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32 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Removable, Sequestration Coatings for Mitigating Hazardous Contaminants Related to Deactivation and Decommissioning Activities

This project is a collaborative effort between InnoSense LLC (ISL) and Oak Ridge National Laboratory (ORNL) aimed at mitigating the mercury (Hg) contamination problem at the Y-12 National Security Complex (NSC). The report summarizes the research and technology development work of the Phase IIB Project, led by Dr. Uma Sampathkumaran at ISL for the period of July 31, 2017–October 31, 2021. The Y-12 site cleanup includes technologies for safe and cost-effective facility demolition, soil remediation, and on-site treatment and disposal of mercury bearing wastes. One of the technology demonstration goals was a reactive strippable coating for targeted pre-demolition and de-contamination to limit Hg mobilization and the volume of debris requiring treatment for disposal. Toward this, ISL has developed a water-based reactive strippable coating (Trap & See-Hg™) to sequester elemental Hg(0) and mercuric Hg(II) species in the coating. The coating provides multiple benefits including (1) Hg vapor suppression, (2) sealing in the hazardous contaminants, (3) visually locating the contaminant through color changes, and (4) remediating the contaminated surfaces upon coating removal. Through collaboration between ORNL and ISL in Phase II work, the team successfully demonstrated the Trap & See-Hg technology to (1) visually locate the presence of Hg on concrete, soil and drywall surfaces, (2) effectively sequester all mercury species (elemental, soluble and insoluble Hg) from lab-generated and ex-situ soil and brick/rubble samples collected from the Y 12 site with 80 to 95% efficiency to capture/reduce Hg vapor concentration, (3) be applied by manual and robotic spray applicators and cure at room ambient, (4) remain a cohesive and peelable coating upon drying, and (5) sequester Hg0 from walls in the alpha-2 building basement at Y-12 during a small scale in-situ field trial. In Phase IIB, ISL’s effort was focused on refining the coating formulations with additives containing passive and reactive sorbents, colorimetric indicator, and thixotropic agents to achieve the desired performance. The paints were then evaluated at ORNL for applicability to metal and concrete surfaces of different sizes and shapes, and soil rubble, Hg-sorption capacity and achieving sag-free coating on surfaces when applied by a manual spray applicator. Ambient cure of the coating resulted in a dry thickness of 16–20 mil. The coatings were removed from smooth or rough surfaces with low to moderate force. Both lab-generated Hg-contaminated samples and soil and brick/rubble samples containing a range of Hg concentrations (collected from the Y-12 site by UCOR) were used in this project. Optimized formulations were applied to these samples and evaluated for ability to suppress Hg vapors, sequester Hg 0 and Hg(II) species and color mapping of mercury species on the test surface. The ORNL team initially identified three to four potential sites at Y-12 and ORNL for potential demonstration. However, the pandemic closed any possible avenues for on-site demonstration of the robotic spray applicator. The metal and concrete samples with low to high Hg content provided by UCOR from an ongoing demolition were subsequently used for ex-situ sample characterization and analysis at ORNL over a period of 25 days. The coatings suppressed Hg vapors with an efficiency of 95–99% from heavily contaminated metal and 60% from concrete substrate. Analysis of total Hg in the peeled paints indicates sorption capacities ranging from 12 µg Hg/g of paint from concrete to 1.2 mg Hg/g of paint from the metal substrates while peeled paints from soil samples could capture a total Hg from 2.3 mg Hg/g to 66 mg/g paint. Toxicity characteristic leaching procedure (TCLP) tests recovered total mercury leached at 0.15±0.0008 µg/L for concrete to 126.81±0.67 µg/L and 377.25±5.67 µg/L for the two metal substrates, to allow for informed decisions on downstream disposal considerations. Together, this Phase IIB demonstrated the potential value of the Trap & See-Hg for Hg uptake, vapor suppression, and color mapping, and may thus be used to enhance worker safety during site cleanup, facility demolition, and downstream waste disposal at Y-12 NSC.

