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71.
Haydon P. Mort Thierry Adatte Gerta Keller David Bartels Karl B. Fllmi Philipp Steinmann Zsolt Berner E.H. Chellai 《Cretaceous Research》2008,29(5-6):1008
With a multi-proxy approach, an attempt was made to constrain productivity and bottom-water redox conditions and their effects on the phosphorus accumulation rate at the Mohammed Plage section on the Tarfaya coast, Morocco, during the Cenomanian-Turonian Anoxic Event (OAE 2). A distinct δ13Corg isotope excursion of +2.5‰ occurs close to the top of the section. The unusually abrupt shift of the isotope excursion and disappearance of several planktonic foraminiferal species (e.g. Rotalipora cushmani and Rotalipora greenhornensis) in this level suggests a hiatus of between 40–60 kyrs at the excursion onset. Nevertheless, it was possible to determine both the long-term environmental history as well as the processes that took place immediately prior to and during OAE 2. TOC% values increase gradually from the base of the section to the top (from 2.5% to 10%). This is interpreted as the consequence of a long-term eustatic sea-level rise and subsidence causing the encroachment of less oxic waters into the Tarfaya Basin. Similarly a reduction in the mineralogically constructed ‘detrital index’ can be explained by the decrease in the continental flux of terrigenous material due to a relative sea-level rise. A speciation of phosphorus in the upper part of the section, which spans the start and mid-stages of OAE 2, shows overall higher abundances of Preactive mass accumulation rates before the isotope excursion onset and lower values during the plateau. Due to the probable short hiatus, the onset of the decrease in phosphorus content relative to the isotope excursion is uncertain, although the excursion plateau already contains lower concentrations. The Corg/Ptotal and V/Al ratios suggest that this reduction was mostly likely caused by a decrease in the available bottom oxygen content (probably as a result of higher productivity) and a corresponding fall in the phosphorus retention ability of the sediment. Productivity appears to have remained high during the isotope plateau possibly due to a combination of ocean-surface fertilisation via increased aridity (increased K/Al and Ti/Al ratios) and/or higher dissolved inorganic phosphorus content in the water column as a result of the decrease in sediment P retention. The evidence for decreased P-burial has been observed in many other palaeoenvironments during OAE 2. Tarfaya's unique upwelling paleosituation provides strong evidence that the nutrient recycling was a global phenomenon and therefore a critical factor in starting and sustaining OAE 2. 相似文献
72.
Thomas B. Boving Mark H. Stolt Janelle Augenstern Brian Brosnan 《Environmental Geology》2008,55(3):571-582
The control of polluted surface runoff and the assessment of possible impacts on groundwater is a concern at the local and
regional scale. On this background, a study investigates possible impacts of organic and inorganic pollutants (including bacteria)
originating from a permeable asphalt parking lot on the water quality immediately beneath it. The functioning of the permeable
pavement, including clogging and restricted vertical percolation, was also evaluated. Four nested sample ports (shallow and
deep) were installed below low- and high-traffic areas, including one port outside the parking lot. At least initially there
was a good hydraulic connection between the parking surface and the shallow sample ports. The presence of a geotextile layer
at the base of the parking lot structure, however, was identified in lab tests as one factor restricting vertical percolation
to the deeper ports. Clogging of the permeable surface was most pronounced in heavy traffic areas and below snow pile storage
areas. Corroborated by high electric conductivity and chloride measurements, sand brought in by cars during winter was the
principal cause for clogging. No bacteria or BOD were found in percolating water. Polycyclic aromatic hydrocarbons (PAH) were
present at concentrations near minimum detection limit. Nutrients (nitrate and phosphate) were being leached into the ground
via the permeable parking lot surface at annual flux rates of 0.45–0.84 g/m2/year. A multi-species tracer test demonstrated a retention capacity of the permeable parking lot structure of >90% for metals
and 27% for nutrients, respectively. 相似文献
73.
