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For sites with vadose zone contamination, the nature and extent of groundwater contaminant plumes are related to the flux into groundwater. In thick vadose zones at arid sites, transport is likely relative slow, complicating direct measurement of contaminant flux. A predictive numerical analysis was applied to estimate contaminant flux to groundwater at the Hanford BY Cribs site. The site received large amounts of waste water in the 1950’s, containing contaminants such as technetium-99 and nitrate. Recently, large increases in groundwater concentrations have been observed in site groundwater wells and, for potential remediation purposes, vadose zone fluxes into groundwater needed to be evaluated. The analysis approach uses forward simulations, tracking contaminants during and after disposal, and imposed concentration (IC) simulations, where concentrations, derived from electrical conductivity data obtained in 2007, are imposed on the flow field. A total of three IC methods, relating electrical conductivity to nitrate concentrations, are developed and tested. The numerical analysis predicts high fluxes during and directly after disposal, with decreasing trends beginning in 1970. The IC simulations also show declining nitrate fluxes over time. The predicted fluxes of the forward and IC simulations after 2007 are in reasonable agreement. The observed concentration increases in the groundwater below the BY Cribs site cannot be explained by an increase in contaminant flux from the vadose zone. An alternative explanation, based on the observed decrease in aquifer thickness below the site, is presented.

Model-based decision making is commonly used in performance assessments to assure water resource protection for both human health and the environment for hundreds of years into the future. To make decisions regarding aquifer protection against potential contamination, a conceptual site model (CSM) describing the hydrodynamic behavior needs to account for subsurface heterogeneities in sufficient detail. When site-specific data are sparse, larger-scale geologic descriptions are adopted with the consequence of losing small-scale features (at the cm scale) that can control contaminant transport. In this study, a multiple lines of evidence approach is used to construct vadose zone CSMs based on an evaluation of several types of data, including geologic logs, borehole moisture content and concentration data, geophysical spectral gamma logging data, and groundwater concentration data for a tank farm at the Hanford Site in southeastern Washington State. The resulting CSMs of the unsaturated zone represent a synthesis of what is known about flow and transport processes at the site-scale and maintain consistency with knowledge that has been accumulated at the regional scale. Through a process of extensive data analyses, a systematic approach is described to create an evidence base that supports the evaluation and development of CSMs. Numerical models are then used to evaluate the impact that smaller-scale heterogeneities have on contaminant transport through the vadose zone for a performance assessment on waste tank closure. Together, the field data and the numerical experiments suggest that although small-scale features close to source releases can have an impact on horizontal spreading, overall there is a relatively minor impact on transport for the site under study as evaluated by differences in peak fluxes and arrival times for historical leak events, and for potential releases resulting from waste tank closure. Use of alternative CSMs, developed through careful examination of available characterization and monitoring data, provides confidence that geologic heterogeneities do not impact contaminant transport behavior significantly enough to alter the assessment of risk for closure at this site.

Long-term monitoring solutions at contaminated sites are necessary to track plume migration and evaluate the performance of remediation efforts. Electrical resistivity imaging (ERI) can potentially provide information about plume dynamics; however, the feasibility and likelihood of success are seldom evaluated before conducting a field study. Coupling flow and transport models with geoelectrical models provide a powerful way to assess the potential effectiveness of an actual ERI field campaign. We present a coupled approach for evaluating the feasibility of monitoring nitrate migration and remediation using 4D time-lapse ERI at a legacy nuclear waste facility. This kilometer-scale study focuses on depths below the water table (∼70 m). A flow and transport model is developed to perform simulations of nitrate migration and removal via a hypothetical pump-and-treat system. A tracer injection is also simulated at the leading edge of the nitrate plume to enhance the conductivity contrast between the native subsurface and the groundwater fluids. Images of absolute bulk conductivity provide limited information concerning plume migration while time-lapse difference images, which remove the static effects of geology, provide more useful information concerning plume dynamics over time. A spatial moment analysis performed on flow and transport and ERI models matches well during the tracer injection; however, inversion regularization smoothing otherwise limits the value in terms of locating the center of mass. We find that the addition of a tracer enables ERI to characterize plume dynamics during pump-and-treat operations, and late-time ERI monitoring provides a conservative estimate of nitrate plume boundaries in this synthetic study.

