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61.
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
62.
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
63.
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
64.
Complexity theory has received considerable attention over the past decade from a wide variety of disciplines. Some who write on this topic suggest that complexity theory will lead to a unifying understanding of complex phenomena; others dismiss it as a passing and disruptive fad. We suggest that for the analysis of coupled natural/human systems, the truth emerges from the middle ground. As an approach focused as much on the connections among system elements as the elements themselves, we argue that complexity theory provides a useful conceptual framework for the study of coupled natural/human systems. It is, if nothing else, a framework that leads us to ask interesting questions about, for example, sustainability, resilience, threshold events, and predictability.In this paper we attempt to demystify the ongoing discussions on complexity theory by linking its evocative and overloaded terminology to real-world processes. We illustrate how a shift in focus from system elements to connections among elements can lead to meaningful insight into human-environment interactions that might otherwise be overlooked. We ground our discussion in ongoing interdisciplinary research surrounding Yellowstone National Park’s northern elk winter range; a tightly coupled natural/human system that has been the center of debate, conflict, and compromise for more than 135 years. 相似文献
65.
Almeev Renat; Holtz Francois; Koepke Jurgen; Haase Karsten; Devey Colin 《Journal of Petrology》2008,49(1):25-45
Phase equilibria simulations were performed on naturally quenchedbasaltic glasses to determine crystallization conditions priorto eruption of magmas at the Mid-Atlantic Ridge (MAR) east ofAscension Island (7–11°S). The results indicate thatmid-ocean ridge basalt (MORB) magmas beneath different segmentsof the MAR have crystallized over a wide range of pressures(100–900 MPa). However, each segment seems to have a specificcrystallization history. Nearly isobaric crystallization conditions(100–300 MPa) were obtained for the geochemically enrichedMORB magmas of the central segments, whereas normal (N)-MORBmagmas of the bounding segments are characterized by polybariccrystallization conditions (200–900 MPa). In addition,our results demonstrate close to anhydrous crystallization conditionsof N-MORBs, whereas geochemically enriched MORBs were successfullymodeled in the presence of 0·4–1 wt% H2O in theparental melts. These estimates are in agreement with direct(Fourier transform IR) measurements of H2O abundances in basalticglasses and melt inclusions for selected samples. Water contentsdetermined in the parental melts are in the range 0·04–0·09and 0·30–0·55 wt% H2O for depleted and enrichedMORBs, respectively. Our results are in general agreement (within±200 MPa) with previous approaches used to evaluate pressureestimates in MORB. However, the determination of pre-eruptiveconditions of MORBs, including temperature and water contentin addition to pressure, requires the improvement of magma crystallizationmodels to simulate liquid lines of descent in the presence ofsmall amounts of water. KEY WORDS: MORB; Mid-Atlantic Ridge; depth of crystallization; water abundances; phase equilibria calculations; cotectic crystallization; pressure estimates; polybaric fractionation 相似文献
66.
To investigate eclogite melting under mantle conditions, wehave performed a series of piston-cylinder experiments usinga homogeneous synthetic starting material (GA2) that is representativeof altered mid-ocean ridge basalt. Experiments were conductedat pressures of 3·0, 4·0 and 5·0 GPa andover a temperature range of 1200–1600°C. The subsolidusmineralogy of GA2 consists of garnet and clinopyroxene withminor quartz–coesite, rutile and feldspar. Solidus temperaturesare located at 1230°C at 3·0 GPa and 1300°C at5·0 GPa, giving a steep solidus slope of 30–40°C/GPa.Melting intervals are in excess of 200°C and increase withpressure up to 5·0 GPa. At 3·0 GPa feldspar, rutileand quartz are residual phases up to 40°C above the solidus,whereas at higher pressures feldspar and rutile are rapidlymelted out above the solidus. Garnet and clinopyroxene are theonly residual phases once melt fractions exceed 20% and garnetis the sole liquidus phase over the investigated pressure range.With increasing melt fraction garnet and clinopyroxene becomeprogressively more Mg-rich, whereas coexisting melts vary fromK-rich dacites at low degrees of melting to basaltic andesitesat high melt fractions. Increasing pressure tends to increasethe jadeite and Ca-eskolaite components in clinopyroxene andenhance the modal proportion of garnet at low melt fractions,which effects a marked reduction in the Al2O3 and Na2O contentof the melt with pressure. In contrast, the TiO2 and K2O contentsof the low-degree melts increase with increasing pressure; thusNa2O and K2O behave in a contrasted manner as a function ofpressure. Altered oceanic basalt is an important component ofcrust returned to the mantle via plate subduction, so GA2 maybe representative of one of many different mafic lithologiespresent in the upper mantle. During upwelling of heterogeneousmantle domains, these mafic rock-types may undergo extensivemelting at great depths, because of their low solidus temperaturescompared with mantle peridotite. Melt batches may be highlyvariable in composition depending on the composition and degreeof melting of the source, the depth of melting, and the degreeof magma mixing. Some of the eclogite-derived melts may alsoreact with and refertilize surrounding peridotite, which itselfmay partially melt with further upwelling. Such complex magma-genesisconditions may partly explain the wide spectrum of primitivemagma compositions found within oceanic basalt suites. KEY WORDS: eclogite; experimental petrology; mafic magmatism; mantle melting; oceanic basalts 相似文献
67.
