https://digitalcommons.unl.edu/cgi/viewcontent.cgi?article=1162&context=usdoepub

Heterogeneous reduction of Tc(VII) by Fe(II) at the solid-water interface

This report presents the results of groundwater and vadose zone monitoring and remediation for fiscal year 2002 on the U.S. Department of Energy's Hanford Site in Washington State. This report is written to meet the requirements in CERCLA, RCRA, the Atomic Energy Act of 1954, and Washington State Administrative Code.

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Hanford Site Groundwater Monitoring for Fiscal Year 2002

Land-use change and management practices are normally enacted to manipulate environments to improve conditions that relate to production, remediation, and accommodation. However, their effect on the soil microbial community and their subsequent influence on soil function is still difficult to quantify. Recent applications of molecular techniques to soil biology, especially the use of 16S rRNA, are helping to bridge this gap. In this study, the influence of three land-use systems within a demonstration farm were evaluated with a view to further understand how these practices may impact observed soil bacterial communities. Replicate soil samples collected from the three land-use systems (grazed pine forest, cultivated crop, and grazed pasture) on a single soil type. High throughput 16S rRNA gene pyrosequencing was used to generate sequence datasets. The different land use systems showed distinction in the structure of their bacterial communities with respect to the differences detected in cluster analysis as well as diversity indices. Specific taxa, particularly Actinobacteria, Acidobacteria, and classes of Proteobacteria, showed significant shifts across the land-use strata. Families belonging to these taxa broke with notions of copio- and oligotrphy at the class level, as many of the less abundant groups of families of Actinobacteria showed a propensity for soil environments with reduced carbon/nutrient availability. Orders Actinomycetales and Solirubrobacterales showed their highest abundance in the heavily disturbed cultivated system despite the lowest soil organic carbon (SOC) values across the site. Selected soil properties ([SOC], total nitrogen [TN], soil texture, phosphodiesterase [PD], alkaline phosphatase [APA], acid phosphatase [ACP] activity, and pH) also differed significantly across land-use regimes, with SOM, PD, and pH showing variation consistent with shifts in community structure and composition. These results suggest that use of pyrosequencing along with traditional analysis of soil physiochemical properties may provide insight into the ecology of descending taxonomic groups in bacterial communities.

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Distinct soil bacterial communities revealed under a diversely managed agroecosystem.

Nuclear wastes from Hanford’s processing for separation of plutonium are stored in massive, buried, single-shell tanks in 18 tank farms. These so-called tank wastes were initially thermally hot because of radioactive decay, and many exhibited extreme chemical character in terms of pH, salinity, and radionuclide concentration. At present, 67 of the 149 single shell tanks are suspected to have released over 1.9 million L of tank waste to the vadose zone, with most leak events occurring between 1950 and 1975. Boreholes have been placed through the largest vadose zone plumes to defi ne the extent of contaminant migration and to develop conceptual models of processes governing the transformation, retardation, and overall transport of tank waste residuals. Laboratory studies with sediments so collected have shown that ion exchange, precipitation and dissolution, and surface complexation reactions have occurred between the tank wastes and subsurface sediments, moderating their chemical character and retarding the migration of select contaminants. Processes suspected to facilitate the far-fi eld migration of immobile radionuclides including stable aqueous complex formation and mobile colloids were found to be potentially operative but unlikely to occur in the fi eld, with the exception of cyanide-facilitated migration of 60 Co. Certain fi ssion product oxyanions (Mo, Ru, Se, Tc) and nitrates are the most mobile of tank waste constituents because their adsorption is suppressed by large concentrations of waste anions, the vadose zone clay fraction is negative in surface charge, and, unlike Cr, their reduced forms are unstable in oxidizing environments. Reaction/process-based transport modeling is beginning to be used for predictions of future contaminant mobility and plume evolution.