We examine subsurface uranium (U) plumes at two U.S. Department of Energy sites that are located near large river systems and that are influenced by groundwater-river hydrologic interaction. Following surface excavation of contaminated materials, both sites were projected to naturally flush remnant uranium contamination to levels below regulatory limits (e.g., 30 µg/L or 0.126 µmol/L; U.S. EPA drinking water standard), with 10 years projected for the Hanford 300 Area (Columbia River) and 12 years for the Rifle site (Colorado River). The rate of observed uranium decrease was much lower than expected at both sites. While uncertainty remains, a comparison of current understanding suggests that the two sites have common, but also different mechanisms controlling plume persistence. At the Hanford 300 A, the persistent source is adsorbed U(VI) in the vadose zone that is released to the aquifer during spring water table excursions. The release of U(VI) from the vadose zone and its transport within the oxic, coarse-textured aquifer sediments is dominated by kinetically-limited surface complexation. Modeling implies that annual plume discharge volumes to the Columbia River are small (< one pore volume). At the Rifle site, slow oxidation of naturally reduced, contaminant U(IV) in the saturated zone and a continuousmore » influx of U(VI) from natural, up-gradient sources influences plume persistence. Rate-limited mass transfer and surface complexation also control U(VI) migration velocity in the sub-oxic Rifle groundwater. Flux of U(VI) from the vadose zone at the Rifle site may be locally important, but it is not the dominant process that sustains the plume. A wide range in microbiologic functional diversity exists at both sites. Strains of Geobacter and other metal reducing bacteria are present at low natural abundance that are capable of enzymatic U(VI) reduction in localized zones of accumulated detrital organic carbon or after organic carbon amendment. Major differences between the sites include the geochemical nature of residual, contaminant U; the rates of current kinetic processes (both biotic and abiotic) influencing U(VI) solid-liquid distribution; the presence of detrital organic matter and the resulting spatial heterogeneity in microbially-driven redox properties; and the magnitude of groundwater hydrologic dynamics controlled by river-stage fluctuations, geologic structures, and aquifer hydraulic properties. The comparative analysis of these sites provides important guidance to the characterization, understanding, modeling, and remediation of groundwater contaminant plumes influenced by surface water interaction that are common world-wide.« less

Bacterial-induced changes in the hydraulic properties of porous media are important in a variety of disciplines. Most of the previous research on this topic has focused on liquid-saturated porous media systems that are representative of aquifer sediments. Unsaturated or variably saturated systems such as soils require additional considerations that have not been fully addressed in the literature. This paper reviews some of the earlier studies on bacterial-induced changes in the hydraulic properties of saturated porous media, and discusses characteristics of unsaturated or variably saturated porous media that may be important to consider when modeling such phenomena in these systems. New data are presented from experiments conducted in sand-packed columns with initially steady unsaturated flow conditions that show significant biomass-induced changes in pressure heads and water contents and permeability reduction during growth of a Pseudomonas fluorescens bacterium.

