Re-Inversion of Surface Electrical Resistivity Tomography Data from the Hanford Site B-Complex

This report documents the three-dimensional (3D) inversion results of surface electrical resistivity tomography (ERT) data collected over the Hanford Site B-Complex. The data were collected in order to image the subsurface distribution of electrically conductive vadose zone contamination resulting from both planned releases of contamination into subsurface infiltration galleries (cribs, trenches, and tile fields), as well as unplanned releases from the B, BX, and BY tank farms and/or associated facilities. Electrically conductive contaminants are those which increase the ionic strength of pore fluids compared to native conditions, which comprise most types of solutes released into the subsurface B-Complex. The ERT data were collected and originally inverted as described in detail in report RPP-34690 Rev 0., 2007, which readers should refer to for a detailed description of data collection and waste disposal history. Although the ERT imaging results presented in that report successfully delineated the footprint of vadose zone contamination in areas outside of the tank farms, imaging resolution was not optimized due to the inability of available inversion codes to optimally process the massive ERT data set collected at the site. Recognizing these limitations and the potential for enhanced ERT characterization and time-lapse imaging at contaminated sites, a joint effort was initiated in 2007 by the U.S. Department of Energy – Office of Science (DOE-SC), with later support by the Office of Environmental Management (DOE-EM), and the U.S. Department of Defense (DOD), to develop a high-performance distributed memory parallel 3D ERT inversion code capable of optimally processing large ERT data sets. The culmination of this effort was the development of E4D (Johnson et al., 2010,2012) In 2012, under the Deep Vadose Zone Applied Field Research Initiative (DVZ-AFRI), the U.S. Department of Energy – Richland Operations Office (DOE-RL) and CH2M Hill Plateau Remediation Company (CHPRC) commissioned an effort for the Pacific Northwest National Laboratory (PNNL) to re-invert the ERT data collected over the B-Complex using E4D, with the objective to improve imaging resolution and better understand the distribution of vadose zone contamination at the B-Complex. The details and results of that effort as documented in this report display a significant improvement in ERT image resolution, revealing the nature and orientation of contaminant plumes originating in former infiltration galleries and extending toward the water table. In particular, large plumes originating in the BY-Cribs area appear to have intercepted, or are close to intercepting the water table after being diverted eastward, possibly by the same low permeability unit causing perched water north of the B-Tank Farm boundary. Contaminant plumes are also evident beneath the BX-Trenches, but do not appear to have intercepted the water table. Imaging results within the tank farms themselves are highly biased by the dense network of electrically conductive tanks and dry wells, and are therefore inconclusive concerning contaminant distributions beneath tanks. However, beneath the diversion boxes, the results do reveal highly conductive anomalies that are not associated with metallic infrastructure, and may be diagnostic of extensive contamination. Overall, the parallel ERT inversion provides additional detail concerning contaminated zones in terms of conductive anomalies. These anomalies are consistent with waste disposal histories, and in several cases reveal lateral contaminant transport caused by heterogeneity within the vadose zone

Re-Inversion of Surface Electrical Resistivity Tomography Data from the Hanford Site B-Complex