Mark A. Engle Michael T. Tate David P. Krabbenhoft Allan Kolker Mark L. Olson Eric S. Edgerton John F. DeWild Ann K. McPherson 《Applied Geochemistry》2008
Concentrations of atmospheric Hg species, elemental Hg (Hg°), reactive gaseous Hg (RGM), and fine particulate Hg (Hg-PM2.5) were measured at a coastal site near Weeks Bay, Alabama from April to August, 2005 and January to May, 2006. Mean concentrations of the species were 1.6 ± 0.3 ng m−3, 4.0 ± 7.5 pg m−3 and 2.7 ± 3.4 pg m−3, respectively. A strong diel pattern was observed for RGM (midday maximum concentrations were up to 92.7 pg m−3), but not for Hg° or Hg-PM2.5. Elevated RGM concentrations (>25 pg m−3) in April and May of 2005 correlated with elevated average daytime O3 concentrations (>55 ppbv) and high light intensity (>500 W m−2). These conditions generally corresponded with mixed continental-Gulf and exclusively continental air mass trajectories. Generally lower, but still elevated, RGM peaks observed in August, 2005 and January–March, 2006 correlated significantly (p < 0.05) with peaks in SO2 concentration and corresponded to periods of high light intensity and lower average daytime O3 concentrations. During these times air masses were dominated by trajectories that originated over the continent. Elevated RGM concentrations likely resulted from photochemical oxidation of Hg° by atmospheric oxidants. This process may have been enhanced in and by the near-shore environment relative to inland sites. The marine boundary layer itself was not found to be a significant source of RGM. 相似文献
68.
Nicolas Seignez Arnaud Gauthier David Bulteel Denis Damidot Jean-Luc Potdevin 《Applied Geochemistry》2008,23(12):3699-3711
Lead metallurgical slags are partially vitrified materials containing residual amounts of Zn, Pb, Cr, Cd and As. These hazardous materials are generally buried on heaps exposed to weathering. In this study, leaching behavior of lead blast furnace slags has been tested using pure water and open flow experiments. It appears that in such far from equilibrium and slightly acidic conditions, the main phase to be altered is the vitreous phase. As for lunar, basaltic and nuclear glasses, alkalis/proton exchanges prevail and lead to the formation of a non-protective altered layer enriched in Si, Fe and Al. The composition of the altered layer is quite constant except for Si whose concentration decreases towards the leachate interface. Owing to their sizes, micrometric Pb droplets are not always totally dissolved at the slag surface. Nevertheless, nanometric Pb droplets are instantaneously dissolved while a surrounding altered layer is formed. This leads to high Pb releases in open flow systems. Leachate chemistry and dissolution rates of the vitreous phase are closely comparable to previous leaching tests with basaltic and nuclear glasses in conditions far from equilibrium. Moreover, this study confirms that Fe is a stable element in such conditions. 相似文献
69.
Rice is a major exposure route for arsenic in Chakdaha block,Nadia district,West Bengal,India: A probabilistic risk assessment 总被引:2,自引:0,他引:2
The importance or otherwise of rice as an exposure pathway for As ingestion by people living in Bengal and other areas impacted by hazardous As-bearing groundwaters is currently a matter of some debate. Here this issue is addressed by determining the overall increased cancer risk due to ingestion of rice in an As-impacted district of West Bengal. Human target cancer health risks have been estimated through the intake of As-bearing rice by using combined field, laboratory and computational methods. Monte Carlo simulations were run following fitting of model probability curves to measured distributions of (i) As concentration in rice and drinking water and (ii) inorganic As content of rice and fitting distributions to published data on (i) ingestion rates and (ii) body weight and point estimates on bioconcentration factors, exposure duration and other input variables. The distribution of As in drinking water was found to be substantially lower than that reported by previous authors for As in tube wells in the same area, indicating that the use of tube well water as a proxy for drinking water is likely to result in human health risks being somewhat overestimated. The calculated median increased lifetime cancer risk due to cooked rice intake was 7.62 × 10−4, higher than the 10−4–10−6 range typically used by the USEPA as a threshold to guide determination of regulatory values and similar to the equivalent risk from water intake. The median total risk from combined rice and water intake was 1.48 × 10−3. The contributions to this median risk from drinking water, rice and cooking of rice were found to be 48%, 44% and 8%, respectively. Thus, rice is a major potential source of As exposure in the As-affected study areas in West Bengal and the most important exposure pathway for groups exposed to low or no As in drinking water. 相似文献
70.
Estimation of Rn transfer from water to indoor air based on multi-day measurements may underestimate alpha exposure that occurs at short time scales in confined spaces, such as from showering, in houses with high Rn activities in the water supply. In order to examine one such incremental increase in exposure, variations in Rn in water and indoor air in 18 houses with private wells in western North Carolina (USA) were investigated. Radon in well water ranged from 158 to 811 Bq L−1 (median 239 Bq L−1). After 20-min showers in bathrooms with closed doors, peak Rn in air increases (above background) ranged from 71 to 4420 Bq m−3 (median 1170 Bq m−3). Calculated transfer coefficients at the scale of a 40-min closed bathroom (20-min shower plus 20 min post-shower) are described by a lognormal distribution whose geometric mean exceeds the widely-used ∼10−4 whole-house transfer coefficient by about one order of magnitude. As short-lived decay products grow from shower-derived Rn, short-term alpha energy exposure occurs in bathrooms in addition to the exposure caused by Rn mixed throughout the volume of the house. Due to the increasing ratio of Rn decay products to Rn, alpha energy exposure is greatest several minutes after the shower is turned off. For a 7.2-min shower with 10 min of additional exposure before opening the door, a geometric mean 5.6% increase in exposure over the ∼10−4 whole-house transfer coefficient derived from longer measurement periods was estimated. In addition to Rn activity in water, short-term shower exposure to Rn progeny depends on exposure time, ventilation, attachment and deposition, among other variable factors that characterize individual houses and residents. 相似文献