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561.
Thermodynamic model for arsenic speciation in sulfidic waters: A novel use of ab initio computations
Recent discoveries demonstrate that the chemistry of arsenic in sulfidic waters is much more complex that previously believed. One implication is that all earlier thermodynamic data on stabilities of As thioanions require revision. Previously used experimental approaches for determining As thioanion stabilities may be inadequate to deal with the full range of complexity. Here we use computational as well as empirical information to construct a provisional model for equilibrium As thioanion distributions in sulfidic waters. Whereas previous authors have argued for either As(III) or As(V) thioanions, the new model predicts that both are important and can occur simultaneously under commonly encountered pH and ΣS−II conditions. At the order of magnitude level, the model reasonably predicts the solubility of As2S3 in sulfidic solutions, provides tentative peak assignments for published Raman spectroscopic data and plausibly accounts for how sulfide modifies the bacterial toxicity of As. The model yields a thermodynamic justification for how sulfide, which is usually regarded as a reducing agent, can counter-intuitively drive oxidation of As(III) to As(V), as has been observed both in the laboratory and in the field. Despite its uncertain accuracy, the model serves as a useful source of new, testable hypotheses about As geochemistry and highlights crucial experimental data needs. 相似文献
562.
563.
A. van Geen K. Radloff Z. Aziz Z. Cheng M.R. Huq K.M. Ahmed B. Weinman S. Goodbred H.B. Jung Y. Zheng M. Berg P.T.K. Trang L. Charlet J. Metral D. Tisserand S. Guillot S. Chakraborty A.P. Gajurel B.N. Upreti 《Applied Geochemistry》2008
One of the reasons the processes resulting in As release to groundwater in southern Asia remain poorly understood is the high degree of spatial variability of physical and chemical properties in shallow aquifers. In an attempt to overcome this difficulty, a simple device that collects groundwater and sediment as a slurry from precisely the same interval was developed in Bangladesh. Recently published results from Bangladesh and India relying on the needle-sampler are augmented here with new data from 37 intervals of grey aquifer material of likely Holocene age in Vietnam and Nepal. A total of 145 samples of filtered groundwater ranging in depth from 3 to 36 m that were analyzed for As (1–1000 μg/L), Fe (0.01–40 mg/L), Mn (0.2–4 mg/L) and S (0.04–14 mg/L) are compared. The P-extractable (0.01–36 mg/kg) and HCl-extractable As (0.04–36 mg/kg) content of the particulate phase was determined in the same suite of samples, in addition to Fe(II)/Fe ratios (0.2–1.0) in the acid-leachable fraction of the particulate phase. Needle-sampler data from Bangladesh indicated a relationship between dissolved As in groundwater and P-extractable As in the particulate phase that was interpreted as an indication of adsorptive equilibrium, under sufficiently reducing conditions, across 3 orders of magnitude in concentrations according to a distribution coefficient of 4 mL/g. The more recent observations from India, Vietnam and Nepal show groundwater As concentrations that are often an order of magnitude lower at a given level of P-extractable As compared to Bangladesh, even if only the subset of particularly reducing intervals characterized by leachable Fe(II)/Fe >0.5 and dissolved Fe >0.2 mg/L are considered. Without attempting to explain why As appears to be particularly mobile in reducing aquifers of Bangladesh compared to the other regions, the consequences of increasing the distribution coefficient for As between the particulate and dissolved phase to 40 mL/g for the flushing of shallow aquifers of their initial As content are explored. 相似文献
564.
Summary Left in place pillars of abandoned mines are subject to weathering (e.g action of water, bacteria) that degrades their mechanical
strength and eventually leads to collapse. A simple weathering model is proposed, that is governed by two parameters: the
rate of progression of weathered front and the rate of degradation of the compressive strength with time. Both plane strain
and axisymmetric analyses are performed and closed form solutions of the variation with time of the bearing capacity of the
pillar are given. Experimental data of the tests conducted on gypsum and anhydrite specimens attacked by water are presented.
It is shown that in order to fit the experimental data a third parameter must be introduced. New closed form solutions are
given and the data are used for estimating the time to failure of abandoned gypsum mines in Northern Italy.
Authors’ address: Dr. Riccardo Castellanza, Research Assistant, Department of Structural Engineering, Milan University of
Technology (Politecnico), Piazza Leonardo da Vinci 32, 20133 Milan, Italy 相似文献
565.
High levels of Cd and Zn in Jamaican soils observed in geochemical surveys are related to the presence of phosphorites of possible Late-Miocene or Pliocene age. The trace element and REE geochemistry of the phosphorites, together with SEM studies, indicate a guano origin for the phosphorites. No specific host minerals for Cd could be identified in the fossiliferous phosphorite which is characterized by uniquely high levels of Cd, Zn, Ag, Be, U and Y. However, in the soil Cd is present in lithiophorite and a complex history of pedological development is preserved in the aluminous–goethite present in the soil. The unique guano signature is preserved in the soil despite the fact that guanos themselves have either not been observed or have been destroyed by continuing karst and soil development. The phosphorite geochemical signature can be traced in the data of a 1988 island-wide soil geochemical survey, identifying areas where the Palaeo-environment that supported bird ‘rookeries’ existed in the Late-Miocene or Pliocene. 相似文献
566.
