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1.
Glassy nuclear fallout debris from near-surface nuclear tests is fundamentally reprocessed earth material. A geochemical approach to analysis of glassy fallout is uniquely suited to determine the means of reprocessing and shed light on the mechanisms of fallout formation. An improved understanding of fallout formation is of interest both for its potential to guide post-detonation nuclear forensic investigations and in the context of possible affinities between glassy debris and other glasses generated by high-energy natural events, such as meteorite impacts and lightning strikes. This study presents a large major-element compositional dataset for glasses within aerodynamic fallout from the Trinity nuclear test (“trinitite”) and a geochemically based analysis of the glass compositional trends. Silica-rich and alkali-rich trinitite glasses show compositions and textures consistent with formation through melting of individual mineral grains—quartz and alkali feldspar, respectively—from the test-site sediment. The volumetrically dominant glass phase—called the CaMgFe glass—shows extreme major-element compositional variability. Compositional trends in the CaMgFe glass are most consistent with formation through volatility-controlled condensation from compositionally heterogeneous plasma. Radioactivity occurs only in CaMgFe glass, indicating that co-condensation of evaporated bulk ground material and trace device material was the main mechanism of radioisotope incorporation into trinitite. CaMgFe trinitite glasses overlap compositionally with basalts, rhyolites, fulgurites, tektites, and microtektites but display greater compositional diversity than all of these naturally formed glasses. Indeed, the most refractory CaMgFe glasses compositionally resemble early solar system condensates—specifically, CAIs.  相似文献   

2.
Melt glasses for seven types of rock ranging from acid to basic were prepared under 1.0 GPa on a multi-anvil pressure apparatus, YJ-3000 ton press. Densities and elastic properties of the melt glasses were compared with those described in previous studies. It was found that the glasses melted under 1.0 GPa were consistent in density with both naturally-occurring glassy rocks and artificially prepared glasses melted at ambient pressure. The densities of glasses are negatively correlated with the SiO2 contents and positively correlated with the （MgO＋FeO） contents. The compressive velocity （Vp） of glass tends to increase with decreasing SiO2 contents and increasing （MgO＋FeO） contents. The shear velocity （Vs） of glass tends to increase slightly with increasing SiO2 contents, which has little connection with the （MgO＋FeO） contents. It was calculated from densities and velocities that the elastic moduli of glasses are negatively correlated with the SiO2 contents and positively correlated with the （MgO＋FeO） contents.  相似文献   

3.
大洋底的玻璃微粒   总被引：1，自引：0，他引：1  
大洋沉积物中的微玻璃陨石和火山玻璃是两类性质截然不同的微玻璃体,前者SiO2含量十分稳定,MgO含量比较高,Na2O和MnO含量都很低,并具有Os、Ir等重要地外元素丰度特征。另外,还具有特殊的表面结构以及一定的形成年代。后者的SiO2含量不稳定,MgO含量很低,Na2O和MgO含量比较高,不具有Os、Ir等地外元素丰度特征。因此,不可将它们混为一谈。  相似文献   

4.
In the formation of zeolites by hydrothermal alteration volcanic glasses are the starting material in most cases. The experiments aimed at demonstrating in what way the chemistry of the volcanic glass influences:
  1. the alteration rate of the volcanic glass to zeolites,
  2. the kind of zeolites being formed and their formation conditions.
Three volcanic glasses were used, a basaltic, a phonolitic, and a rhyolitic one. The experimental conditions were as similar as possible to the natural alteration conditions. Solutions being used: H2O dist (pH ～5.5), 0.01 n NaOH (pH ～10.5), and solutions of similar chemistry to the natural ones. The temperatures were 180 °, 200 °, 250 ° C. The experiments were carried out both in closed and in open systems. The experimental results show a difference in the alteration rate and in the zeolites being formed between the basaltic and the phonolitic glasses on the one hand and the rhyolitic one on the other. In case of the closed system the SiO2-poor volcanic glasses react more rapidly than the SiO2-rich one. The zeolites being formed are chabazite, phillipsite, analcime respectively mordenite, analcime. In case of the open system the influence of the chemistry of the volcanic glass on the alteration rate and the zeolite being formed is less significant. Which zeolite is formed at a given temperature depends on: the chemistry of the starting material, the chemistry of the reacting solution and wether there is a closed or an open system.  相似文献   