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DOE OSTI2023

Review of Mercury Sequestration in Cementitious Waste Forms

Decontaminated salt solution from Tank 50 at the Savannah River Site (SRS) is known to contain dissolved mercury species which are present as hydroxides and oxides. These species are reported in analytical measurements as the organic cation [CH 3 Hg] + and the inorganic cation Hg 2+ . The salt solution is mixed with cementitious reagents, blast-furnace slag (BFS) and thermally beneficiated Class F fly ash in the Saltstone Processing Facility and pumped into engineered Saltstone Disposal Units, (SDUs), to produce a solidified waste form. The solidified waste form, saltstone, encapsulates and chemically stabilizes the mercury and other contaminants, sequestering them from release into the environment. With the discovery of methylmercury in the salt solution, testing was performed to determine the extent to which saltstone prepared with methylmercury (MeHg) retains mercury in the Toxicity Characteristic Leaching Procedure (TCLP). Results from this testing indicated that the amount of mercury extracted remained below the regulatory limit, and that the saltstone formulation with a greater proportion of BFS performed slightly better at retaining Hg in the solid.

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DOE OSTI2024

Regulatory Testing of WTP HL W Glasses for Compliance with Delisting Requirements, VSL-03R3780-1, Rev. 1

(Part of the data collected for this work and discussed in this report was subject to data quality and bias issues. All the affected tests have subsequently been repeated, as directed by the Waste Treatment Plant Project, and new statistical analyses have been performed on the revised data set. A subsequently-issued report supercedes this report and describes the revised data, together with the revised composition-property models (Kot et al. 2004). The reader should refer to the new report for discussion of the revised data set and composition-property (TCLP cadmium release) models. None of the data for the spike glasses, designed for Case 1 and Case 2 COPCs testing, were affected by this issue.)

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DOE OSTI2024

Integrated Off-Gas System Tests on the DM1200 Melter with RPP-WTP LAW Sub-Envelope C1 Simulants (Final Report)

The report documents melter and off-gas performance results obtained on the DM1200 during processing of LAW Sub-Envelope Cl feed. The principal objectives of the DM1200 melter testing were to demonstrate suitable processing and production rates for LAW Cl feed; characterize the glass product for elemental composition, the presence of organic compounds, and TCLP response for metals; and measure destruction and removal efficiencies (DREs) for organic compounds across the melter and off-gas treatment components. The feed was spiked with organic compounds for part of the testing duration. Data were collected for both process engineering needs and to support regulatory activities. The data needed for regulatory support were collected using EPA methods and independent data analyses and data checking were performed.

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DOE OSTI2025

Affinity of LDR Organics to Cementitious Materials: Sorption and Leaching Tests

SRNL is working to identify and test the physiochemical interactions of organic contaminants of potential concern with minerals in grout/cementitious materials. Organic species may interact with cementitious minerals including slag, fly ash, cement, and other components/dopants like carbon in fly ash. The identification of such interactions will support the solidification process design, performance assessments for the chemicals of concern, and a proposed Resource Conservation and Recovery Act (RCRA) treatment variance specified for the Land Disposal Restriction (LDR) organics associated with Hanford tank waste. Inably expected to be present LDR organics associated with Hanford tank waste (RPP-RPT-63493, Rev 1a) was screened by functional groups, octanol-water partitioning coefficients, and detection frequency in Hanford tank waste samples. A subset of 10 compounds, spanning the identified properties, were tested using sorption and leachate tests. These compounds were subjected to traditional batch sorption tests and leaching tests on/from Cast Stone cementitious material with and without activated carbon (a potential organic adsorption additive). The interactions between organic compounds were observed in traditional batch sorption and modified Toxic Characteristic Leaching Procedure (TCLP) leachate tests for a surrogate Cast Stone material with and without an activated carbon addition. Specifically, phthalic acids (negatively charged) and 4-chloroaniline (polar) sorbed strongly to unmodified Cast Stone and a group of 3 phenolic compounds (2,4,6-Trichlorophenol, Pentachlorophenol, o-Cresol) were sorbed to and were retained by Cast Stone with a 1% activated carbon amendment.