Kathleen A. Radloff Anya R. Manning Brian Mailloux Yan Zheng M. Moshiur Rahman M. Rezaul Huq Kazi M. Ahmed Alexander van Geen 《Applied Geochemistry》2008
Microbial Fe reduction is widely believed to be the primary mechanism of As release from aquifer sands in Bangladesh, but alternative explanations have been proposed. Long-term incubation studies using natural aquifer material are one way to address such divergent views. This study addresses two issues related to this approach: (1) the need for suitable abiotic controls and (2) the spatial variability of the composition of aquifer sands. Four sterilization techniques were examined using orange-colored Pleistocene sediment from Bangladesh and artificial groundwater over 8 months. Acetate (10 mM) was added to sacrificial vials before sterilization using either (1) 25 kGy of gamma irradiation, (2) three 1-h autoclave cycles, (3) a single addition of an antibiotic mixture at 1× or (4) 10× the typical dose, and (5) a 10 mM addition of azide. The effectiveness of sterilization was evaluated using two indicators of microbial Fe reduction, changes in diffuse spectral reflectance and leachable Fe(II)/Fe ratios, as well as changes in P-extractable As concentrations in the solid phase. A low dose of antibiotics was ineffective after 70 days, whereas autoclaving significantly altered groundwater composition. Gamma irradiation, a high dose of antibiotics, and azide were effective for the duration of the experiment. 相似文献
567.
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
568.
The Simpevarp area is one of the alternative sites being considered for the deep geological disposal of high level radioactive waste in Sweden. In this paper, a coupled regional groundwater flow and reactive solute transport model of the Simpevarp area is presented that integrates current hydrogeological and hydrochemical data of the area. The model simulates the current hydrochemical pattern of the groundwater system in the area. To that aim, a conceptual hydrochemical model was developed in order to represent the dominant chemical processes. Groundwater flow conditions were reproduced by taking into account fluid-density-dependent groundwater flow and regional hydrogeologic boundary conditions. Reactive solute transport calculations were performed on the basis of the velocity field so obtained. The model was calibrated and sensitivity analyses were carried out in order to investigate the effects of heterogeneities of hydraulic conductivity in the subsurface medium. Results provided by the reactive transport model are in good agreement with much of the measured hydrochemical data. This paper emphasizes the appropriateness of the use of reactive solute transport models when water-rock interaction reactions are involved, and demonstrates what powerful tools they are for the interpretation of hydrogeological and hydrochemical data from site geological repository characterization programs, by providing a qualitative framework for data analysis and testing of conceptual assumptions in a process-oriented approach. 相似文献
569.
570.
Quantitative sinkhole hazard assessments in karst areas allow calculation of the potential sinkhole risk and the performance
of cost-benefit analyses. These estimations are of practical interest for planning, engineering, and insurance purposes. The
sinkhole hazard assessments should include two components: the probability of occurrence of sinkholes (sinkholes/km2 year) and the severity of the sinkholes, which mainly refers to the subsidence mechanisms (progressive passive bending or
catastrophic collapse) and the size of the sinkholes at the time of formation; a critical engineering design parameter. This
requires the compilation of an exhaustive database on recent sinkholes, including information on the: (1) location, (2) chronology
(precise date or age range), (3) size, and (4) subsidence mechanisms and rate. This work presents a hazard assessment from
an alluvial evaporite karst area (0.81 km2) located in the periphery of the city of Zaragoza (Ebro River valley, NE Spain). Five sinkholes and four locations with features
attributable to karstic subsidence where identified in an initial investigation phase providing a preliminary probability
of occurrence of 0.14 sinkholes/km2 year (11.34% in annual probability). A trenching program conducted in a subsequent investigation phase allowed us to rule
out the four probable sinkholes, reducing the probability of occurrence to 0.079 sinkholes/km2 year (6.4% in annual probability). The information on the severity indicates that collapse sinkholes 10–15 m in diameter
may occur in the area. A detailed study of the deposits and deformational structures exposed by trenching in one of the sinkholes
allowed us to infer a modern collapse sinkhole approximately 12 m in diameter and with a vertical throw of 8 m. This collapse
structure is superimposed on a subsidence sinkhole around 80 m across that records at least 1.7 m of synsedimentary subsidence.
Trenching, in combination with dating techniques, is proposed as a useful methodology to elucidate the origin of depressions
with uncertain diagnosis and to gather practical information with predictive utility about particular sinkholes in alluvial
karst settings: precise location, subsidence mechanisms and magnitude, and timing and rate of the subsidence episodes. 相似文献