hydrocarbons for kerogen with montmorillonite than for kerogen alone, and by the dominance of branched hydrocarbons in the C4–C6 range (up to 90% of the total amount at any single carbon number). This latter effect in the presence of montmorillonite is attributed to cracking via a carbonium-ion [carbocation] intermediate which forms on the acidic sites of the clay. No catalytic effect, however, was observed for generation of methane and C2 hydrocarbons which form by thermal cracking. The catalysis of montmorillonite was significantly greater during pyrolysis of bitumen than for kerogen, which may point to the importance of the early formed bitumen as an intermediate in the production of low molecular weight hydrocarbons. Catalysis by minerals was also observed for the production of carbon dioxide.These results stress the importance of the mineral matrix in determining the type and amount of gases and condensates forming from the associated organic matter under thermal stress. The literature contains examples of gas distributions in the geologic column which can be accounted for by selective mineral catalysis, mainly during early stages of organic matter maturation. 相似文献
13.
Noble gases trapped in primitive meteorites are quantitatively hosted by a poorly defined organic phase, labeled phase Q. Xenon is enriched in heavy isotopes by +1.30 ± 0.06% per atomic mass unit (amu, 1σ) in phase Q relative to solar. To understand the origin of this fractionation, we have performed adsorption experiments of xenon atoms and ions, ionized in a radiofrequency plasma. Within the reaction vessel, anthracite was heated and the resulting smoke deposited onto the walls of the vessel, resulting in carbon-rich films. Xenon was trapped in the carbon films either as ions in the ionization zone of the vessel, or as neutral atoms outside this zone. Xenon trapped as ionic Xe is tightly bound and is enriched by +1.36 ± 0.05%/amu (1σ) in heavy isotopes, reproducing the isotopic fractionation of xenon trapped in phase Q relative to solar. Neutral xenon is more loosely trapped, is in much lower concentration, and is not isotopically fractionated. Ionized conditions allow the constant xenon isotopic composition observed in meteorite during stepwise heating release to be reproduced. Furthermore, the trapping efficiency of Xe+ estimated from these experiments is consistent with the high xenon concentration measured in phase Q of primitives meteorites.Xenon was not trapped in the film by implantation because the energies of the incident Xe atoms and ions were far too low (<1 eV). From the difference of behavior between ionic and neutral forms, we propose that xenon ions were trapped via chemical bonding at the surface of the newly created C-rich film. The observed mass-dependent fractionation of xenon is unlikely to have occurred in the gas phase. It is more probably related to variations in chemical bonding strengths of Xe isotopes as chemical bonds involving heavy Xe isotopes are more stable than those involving light ones. For young stars, including the young Sun, photons emitted in the far UV energy range able to ionize noble gases (<100 nm) were orders of magnitude more abundant than for the Present-day Sun, allowing efficient ionization of gaseous species. A way to achieve Q-noble gas fractionation and trapping was UV irradiation by nearby young stars from O/B association of the surface of growing organic grains in the outer part of the solar system or by the young Sun at the edge of the disk. 相似文献
14.