5.
Raman microprobe spectra were made on three post shock, diaplectic plagioclase feldspars. Optical and X-ray diffraction studies indicated that feldspars maintained a partially or totally crystalline state after having passed through the mixed phase zone of Hugoniot response to shock waves (15–38 GPa). The appearance of uniquely glass-type spectra occurs at different shock pressures for each specimen according to its atomic structural arrangement, below 38 GPa for mosaic structured labradorite, near 40 GPa for anorthite and above 50 GPa for the highly ordered low albite. The diaplectic anorthite and labradorite glasses give spectra which indicate the presence of two glass types. Shifts in the band envelope frequencies compared to spectra of fused glass and statically pressure densified glass suggest that these glasses have specific structural arrangements. These differences suggest that the shock and fusion glass-forming processes are not exactly identical. The results from material shocked in the mixed phase region of Hugoniot response show that the phase transitions are effected at different pressures depending upon the feldspar structural type.  相似文献   

6.
Two kinds of glasses are to be found in the breccias of the Ries basin both which have been generated by shock wave action on the rocks of the crystalline basement: a) Normal glasses, containing flow structures and vesicles; they are formed by shock waves of high energy which after unloading, leave behind material, the temperature of which is above the melting point. b) Diaplectic glasses without vesicles and flow structures, preserving the grain boundaries, cleavages and twin lamellae of the primary minerals; they are formed by shock waves of lower energy which destroy the crystal lattice but after unloading, leave behind material, the temperature of which is below the melting point. — Measurements have been taken of the density and index of refraction of diaplectic quartz- and plagioclase-glasses. The values obtained proved to be higher than those of the normal glasses and lower than those of the crystalline phases. Diaplectic glasses are distinguishable from normal glasses by their physical properties. They represent intermediate stages of structural order between the crystalline and normal glass phases.  相似文献   

7.
The vesicular glass from Köfels, Tyrol, contains grains of quartz that have been partially melted but not dissolved in the matrix glass. This phenomenon has been observed in similar glasses formed by friction along a thrust fault and by meteorite impact, but not in volcanic glasses. The explosion of a small nuclear device buried behind a steep slope produced a geologic structure that is a good small-scale model of that at Köfels. Impact of a large meteorite would have an effect analogous to that of a subsurface nuclear explosion and is the probable cause of the Köfels feature.
Zusammenfassung Der Bimsstein von Köfels, Tirol, enthält Körner von Quarz, welche teilweise geschmolzen, aber nicht im Mutterglas gelöst sind. Diese Erscheinung wurde in ähnlichen Gläsern beobachtet, welche durch Reibung entlang von Rutschverwerfungen und durch Meteoriteneinschläge entstanden, aber nicht in vulkanischen Gläsern. Die Explosion eines kleinen nuklearen Gerätes, eingegraben in einem steilen Abhang, brachte eine geologische Struktur hervor, welche ein gutes Modell im kleinen Maßstab des Vorganges bei Köfels darstellt. Der Einschlag eines großen Meteoriten würde einen Effekt hervorrufen, der analog ist einer unterirdischen nuklearen Explosion, und ist wahrscheinlich der Grund für die Bildungen von Köfels.