This report documents the three-dimensional (3D) inversion results of surface electrical resistivity tomography (ERT) data collected over the Hanford Site B-Complex. The data were collected in order to image the subsurface distribution of electrically conductive vadose zone contamination resulting from both planned releases of contamination into subsurface infiltration galleries (cribs, trenches, and tile fields), as well as unplanned releases from the B, BX, and BY tank farms and/or associated facilities. Electrically conductive contaminants are those which increase the ionic strength of pore fluids compared to native conditions, which comprise most types of solutes released into the subsurface B-Complex. The ERT data were collected and originally inverted as described in detail in report RPP-34690 Rev 0., 2007, which readers should refer to for a detailed description of data collection and waste disposal history. Although the ERT imaging results presented in that report successfully delineated the footprint of vadose zone contamination in areas outside of the tank farms, imaging resolution was not optimized due to the inability of available inversion codes to optimally process the massive ERT data set collected at the site. Recognizing these limitations and the potential for enhanced ERT characterization and time-lapse imaging at contaminated sites, a joint effort was initiated in 2007 by the U.S. Department of Energy – Office of Science (DOE-SC), with later support by the Office of Environmental Management (DOE-EM), and the U.S. Department of Defense (DOD), to develop a high-performance distributed memory parallel 3D ERT inversion code capable of optimally processing large ERT data sets. The culmination of this effort was the development of E4D (Johnson et al., 2010,2012) In 2012, under the Deep Vadose Zone Applied Field Research Initiative (DVZ-AFRI), the U.S. Department of Energy – Richland Operations Office (DOE-RL) and CH2M Hill Plateau Remediation Company (CHPRC) commissioned an effort for the Pacific Northwest National Laboratory (PNNL) to re-invert the ERT data collected over the B-Complex using E4D, with the objective to improve imaging resolution and better understand the distribution of vadose zone contamination at the B-Complex. The details and results of that effort as documented in this report display a significant improvement in ERT image resolution, revealing the nature and orientation of contaminant plumes originating in former infiltration galleries and extending toward the water table. In particular, large plumes originating in the BY-Cribs area appear to have intercepted, or are close to intercepting the water table after being diverted eastward, possibly by the same low permeability unit causing perched water north of the B-Tank Farm boundary. Contaminant plumes are also evident beneath the BX-Trenches, but do not appear to have intercepted the water table. Imaging results within the tank farms themselves are highly biased by the dense network of electrically conductive tanks and dry wells, and are therefore inconclusive concerning contaminant distributions beneath tanks. However, beneath the diversion boxes, the results do reveal highly conductive anomalies that are not associated with metallic infrastructure, and may be diagnostic of extensive contamination. Overall, the parallel ERT inversion provides additional detail concerning contaminated zones in terms of conductive anomalies. These anomalies are consistent with waste disposal histories, and in several cases reveal lateral contaminant transport caused by heterogeneity within the vadose zone

Characterization of Material from Wells 299-W10-35 (C7573) and 299-W14-74 (C7024)

The objective of this work was to characterize material accumulating on wells 299-W10-35 (C7573) and 299-W14-74 (C7024) to determine the type of material (i.e., chemical or biological) and, if the material is biological, to identify the microorganisms present

Radionuclide Retention in Concrete Wasteforms

Assessing long-term performance of Category 3 waste cement grouts for radionuclide encasement requires knowledge of the radionuclide-cement interactions and mechanisms of retention (i.e., sorption or precipitation); the mechanism of contaminant release; the significance of contaminant release pathways; how wasteform performance is affected by the full range of environmental conditions within the disposal facility; the process of wasteform aging under conditions that are representative of processes occurring in response to changing environmental conditions within the disposal facility; the effect of wasteform aging on chemical, physical, and radiological properties; and the associated impact on contaminant release. This knowledge will enable accurate prediction of radionuclide fate when the wasteforms come in contact with groundwater. Data collected throughout the course of this work will be used to quantify the efficacy of concrete wasteforms, similar to those used in the disposal of LLW and MLLW, for the immobilization of key radionuclides (i.e., uranium, technetium, and iodine). Data collected will also be used to quantify the physical and chemical properties of the concrete affecting radionuclide retention

Experimental Plan: Uranium Stabilization Through Polyphosphate Injection 300 Area Uranium Plume Treatability Demonstration Project

This Test Plan describes a laboratory-testing program to be performed at Pacific Northwest National Laboratory (PNNL) in support of the 300-FF-5 Feasibility Study (FS). The objective of the proposed treatability test is to evaluate the efficacy of using polyphosphate injections to treat uranium contaminated groundwater in situ. This study will be used to: (1) Develop implementation cost estimates; (2) Identify implementation challenges; and (3) Investigate the technology's ability to meet remedial objectives These activities will be conducted in parallel with a limited field investigation, which is currently underway to more accurately define the vertical extent of uranium in the vadose zone, and in the capillary fringe zone laterally throughout the plume. The treatability test will establish the viability of the method and, along with characterization data from the limited field investigation, will provide the means for determining how best to implement the technology in the field. By conducting the treatability work in parallel with the ongoing Limited Field Investigation, the resulting Feasibility Study (FS) will provide proven, site-specific information for evaluating polyphosphate addition and selecting a suitable remediation strategy for the uranium plume within the FS time frame at an overall cost savings