V. B. Naumov V. S. Kamenetsky R. Thomas N. N. Kononkova B. N. Ryzhenko 《Geochemistry International》2008,46(6):554-564
Melt inclusions were studied in chrome diopside from the Inagli deposit of gemstones in the Inagli massif of alkaline ultrabasic rocks of potassic affinity in the northwestern Aldan shield, Yakutia, Russia. The chrome diopside is highly transparent and has an intense green color. Its Cr2O3 content varies from 0.13 to 0.75 wt %. Primary and primary-secondary polyphase inclusions in chrome diopside are dominated by crystal phases (80–90 vol %) and contain aqueous solution and a gas phase. Using electron microprobe analysis and Raman spectroscopy, the following crystalline phases were identified. Silicate minerals are represented by potassium feldspar, pectolite [NaCa2Si3O8(OH)], and phlogopite. The most abundant minerals in the majority of inclusions are sulfates: glaserite (aphthitalite) [K3Na(SO4)2], glauberite [Na2Ca(SO4)2], aluminum sulfate, anhydrite (CaSO4), gypsum (CaSO4 × 2H2O), barite (BaSO4), bloedite [Na2Mg(SO4)2 × 4H2O], thenardite (NaSO4), polyhalite [K2Ca2Mg(SO4)4 × 2H2O], arcanite (K2SO4), and celestite (SrSO4). In addition, apatite was detected in some inclusions. Chlorides are probably present among small crystalline phases, because some analyses of aggregates of silicate and sulfate minerals showed up to 0.19–10.3 wt % Cl. Hydrogen was identified in the gas phase of polyphase inclusions by Raman spectroscopy. The composition of melt from which the chrome diopside crystallized was calculated on the basis of the investigation of silicate melt inclusions. This melt contains 53.5 wt % SiO2, considerable amounts of CaO (16.3 wt %), K2O (7.9 wt %), Na2O (3.5 wt %), and SO3 (1.4 wt %) and moderate amounts of Al2O3 (7.5 wt %), MgO (5.8 wt %), FeO (1.1 wt %), and H2O (0.75 wt %). The content of Cr2O3 in the melt was 0.13 wt %. Many inclusions were homogenized at 770–850°C, when all of the crystals and the gas phase were dissolved. The material of inclusions heated up to the homogenization temperature became heterogeneous even during very fast quenching (two seconds) producing numerous small crystals. This fact implies that most of the inclusions contained a salt (rather than silicate) melt of sulfate-dominated composition. Such inclusions were formed from salt globules (with a density of about 2.5 g/cm3) occurring as an emulsion in the denser (2.6 g/cm3) silicate melt from which the chrome diopside crystallized. 相似文献
74.
Pedro J. Marenco Frank A. Corsetti Douglas E. Hammond Alan J. Kaufman David J. Bottjer 《Chemical Geology》2008,247(1-2):124-132
The sulfur isotopic composition of carbonate associated sulfate (CAS) has been used to investigate the geochemistry of ancient seawater sulfate. However, few studies have quantified the reliability of δ34S of CAS as a seawater sulfate proxy, especially with respect to later diagenetic overprinting. Pyrite, which typically has depleted δ34S values due to authigenic fractionation associated with bacterial sulfate reduction, is a common constituent of marine sedimentary rocks. The oxidation of pyrite, whether during diagenesis or sample preparation, could thus adversely influence the sulfur isotopic composition of CAS. Here, we report the results of CAS extractions using HCl and acetic acid with samples spiked with varying amounts of pyrite. The results show a very strong linear relationship between the abundance of fine-grained pyrite added to the sample and the resultant abundance and δ34S value of CAS. This data represents the first unequivocal evidence that pyrite is oxidized during the CAS extraction process. Our mixing models indicate that in samples with much less than 1 wt.% pyrite and relatively high δ34Spyrite values, the isotopic offset imparted by oxidation of pyrite should be much less than ? 4‰. A wealth of literature exists on the oxidation of pyrite by Fe3+ and we believe this mechanism drives the oxidation of pyrite during CAS extraction, during which the oxygen used to form sulfate is taken from H2O, not O2. Consequently, extracting CAS under anaerobic conditions would only slow, but not halt, the oxidation of pyrite. Future studies of CAS should attempt to quantify pyrite abundance and isotopic composition. 相似文献
75.
David M. Hirsch 《Contributions to Mineralogy and Petrology》2008,155(4):401-415
Garnet-bearing schists from the Waterville Formation of south-central Maine provide an opportunity to examine the factors
governing porphyroblast size over a range of metamorphic grade. Three-dimensional sizes and locations for all garnet porphyroblasts
were determined for three samples along the metamorphic field gradient spanning lowest garnet through sillimanite grade, using
high-resolution X-ray computed tomography. Comparison of crystal size distributions to previous data sets obtained by stereological
methods for the same samples reveals significant differences in mode, mean, and shape of the distributions. Quantitative textural
analysis shows that the garnets in each rock crystallized in a diffusion-controlled nucleation and growth regime. In contrast
to the typical observation of a correlation between porphyroblast size and position along a metamorphic field gradient, porphyroblast
size of the lowest-grade specimen is intermediate between the high- and middle-grade specimens’ sizes. Mean porphyroblast
size does not correlate with peak temperatures from garnet-biotite Fe-Mg exchange thermometry, nor is post-crystallization
annealing (Ostwald Ripening) required to produce the observed textures, as was previously proposed for these rocks. Robust
pseudosection calculations fail to reproduce the observed garnet core compositions for two specimens, suggesting that these
calc-pelites experienced metasomatism. For each of these two specimens, Monte Carlo calculations suggest potential pre-metasomatism
bulk compositions that replicate garnet core compositions. Pseudosection analyses allow the estimation of the critical temperatures
for garnet growth: ∼481, ∼477, and ∼485°C for the lowest-garnet-zone, middle-garnet-zone, and sillimanite-zone specimens,
respectively. Porphyroblast size appears to be determined in this case by a combination of the heating rate during garnet
crystallization, the critical temperature for the garnet-forming reaction and the kinetics of nucleation. Numerical simulations
of thermally accelerated, diffusion-controlled nucleation, and growth for the three samples closely match measured crystal
size distributions. These observations and simulations suggest that previous hypotheses linking the garnet size primarily
to the temperature at the onset of porphyroblast nucleation can only partially explain the observed textures. Also important
in determining porphyroblast size are the heating rate and the distribution of favorable nucleation sites. 相似文献
76.