C.M. Hansel D.R. Learman C.J. Lentini E.B. Ekstrom 《Geochimica et cosmochimica acta》2011,75(16):4653-4666
The poorly crystalline Fe(III) hydroxide ferrihydrite is considered one of the most important sinks for (in)organic contaminants and nutrients within soils, sediments, and waters. The ripening of ferrihydrite to more stable and hence less reactive phases such as goethite is catalyzed by surface reaction with aqueous Fe(II). While ferrihydrite within most natural environments contains high concentrations of adsorbed or co-precipitated cations (particularly Al), little is known regarding the impact of these cations on Fe(II)-induced transformation of ferrihydrite to secondary phases. Accordingly, we explored the extent, rates, and pathways of Fe(II)-induced secondary mineralization of Al-ferrihydrites by reacting aqueous Fe(II) (0.2 and 2.0 mM) with 2-line ferrihydrite containing a range of Al levels substituted within (6-24 mol% Al) or adsorbed on the surface (0.1-27% Γmax). Here, we show that regardless of the Fe(II) concentration, Al substituted within or adsorbed on ferrihydrite results in diminished secondary mineralization and preservation of ferrihydrite. In contrast to pure ferrihydrite, the concentration of Fe(II) may not in fact influence the mineralization products of Al-compromised ferrihydrites. Furthermore, the secondary mineral profiles upon Fe(II) reaction with ferrihydrite are not only a function of Al concentration but also the mode of Al incorporation. While Al substitution impedes lepidocrocite formation and magnetite nucleation, Al adsorption completely inhibits goethite formation and appears to have a lesser impact on magnetite nucleation. When normalized to total Al content associated with ferrihydrite, Al adsorption results in greater degree of ferrihydrite preservation relative to Al substitution. These findings provide insight into mechanisms that may be responsible for ferrihydrite preservation and low levels of secondary magnetite typically found in sedimentary environments. Considering the preponderance of cation substitution within and adsorption on ferrihydrite in soils and sediments, the reactivity of natural (compromised) ferrihydrites and the subsequent impact on mineral evolution needs to be more fully explored. 相似文献
15.
海相干酪根与原油裂解气甲烷生成及碳同位素分馏的差异研究 总被引：10，自引：3，他引：10
利用封闭金管高压釜体系对海相原油和成熟干酪根进行了热解生气实验,获取了两类裂解气的组分和甲烷碳同位素数据,对比研究了两类母质在生气机理上的差异,并借助碳同位素分馏动力学参数讨论了甲烷碳同位素分馏的异同点.结果表明,原油裂解气富含C2-5重烃,其后期裂解是甲烷的重要来源;而干酪根裂解气中C2-5的含量较低,其后期裂解对干酪根甲烷气的贡献较小.这是两类甲烷气体生成的最大差异之一.两类裂解气甲烷碳同位素都有随着热解温度增高,碳同位素值先变轻再变重的特点,但原油裂解气甲烷碳同位素的最小值对应的温度较高;在相同热解温度下,干酪根裂解气甲烷碳同位素值要重于原油裂解气甲烷碳同位素值,这与后者前系物经过多次碳同位素分馏有关.因此,生气机理的差异是造成同位素分馏差异的根本原因,两类甲烷气体碳同位素分馏动力学参数的差异也是有成因意义的. 相似文献
16.
Chronology and shock history of the Bencubbin meteorite: A nitrogen, noble gas, and Ar-Ar investigation of silicates, metal and fluid inclusions 总被引：1，自引：0，他引：1
We have investigated the distribution and isotopic composition of nitrogen and noble gases, and the Ar-Ar chronology of the Bencubbin meteorite. Gases were extracted from different lithologies by both stepwise heating and vacuum crushing. Significant amounts of gases were found to be trapped within vesicles present in silicate clasts. Results indicate a global redistribution of volatile elements during a shock event caused by an impactor that collided with a planetary regolith. A transient atmosphere was created that interacted with partially or totally melted silicates and metal clasts. This atmosphere contained 15N-rich nitrogen with a pressure ?3 × 105 hPa, noble gases, and probably, although not analyzed here, other volatile species. Nitrogen and noble gases were re-distributed among bubbles, metal, and partly or totally melted silicates, according to their partition coefficients among these different phases. The occurrence of N2 trapped in vesicles and dissolved in silicates indicates that the oxygen fugacity (fO2) was greater than the iron-wüstite buffer during the shock event. Ar-Ar dating of Bencubbin glass gives an age of 4.20 ± 0.05 Ga, which probably dates this impact event. The cosmic-ray exposure age is estimated at ∼40 Ma with two different methods. Noble gases present isotopic signatures similar to those of “phase Q” (the major host of noble gases trapped in chondrites) but elemental patterns enriched in light noble gases (He, Ne and Ar) relative to Kr and Xe, normalized to the phase Q composition. Nitrogen isotopic data together with 40Ar/36Ar ratios indicate mixing between a 15N-rich component (δ15N = +1000‰), terrestrial N, and an isotopically normal, chondritic N.Bencubbin and related 15N-rich meteorites of the CR clan do not show stable isotope (H and C) anomalies, precluding contribution of a nucleosynthetic component as the source of 15N enrichments. This leaves two possibilities, trapping of an ancient, highly fractionated atmosphere, or degassing of a primitive, isotopically unequilibrated, nitrogen component. Although the first possibility cannot be excluded, we favor the contribution of primitive material in the light of the recent finding of extremely 15N-rich anhydrous clasts in the CB/CH Isheyevo meteorite. This unequilibrated material, probably carried by the impactor, could have been insoluble organic matter extremely rich in 15N and hosting isotopically Q-like noble gases, possibly from the outer solar system. 相似文献
17.