Experimental Plan: 300 Area Treatability Test: In Situ Treatment of the Vadose Zone and Smear Zone Uranium Contamination by Polyphosphate Infiltration

The overall objectives of the treatability test is to evaluate and optimize polyphosphate remediation technology for infiltration either from ground surface, or some depth of excavation, providing direct stabilization of uranium within the deep vadose and capillary fringe above the 300 Area aquifer. Expected result from this experimental plan is a data package that includes: 1) quantification of the retardation of polyphosphate, 2) the rate of degradation and the retardation of degradation products as a function of water content, 3) an understanding of the mechanism of autunite formation via the reaction of solid phase calcite-bound uranium and aqueous polyphosphate remediation technology, 4) an understanding of the transformation mechanism, identity of secondary phases, and the kinetics of the reaction between uranyl-carbonate and –silicate minerals with the polyphosphate remedy under solubility-limiting conditions, 5) quantification of the extent and rate of uranium released and immobilized based on the infiltration rate of the polyphosphate remedy and the effect of and periodic wet-dry cycling on the efficacy of polyphosphate remediation for uranium in the vadose zone and capillary fringe, and 6) quantification of reliable equilibrium solubility values for autunite under hydraulically unsaturated conditions allowing accurate prediction of the long-term stability of autunite. Moreover, results of intermediate scale testing will quantify the transport of polyphosphate and degradation products, and yield degradation rates, at a scale that is bridging the gap between the small-scale UFA studies and the field scale. These results will be used to test and verify a site-specific, variable saturation, reactive transport model and to aid in the design of a pilot-scale field test of this technology. In particular, the infiltration approach and monitoring strategy of the pilot test would be primarily based on results from intermediate-scale testing. Results from this experimental plan will be documented in a PNNL report

Adsorption of Carbon Tetrachloride to Sediments from the UP-1 Operable Unit

In 2004, Fluor Hanford, Inc. (FHI) drilled several groundwater wells within the 200-UP-1 operable unit to monitor plumes that have been the focus of past remediation activities. Thirteen cores taken from three wells (C4298, C4299, and C4300) were sent to Pacific Northwest National Laboratory for characterization and quantification of contaminant retardation. These cores were 4-inches in diameter by 6-inches in length and were taken from depths near the unconfined aquifer surface (water table) to locations approximately 150 to 180 ft below the water table. Prior to this work, no 200-UP-1 site-specific adsorption data (i.e., values of distribution coefficient [Kd ]) were available for the sediments or key contaminants present in the 200-UP-1 operable unit groundwater plume. Site-specific sorption data for carbon tetrachloride (CCl4) was obtained with the <2 mm size fractions of uncontaminated 200-UP-1 sediments taken from two of these boreholes (C4299 and C4300) and distribution coefficients determined. Each fraction exhibited bimodal CCl4 adsorption isotherms over the concentration range (15 – 2500 g L-1) for total CCl4 in solution. Sorption of CCl4 was linear over the concentration ranges of 15 to 400 g L-1 and 400 to 2500 g L-1. The Kd values measured for the three 200-UP-1 sediments exhibited bimodal sorption with initial Kd values ranging from 0.0002 to 0.0005, and phase 2 values approximately 0.003 for all sediments. The measure Kd values are lower than the range calculated for CCl4 in a Hanford soil (0.016 to 0.83 L/Kg) containing an average organic carbon content of 0.2% (Truex et al., 2001). The best estimate value of Truex et al. (2001) is 0.06 L/Kg based on a 0.1% sediment organic carbon content. However, this estimate is based on an organic carbon content up to an order of magnitude greater than the organic carbon content of the sediments tested herein. Prolonged contact may increase adsorption of CCl4 as a result of mineral driven sorption and intraparticle diffusion. Kd values obtained on sediment samples from 200-UP-1 contributes to a larger Kd database that exists for other Hanford sediments, and contains significant desorption data for CCl4. Comparison of previous data with new results (e.g., from this study) will allow inferences to be made on how the 200-UP-1 Kd values for CCl4 may compare with sediments from other Hanford locations. Adsorption results presented here validate the use of a linear adsorption isotherm (Kd) to predict short contact time CCl4 adsorption to sediments in 200-UP-1 groundwater plume for a distinct ranges in CCl4 concentration. However, this does not imply that values of Kd will be constant if the groundwater chemical composition at 200-UP-1 changes with space or time. This site-specific sorption data, when complemented by the chemical, geologic, mineralogic, hydrologic, and physical characterization data that are also being collected (see Sampling and Analysis Plan for the 200-UP-1 Groundwater Monitoring Well Network, DOE 2002) can be used to develop a robust, scientifically defensible data base to allow risk predictions to be generated and to aid in future remediation decisions for the 200-UP-1 operable unit

