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DOE OSTI2025

SaltStone Wastewater Cement Study Using Isothermal Calorimetry, Standard Concrete Characterization Techniques, and CemGEMS - 25169

Cementitious reagents are used to solidify/stabilize aqueous radioactive, hazardous, and mixed salt solutions, and sludges to meet low-level radioactive waste (LLW) and Resource Conservation and Recovery Act (RCRA) requirements for disposal at Department of Energy (DOE). It is flexible enough to solidify radioactive wastewater saturated in complex species that include but are not limited to radioactive isotopes from the bombardment of neutrons in reactor operation, corrosion products from metallic components, and a variety of soluble organic compounds. [1,2]. Waste form testing typically includes processing or fresh properties, cured properties, compressive strength and hydraulic properties, porosity, density, saturated and unsaturated moisture transport, and leachability of contaminants in the waste form pore solution. Properties are collected over a relatively limited time, typically 28 to 365 days [3]. In addition, changes in the waste form as the result of time and changing conditions are important for concrete engineers to predict overall performance of the forms and potential release of contaminants in the disposal process via unintended filtration into the environment [4]. These predictions are determined/calculated characterizing young waste forms (relative to the standard age of concrete) and are based on transport through soluble ions in pore solutions. Characterization methods include X-ray, SEM, and isothermal calorimetry among other methods used to define the composition, amorphous vs. crystalline nature of the components, and the energetic formation mechanisms for multi-phase mineral systems. [5–7] Isothermal calorimetry is a well standardized technique for cements and concretes and can be used to predict the timing and nature of the hydration reactions.[8] The technique can measure long term energetic

Bustamante, Michael E. [Savannah River National La↗
DOE OSTI2013

Method development for determining the hydraulic conductivity of fractured porous media

Plausible, but unvalidated, theoretical model constructs for unsaturated hydraulic conductivity of fractured porous media are currently used in Performance Assessment (PA) modeling for cracked saltstone and concrete (Flach 2011). The Nuclear Regulatory Commission (NRC) has expressed concern about the lack of model support for these assumed Moisture Characteristic Curves (MCC) data, as noted in Requests for Additional Information (RAIs) PA-8 and SP-4 (Savannah River Remediation, LLC, 2011). The objective of this task was to advance PA model support by developing an experimental method for determining the hydraulic conductivity of fractured cementitious materials under unsaturated conditions, and to demonstrate the technique on fractured saltstone samples. The task was requested through Task Technical Request (TTR) HLW-SSF-TTR-2012-0016 and conducted in accordance with Task Technical & Quality Assurance Plan (TTQAP) SRNL-TR-2012-00090. Preliminary method development previously conducted by Kohn et al. (2012) identified transient outflow extraction as the most promising method for characterizing the unsaturated properties of fractured porous media. While the research conducted by Kohn et al. (2012) focused on fractured media analogs such as stacked glass slides, the current task focused directly on fractured saltstone. For this task, four sample types with differing fracture geometries were considered: 1) intact saltstone, 2) intact saltstone with a single saw cut, smooth surface fracture, 3) micro-fractured saltstone (induced by oven drying), and 4) micro-fractured saltstone with a single, fully-penetrating, rough-surface fracture. Each sample type was tested initially for saturated hydraulic conductivity following method ASTM D 5084 using a flexible wall permeameter. Samples were subsequently tested using the transient outflow extraction method to determine cumulative outflow as a function of time and applied pressure. Of the four sample types tested, two yielded datasets suitable for analysis (sample types 3 and 4). The intact saltstone sample (sample type 1) did not yield any measureable outflow over the pressure range of the outflow test (0-1000 cm H 2 O). This was expected because the estimated air entry pressure for intact saltstone is on the order of 100,000 cm H 2 O (Dixon et al., 2009). The intact saltstone sample with a single saw cut smooth surface fracture (sample type 2) did not produce useable data because the fracture completely drained at less than 10 cm H 2 O applied pressure. The cumulative outflow data from sample types 3 and 4 were analyzed using an inverse solution of the Richard’s equation for water flow in variably saturated porous media. This technique was implemented using the computer code Hydrus-1D (Šimunek et al., 2008) and the resulting output included the van Genuchten-Mualem water retention and relative permeability parameters and predicted saturated hydraulic conductivity (Van Genuchten, 1980; Van Genuchten et al., 1991). Estimations of relative permeability and saturated conductivity are possible because the transient response of the sample to pressure changes is recorded during the multi-step outflow extraction test. Characteristic curves were developed for sample types 3 and 4 based on the results of the transient outflow method and compared to that of intact saltstone previously reported by Dixon et al. (2009). The overall results of this study indicate that the outflow extraction method is suitable for measuring the hydraulic properties of micro-fractured porous media. The resulting cumulative outflow data can be analyzed using the computer code Hydrus-1D to generate the van Genuchten curve fitting parameters that adequately describe fracture drainage. The resulting characteristic curves are consistent with blended characteristic curves that combine the behaviors of low pressure drainage associated with fracture flow with high pressure drainage from the bulk saltstone matrix.