Arsenate and antimonate are water-soluble toxic mining waste species which often occur together and can be sequestered with varying success by a hydrous ferric oxide known as ferrihydrite. The competitive adsorption of arsenate and antimonate to thin films of 6-line ferrihydrite has been investigated using primarily adsorption/desorption kinetics monitored by in situ attenuated total reflectance infrared (ATR-IR) spectroscopy on flowed solutions containing 10−3 and 10−5 mol L−1 of both species at pH 3, 5, and 7. ICP-MS analysis of arsenate and antimonate adsorbed to 6-line ferrihydrite from 10−3 mol L−1 mixtures in batch adsorption experiments at pH 3 and 7 was carried out to calibrate the relative surface concentrations giving rise to the IR spectral absorptions. The kinetic data from 10−3 and 10−5 mol L−1 mixtures showed that at pH 3 antimonate achieved a greater surface concentration than arsenate after 60 min adsorption on 6-line ferrihydrite. However, at pH 7, the adsorbed arsenate surface concentration remained relatively high while that of adsorbed antimonate was much reduced compared with pH 3 conditions. Both species desorbed slowly into pH 3 solution while at pH 7 most adsorbed arsenate showed little desorption and adsorbed antimonate concentration was too low to register its desorption behaviour. The nature of arsenate which is almost irreversibly adsorbed to 6-line ferrihydrite remains to be clarified. 相似文献
18.
Sixteen amorphous carbon (lampblack) samples that had been exposed to Xe127 and pumped for >9 hrs to remove the most labile gas were examined by etching with HNO3, for comparison with the release pattern of meteoritic xenon. Samples originally exposed at 100–200°C lost 90% of their Xe very readily, when the surface had been etched to a mean depth of only ~0.2 Å. This suggests that the Xe is adsorbed mainly at rare sites that are unusually reactive to HNO3. The adsorbed Xe survived several months' storage in vacuum, but on exposure to air, part of it was lost within a few hours, while the remainder persisted without measurable exchange. Samples exposed at 800–1000°C had a similar adsorbed component, as well as a second, tightly bound component extending to a mean depth of up to 30 Å; this component had apparently diffused into the carbon during exposure. The (microscopic) diffusion coefficient for graphitic crystallites is 5 × 10?20 cm2/sec at 1000°C.PVDC carbon lost its adsorbed Xe at about the same rate as lampblack on exposure to air or HNO3, though it differs from lampblack in being non-graphitizable and more porous. It had only a small diffused component, however.The most tightly bound part of the Xe adsorbed on lampblack resembles planetary Xe in most characteristics: surface siting, etchability, persistence in vacuum, and lack of exchange with atmospheric Xe. The Xe concentrations—if interpreted as equilibrium distribution coefficients—are some 106× too small to account for meteoritic Xe, but it appears that equilibrium had not been reached by any of the samples, even after 1 day's exposure to Xe. If the uptake of Xe is controlled by rate rather than equilibrium, then the high noble gas concentrations in meteorites may simply reflect the much longer uptake times in the solar nebula. It seems likely that the trapping mechanisms discussed here can also explain two other features: elemental fractionations of noble gases, and the close correlation between planetary Xe and CCFXe. 相似文献
19.