Some of the defense wastes at the Hanford Site in southeastern Washington State are stored in the vadose zone. It is possible that natural recharge could mobilize and transport the contaminants in these wastes to the groundwater, as well as influence groundwater velocities and directions. The objective of this study was to estimate the areal distribution of natural recharge for use as a boundary condition for a groundwater flow and transport model. A geographic information system (GIS) was used to identify all possible combinations of soil type and vegetation and assign to each an appropriate estimate of recharge. The strategy was to assign estimates based on field data and supplement with simulation results only when necessary. The estimated rates varied from 0.7 to 127.1 mm/yr. The order of preference for assigning estimates was lysimetry > water content measurements > tracers > modeling, based on qualitative estimates of the relative error of each method as applied.The GIS software was used to estimate the annual recharge volume attributable to specific soil-vegetation combinations. The total annual recharge volume was 8.47 x 10' L for the 765 km 2 portion of the site containing the major waste storage areas. This volume is from 2 to 10 times higher than estimates of runoff and groundwater flow from adjacent higher elevations and is equivalent to facility discharges in 1992. The recharge map showed the impact of a 1984 fire on increasing recharge ; it also illustrated the higher recharge rates associated with disturbed soils in the waste storage areas.

The Integrated Field Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex subsurface biogeochemical setting where groundwater and riverwater interact. A series of forefront science questions on reactive mass transfer motivates research. These questions relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated biogeochemical system. The project was initiated in February 2007, with CY 2007, CY 2008, CY 2009, and CY 2010 progress summarized in preceding reports. A project peer review was held in March 2010, and the IFRC project acted upon all suggestions and recommendations made in consequence by reviewers and SBR/DOE. These responses have included the development of 'Modeling' and 'Well-Field Mitigation' plans that are now posted on the Hanford IFRC web-site, and modifications to the IFRC well-field completed in CY 2011. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2011 including: (i) well modifications to eliminate well-bore flows, (ii) hydrologic testing of the modified well-field and upper aquifer, (iii) geophysical monitoring of winter precipitation infiltration through the U-contaminated vadose zone and spring river water intrusion to the IFRC, (iv) injection experimentation to probe the lower vadose zone and to evaluate the transport behavior of high U concentrations, (v) extended passive monitoring during the period of water table rise and fall, and (vi) collaborative down-hole experimentation with the PNNL SFA on the biogeochemistry of the 300 A Hanford-Ringold contact and the underlying redox transition zone. The modified well-field has functioned superbly without any evidence for well-bore flows. Beyond these experimental efforts, our site-wide reactive transport models (PFLOTRAN and eSTOMP) have been updated to include site geostatistical models of both hydrologic properties and adsorbed U distribution; and new hydrologic characterization measurements of the upper aquifer. These increasingly robust models are being used to simulate past and recent U desorption-adsorption experiments performed under different hydrologic conditions, and heuristic modeling to understand the complex functioning of the smear zone. We continued efforts to assimilate geophysical logging and 3D ERT characterization data into our site wide geophysical model, with significant and positive progress in 2011 that will enable publication in 2012. Our increasingly comprehensive field experimental results and robust reactive transport simulators, along with the field and laboratory characterization, are leading to a new conceptual model of U(VI) flow and transport in the IFRC footprint and the 300 Area in general, and insights on the microbiological community and associated biogeochemical processes influencing N, S, C, Mn, and Fe. Collectively these findings and higher scale models are providing a unique and unparalleled system-scale understanding of the biogeochemical function of the groundwater-river interaction zone.