Wit 4 Figures

Publication authorized by the Director, U. S. Geological Survey.  相似文献   

8.
The regolith of the Apollo 16 lunar landing site is composed mainly of feldspathic lithologies but mafic lithologies are also present. A large proportion of the mafic material occurs as glass. We determined the major element composition of 280 mafic glasses (>10 wt% FeO) from six different Apollo 16 soil samples. A small proportion (5%) of the glasses are of volcanic origin with picritic compositions. Most, however, are of impact origin. Approximately half of the mafic impact glasses are of basaltic composition and half are of noritic composition with high concentrations of incompatible elements. A small fraction have compositions consistent with impact mixtures of mare material and material of the feldspathic highlands. On the basis of major-element chemistry, we identified six mafic glass groups: VLT picritic glass, low-Ti basaltic glass, high-Ti basaltic glass, high-Al basaltic glass, KREEPy glass, and basaltic-andesite glass. These glass groups encompass 60% of the total mafic glasses studied. Trace-element analyses by secondary ion mass spectroscopy for representative examples of each glass group (31 total analyses) support the major-element classifications and groupings. The lack of basaltic glass in Apollo 16 ancient regolith breccias, which provide snapshots of the Apollo 16 soil just after the infall of Imbrium ejecta, leads us to infer that most (if not all) of the basaltic glass was emplaced as ejecta from small- or moderate-sized impacts into the maria surrounding the Apollo 16 site after the Imbrium impact. The high-Ti basaltic glasses likely represent a new type of basalt from Mare Tranquillitatis, whereas the low-Ti and high-Al basaltic glasses possibly represent the composition of the basalts in Mare Nectaris. Both the low-Ti and high-Al basaltic glasses are enriched in light-REEs, which hints at the presence of a KREEP-bearing source region beneath Mare Nectaris. The basaltic andesite glasses have compositions that are siliceous, ferroan, alkali-rich, and moderately titaniferous; they are unlike any previously recognized lunar lithology or glass group. Their likely provenance is within the Procellarum KREEP Terrane, but they are not found within the Apollo 16 ancient regolith breccias and therefore were likely deposited at the Apollo 16 site post-Imbrium. The basaltic-andesite glasses are the most ferroan variety of KREEP yet discovered.  相似文献   

9.
核爆炸玻璃、撞击玻璃和玻璃陨石源岩   总被引：3，自引：0，他引：3       下载免费PDF全文
本文根据核爆炸岩石熔融玻璃的地球化学研究结果,与超速陨石撞击坑的熔岩进行比较,获得在远离热力学平衡条件下,各种玻璃和熔岩在化学成分上分布十分均匀的重要结论。岩石玻璃和熔岩是由基岩各组成岩石按一定比例混合熔融形成的。它们的主量元素和痕量元素丰度受基岩元素背景值制约。文中根据熔体和靶岩的化学成分,计算了熔岩各组成岩石的百分比。玻璃陨石是地壳岩石受撞击熔融形成的。同一撒布区的玻璃陨石化学成分相近,说明起源于同一源坑;而玻璃陨石化学成分的不同,则说明母岩组成分量的差异。因此,文中通过模拟计算,得出各玻璃陨石的组成源岩。澳大利亚撒布区的玻璃陨石,Al2O3,K2O 和Na2O 与 SiO2及 K2O/Na2O 比值不完全相同,说明澳大利亚撒布区存在着几个不同的源岩和源坑,至少有印支、爪哇、菲律宾和澳大利亚四个相应撞击坑。  相似文献   

10.
A petrographic study was conducted on a suite of bottom ash particles from 3 different modern municipal solid waste combustors. The object of the study was to evaluate the mineralogical characteristics and formation process of the bottom ash by using standard geological techniques of light microscopy, electron microscopy, and X-ray microanalysis. This information was subsequently used to model the bottom ash petrogenesis based upon an examination of the mineralogy, melt structure, and composition of the ash.Bottom ash can be divided into two major groups: 1) refractory waste products and 2) melt products. The refractory waste products consist largely of rock and mineral fragments, various waste metals, and unmelted glass shards. The melt products consist of two distinct glasses: 1) isotropic glass, and 2) opaque glass. Complex silicate minerals are precipitated from and are abundant in the isotropic glass whereas both metal oxide and silicate minerals are precipitated from the opaque glass.The isotropic and opaque glasses formed simultaneously in different locations on the combustor grate. The contrast in melting (liquidus) temperatures shown by these glasses suggests that the isotropic melts were produced at localized hot spots (1500°C to 1650°C) and the opaque melts formed at cold spots (1150°C to 1400°C) on the grate. This could be the result of heterogeneous distribution of combustible municipal solid waste on the grate or from localized hot spots where air is introduced through the grates. In some instances the two glasses then had the opportunity to variably mix with each other. Fe-oxides represent waste metal fragments that were assimilated by melting and later recrystallized.Bottom ash is produced via a co-mingled two melt system that forms melilite-bearing, alkaline, volcanic-like rocks. The great similarity of the bottom ash residues between these 3 different MSW combustors suggests that, despite variable combustor designs and heterogeneous waste feed, high temperature combustion of MSW produces bottom ash of fairly uniform composition and structure that formed via the petrogenetic process described above. Alterations to the combustion process or implementations of secondary treatment technologies may render the bottom ash residue into a more environmentally stable material better suited for aggregate or long term secure disposal in landfills.  相似文献   