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Geochemical Processes Controlling Migration of Tank Wastes in Hanford's Vadose Zone

[1] While pedotransfer functions (PTFs) have long been applied to estimate soil hydraulic parameters for unsaturated flow and solute transport modeling, the uncertainty associated with the estimates is often ignored. The objective of this study is to evaluate uncertainty of the PTF-estimated soil hydraulic parameters and its effect on numerical simulation of moisture flow. Contributing to the parameter estimation uncertainty are (1) the PTF intrinsic uncertainty caused by limited data used for PTF training and (2) the PTF input uncertainty in pedotransfer variables (i.e., PTF inputs). The PTF intrinsic uncertainty is assessed using the bootstrap method by generating multiple bootstrap realizations of the soil hydraulic parameters; the realizations follow normal or lognormal distributions. The PTF input variables (i.e., bulk density and soil texture) are obtained using the cokriging technique. The PTF input uncertainty is quantified by assuming that the cokriging estimates follow a normal distribution. Our results show that the PTF input uncertainty dominates over the PTF intrinsic uncertainty and determines the spatial distribution of the PTF parameter estimation uncertainty. When the parameter estimation uncertainty is included, the spatial variability of the measured soil hydraulic parameters is better captured. This is also the case for the observed moisture contents, whose spatial variability is well bracketed by the prediction intervals. However, this is only possible after the PTF input uncertainty is considered. These results suggest that additional sample acquisition for the PTF input variables would have a more favorable impact on reduction of the parameter estimation uncertainty than collecting additional soil hydraulic parameter measurements for PTF development.

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Quantification of uncertainty in pedotransfer function-based parameter estimation for unsaturated flow modeling

[1] Optimization of water use in agriculture and quantification of percolation from landfills and watersheds require reliable estimates of vadose zone water fluxes. Current technology is limited primarily to lysimeters, which directly measure water flux but are expensive and may in some way disrupt flow, causing errors in the measured drainage. We report on design considerations and field tests of an alternative approach, passive wick fluxmeters, which use a control tube to minimize convergent or divergent flow. Design calculations with a quasi-three-dimensional model illustrate how convergence and divergence can be minimized for a range of soil and climatic conditions under steady state and transient fluxes using control tubes of varying heights. There exists a critical recharge rate for a given wick length, where the fluxmeter collection efficiency is 100% regardless of the height of the control tube. Otherwise, convergent or divergent flow will occur, especially when the control tube height is small. While divergence is eliminated in coarse soils using control tubes, it is reduced but not eliminated in finer soils, particularly for fluxes 60% annual precipitation) from gravel surfaces and least (no drainage) from silt loam soils. In Oregon and New Mexico, United States, and in New Zealand, drainage showed substantial spatial variability. The New Mexico tests were located in semiarid canyon bottom terraces, with flash flood prone locations having extremely high drainage/precipitation ratios. In the wettest environments, drainage was found to be closely linked to the rate and duration of precipitation events.

https://agupubs.onlinelibrary.wiley.com/doi/pdf/10.1029/2008WR007088

Passive wick fluxmeters: Design considerations and field applications

In desert environments, non-vegetated (bare) soils and sediments can act as recharge basins, allowing water infiltration but restricting evaporation. When such sediments are located over buried wastes, drainage can lead to groundwater contamination. Lysimeters were used to quantify drainage from bare sediments at the U.S. Department of Energy's Hanford Site in Washington State, USA. Drainage varied widely from zero to more than half of the annual precipitation for sediments ranging from fine silts to coarse rock-fragments. Decade-long drainage records were used to develop two empirical models relating annual drainage and textural properties of bare sediments. A 23-year drainage record for bare, coarse sand was tested, and the calibration developed for the past 10 years (1994 to 2004) was found to reliably predict drainage from the previous 12 years. The texture models were also compared against Darcy's Law estimates (i.e., unsaturated hydraulic conductivity) for coarse sand and found to agree within 15% of the long-term drainage average. For cases where unsaturated hydraulic-property estimates were not available, the texture models reasonably predicted annual drainage rates for bare sediments containing significant fines (materials less than 50 microns). Clean rock and gravels with little or no fines yielded less drainage (more evaporation) than gravelsmore » with fines, and this was attributed to advective drying in the open work gravel and rock. Because of advective drying, no single empirical texture function could be found to predict drainage from all the coarse sediments tested. However, drainage rates from sediments ranging from silts to coarse sediments mixed with fines appear to be predictable with the models tested. To minimize drainage at desert waste sites, only modest quantities of fines need to be added to the coarse sediments to substantially reduce the potential for groundwater contamination.« less

Measurement and Prediction of Deep Drainage from Bare Sediments at a Semiarid Site