The Integrated Field Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex subsurface hydrogeologic setting where groundwater and riverwater interact. A series of forefront science questions on reactive mass transfer focus research. These questions relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated system. The project was initiated in February 2007, with CY 2007, CY 2008, and CY 2009 progress summarized in preceding reports. A project peer review was held in March 2010, and the IFRC project has responded to all suggestions and recommendations made in consequence by reviewers and SBR/DOE. These responses have included the development of “Modeling” and “Well-Field Mitigation” plans that are now posted on the Hanford IFRC web-site. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2010 including the quantification of well-bore flows in the fully screened wells and the testing of means to mitigate them; the development of site geostatistical models of hydrologic and geochemical properties including the distribution of U; developing and parameterizing a reactive transport model of the smear zone that supplies contaminant U to the groundwater plume; performance of a second passive experiment of the spring water table rise and fall event with a associated multi-point tracer test; performance of downhole biogeochemical experiments where colonization substrates and discrete water and gas samplers were deployed to the lower aquifer zone; and modeling of past injection experiments for model parameterization, deconvolution of well-bore flow effects, system understanding, and publication. We continued efforts to assimilate geophysical logging and 3D ERT characterization data into our site wide geophysical model, and have now implemented a new strategy for this activity to bypass an approach that was found unworkable. An important focus of CY 2010 activities has been infrastructure modification to the IFRC site to eliminate vertical well bore flows in the fully screened wells. The mitigation procedure was carefully evaluated and is now being implementated. A new experimental campaign is planned for early spring 2011 that will utilize the modified well-field for a U reactive transport experiment in the upper aquifer zone. Preliminary geophysical monitoring experiments of rainwater recharge in the vadose zone have been initiated with promising results, and a controlled infiltration experiment to evaluate U mobilization from the vadose zone is now under planning for the September 2011. The increasingly comprehensive field experimental results, along with the field and laboratory characterization, are leading to a new conceptual model of U(VI) flow and transport in the IFRC footprint and the 300 Area in general, and insights on the microbiological community and associated biogeochemical processes.

[1] This study explores field-scale modeling of U(VI) reactive transport through incorporation of laboratory and field data. A field-scale reactive transport model was developed on the basis of laboratory-characterized U(VI) surface complexation reactions (SCRs) and multirate mass transfer processes, as well as field-measured hydrogeochemical conditions at the U.S. Department of Energy, Hanford 300 Area (300 A), Washington. The model was used to assess the importance of multirate mass transfer processes on U(VI) reactive transport and to evaluate the effect of variable geochemical conditions caused by dynamic river water-groundwater interactions on U(VI) plume migration. Model simulations revealed complex spatiotemporal relationships between groundwater composition and U(VI) speciation, adsorption, and plume migration. In general, river water intrusion enhances uranium adsorption and lowers aqueous uranium concentration because river water dilution increases pH and decreases aqueous bicarbonate concentration, leading to overall enhanced U(VI) surface complexation. Strong U(VI) retardation was computed for the field-measured hydrogeochemical conditions, suggesting a slow dissipation of the U(VI) plume, a phenomenon consistent with field observations. The simulations also showed that SCR-retarded U(VI) migration becomes more dynamic and synchronous with the groundwater flow field when multirate mass transfer processes are involved. Breakthrough curves at selected locations and the temporal changes in the calculated mass during the 20 year simulation period indicated that uranium adsorption/desorption never attained steady state because of the dynamic flow field and groundwater composition variations caused by river water intrusion. Thus, the multirate SCR model appears to be a crucial consideration for future reactive transport simulations of uranium contaminants at the Hanford 300 A site and elsewhere under similar hydrogeochemical conditions.