11.
Shock veins and melt pockets in Lithology A of Martian meteorite Elephant Moraine (EETA) 79001 have been investigated using electron microprobe (EM) analysis, petrography and X-ray Absorption Near Edge Structure (XANES) spectroscopy to determine elemental abundances and sulfur speciation (S2− versus S6+). The results constrain the materials that melted to form the shock glasses and identify the source of their high sulfur abundances. The XANES spectra for EETA79001 glasses show a sharp peak at 2.471 keV characteristic of crystalline sulfides and a broad peak centered at 2.477 keV similar to that obtained for sulfide-saturated glass standards analyzed in this study. Sulfate peaks at 2.482 keV were not observed. Bulk compositions of EETA79001 shock melts were estimated by averaging defocused EM analyses. Vein and melt pocket glasses are enriched in Al, Ca, Na and S, and depleted in Fe, Mg and Cr compared to the whole rock. Petrographic observations show preferential melting and mobilization of plagioclase and pyrrhotite associated with melt pocket and vein margins, contributing to the enrichments. Estimates of shock melt bulk compositions obtained from glass analyses are biased towards Fe- and Mg- depletions because, in general, basaltic melts produced from groundmass minerals (plagioclase and clinopyroxene) will quench to a glass, whereas ultramafic melts produced from olivine and low-Ca pyroxene megacrysts crystallize during the quench. We also note that the bulk composition of the shock melt pocket cannot be determined from the average composition of the glass but must also include the crystals that grew from the melt - pyroxene (En72-75Fs20-21Wo5-7) and olivine (Fo75-80). Reconstruction of glass + crystal analyses gives a bulk composition for the melt pocket that approaches that of lithology A of the meteorite, reflecting bulk melting of everything except xenolith chromite.Our results show that EETA79001 shock veins and melt pockets represent local mineral melts formed by shock impedance contrasts, which can account for the observed compositional anomalies compared to the whole rock sample. The observation that melts produced during shock commonly deviate from the bulk composition of the host rock has been well documented from chondrites, rocks from terrestrial impact structures and other Martian meteorites. The bulk composition of shock melts reflects the proportions of minerals melted; large melt pockets encompass more minerals and approach the whole rock whereas small melt pockets and thin veins reflect local mineralogy. In the latter, the modal abundance of sulfide globules may reach up to 15 vol%. We conclude the shock melt pockets in EETA79001 lithology A contain no significant proportion of Martian regolith.  相似文献   

12.
Dolomite (CaMg(CO3)2) is one of the common rock-forming minerals in many geological media, in particular in clayey layers that are currently considered as potential host formations for a deep radioactive waste disposal facility. Magnesium in solution is one of the elements known to potentially enhance the alteration of nuclear glasses. The alteration of borosilicate glasses with dolomite as a Mg-bearing mineral source was investigated for 8 months in batch tests at 90 °C. Glass composition effects were investigated through two compositions (SiBNaAlCaZrO and SiBNaAlZrO) differing in their Ca content. The Ca-rich glass alteration is slightly enhanced in the presence of dolomite compared to the alteration observed in pure water. This greater alteration is explained by the precipitation of Mg silicate phases on the dolomite and glass surfaces. In contrast, the Ca-free glass alteration decreases in the presence of dolomite compared to the alteration observed in pure water. This behavior is explained by Ca incorporation in the amorphous layer (formed during glass alteration) coming from dolomite dissolution. Calcium acts as a layer reorganizer and limits glass alteration by reducing the diffusion of reactive species through the altered layer. Modeling was performed using the GRAAL model implemented within the CHESS/HYTEC geochemical code to discriminate and interpret the mechanisms involved in glass/dolomite interactions. Magnesium released by dolomite dissolution reacts with silica provided by glass alteration to form Mg silicates. This reaction leads to a pH decrease. The main mechanism controlling glass alteration is the ability of dolomite to dissolve. During the experiment the quantities of secondary phases formed were very small, but for longer time scales, this mechanism could supply sufficient Mg in solution to form large amounts of Mg silicates and sustain glass alteration. The ability of the GRAAL model to reproduce the concentrations of elements in solution and solid phases regardless of the amount of dolomite and the glass composition strongly supports the basic modeling hypothesis.  相似文献   