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DOE OSTI2014

Degradation of cementitious materials associated with salstone disposal units

The Saltstone facilities at the DOE Savannah River Site (SRS) stabilize and dispose of low-level radioactive salt solution originating from liquid waste storage tanks at the site. The Saltstone Production Facility (SPF) receives treated salt solution and mixes the aqueous waste with dry cement, blast furnace slag, and fly ash to form a grout slurry which is mechanically pumped into concrete disposal cells that compose the Saltstone Disposal Facility (SDF). The solidified grout is termed “saltstone”. Cementitious materials play a prominent role in the design and long-term performance of the SDF. The saltstone grout exhibits low permeability and diffusivity, and thus represents a physical barrier to waste release. The waste form is also reducing, which creates a chemical barrier to waste release for certain key radionuclides, notably Tc-99. Similarly, the concrete shell of a saltstone disposal unit (SDU) represents an additional physical and chemical barrier to radionuclide release to the environment. Together the waste form and the SDU compose a robust containment structure at the time of facility closure. However, the physical and chemical state of cementitious materials will evolve over time through a variety of phenomena, leading to degraded barrier performance over Performance Assessment (PA) timescales of thousands to tens of thousands of years. Previous studies of cementitious material degradation in the context of low-level waste disposal have identified sulfate attack, carbonation influenced steel corrosion, and decalcification (primary constituent leaching) as the primary chemical degradation phenomena of most relevance to SRS exposure conditions. In this study, degradation time scales for each of these three degradation phenomena are estimated for saltstone and concrete associated with each SDU type under conservative, nominal, and best estimate assumptions.

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DOE OSTI2025

April 2025 Semiannual Composite Salt Waste Processing Facility (SWPF) Decontaminated Salt Solution (DSS) Toxicity Characteristic Leaching Procedure (TCLP) Results

The aqueous waste from the Salt Waste Processing Facility is sampled semiannually for transfers to the Saltstone Production Facility. Salt solution is treated at the Saltstone Production Facility and disposed of in the Saltstone Disposal Facility. Per request of customer, X-TTR-Z-00027, Revision 0, one Saltstone Disposal Facility waste form was prepared at Savannah River National Laboratory using the Salt Waste Processing Facility Decontaminated Salt Solution and Z-area premix material for the April 2025 semiannual Toxicity Characteristic Leaching Procedure sample. The sample contained 60:40 (by weight) of slag and fly ash (referred to as the “Cement-Free grout sample”). Results from the technical report support Task 2: ‘Grout Leaching Analyses’ of the Task Technical Request prepared by Savannah River Mission Completion. At 43 days cured, the Saltstone sample was collected and shipped to a certified laboratory for analysis using the Toxicity Characteristic Leaching Procedure. The April 2025 semiannual Cement-Free grout sample met the South Carolina Code of Regulations for Hazardous Waste Management Regulations 61-79.261.24 and 61-79.268.48 requirements for a non-hazardous waste form with respect to the Resource Conservation and Recovery Act metals and Underlying Hazardous Constituents, and met the Saltstone Production Facility Waste Acceptance Criteria that was in effect at the time of the sample collection at the Salt Waste Processing Facility.