From FY 2000 through FY 2003, a series of vadose zone transport field experiments were conducted as part of the U.S. Department of Energy’s Groundwater/Vadose Zone Integration Project Science and Technology Project, now known as the Remediation and Closure Science Project, and managed by the Pacific Northwest National Laboratory (PNNL). The series of experiments included two major field campaigns, one at a 299-E24-11 injection test site near PUREX and a second at a clastic dike site off Army Loop Road. The goals of these experiments were to improve our understanding of vadose zone transport processes; to develop data sets to validate and calibrate vadose zone flow and transport models; and to identify advanced monitoring techniques useful for evaluating flow-and-transport mechanisms and delineating contaminant plumes in the vadose zone at the Hanford Site. This report summarizes the key findings from the field studies and demonstrates how data collected from these studies are being used to improve conceptual models and develop numerical models of flow and transport in Hanford’s vadose zone. Results of these tests have led to a better understanding of the vadose zone. Fine-scale geologic heterogeneities, including grain fabric and lamination, were observed to have a strong effect on the large-scale behavior of contaminant plumes, primarily through increased lateral spreading resulting from anisotropy. Conceptual models have been updated to include lateral spreading and numerical models of unsaturated flow and transport have revised accordingly. A new robust model based on the concept of a connectivity tensor was developed to describe saturation-dependent anisotropy in strongly heterogeneous soils and has been incorporated into PNNL’s Subsurface Transport Over Multiple Phases (STOMP) simulator. Application to field-scale transport problems have led to a better understanding plume behavior at a number of sites where lateral spreading may have dominated waste migration (e.g. BC Cribs and Trenches). The improved models have been also coupled with inverse models and newly-developed parameter scaling techniques to allow estimation of field-scale and effective transport parameters for the vadose zone. The development and utility of pedotransfer functions for describing fine-scale hydrogeochemical heterogeneity and for incorporating this heterogeneity into reactive transport models was explored. An approach based on grain-size statistics appears feasible and has been used to describe heterogeneity in hydraulic properties and sorption properties, such as the cation exchange capacity and the specific surface area of Hanford sediments. This work has also led to the development of inverse modeling capabilities for time-dependent, subsurface, reactive transport with transient flow fields using an automated optimization algorithm. In addition, a number of geophysical techniques investigated for their potential to provide detailed information on the subtle changes in lithology and bedding surfaces; plume delineation, leak detection. High-resolution resistivity is now being used for detecting saline plumes at several waste sites at Hanford, including tank farms. Results from the field studies and associated analysis have appeared in more than 46 publications generated over the past 4 years. These publications include test plans and status reports, in addition to numerous technical notes and peer reviewed papers.

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Vadose Zone Transport Field Study: Summary Report

The BC Cribs and Trenches, part of the 200 TW 1 OU waste sites, received about 30 Mgal of scavenged tank waste, with possibly the largest inventory of 99Tc ever disposed to the soil at Hanford and site remediation is being accelerated. The purpose of this work was to develop a conceptual model for contaminant fate and transport at the 216-B-26 Trench site to support identification and development and evaluation of remediation alternatives. Large concentrations of 99Tc high above the water table implicated stratigraphy in the control of the downward migration. The current conceptual model accounts for small-scale stratigraphy; site-specific changes soil properties; tilted layers; and lateral spreading. It assumes the layers are spatially continuous causing water and solutes to move laterally across the boundary if conditions permit. Water influx at the surface is assumed to be steady. Model parameters were generated with pedotransfer functions; these were coupled high resolution neutron moisture logs that provided information on the underlying heterogeneity on a scale of 3 inches. Two approaches were used to evaluate the impact of remedial options on transport. In the first, a 1-D convolution solution to the convective-dispersive equation was used, assuming steady flow. This model was used to predict future movement of the existing plume using the mean and depth dependent moisture content. In the second approach, the STOMP model was used to first predict the current plume distribution followed by its future migration. Redistribution of the 99Tc plume was simulated for the no-action alternative and on-site capping. Hypothetical caps limiting recharge to 1.0, 0.5, and 0.1 mm yr-1 were considered and assumed not to degrade in the long term. Results show that arrival time of the MCLs, the peak arrival time, and the arrival time of the center of mass increased with decreasing recharge rate. The 1-D convolution model is easy to apply and can easily accommodate initial contaminant inventory and water content depth distributions of any complexity. However, the results are somewhat conservative in that the model does not take credit for stratification and its dimensionality effects. Transient analysis shows transport to be controlled by small-scale stratification that resulted in laterally movement of contaminants and their failure to reach the ground water. Multiple discharges quickly merged into a single plume that migrated beyond the domain boundaries. However, it appears that this very feature that was effective in mitigating deep transport of the contaminants for almost 50 years now functions to confound expected barrier effects. Simulations suggest that a barrier provides no additional protection above the no-action alternative. Although continuous layers are assumed, in reality, there may be discontinuities that could lead to vertical movement. Episodic recharge events could also be conducive to downward movement. As more data becomes available, the conceptual model will be revised. Based on the analyses, capping appears to be no better than the no-action alternative. Projected 99Tc concentrations reaching the groundwater suggest that alternate source control actions may be necessary to reach soil screening levels. The benefits of active remediation are therefore readily apparent. Because none of the alternatives reduce soil concentrations, they effect no active reduction in the groundwater concentrations therefore the residual risk will remain high.