Challenges Associated with Apatite Remediation of Uranium in the 300 Area Aquifer

Sequestration of uranium as insoluble phosphate phases appears to be a promising alternative for treating the uranium-contaminated groundwater at the Hanford 300 Area. The proposed approach involves both the direct formation of autunite by the application of a polyphosphate mixture, as well as the formation of apatite in the aquifer as a continuing source of phosphate for long-term treatment of uranium. After a series of bench-scale tests, a field treatability test was conducted in a well at the 300 Area. The objective of the treatability test was to evaluate the efficacy of using polyphosphate injections to treat uranium-contaminated groundwater in situ. A test site consisting of an injection well and 15 monitoring wells was installed in the 300 Area near the process trenches that had previously received uranium-bearing effluents. The results indicated that while the direct formation of autunite appears to have been successful, the outcome of the apatite formation of the test was more limited. Two separate overarching issues impact the efficacy of apatite remediation for uranium sequestration within the 300 Area: 1) the efficacy of apatite for sequestering uranium under the present geochemical and hydrodynamic conditions, and 2) the formation and emplacement of apatite via polyphosphate technology. This paper summarizes these issues

Corrosion of Metal Inclusions In Bulk Vitrification Waste Packages

The primary purpose of the work reported here is to analyze the potential effect of the release of technetium (Tc) from metal inclusions in bulk vitrification waste packages once they are placed in the Integrated Disposal Facility (IDF). As part of the strategy for immobilizing waste from the underground tanks at Hanford, selected wastes will be immobilized using bulk vitrification. During analyses of the glass produced in engineering-scale tests, metal inclusions were found in the glass product. This report contains the results from experiments designed to quantify the corrosion rates of metal inclusions found in the glass product from AMEC Test ES-32B and simulations designed to compare the rate of Tc release from the metal inclusions to the release of Tc from glass produced with the bulk vitrification process. In the simulations, the Tc in the metal inclusions was assumed to be released congruently during metal corrosion as soluble TcO4-. The experimental results and modeling calculations show that the metal corrosion rate will, under all conceivable conditions at the IDF, be dominated by the presence of the passivating layer and corrosion products on the metal particles. As a result, the release of Tc from the metal particles at the surfaces of fractures in the glass releases at a rate similar to the Tc present as a soluble salt. The release of the remaining Tc in the metal is controlled by the dissolution of the glass matrix. To summarize, the release of 99Tc from the BV glass within precipitated Fe is directly proportional to the diameter of the Fe particles and to the amount of precipitated Fe. However, the main contribution to the Tc release from the iron particles is over the same time period as the release of the soluble Tc salt. For the base case used in this study (0.48 mass% of 0.5 mm diameter metal particles homogeneously distributed in the BV glass), the release of 99Tc from the metal is approximately the same as the release from 0.3 mass% soluble Tc salt in the castable refractory block and it is released over the same time period as the salt. Therefore, to limit the impact of precipitated Fe on the release of 99Tc, both the amount of precipitated Fe in the BV glass and the diameter of these particles should be minimized