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DOE OSTI2026

Enhanced HLW glass property-composition models - phase 3

During the present phase (Phase 3) of work to enhance and expand the HLW glass property-composition models, test data for 137 glasses were collected and incorporated into the combined WTP/ORP database. The new data include those collected on glasses from two statistically designed matrices to augment the moderate alumina region (the HLW16-MA matrix covering the region of 9 wt% < Al2O3 < 12 wt% with 16 glasses) and the ultra-high alumina region (the HLW16-UHA matrix covering the region of 26 wt% < Al2O3 < 29 wt% with 29 glasses). The addition of ORP glasses over the different phases of testing has significantly expanded the combined WTP/ORP database. The compiled data include glass compositions, PCT (B, Li and Na) releases, spinel T1%, electrical conductivity, viscosity, TCLP-Cd releases, and nepheline formation upon CCC. With the exception of the CCC spinel formation data – the CCC data will be used to support the further development of nepheline models for Hanford HLW glasses.

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DOE OSTI2026

Enhancement of HLW glass property-composition models

Since the WTP compositional space of HLW glasses is extremely large, development of HLW property-composition models is a multi-year task consisting of multiple phases. The primary focus of this work was to enhance the WTP HLW models of interest including PCT releases, spinel crystallization (T1%), viscosity, electrical conductivity, and TCLP-Cd response. Model development to predict nepheline formation upon CCC is the subject of a separate task. In particular, the earlier work has produced property-composition models for glass melt viscosity and glass melt electrical conductivity that showed good performance, while models for PCT releases and spinel crystallization (T1%) required improvement. Therefore, more efforts were directed in the present work to collect data and improve model performance for HLW glass PCT releases and spinel crystallization than for other properties. The present work is a continuation of earlier development phases and is responsive to the applicable Test Plan.

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DOE OSTI2026

Retention of LDR Inorganics in Solidified/Immobilized Waste

This report provides a summary of the laboratory data and statistical analysis used to calculate retention factors in solidified/stabilized Hanford tank waste for the 13 LDR inorganic species associated with Hanford tank waste (SRNL-STI-2020-00228). The data presented is a summary of the results of research performed to build a correlation between the untreated waste concentration and the TCLP response of a solidified/stabilized waste form. This report establishes the efficacy of two treatment technologies found in 40 CFR 268.42, CHRED (chemical reduction) and STABL (stabilization), that are key to the Sample-and-Send strategy.

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DOE OSTI2026

Testing of High S Matrix Glasses to Expand DFHLW Glass Compositional Ranges (Rev.1)

Gaps in glass composition-property data for direct-feed high-level waste (DFHLW) have recently been identified. One such gap is the region of high sulfur solubility since previous, pretreated, high-level wastes contained very little sulfur. Filling this data gap will significantly broaden the range of process flowsheet options including minimal washing and will allow for optimized waste loading in DFHLW glasses. This report summarizes the data collected during the characterization of the DFHLW High S Glass Matrix (HS24). A glass matrix of 50 glass compositions was developed to evenly cover the DFHLW composition region for high sulfur glass. Matrix glasses were designed to expand the composition region outside the current component concentration and property limits so as to reduce uncertainties at the limits. The 50 matrix glasses were fabricated and tested for properties important to the success of DFHLW vitrification including: compositions, canister centerline cooling (CCC) crystallinity and isothermal crystallinity, density, viscosity, electrical conductivity (EC), product consistency test (PCT) response, toxicity, and sulfate solubility. Melter materials corrosion testing is reported elsewhere. These glasses were intentionally designed to have high SO 3 solubilities (0.7 to 2.2 SO 3 wt%) in compositional regions that had not been previously explored. Forty-eight glasses showed the measured SO 3 content retained >80% of the target SO 3 and the densities of all the glasses ranged from 2.49 g·cm -3 to 2.74 g·cm -3 . While the model predicted nepheline formation in 5 glasses, one of the tested 50 CCC glasses formed nepheline, and 35 glasses formed Cr-containing phases such as spinels and eskolaite. Only five glasses were amorphous after CCC treatment where 44 glasses with detectable crystals contained =10 wt% crystals and only one glass had > 10 wt% crystals. None of the glasses exceeded the allowable T 2% for spinel crystal formation at 950 ºC (i.e., no glasses had >2 wt% spinel at 950 ºC) during isothermal crystal fraction tests where 10 glasses showed no crystalline phases at or below 950 ºC. All the glasses (except one which failed being slightly lower than the target) satisfied the SO 3 constraint while 98 glasses did not meet the viscosity constraints and 4 failed the EC constraints. Six quenched (Q) and six CCC glasses failed the Defense Waste Processing Facility (DWPF) Environmental Assessment (EA) glass PCT threshold and 3 Q and 4 CCC failed the PCT design constraint. One glass exceeded the WTP delisting limits for Cr via EPA Method 1311 (i.e., Toxicity Characteristic Leaching Procedure, TCLP). It should be emphasized that some of these glasses were specifically designed to approach or even exceed certain property constraints, as filling data gaps in these regions will provide the greatest benefit for future model development by improving accuracy and reducing uncertainties. These insights will ultimately support the development of more robust glass formulation strategies, enabling higher waste loading, reducing operational risks, and expanding the processing envelope.