The Integrated Field-Scale Subsurface Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex hydrogeologic setting where groundwater and riverwater interact. A series of forefront science questions on mass transfer are posed for research which relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated system. The project was initiated in February 2007, with CY 2007 and CY 2008 progress summarized in preceding reports. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2009 with completion of extensive laboratory measurements on field sediments, field hydrologic and geophysical characterization, four field experiments, and modeling. The laboratory characterization results are being subjected to geostatistical analyses to develop spatial heterogeneity models of U concentration and chemical, physical, and hydrologic properties needed for reactive transport modeling. The field experiments focused on: (1) physical characterization of the groundwater flow field during amore » period of stable hydrologic conditions in early spring, (2) comprehensive groundwater monitoring during spring to characterize the release of U(VI) from the lower vadose zone to the aquifer during water table rise and fall, (3) dynamic geophysical monitoring of salt-plume migration during summer, and (4) a U reactive tracer experiment (desorption) during the fall. Geophysical characterization of the well field was completed using the down-well Electrical Resistance Tomography (ERT) array, with results subjected to robust, geostatistically constrained inversion analyses. These measurements along with hydrologic characterization have yielded 3D distributions of hydraulic properties that have been incorporated into an updated and increasingly robust hydrologic model. Based on significant findings from the microbiologic characterization of deep borehole sediments in CY 2008, down-hole biogeochemistry studies were initiated where colonization substrates and spatially discrete water and gas samplers were deployed to select wells. The increasingly comprehensive field experimental results, along with the field and laboratory characterization, are leading to a new conceptual model of U(VI) flow and transport in the IFRC footprint and the 300 Area in general, and insights on the microbiological community and associated biogeochemical processes. A significant issue related to vertical flow in the IFRC wells was identified and evaluated during the spring and fall field experimental campaigns. Both upward and downward flows were observed in response to dynamic Columbia River stage. The vertical flows are caused by the interaction of pressure gradients with our heterogeneous hydraulic conductivity field. These impacts are being evaluated with additional modeling and field activities to facilitate interpretation and mitigation. The project moves into CY 2010 with ambitious plans for a drilling additional wells for the IFRC well field, additional experiments, and modeling. This research is part of the ERSP Hanford IFRC at Pacific Northwest National Laboratory.« less

Researchers at Pacific Northwest National Laboratory developed field-scale groundwater flow and transport simulations of the 300 Area to support the 300-FF-5 Operable Unit Phase III Feasibility Study. The 300 Area is located in the southeast portion of the U.S. Department of Energy’s Hanford Site in Washington State. Historical operations involving uranium fuel fabrication and research activities at the 300 Area have contaminated engineered liquid-waste disposal facilities, the underlying vadose zone, and the uppermost aquifer with uranium. The main objectives of this research were to develop numerical groundwater flow and transport models to help refine the site conceptual model, and to assist assessment of proposed alternative remediation technologies focused on the 300 Area uranium plume.

This report provides a description of uranium contamination in the subsurface at the Hanford Site's 300 Area. The principal focus is a persistence plume in groundwater, which has not attenuated as predicted by earlier remedial investigations. Included in the report are chapters on current conditions, hydrogeologic framework, groundwater flow modeling, and geochemical considerations. The report is intended to describe what is known or inferred about the uranium contamination for the purpose of making remedial action decisions.

Four new CERCLA groundwater monitoring wells were installed in the 300-FF-5 Operable Unit in FY 2006 to fulfill commitments for well installations proposed in the Hanford Federal Facility Agreement and Consent Order Milestone M-24-57. Wells were installed to collect data to determine the distribution of process uranium and other contaminants of potential concern in groundwater. These data will also support uranium contaminant transport simulations and the wells will supplement the water quality monitoring network for the 300-FF-5 OU. This report supplies the information obtained during drilling, characterization, and installation of the new groundwater monitoring wells. This document also provides a compilation of hydrogeologic, geochemical, and well construction information obtained during drilling, well development, and sample collection/analysis activities.

[1] A novel analytical method was developed that permitted real-time, noninvasive measurements of microbial growth and associated changes in hydrodynamic properties in porous media under unsaturated flowing conditions. Salicylate-induced, lux gene-based bioluminescence was used to quantify the temporal and spatial development of colonization over a 7-day time course. Water contents were determined daily by measuring light transmission through the system. Hydraulic flow paths were determined daily by pulsing a bromophenol blue dye solution through the colonized region of the sand. Bacterial growth and accumulation had a significant impact on the hydraulic properties of the porous media. Microbial colonization caused localized drying within the colonized zone, with decreases in saturation approaching 50% of antecedent values, and a 25% lowering of the capillary fringe height. Flow was retarded within the colonized zone and diverted around it concurrent with the expansion of the colonized zone between days 3 and 6. The location of horizontal dispersion corresponded with the cell densities of 1–3 × 109 cells g−1 dry sand. The apparent solute velocity through the colonized region was reduced from 0.41 cm min−1 (R2 = 0.99) to 0.25 cm min−1 (R2 = 0.99) by the sixth day of the experiment, associated with population densities that would occupy approximately 7% of the available pore space within the colonized region. Changes in the extent of colonization occurred over the course of the experiment, including upward migration against flow. The distribution of cells was not determined by water flow alone, but rather by a dynamic interaction between water flow and microbial growth. This experimental system provides rich data sets for the testing of conceptualizations expressed through numerical modeling.