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Vadose Zone Contaminant Fate and Transport Analysis for the 216-B-26 Trench

In FY 2004, monitoring of the prototype Hanford barrier focused on barrier stability, vegetative cover, evidence of plant and animal intrusion, and the main components of the water balance. Monitored water-balance components included precipitation, runoff, storage, drainage, and deep percolation. Precipitation in FY 2004 was 26 percent less than in FY 2003 but was still higher than normal. The seasonal distribution in precipitation was also different from the previous year with a 43 percent reduction in spring precipitation and a 46 percent increase in summer precipitation. The cumulative amount of water received from October 1994, through September 2004, was 2,559.58 mm on the northern half of the barrier, which is the formerly irrigated treatment, and 1,886.71 mm on the southern non-irrigated treatments. Water storage continued to show a cyclic pattern, increasing in the winter and declining in the spring and summer to a lower limit of about 100 mm in response to evapotranspiration. The 600-mm design storage has never been exceeded. Total drainage from the soil-covered plots range from 2.9E-4 mm to 0.22 mm or 0.003 6 0.004 percent of precipitation. Side-slope drainage was much higher at 20.9 6 2.3 percent of precipitation from the gravel and 18.6 6 5.1more » percent from the riprap. There was no runoff from the barrier, but runoff from the BY tank farm following a thunderstorm in May eroded a 45-inch-deep channel into the structural fill at the toe of the riprap slope. Above-asphalt and below-asphalt moisture measurements show no evidence of deep percolation of water. Topographic surveys were conducted on the barrier surface, including the two settlement gauges and 12 creep gauges on the riprap slope using aerial photogrammetry (AP) and a global positioning system (GPS). Comparing the aerial photogrammetry (AP) and global positioning system (GPS) surveys with the traditional survey shows the barrier and side slopes to be stable. Both AP and GPS show potential for considerable cost savings without any loss in accuracy. A relatively high coverage of native plants still persists after the initial revegetation in 1994. The formerly irrigated treatments continue to show greater cover of grasses and litter than the non-irrigated treatments. On the formerly irrigated treatments, the mean cover class was 25 to 50 percent for both grasses and shrubs. On the non-irrigated treatments, the mean cover class was 5 to 25 percent from grasses and 25 to 50 percent for shrubs. Species diversity of the vegetative community appears to have stabilized over the past several years. In addition to 12 of 17 species present in 2003 being present in 2004, two additional species were encountered. Sagebrush continues to flourish with shrubs along the perimeter showing higher biomass yield than the interior shrubs. There is evidence of sagebrush seedlings recruitment but not of rabbitbrush; the presence of gray rabbitbrush appears is declining as the barrier surface continues to stabilize. Use of the barrier surface by insects and small mammals is also evident. Small mammal burrowing on the barrier surface has become more prevalent in recent years, suggesting that the restored barrier surface is beginning to function as a recovering ecosystem. Small-mammal burrowing on the top and sides of the barrier is most prevalent on the finer-grained and disturbed soils while active ant mounds were observed on the northern and western slopes.« less

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Jason M. Keller

Papers

Passive wick fluxmeters: Design considerations and field applications

Measurement and Prediction of Deep Drainage from Bare Sediments at a Semiarid Site

Vadose Zone Transport Field Study: Summary Report

Vadose Zone Contaminant Fate and Transport Analysis for the 216-B-26 Trench

200-BP-1 Prototype Hanford Barrier Annual Monitoring Report for Fiscal Year 2004