Thermal history of the unsaturated zone at Yucca Mountain,Nevada, USA     

Joseph F. Whelan  Leonid A. Neymark  Richard J. Moscati  Brian D. Marshall  Edwin Roedder 《Applied Geochemistry》2008

Secondary calcite, silica and minor amounts of fluorite deposited in fractures and cavities record the chemistry, temperatures, and timing of past fluid movement in the unsaturated zone at Yucca Mountain, Nevada, the proposed site of a high-level radioactive waste repository. The distribution and geochemistry of these deposits are consistent with low-temperature precipitation from meteoric waters that infiltrated at the surface and percolated down through the unsaturated zone. However, the discovery of fluid inclusions in calcite with homogenization temperatures (T_h) up to ∼80 °C was construed by some scientists as strong evidence for hydrothermal deposition. This paper reports the results of investigations to test the hypothesis of hydrothermal deposition and to determine the temperature and timing of secondary mineral deposition. Mineral precipitation temperatures in the unsaturated zone are estimated from calcite- and fluorite-hosted fluid inclusions and calcite δ¹⁸O values, and depositional timing is constrained by the ²⁰⁷Pb/²³⁵U ages of chalcedony or opal in the deposits. Fluid inclusion T_h from 50 samples of calcite and four samples of fluorite range from ∼35 to ∼90 °C. Calcite δ¹⁸O values range from ∼0 to ∼22‰ (SMOW) but most fall between 12 and 20‰. The highest T_h and the lowest δ¹⁸O values are found in the older calcite. Calcite T_h and δ¹⁸O values indicate that most calcite precipitated from water with δ¹⁸O values between −13 and −7‰, similar to modern meteoric waters.  相似文献   

Reply to the comment on “Some numerical considerations in the geochemical analysis of distal microtephra”, by Nicholas J.G. Pearce,Charles A. Bendall and John A. Westgate     

A.M. Pollard  S.P.E. BlockleyC.S. Lane 《Applied Geochemistry》2008

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The arsenic source term for an in-pit uranium mine tailings facility and its long-term impact on the regional groundwater     

Brett J. Moldovan  M. Jim Hendry  Glenn A. Harrington 《Applied Geochemistry》2008

Detailed field sampling and analyses and laboratory-based diffusion-cell experiments were used in conjunction with 3-D reactive transport modeling (MODFLOW and MT3D99) to quantify the fate and long-term (10 ka) transport of As in the Rabbit Lake In-pit Tailings Management Facility (RLITMF), northern Saskatchewan, Canada. The RLITMF (300 m × 425 m × 90 m thick) was engineered to ensure solute transport within the RLITMF is dominated by diffusion. Concentrations of As in the tailings pore fluids ranged from 0.24 to 140 mg/L (n = 43). Arsenic speciation analyses indicate 90% of this arsenic exists as As⁵⁺. This observation is supported by pH–Eh measurements of pore fluids (n = 135). Geochemical analyses yielded a strong inverse correlation between the Fe/As molar ratio in the tailings solids and the corresponding concentration of dissolved As, which is attributed to the adsorption of As to secondary 2-line ferrihydrite present in the tailings. Diffusion-cell testing yielded values for the effective diffusion coefficient, sorption coefficient, and effective porosity of As in the tailings of 4.5 × 10⁻¹⁰ m²/s, 2–4 cm³/g and 0.36, respectively. Reactive transport simulations using the field and laboratory data show adsorption of As to the tailings and diffusive transport of dissolved As in the tailings should reduce the source term concentration of As to between 40% and 70% of the initial concentrations over the 10 ka simulation period. Based on these simulations, the As concentrations in the regional groundwater, 50 m down gradient of the tailings facility, should be maintained at background concentrations of 0.001 mg/L over the 10 ka period. These findings suggest the engineered in-pit disposal of U mine tailings can provide long-term protection for the local groundwater regime from As contamination.  相似文献   

A consistent geochemical modelling approach for the leaching and reactive transport of major and trace elements in MSWI bottom ash     

Joris J. Dijkstra  Johannes C.L. Meeussen  Hans A. Van der Sloot  Rob N.J. Comans 《Applied Geochemistry》2008

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Site descriptive modelling during characterization for a geological repository for nuclear waste in Sweden     

A. Ström  J. Andersson  K. Skagius  A. Winberg 《Applied Geochemistry》2008

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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  

Debapriya Mondal  David A. Polya 《Applied Geochemistry》2008

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   

Geochemistry and mineralogy of arsenic in (natural) anaerobic groundwaters     

J.A. Saunders  M.-K. Lee  M. Shamsudduha  P. Dhakal  A. Uddin  M.T. Chowdury  K.M. Ahmed 《Applied Geochemistry》2008

Here new data from field bioremediation experiments and geochemical modeling are reported to illustrate the principal geochemical behavior of As in anaerobic groundwaters. In the field bioremediation experiments, groundwater in Holocene alluvial aquifers in Bangladesh was amended with labile water-soluble organic C (molasses) and MgSO₄ to stimulate metabolism of indigenous SO₄-reducing bacteria (SRB). In the USA, the groundwater was contaminated by Zn, Cd and SO₄, and contained <10 μg/L As under oxidized conditions, and a mixture of sucrose and methanol were injected to stimulate SRB metabolism. In Bangladesh, groundwater was under moderately reducing conditions and contained ∼10 mg/L Fe and ∼100 μg/L As. In the USA experiment, groundwater rapidly became anaerobic, and dissolved Fe and As increased dramatically (As > 1000 μg/L) under geochemical conditions consistent with bacterial Fe-reducing conditions. With time, groundwater became more reducing and biogenic SO₄ reduction began, and Cd and Zn were virtually completely removed due to precipitation of sphalerite (ZnS) and other metal sulfide mineral(s). Following precipitation of chalcophile elements Zn and Cd, the concentrations of Fe and As both began to decrease in groundwater, presumably due to formation of As-bearing FeS/FeS₂. By the end of the six-month experiment, dissolved As had returned to below background levels. In the initial Bangladesh experiment, As decreased to virtually zero once biogenic SO₄ reduction commenced but increased to pre-experiment level once SO₄ reduction ended. In the ongoing experiment, both SO₄ and Fe(II) were amended to groundwater to evaluate if FeS/FeS₂ formation causes longer-lived As removal. Because As-bearing pyrite is the common product of SRB metabolism in Holocene alluvial aquifers in both the USA and Southeast Asia, it was endeavored to derive thermodynamic data for arsenian pyrite to better predict geochemical processes in naturally reducing groundwaters. Including the new data for arsenian pyrite into Geochemist’s Workbench, its stability field completely dominates in reducing Eh–pH space and “displaces” other As-sulfides (orpiment, realgar) that have been implied to be important in previous modeling exercises and reported in rare field conditions.  相似文献   

Considerations for conducting incubations to study the mechanisms of As release in reducing groundwater aquifers     

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   

Radon transfer from groundwater used in showers to indoor air     

David S. Vinson  Ted R. Campbell  Avner Vengosh 《Applied Geochemistry》2008

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   

Calibration of regional palaeohydrogeology and sensitivity analysis using hydrochemistry data in site investigations     

F.M.I. Hunter  L.J. Hartley  A. Hoch  C.P. Jackson  R. McCarthy  N. Marsic  B. Gylling 《Applied Geochemistry》2008

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