13.
Rock 14318 is a complex microbreccia consisting of lithic fragments, chondrules, glass spherules, and glass and mineral fragments that are embedded into a fine-grained, partly glassy matrix. Rock fragmenta, chondrules, and glasses are tightly welded to the matrix and partly recrystallized, indicating a relatively high-temperature agglomeration history. Few lithic fragments have igneous textures; most are miorobreccias that have suffered various degrees of recrystallization before they were embedded into rock 14318. Compositions of lithic fragments, glasses and chondrules, in terms of compositional rock and rock suite equivalents, represent members of the ANT (anorthositic-noritic-troctolite) suite; the alkalic high-alumina basalt (KREEP) group; high-alkali quartz basalt; basalt; and dunite. The polymict nature of many lithic fragments suggests that rook 14318 require at least two, and probably more, impact episodes for its formation. Final agglomeration took place while part of the material was hot, as is indicated by the welded texture, suggesting that the final impact event was a large one, producing a fiery cloud similar to a nuée ardente. The close similarity in texture of lunar rock 14318 to certain polymict-brecciated meteorites such as Siena suggests that meteorites of this type were also formed by complex and successive impact events on the surface of the meteorite parent body, rather than during agglomeration of the parent body.  相似文献   

14.
The paper reports scanning electron microscopy (FEG-SEM) and transmission electron microscopy (TEM) data on three cryptocrystalline (CC) cosmic spherules of chondritic composition (Mg/Si ≈ 1) from two collections taken up at glaciers at the Novaya Zemlya and in the area of the Tunguska event. The spherules show “brickwork” microtextures formed by minute parallel olivine crystals set in glass of pyroxene–plagioclase composition. The bulk-rock silicate chemistry, microtexture, mineralogy, and the chemical composition of the olivine and the local chemistry of the glass in these spherules testify to a chondritic source of the spherules. The solidification of the spherules in the Earth’s atmosphere was proved to be a highly unequilibrated process. A metastable state of the material follows, for example, from the occurrence of numerous nanometer-sized SiO2 globules in the interstitial glass. These globules were formed by liquid immiscibility in the pyroxene–SiO2 system. Troilite FeS and schreibersite (Fe,Ni)3P globules were found in the FeNi metal in one of the spherules, which suggests that the precursor was not chemically modified when melted in the Earth’s atmosphere. Our results allowed us to estimate the mineralogy of the precursor material and correlate the CC spherules with the chondrule material of chondrites. The bulk compositions of the spherules are closely similar to those of type-IIA chondrules.  相似文献   

15.
Inclusions of troilite and metallic Fe,Ni 0.2–4 mm in size with a dendritic or cellular texture were observed in 12 ordinary chondrites. Cooling rates in the interval 1400?950°C calculated from the spacing of secondary dendrite arms or cell widths and published experimental data range from 10?7 to 104°C/sec. In 8 of these chondrites, which are breccias containing some normal slow-cooled metal grains, the inclusions solidified before they were incorporated into the breccias. Their cooling rates of 1–300 °C/sec indicate cooling by radiation, or by conduction in contact with cold silicate or hot silicate volumes only 6–40 mm in size. This is quantitative evidence that these inclusions and their associated clasts were melted on the surface of a parent body (by impact), and were not formed at depth from an internally derived melt. In Ramsdorf, Rose City and Shaw, which show extensive reheating to ? 1000°C, Fe-FeS textures in melted areas are coarser and indicate cooling rates of 10?1 to 10?4°C/sec during solidification. This metal may have solidified inside hot silicate volumes that were 10–300 cm in size. As Shaw and Rose City are breccias of unmelted and melted material, their melted metal did not necessarily cool through 1000°C within a few m of the surface. Shock-melted, fine-grained, irregular intergrowths of metal and troilite formed in situ in many irons and some chondrites by rapid solidification at cooling rates of ? 105°C/sec. Their kamacite and taenite compositions may result from annealing at ~250°C of metallic glass or exceedingly fine-grained quench products.  相似文献   