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DOE OSTI2026

October 2025 Semiannual Composite Salt Waste Processing Facility Decontaminated Salt Solution Toxicity Characteristic Leaching Procedure Results

The aqueous waste from the Salt Waste Processing Facility is sampled semiannually for transfers to the Saltstone Disposal Facility. Salt solution is treated at the Saltstone Production Facility and disposed of in the Saltstone Disposal Facility. Per request of customer, X-TTR-Z-00027, Revision 0, one Saltstone Processing Facility Decontaminated Salt Solution and Z area premix material for the October 2025 semiannual Toxicity Characteristic Leaching Procedure sample. The sample contained 60:40 (by weight) of slag and fly ash (referred to as the “Cement-Free grout sample”). Results from the technical report support Task 2: ‘Grout Leaching Analyses’ of the Task Technical Request prepared by Savannah River Mission Completion. At 51 days cured, the Saltstone sample was collected and shipped to a certified laboratory for analysis using the Toxicity Characteristic Leaching Procedure. The October 2025 Semiannual Cement-Free grout sample met 61 79.268.48 requirements for a non-hazardous waste form with respect to the Resource Conservation and Recovery Act metals and Underlying Hazardous Constituents and met the Saltstone Production Facility Waste Acceptance Criteria that was in effect at the time of the sample collection at the Salt Waste Processing Facility.

Hsieh, Madison [Savannah River National Laboratory↗
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 OSTI2016

Results for the Fourth Quarter Calendar Year 2015 Tank 50H Salt Solution Sample

In this memorandum, the chemical and radionuclide contaminant results from the Fourth Quarter Calendar Year 2015 (CY15) sample of Tank 50H salt solution are presented in tabulated form. The Fourth Quarter CY15 Tank 50H samples were obtained on October 29, 2015 and received at Savannah River National Laboratory (SRNL) on October 30, 2015. The information from this characterization will be used by Defense Waste Processing Facility (DWPF) & Saltstone Facility Engineering for the transfer of aqueous waste from Tank 50H to the Salt Feed Tank in the Saltstone Production Facility, where the waste will be treated and disposed of in the Saltstone Disposal Facility. This memorandum compares results, where applicable, to Saltstone Waste Acceptance Criteria (WAC) limits and targets. Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals will be documented at a later time per the Task Technical and Quality Assurance Plan (TTQAP) for the Tank 50H saltstone task. The chemical and radionuclide contaminant results from the characterization of the Fourth Quarter Calendar Year 2015 (CY15) sampling of Tank 50H were requested by SRR personnel and details of the testing are presented in the SRNL Task Technical and Quality Assurance Plan.

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DOE OSTI2016

Results For The Third Quarter Calendar Year 2016 Tank 50H Salt Solution Sample

In this memorandum, the chemical and radionuclide contaminant results from the Third Quarter Calendar Year 2016 (CY16) sample of Tank 50H salt solution are presented in tabulated form. The Third Quarter CY16 Tank 50H samples (a 200 mL sample obtained 6” below the surface (HTF-5-16-63) and a 1 L sample obtained 66” from the tank bottom (HTF-50-16-64)) were obtained on July 14, 2016 and received at Savannah River National Laboratory (SRNL) on the same day. Prior to obtaining the samples from Tank 50H, a single pump was run at least 4.4 hours, and the samples were pulled immediately after pump shut down. The information from this characterization will be used by Defense Waste Processing Facility (DWPF) & Saltstone Facility Engineering for the transfer of aqueous waste from Tank 50H to the Saltstone Production Facility, where the waste will be treated and disposed of in the Saltstone Disposal Facility. This memorandum compares results, where applicable, to Saltstone Waste Acceptance Criteria (WAC) limits and targets. Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals will be documented at a later time per the Task Technical and Quality Assurance Plan (TTQAP) for the Tank 50H saltstone task. The chemical and radionuclide contaminant results from the characterization of the Third Quarter CY16 sampling of Tank 50H were requested by Savannah River Remediation (SRR) personnel and details of the testing are presented in the SRNL TTQAP.