David M. Sherman Caroline L. Peacock Christopher G. Hubbard 《Geochimica et cosmochimica acta》2008,72(2):298-310
Sorption of U(VI) to goethite is a fundamental control on the mobility of uranium in soil and groundwater. Here, we investigated the sorption of U on goethite using EXAFS spectroscopy, batch sorption experiments and DFT calculations of the energetics and structures of possible surface complexes. Based on EXAFS spectra, it has previously been proposed that U(VI), as the uranyl cation , sorbs to Fe oxide hydroxide phases by forming a bidentate edge-sharing (E2) surface complex, >Fe(OH)2UO2(H2O)n. Here, we argue that this complex alone cannot account for the sorption capacity of goethite (α-FeOOH). Moreover, we show that all of the EXAFS signal attributed to the E2 complex can be accounted for by multiple scattering. We propose that the dominant surface complex in CO2-free systems is a bidentate corner-sharing (C2) complex, (>FeOH)2UO2(H2O)3 which can form on the dominant {101} surface. However, in the presence of CO2, we find an enhancement of UO2 sorption at low pH and attribute this to a (>FeO)CO2UO2 ternary complex. With increasing pH, U(VI) desorbs by the formation of aqueous carbonate and hydroxyl complexes. However, this desorption is preceded by the formation of a second ternary surface complex (>FeOH)2UO2CO3. The three proposed surface complexes, (>FeOH)2UO2(H2O)3, >FeOCO2UO2, and (>FeOH)2UO2CO3 are consistent with EXAFS spectra. Using these complexes, we developed a surface complexation model for U on goethite with a 1-pK model for surface protonation, an extended Stern model for surface electrostatics and inclusion of all known UO2-OH-CO3 aqueous complexes in the current thermodynamic database. The model gives an excellent fit to our sorption experiments done in both ambient and reduced CO2 environments at surface loadings of 0.02-2.0 wt% U. 相似文献
77.
Gregory K. Druschel David Emerson R. Sutka P. Suchecki 《Geochimica et cosmochimica acta》2008,72(14):3358-3370
Neutrophilic iron oxidizing bacteria (FeOB) must actively compete with rapid abiotic processes governing Fe(II) oxidation and as a result have adapted to primarily inhabit low-O2 environments where they can more successfully compete with abiotic Fe(II) oxidation. The spatial distribution of these microorganisms can be observed through the chemical gradients they affect, as measured using in situ voltammetric analysis for dissolved Fe(II), Fe(III), O2, and FeS(aq). Field and laboratory determination of the chemical environments inhabited by the FeOB were coupled with detailed kinetic competition studies for abiotic and biotic oxidation processes using a pure culture of FeOB to quantify the geochemical niche these organisms inhabit. In gradient culture tubes, the maximum oxygen levels, which were associated with growth bands of Sideroxydans lithotrophicus (ES-1, a novel FeOB), were 15-50 μM. Kinetic measurements made on S. lithotrophicus compared biotic/abiotic (killed control) Fe oxidation rates. The biotic rate can be a significant and measurable fraction of the total Fe oxidation rate below O2 concentrations of approximately 50 μM, but biotic Fe(II) oxidation (via the biotic/abiotic rate comparison) becomes difficult to detect at higher O2 levels. These results are further supported by observations of conditions supporting FeOB communities in field settings. Variablity in cell densities and cellular activity as well as variations in hydrous ferrous oxide mineral quantities significantly affect the laboratory kinetic rates. The microbial habitat (or geochemical niche) where FeOB are active is thus largely controlled by the competition between abiotic and biotic kinetics, which are dependent on Fe(II) concentration, PO2, temperature and pH in addition to the surface area of hydrous ferric oxide minerals and the cell density/activity of FeOB. Additional field and lab culture observations suggest a potentially important role for the iron-sulfide aqueous molecular cluster, FeS(aq), in the overall cycling of iron associated with the environments these microorganisms inhabit. 相似文献
78.