16.
An analytical artefact is reported here related to differences in instrumental mass fractionation between NIST SRM glasses and natural geological glasses during SIMS boron isotope determinations. The data presented demonstrated an average 3.4‰ difference between the NIST glasses and natural basaltic to rhyolitic glasses mainly in terms of their sputtering-induced fractionation of boron isotopes. As no matrix effect was found among basaltic to rhyolitic glasses, instrumental mass fractionation of most natural glass samples can be corrected by using appropriate glass reference materials. In order to confirm the existence of the compositionally induced variations in boron SIMS instrumental mass bias, the observed offset in SIMS instrumental mass bias has been independently reproduced in two laboratories and the phenomenon has been found to be stable over a period of more than one year. This study highlights the need for a close match between the chemical composition of the reference material and the samples being investigated.  相似文献   

17.
Measured were the abundance and distribution of nitrogen in glasses of glass inclusions in olivines of CV3, CO3, CR, C4, CH3, and LL chondritic meteorites by means of the 14N(d, p)15N nuclear reaction. Similar to what was observed with carbon, nitrogen is present in low concentrations (<20 ppm) in the structure of olivines but can by stored in variable amounts in glasses of glass inclusions. These primitive glasses, characterized by a Si-Al-Ca-rich composition, have highly variable nitrogen contents (30 to 1500 ppm) and highly inhomogeneous nitrogen distribution. Nitrogen contents are independent of the chemical composition of the glasses. The heterogeneous distribution is a common feature of all studied inclusions, as is evidenced by the variable contents of nitrogen in glass inclusions occurring in the same olivine grain. Nitrogen heterogeneity is suggestive of trapping of solid nitrogen carrier phases during formation of the constituents of chondrules. However, part of the originally trapped nitrogen appears to have been lost, possibly, by ulterior oxidation and subsequent transformation into volatile species.  相似文献   

18.
Reprocessing of spent nuclear fuel (SNF) for recovery of fissionable elements is a precondition of long-term development of nuclear energetics. Solution of this problem is hindered by the production of a great amount of liquid waste; 99% of its volume is low- and intermediate-level radioactive waste (LILW). The volume of high-level radioactive waste (HLW), which is characterized by high heat release, does not exceed a fraction of a percent. Solubility of glasses at an elevated temperature makes them unfit for immobilization of HLW, the insulation of which is ensured only by mineral-like matrices. At the same time, glasses are a perfect matrix for LILW, which are distinguished by low heat release. The solubility of borosilicate glass at a low temperature is so low that even a glass with relatively low resistance enables them to retain safety of under-ground LILW depositories without additional engineering barriers. The optimal technology of liquid confinement is their concentration and immobilization in borosilicate glasses, which are disposed in shallow-seated geological repositories. The vitrification of 1 m3 liquid LILW with a salt concentration of ～300 kg/m3 leaves behind only 0.2 m3 waste, that is, 4–6 times less than by bitumen impregnation and 10 times less than by cementation. Environmental and economic advantages of LILW vitrification result from (1) low solubility of the vitrified LILW in natural water; (2) significant reduction of LILW volume; (3) possibility to dispose the vitrified waste without additional engineering barriers under shallow conditions and in diverse geological media; (4) the strength of glass makes its transportation and storage possible; and finally (5) reliable longterm safety of repositories. When the composition of the glass matrix for LILW is being chosen, attention should be paid to the factors that ensure high technological and economic efficiency of vitrification. The study of vitrified LILW from the Kursk nuclear power plant with high-power channel reactors (HPCR; equivalent Russian acronym, RBMK) and the Kalinin nuclear power plant with pressurized water reactors (PWR; equivalent Russian acronym VVER) after their 14-yr storage in the shallow-seated repository at the MosNPO Radon testing ground has confirmed the safety of repositories ensured by confinement properties of borosilicate matrix. The most efficient vitrification technology is based on cold crucible induction melting. If the content of a chemical element in waste exceeds its solubility in glass, a crystalline phase is formed in the course of vitrification, so that the glass ceramics become a matrix for such waste. Vitrified waste with high Fe; Na and Al; Na, Fe, and Al; Na and B is characterized. The composition of frit and its proportion to waste depends on waste composition. This procedure requires careful laboratory testing.  相似文献   

