Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) has been applied to determine the elemental composition of the surface layer, as well as of the first interior layer, of quartz grains from the mine tailings from Kristineberg (northern Sweden) in order to determine concentration gradients between these two layers. The quartz grains were collected from the oxidized and unoxidized zones within the tailings. The aim of this study is to assess the role of quartz surfaces as sites for the attenuation of solutes from the mine-tailings porewater. Concentrations of Cu, Ag, Sb, Pb and Bi are highest near the surface of each grain and decrease towards the interior. The surface concentration of Cu, Zn and Pb is more pronounced within the unoxidized than within the oxidized zone of the tailings. Cu exhibits a distinct concentration peak at the surface of the quartz grains below the pre-remediation oxidation front. For Zn and Ce the trend of high surface concentration is less pronounced than for Cu or Pb. Silver, Bi and As are preferably adsorbed within the uppermost layers of the oxidized zone where the pH is as high as 6.2. The conversion of intensity signals of the elements to concentration values in ppm was done by using external standards (NIST silicate glass). 相似文献
The electron localization function, η, evaluated for first-principles geometry optimized model structures generated for quartz and coesite, reveals that the oxide anions are coordinated by two hemispherically shaped η-isosurfaces located along each of the SiO bond vectors comprising the SiOSi angles. With one exception, they are also coordinated by larger banana-shaped isosurfaces oriented perpendicular to the plane centered in the vicinity of the apex of each angle. The hemispherical isosurfaces, ascribed to domains of localized bond-pair electrons, are centered ~0.70 Å along the bond vectors from the oxide anions and the banana-shaped isosurfaces, ascribed to domains of localized nonbonding lone-pair electrons, are centered ~0.60 Å from the apex of the angle. The oxide anion comprising the straight SiOSi angle in coesite is the one exception in that the banana-shaped isosurface is missing; however, it is coordinated by two hemispherically shaped isosurfaces that lie along the bond vectors. In the case of a first-principles model structure generated for stishovite, the oxide anion is coordinated by five hemispherically shaped η-isosurfaces, one located along each of the three SiO bond vectors (ascribed to domains of bonding-electron pairs) that are linked to the anion with the remaining two (ascribed to domains of nonbonding-electron pairs) located on opposite sides of the plane defined by three vectors, each isosurface at a distance of ~0.5 Å from the anion. The distribution of the five isosurfaces is in a one-to-one correspondence with the distribution of the maxima displayed by experimental Δρ and theoretical ??2ρ maps. Isosurface η maps calculated for quartz and the (HO)3SiOSi(OH)3 molecule also exhibit maxima that correspond with the (3,?3) maxima displayed by distributions of ??2ρ. Deformation maps observed for the SiOSi bridges for the silica polymorphs and a number of silicates are similar to that calculated for the molecule but, for the majority, the maxima ascribed to lone-pair features are absent. The domains of localized nonbonding-electron pair coordinating the oxide anions of quartz and coesite provide a basis for explaining the flexibility and the wide range of the SiOSi angles exhibited by the silica polymorphs with four-coordinate Si. They also provide a basis for explaining why the SiO bond length in coesite decreases with increasing angle. As found in studies of the interactions of solute molecules with a solvent, a mapping of η-isosurfaces for geometry-optimized silicates is expected to become a powerful tool for deducing potential sites of electrophilic attack and reactivity for Earth materials. The positions of the features ascribed to the lone pairs in coesite correspond with the positions of the H atoms recently reported for an H-doped coesite crystal. 相似文献
Modern and known-age Pleistocene fluvial sediments were investigated by optical dating of quartz to test the suitability of the approach for dating deposits from the deeply incised Middle Rhine Valley. Samples from modern flood sediments revealed skewed distributions indicating different residual levels of equivalent dose (De) within the different aliquots. Nevertheless, a substantial number of aliquots from the modern deposits reflect De values close to zero. For the Pleistocene samples, optical ages are in general consistent with age control given by the presence of the Laacher See Tephra and radiocarbon dating. However, some samples overestimate the known age by a few thousand years when using the arithmetic mean. This is apparently explained by including aliquots in the determination of mean De where the optical signal was incompletely bleached at deposition. The most difficult issue in this context is identifying a suitable approach that can distinguish between the variability of De due to partial bleaching and microdosimetry. However, even when considering these limitations it appears that optical dating will by a quite suitable method to date Pleistocene sediments from such a complex fluvial environment, especially when focusing on a precision scale beyond a few thousand years. 相似文献
Fossil oyster reefs are indicators of past sea levels, and their formation is usually dated by means of radiocarbon. However, radiocarbon dating of the shells from coastal areas may be complicated by the varying sources of carbon. Here we applied optical dating methods to date the samples from above and below a fossil oyster bed in a section on the coast of Bohai Bay, China. The optical ages of the sediments were used to constrain the oyster bed. Single-aliquot regenerative-dose procedures using the OSL signal from fine grain quartz, the IRSL and post-IR OSL signals from polymineral fine grains were employed to determine equivalent dose (De). The behaviors of the different luminescence signals from quartz and polymineral grains during De measurements were examined. The results showed that the quartz OSL signal is more reliable than the polymineral IRSL and post-IR OSL signals with respect to dating for these coastal samples. The optical ages indicated that the oyster reef formed between ca. 6.2 and 5.0 ka. 相似文献
An ESR experimental study of artificial optical bleaching of sedimentary quartz has shown that the aluminum center was maximally bleached after a 6-month illumination equivalent to natural light. This duration seems too long to apply in natural conditions. Nevertheless, the measurement of the ESR intensity of aluminum centers in quartz extracted from modern sediments and deposited in sandy bars shows that the maximum bleaching has effectively been reached.
In order to determine the relationship between the bleaching and the distance covered by a quartz grain in a river, samples were collected along the Creuse River (France) from its spring to about 170 km downstream, where maximum bleaching levels were observed in previous studies. The ESR intensities of the aluminum and titanium centers in quartz were measured, using X-band spectroscopy, before and after artificial bleaching. The difference measured between these sub-samples shows that the maximum bleaching level is obtained in the course of the first kilometer. Hence, the assumption that ESR dating of fluvial sediment is based on the optical bleaching was validated. 相似文献
Six samples were collected from a section of Peoria Loess in Eustis, North America, for optically stimulated luminescence (OSL) dating of quartz, and all except one (LV90) produced narrow dose distributions. A comparative study was conducted on this sample and on a ‘well-behaved’ sample (LV91), involving other dating methods and examination of the quartz OSL. These investigations revealed differences in the quartz OSL growth with dose, OSL response to thermal treatments and the range of components within the OSL signals. An ultra-fast component was found in LV90 that displayed a higher rate of sensitivity change than the fast component and this had a malign influence on the determination of the equivalent dose. The distinctive luminescence characteristics of LV90 imply either a change in wind dynamics and/or the source area for the silt. 相似文献
Sediments attributed to flooding events of River Danube concerning the bleaching of the optical stimulated luminescence (OSL) signal were investigated. It is demonstrated that the OSL signal in both quartz and feldspar is not completely but differentially bleached in the sediment grains. Partial bleaching of the samples is clearly indicated by the scatter of equivalent dose determined for several individual single aliquots. It is also shown that residual ages in feldspars are significantly higher than those calculated for quartz. It is furthermore demonstrated that analysing measurement-time dependent equivalent dose estimates is not a suitable method to identify partial bleaching in the investigated sediment grains. However, the transport and deposition process of the investigated samples was probably disturbed by an artificial input of sediment, and this case study may thus not be representative of undisturbed high flood events in the past. 相似文献