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DOE OSTI2020

Critical Design Elements for an On-Site Mercury Concentration and Holding Facility - 20175

Administrative changes and funding issues have delayed the Department of Energy (DOE) from establishing and commissioning a National Repository for mercury as required under the Mercury Export Ban Act (MEBA) of 2008. In the interim, a few hazardous waste Treatment, Storage, and Disposal Facilities (TSDFs) have been authorized to accept mercury classified as a hazardous waste as under Subtitle C of the Resource Conservation and Recovery Act (RCRA). Waste generators are charged (either by weight or by volume) for the waste they manifest to these TSDFs. In many cases, mercury and mercury compounds have chemically sorbed to (or physically lodged into) the interstitial spaces of a substrate material. This almost always causes the amount of waste generated to be unnecessarily large, due to the extra volume (or weight) of the accompanying, non-mercury materials. Depending on a multitude of factors, it could be financially beneficial for waste generators to take greater control of their mercury affairs by separating these substrate materials from the mercury and mercury compounds that have become associated with them. Building and operating an on-site mercury Concentration and Holding Facility (CHF) could help relieve a waste generator's overall cost burden. The purpose of such CHFs is not to treat or dispose of mercury, but to recover and concentrate mercury from bulky mercury-laden materials to the extent that the host substrate to which the mercury may have previously been sorbed could pass a Toxicity Characteristic Leaching Procedure (TCLP) test and either be disposed of at a conventional landfill, or be disposed of at a hazardous waste landfill, but absent additional restrictions specifically for mercury. A CHF represents a way for waste generators to save money by separating mercury from common host materials, concentrating it, and then safely storing it until transportation to an authorized TSDF takes place This paper focuses on the critical design elements waste generators should consider when designing and operating a mercury CHF. (authors)

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DOE OSTI2026

Affinity and Treatment of LDR Organics in Low Activity Waste by Cementitious Materials – 26109

The physiochemical interactions between organic contaminants, minerals, and polymer additives in grout/cementitious materials are being identified. This research supports a proposed Resource Conservation and Recovery Act (RCRA) treatment variance relevant to the Land Disposal Restriction (LDR) organics present in Hanford tank waste. It provides the technical basis to address the aspects documented by the Environmental Protection Agency in a draft memo necessary to establish that organics can be immobilized/stabilized in a cementitious matrix. The organic species may interact with cementitious minerals, including slag, fly ash, cement, and other components/dopants like activated carbon. A list of 132 reasonably expected LDR organics associated with Hanford tank waste (RPP-RPT-63493, Rev 1a) was screened by functional groups, octanol-water partitioning coefficients, and detection frequency in Hanford tank waste samples. A subset of 15 compounds spanning the identified properties was tested using sorption and leachate tests. These compounds were subjected to traditional batch sorption tests and leaching tests on/from Cast Stone cementitious material with and without activated carbon (a potential organic adsorption additive). The interactions between organic compounds were observed in traditional batch sorption and modified TCLP leachate tests for surrogate Cast Stone material with and without activated carbon addition. Specifically, phthalic acid (negatively charged) and 4-chloroaniline (polar) sorbed strongly to unmodified Cast Stone, while a group of three phenolic compounds (2,4,6-Trichlorophenol, Pentachlorophenol, o-Cresol) sorbed to and were retained by Cast Stone with a 1% activated carbon amendment. Mixtures of these compounds demonstrated visible retention of the organics within the matrix with a quantifiable affinity of the organics to the cement. This novel testing supports the notion that organics within Hanford tank waste would be retained onto the cement phase with the addition of simple materials easily added to the formulation as part of the treatment process. To further provide additional support to this claim, models employing Flory-Huggins theory in conjunction with macromolecular and organic molecule solubility parameters and species activity coefficients are being utilized to better understand these interactions. Within this context, Van Krevelen (VK) and Hansen organic and polymer solubility parameters were used to inform the Flory-Huggins interaction parameter, allowing for a quantifiable method of evaluating polymer-solvent compatibility and, by extension, interactions with proposed binding additives (e.g., activated carbon). These models and measurement should test the hypothesis for our systems understanding and applicability of Flory-Huggins theory, and whether the prediction of organics in the polymer phase versus the aqueous phase can be confidently made using this strategy. The estimation of the organic molecular activity coefficient in these high salt-saturated aqueous systems is another factor that will be assessed. This project aims to predict and understand complicated organic interactions in these heterogenous systems, guiding optimal treatment and stabilization methodologies.