19.
Microscopic distribution and speciation of Na, Mg, Ni and Cs in a simulated (inactive) nuclear waste glass were studied using micro X-ray fluorescence (μ-XRF) and micro X-ray absorption spectroscopy (μ-XAS), after aqueous leaching during 12 years at 90 °C. Na and Mg are major constituents of the glass that can be used to determine the progress of the glass corrosion process and the nature of secondary alteration phases. Ni and Cs represent dose determining long-lived radionuclides (59Ni, 135Cs) in vitrified nuclear waste.The Na-Mg μ-XRF maps revealed that the core regions of the glass fragments are apparently unaltered and compositionally homogeneous, whereas rims and interstitial spaces are enriched with Mg-rich smectite formed during the leaching process. The micro X-ray absorption near edge structure (μ-XANES) spectra collected at the Mg K-edge in the altered zones show three sharp resonances typical for crystalline Mg-silicates. These resonances are distinctive of Mg occupying undistorted octahedral positions. In contrast, the μ-XANES spectra collected in the core zones of the glass fragments lack this resonance pattern and are identical to the spectra measured on the pristine (unleached) MW glass.Micro extended X-ray absorption fine structure (μ-EXAFS) and μ-XANES analyses at the Ni K-edge revealed three distinct Ni(II) species: (a) Ni uniformly distributed in the glass matrix, (b) micro-inclusions with high Ni concentrations and (c) Ni associated to the Mg-clay. The comparison with reference spectra of unleached MW and other Ni-bearing silicate glasses indicated that species (a) represents the original coordinative environment of Ni in the glass. The μ-EXAFS analyses revealed that species (b) is structural Ni in trevorite (NiFe2O4), which probably formed through unmixing processes during the cooling of the glass melt. The μ-EXAFS of species (c) could be successfully modeled assuming specific adsorption or incorporation of Ni into the lattice of trioctahedral Mg-clay minerals. Alternative models assuming other elements (Ni, Al, Fe) in addition to Mg in the second shell could not be fitted successfully.Aqueous concentration data were used to calculate the speciation of the leaching solutions. Saturation index (SI) calculations indicate undersaturation with respect to NiCO3 and NiSO4·7H2O, but oversaturation with respect to β-Ni(OH)2. The latter result is probably due to the omission of Ni borate and Ni silicate complexes in the speciation calculations, for which formation constants are not available. With the help of estimation techniques, we could infer that such complexes would dominate the Ni speciation and consequently reduce the SI below the saturation of β-Ni(OH)2.The μ-XRF maps show that Cs is uniformly distributed in the MW glass, since no region with high Cs concentration could be detected. The Cs LIII-edge μ-XAS spectra were all very similar independently of the degree of alteration, indicating similar coordination environments of Cs in the core regions of the glass as well as in the secondary clays. These spectra largely differ from that measured for pollucite (a potential secondary Cs-phase in altered glasses) implying that the coordination environments of Cs in the MW glass and in pollucite are fundamentally different.The present study shows that μ-XRF and μ-XAS are essential tools in determining the fate and the retention mechanisms of radionuclides released from nuclear waste during aqueous alteration. Our spectroscopic analyses allowed us to exclude formation of specific Ni and Cs secondary solids (e.g. nepouite, β-Ni(OH)2, pollucite) during the aqueous alteration. Ni and Cs are instead distributed as trace elements in the alteration phases formed by major elements during the leaching process. Our results imply that solid solution and/or adsorption equilibria, rather than pure phase solubility equilibria, are the adequate chemical models to determine Ni and Cs aqueous concentrations in performance assessments for radioactive waste repositories.  相似文献   

20.
准噶尔板块东北缘富铌玄武岩的发现及其地质意义   总被引：4，自引：0，他引：4       下载免费PDF全文
富铌玄武岩是硅过饱和,富Ｎａ2Ｏ,ＴｉＯ2,Ｐ2Ｏ5,同时富集高场强元素的一类岛弧玄武岩,这类玄武岩的ｗ(Ｎｂ)>7×10-6,(ｗ(Ｌａ)/ｗ(Ｎｂ))ＭＮ<2。它是由来源于70100ｋｍ深处、受ａｄａｋｉｔｅ熔体交代过的地幔楔橄榄岩部分熔融形成的,是大洋板块俯冲作用的产物。目前发现的富铌玄武岩大多分布在环太平洋新生代岛弧环境,与洋壳俯冲作用密切相关[1 5]。本研究在准噶尔板块东北缘富蕴县的索尔库都克附近首次发现了富铌玄武岩。它产于下泥盆统托让格库都克组中、上部。该地层自下而上的岩石组合为:玄武岩 火山凝灰角砾岩 火山集块岩 含…  相似文献   

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