The current study provides an investigation of abiotic reduction of an oversaturated uranyl solution driven by iron nanoparticle oxidation. The reactivity of nano-scale zero-valent iron (ZVI) under mildly oxic conditions (1.2% O2 and 0.0017% CO2) was studied in 1000 ppm uranyl solution in the pH range 3-7, at reaction times from 10 min to 4 h. Reductive precipitation of UO2 was observed as the main process responsible for the removal of uranium from solution with the kinetics of reaction becoming increasingly favourable at higher pH. Despite working with an oversaturated uranium solution, the precipitation of UO2 occurred in preference to precipitation of UO3·2H2O (metaschoepite) at reaction times between 1 and 4 h and for uranyl solutions initially set up at pH ?5. Characterisation of both solid and solution phases was performed using X-ray photoelectron spectroscopy (XPS), focused ion beam (FIB) imaging, X-ray diffraction (XRD) and inductively coupled plasma atomic emission spectroscopy (ICP-AES). 相似文献
79.
Nancy L. Chabot Andrew J. Campbell David S. Draper Munir Humayun Elizabeth Cottrell 《Geochimica et cosmochimica acta》2008,72(16):4146-4158
Earth’s core may contain C, and it has been suggested that C in the core could stabilize the formation of a solid inner core composed of Fe3C. We experimentally examined the Fe-C system at a pressure of 5 GPa and determined the Fe-C phase diagram at this pressure. In addition, we measured solid metal/liquid metal partition coefficients for 17 trace elements and examined the partitioning behavior between Fe3C and liquid metal for 14 trace elements. Solid metal/liquid metal partition coefficients are similar to those found in one atmosphere studies, indicating that the effect of pressure to 5 GPa is negligible. All measured Fe3C/liquid metal partition coefficients investigated are less than one, such that all trace elements prefer the C-rich liquid to Fe3C. Fe3C/liquid metal partition coefficients tend to decrease with decreasing atomic radii within a given period. Of particular interest, our 5 GPa Fe-C phase diagram does not show any evidence that the Fe-Fe3C eutectic composition shifts to lower C contents with increasing pressure, which is central to the previous reasoning that the inner core may be composed of Fe3C. 相似文献
80.
Laura E. Wasylenki Bryan A. Rolfe Thomas G. Spiro 《Geochimica et cosmochimica acta》2008,72(24):5997-6005
The Mo stable isotope system is being applied to study changes in ocean redox. Such applications implicitly assume that Mo isotope fractionation in aqueous systems is relatively insensitive to frequently changing environmental variables such as temperature (T) and ionic strength (I). A major driver of fractionation is the adsorption of Mo to Mn oxyhydroxide surfaces [Barling J. and Anbar A. D. (2004) Molybdenum isotope fractionation during adsorption by manganese oxides. Earth Planet. Sci. Lett.217(3-4), 315-329]. Here, we report the results of experiments that determine the extent to which Mo isotope fractionation during adsorption of Mo to the Mn oxyhydroxide mineral birnessite is sensitive to T and I. The results are compared to new predictions from quantum chemical computations. We measured fractionation from 1 to 50 °C at I = 0.1 m and found that Δ97/95Modissolved-adsorbed varies from 1.9‰ to 1.6‰ over this temperature range. Experiments were also performed at 25 °C in synthetic seawater (I = 0.7); fractionation at this condition was the same within analytical error as in low ionic strength experiments. These findings confirm that the Mo isotope fractionation during adsorption to Mn oxyhydroxides is relatively insensitive to variations and T and I over environmentally relevant ranges. To relate these findings to potential mechanisms of Mo isotope fractionation, we also report results for density functional theory computations of the fractionation between and various possible structures of molybdic acid as a function of temperature. Because no plausible species fractionates from with a magnitude matching the experiments, we are left with three possibilities to explain the fractionation: (1) solvation effects on the vibrational frequencies of aqueous species considered thus far are significant, such that our calculations in vacuo yield inaccurate fractionations; (2) a trace aqueous species not yet considered fractionates from and then adsorbs to birnessite; or (3) a surface complex not present in solution forms on birnessite in which Mo is not tetrahedrally coordinated. Our findings help validate assumptions underlying paleoceanographic applications of the Mo isotope system and also lead us closer to understanding the mechanism of isotope fractionation during adsorption of Mo to Mn oxyhydroxides. 相似文献