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DOE OSTI2014

Results For the Fourth Quarter 2013 Tank 50 WAC Slurry Sample: Chemical and Radionuclide Contaminants

This report details the chemical and radionuclide contaminant results for the characterization of the 2013 Fourth Quarter sampling of Tank 50 for the Saltstone Waste Acceptance Criteria (WAC) in effect at that time. Information from this characterization will be used by DWPF & Saltstone Facility Engineering (DSFE) to support the transfer of low-level aqueous waste from Tank 50 to the Salt Feed Tank in the Saltstone Facility in Z-Area, where the waste will be immobilized. This information is also used to update the Tank 50 Waste Characterization System. The following conclusions are drawn from the analytical results provided in this report: SRR WAC targets or limits were met for all analyzed chemical and radioactive contaminants unless noted in this section. 59 Ni, 94 Nb, 247 Cm, 249 Cf, and 251 Cf are above the requested SRR target concentrations. However, they are below the detection limits established by SRNL. Norpar 13 and Isopar L have higher detection limits compared with the Saltstone WAC. The data provided in this report is based upon the concentrations in the sub-sample, and due to the limited solubility of these materials in aqueous solution, may not represent the concentrations of the analytes in Tank 50. The low insoluble solids content increases the measurement uncertainty for insoluble species. The semivolatile organic analysis (SVOA) method employed in the measurement of Norpar 13 and tributyl phosphate (TBP) has resulted in the erroneous reporting of a variety of small chain alcohols, including 4-methyl-3-hexanol and 5-methyl-3-hexanol, in previous quarterly sample reports. It has now been determined that these alcohols are an artifact of the sample preparation. Further work is being conducted in SRNL to delineate the conditions that produce these alcohols, and these findings will be reported separately.

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DOE OSTI2014

Results for the Third Quarter 2013 Tank 50 WAC Slurry Sample: Chemical and Radionuclide Contaminants

This report details the chemical and radionuclide contaminant results for the characterization of the 2013 Third Quarter sampling of Tank 50 for the Saltstone Waste Acceptance Criteria (WAC) in effect at that time. 1 Information from this characterization will be used by DWPF & Saltstone Facility Engineering (DSFE) to support the transfer of low-level aqueous waste from Tank 50 to the Salt Feed Tank in the Saltstone Facility in Z-Area, where the waste will be immobilized. This information is also used to update the Tank 50 Waste Characterization System. The following conclusions are drawn from the analytical results provided in this report: SRR WAC targets or limits were met for all analyzed chemical and radioactive contaminates unless noted in this section. 59 Ni, 94 Nb, 247 Cm, 249 Cf, and 251 Cf are above the requested SRR target concentrations. 2 However, they are below the detection limits established by SRNL. 3 Norpar 13 and Isopar L have higher detection limits4 compared with the Saltstone WAC. 1 The data provided in this report is based upon the concentrations in the sub-sample, and due to the limited solubility in aqueous solution, may not represent the concentrations of the analytes in Tank 50. Finally, the low insoluble solids content increases the measurement uncertainty for insoluble species.

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DOE OSTI2016

Characterization of Laboratory Prepared Concrete Pastes Exposed to High Alkaline and High Sodium Salt Solutions

The objective of this study was to identify potential chemical degradation mechanisms for the Saltstone Disposal Unit (SDU) concretes, which over the performance life of the structures may be exposed to highly alkaline sodium salt solutions containing sulfate, hydroxide, and other potentially corrosive chemicals in salt solution and saltstone flush water, drain water, leachate and / or pore solution. The samples analyzed in this study were cement pastes prepared in the SIMCO Technologies, Inc. concrete laboratory. They were based on the paste fractions of the concretes used to construct the Saltstone Disposal Units (SDUs). SDU 1 and 4 concrete pastes were represented by the PV1 test specimens. The paste in the SDU 2, 3, 5, and 6 concrete was represented by the PV2 test specimens. SIMCO Technologies, Inc. selected the chemicals and proportions in the aggressive solutions to approximate proportions in the saltstone pore solution [2, 3, 5, and 6]. These test specimens were cured for 56 days in curing chamber before being immersed in aggressive solutions. After exposure, the samples were frozen to prevent additional chemical transport and reaction. Selected archived (retrieved from the freezer) samples were sent to the Savannah River National Laboratory (SRNL) for additional characterization using x-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive x-ray (EDX) spectroscopy. Characterization results are summarized in this report. In addition, a correlation between the oxide composition of the pastes and their chemical durability in the alkaline salt solutions is provided.