This report supplies the information obtained during drilling, characterization, and installation of the new groundwater monitoring well. This document also provides a compilation of hydrogeologic and well construction information obtained during drilling, well development, and sample collection/analysis activities.

While numerous techniques exist for remediation of contaminant plumes in groundwater or near the soil surface, remediation methods in the deep vadose zone are less established due to complex transport dynamics and sparse microbial populations. There is a lack of knowledge on how physical and hydrologic features of the vadose zone control microbial growth and colonization in response to nutrient delivery during bioremediation. Yet pollution in the vadose zone poses a serious threat to the groundwater resources lying deeper in the sediment. While the contaminants may be slowly degraded by native microbial communities, microbial degradation rates rarely keep pace with the spread of the pollutant. It is crucial to increase indigenous microbial degradation in the vadose zone to combat groundwater contamination.

This letter report documents initial numerical analyses conducted by PNNL to provide support for a feasibility study on decommissioning of the canyon buildings at Hanford. The 221-U facility is the first of the major canyon buildings to be decommissioned. The specific objective of this modeling effort was to provide estimates of potential rates of migration of residual contaminants out of the 221-U facility during the first 40 years after decommissioning. If minimal contaminant migration is predicted to occur from the facility during this time period, then the structure may be deemed to provide a level of groundwater protection that is essentially equivalent to the liner and leachate collection systems that are required at conventional landfills. The STOMP code was used to simulate transport of selected radionuclides out of a canyon building, representative of the 221-U facility after decommissioning, for a period of 40 years. Simulation results indicate that none of the selected radionuclides that were modeled migrated beyond the concrete structure of the facility during the 40-year period of interest. Jacques (2001) identified other potential contaminants in the 221-U facility that were not modeled, however, including kerosene, phenol, and various metals. Modeling of these contaminants was beyond the scope ofmore » this preliminary effort due to increased complexity. Simulation results indicate that contaminant release from the canyon buildings will be diffusion controlled at early times. Advection is expected to become much more important at later times, after contaminants have diffused out of the facility and into the surrounding soil environment. After contaminants have diffused out of the facility, surface infiltration covers will become very important for mitigating further transport of contaminants in the underlying vadose zone and groundwater.« less

[1] Liquid saturation and gas-liquid interfacial area are important parameters for evaluating the transport and fate of contaminants in unsaturated subsurface environments. Recent findings indicate that interfacial surface area controls the relative degree of transmitted light in laboratory systems containing translucent porous media. Equations are derived to estimate the specific gas-liquid interfacial area from the area under the primarydrainage branch of the Seff-h characteristic curve as parameterized using common water retention functions. The total area under the curve provides the maximum available specific gas-liquid interfacial area available at residual saturation, which can be incorporated into the relationship to determine the gas-liquid interfacial area at intermediate degrees of saturation via light transmission. Experimental results, and analysis of external data sets, support these findings. Closed-form relationships are presented as enhancements to a recent method for determination of liquid saturations above residual using light transmission. A physically based model is developed and tested for the quantification of liquid contents below residual saturation. INDEX TERMS: 1829 Hydrology: Groundwater hydrology; 1866 Hydrology: Soil moisture; 1875 Hydrology: Unsaturated zone; 1894 Hydrology: Instruments and techniques; KEYWORDS: light transmission, gas-liquid interfacial surface area, liquid saturation, residual saturation, unsaturated porous media, characteristic curve