本文利用高表面活性矿物蒙脱石、蛭石、沸石在一定的介质条件下对Zn2 +进行吸附实验研究。蒙脱石和蛭石对Zn2 +的等温吸附线呈双“S”型 ,而沸石对Zn2 +的等温吸附线则呈“Langmuir”型。三种矿物对Zn2 +的吸附容量大小顺序为 :蒙脱石 >蛭石 >沸石。运用粉晶X射线衍射、红外光谱、差热及热重分析等技术对矿物及矿物吸附Zn2 +后的结构特征进行了研究。结果表明 ,蒙脱石吸附锌后其层间域中吸附锌大量水解形成新的物相 ,而蛭石与沸石吸附锌后水解很少。这为利用高表面活性矿物控制和治理环境污染及其可循环利用提供了理论依据。 相似文献
20.
《Chemie der Erde / Geochemistry》2016,76(4):463-480
Since about half a century samples from the lunar and asteroidal regoliths been used to derive information about elemental and isotopic composition and other properties of the present and past solar wind, predominantly for the noble gases and nitrogen. Secular changes of several important compositional parameters in the solar wind were proposed, as was a likely secular decrease of the solar wind flux. In 2004 NASA’s Genesis mission returned samples which had been exposed to the solar wind for almost 2.5 years. Their analyses resulted in an unprecendented accuracy for the isotopic and elemental composition of several elements in the solar wind, including noble gases, O and N. The Genesis data therefore also allow to re-evaluate the lunar and meteorite data, which is done here. In particular, claims for long-term changes of solar wind composition are reviewed.Outermost grain layers from relatively recently irradiated lunar regolith samples conserve the true isotopic ratios of implanted solar wind species. This conclusion had been made before Genesis based on the agreement of He and Ne isotopic data measured in the aluminum foils exposed to the solar wind on the Moon during the Apollo missions with data obtained in the first gas release fractions of stepwise in-vacuo etch experiments. Genesis data allowed to strengthen this conclusion and to extend it to all five noble gases. Minor variations in the isotopic compositions of implanted solar noble gases between relatively recently irradiated samples (<100 Ma) and samples irradiated billions of years ago are very likely the result of isotopic fractionation processes that happened after trapping of the gases rather than indicative of true secular changes in the solar wind composition. This is particularly important for the 3He/4He ratio, whose constancy over billions of years indicates that hardly any 3He produced as transient product of the pp-chains has been mixed from the solar interior into its outer convective zone. The He isotopic composition measured in the present-day solar wind therefore is identical to the (D + 3He)/4He ratio at the start of the suns’s main sequence phase and hence can be used to determine the protosolar D/H ratio.Genesis settled the long-standing controversy on the isotopic composition of nitrogen in lunar regolith samples. The 15N/14N ratio in the solar wind as measured by Genesis is lower than in any lunar sample. This proves that nitrogen in regolith samples is dominated by non-solar sources. A postulated secular increase of 15N/14N by some 30% over the past few Ga is not tenable any longer. Genesis also provided accurate data on the isotopic composition of oxygen in the solar wind, invaluable for cosmochemisty. These data superseded but essentially confirmed one value – and disproved a second one – derived from lunar regolith samples shortly prior to Genesis.Genesis also confirmed prior conclusions that lunar regolith samples essentially conserve the true elemental ratios of the heavy noble gases in the solar wind (Ar/Kr, Kr/Xe). Several secular changes of elemental abundances of noble gases in the solar wind had been proposed based on lunar and meteoritic data. I argue here that lunar data – in concert with Genesis – provide convincing evidence only for a long-term decrease of the Kr/Xe ratio by almost a factor of two over the past several Ga. It appears that the enhancement of abundances of elements with a low first ionisation potential in the solar wind (FIP effect) changed with time.Finally, Genesis allows a somewhat improved comparison of the present-day flux of solar wind Kr and Xe with the total amount of heavy solar wind noble gases in the lunar regolith. It remains unclear whether the past solar wind flux has been several times higher on average than it is today. 相似文献