Jolin, Will [Savannah River National Laboratory (S↗
DOE OSTI2023

Functional Predictor Variables for the Leaching Potential of Arsenic and Selenium from Coal Fly Ash

The release of leachates from intact coal ash impoundments is a concern due to the enrichment and mobilization of toxic elements such as arsenic (As) and selenium (Se). This study aims to explore the intrinsic properties of coal fly ash that correlate with the relative leachability of As and Se. We performed leaching experiments with 52 fly ash samples collected from 15 different U.S. power plants and representing coal feedstocks from the three major domestic regions. We assessed the mobilization potential of As and Se in fly ash based on standardized leaching protocols and performed multivariate and lasso regression analyses to explore correlations of leachable As and Se contents with characteristics such as major element contents, loss on ignition, and pH. The results of regression models indicated that major elements (Fe, Ca, and Al) for a wide range of fly ashes can serve as predictor variables for the leaching potential of As but not for Se. LOI and pH were not important predictive variables in the models. Both regression approaches resulted in relatively strong fits for leachable As (correlation coefficient R 2 = 0.78 for both models) compared to models for leachable Se (R 2 = 0.49). Overall, these results suggest that correlation models combined with on-site elemental analysis with portable analyzers may enable a screening method for leachable As in coal ash.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

Methylmercury Retention Evaluation to Support Tank 50 and Saltstone Waste Acceptance Criteria: Parts 2 and 3

The objective of this work was to provide a technical basis for the organic mercury waste acceptance criterion (WAC) for Tank 50 salt solution. The current mercury WAC for Tank 50 solution is 325 mg/L as Hg regardless of the form of mercury, which is about three times higher than any total Hg concentrations measured to date in Tank 50 solution. To date, the highest total Hg and MeHg + concentrations in the Tank 50 solution were 105 and 62 mg/L, respectively.

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DOE OSTI2021

Saltstone Waste Characterization Analysis - Salt Waste Processing Facility (SWPF) Waste Stream (Q4 CY2020)

The Saltstone Production and Disposal Facility is designed and permitted by the state of South Carolina Department of Health and Environmental Control (SCDHEC) to treat and dispose of low-level radioactive and hazardous liquid waste (salt solution) remaining from the processing of radioactive material at the Savannah River Site (SRS). Low-level waste (LEW) aqueous streams from the Effluent Treatment Project (ETP) and decontaminated solutions from the Tank Closure Cesium Removal Unit (TCCR) and the Salt Waste Processing Facility (SWPF) are stored in Tank 50 until the LEW can be transferred to the Saltstone Facility for treatment and disposal. In the past, decontaminated solution from the Modular Caustic Side Solvent Extraction Unit (MCU) was stored in Tank 50 until the LEW could be transferred to the Saltstone Facility for treatment and disposal. MCU is currently in a suspended operations state. LEW that meets the Waste Acceptance Criteria (WAC) can be transferred, stored, and treated in the Saltstone Production Facility (SPF) for subsequent disposal as saltstone grout in the Saltstone Disposal Facility (SDF). Sampling will be conducted as new waste streams are identified for treatment and disposal at the Saltstone Industrial Wastewater Treatment Facility (IWTF) and Z-Area Industrial Solid Waste Landfill (ISWLF), Facility ID# 025500-1603, General Condition B.9 or every six years in accordance with South Carolina (SC) Regulation 61-107.19 Parti C, “Solid Waste Management: Solid Waste Landfills and Structural Fill - General Requirements.”

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