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DOE OSTI2018

Results for the First Quarter Calendar Year 2018 Tank 50 Salt Solution Sample

In this Technical Report, the chemical and radionuclide contaminant results from the First Quarter Calendar Year 2018 (CY18) sample of Tank 50 salt solution are presented in tabulated form. The information from this characterization will be used by Savannah River Remediation (SRR) for the transfer of aqueous waste from Tank 50 to the Saltstone Production Facility, where the waste will be treated and disposed of in the Saltstone Disposal Facility. This Technical Report compares results, where applicable, to Saltstone Waste Acceptance Criteria (WAC) limits and targets. The chemical and radionuclide contaminant results from the characterization of the First Quarter CY18 sampling of Tank 50 were requested by SRR personnel via a Task Technical Request (TTR) 2 and details of the testing are presented in the Savannah River National Laboratory (SRNL)Task Technical and Quality Assurance Plan (TT QAP). This Technical Report is part of Deliverable 2 relating to Task 1 from the SRR request. 2 Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals will be documented at a later time per the TTQAP for the Tank 50 Saltstone task.

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DOE OSTI2014

Porflow modeling supporting the FY14 salstone special analysis

PORFLOW related analyses supporting the Saltstone FY14 Special Analysis (SA) described herein are based on prior modeling supporting the Saltstone FY13 SA. Notable changes to the previous round of simulations include: a) consideration of Saltstone Disposal Unit (SDU) design type 6 under “Nominal” and “Margin” conditions, b) omission of the clean cap fill from the nominal SDU 2 and 6 modeling cases as a reasonable approximation of greater waste grout fill heights, c) minor updates to the cementitious materials degradation analysis, d) use of updated I-129 sorption coefficient (Kd) values in soils, e) assignment of the pH/Eh environment of saltstone to the underlying floor concrete, considering down flow through an SDU, and f) implementation of an improved sub-model for Tc release in an oxidizing environment. These new model developments are discussed and followed by a cursory presentation of simulation results. The new Tc release sub-model produced significantly improved (smoother) flux results compared to the FY13 SA. Further discussion of PORFLOW model setup and simulation results will be presented in the FY14 SA, including dose results.

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DOE OSTI2017

Results for the first quarter calendar year 2017 tank 50H salt solution sample

In this memorandum, the chemical and radionuclide contaminant results from the First Quarter Calendar Year 2017 (CY17) sample of Tank 50H salt solution are presented in tabulated form. The First Quarter CY17 Tank 50H samples [a 200 mL sample obtained 6” below the surface (HTF-50-17-7) and a 1 L sample obtained 66” from the tank bottom (HTF-50-17-8)] were obtained on January 15, 2017 and received at Savannah River National Laboratory (SRNL) on January 16, 2017. Prior to obtaining the samples from Tank 50H, a single pump was run at least 4.4 hours and the samples were pulled immediately after pump shut down. All volatile organic analysis (VOA) and semi-volatile organic analysis (SVOA) were performed on the surface sample and all other analyses were performed on the variable depth sample. The information from this characterization will be used by Savannah River Remediation (SRR) for the transfer of aqueous waste from Tank 50H to the Saltstone Production Facility, where the waste will be treated and disposed of in the Saltstone Disposal Facility. This memorandum compares results, where applicable, to Saltstone Waste Acceptance Criteria (WAC) limits and targets. The chemical and radionuclide contaminant results from the characterization of the First Quarter CY17 sampling of Tank 50H were requested by SRR personnel and details of the testing are presented in the SRNL Task Technical and Quality Assurance Plan (TTQAP). This memorandum is part of Deliverable 2 from SRR request. Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals will be documented at a later time per the TTQAP for the Tank 50H saltstone task.

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DOE OSTI2019

Results for the Third Quarter Calendar Year 2018 Tank 50 Salt Solution Sample

In this Technical Report, the chemical and radionuclide contaminant results from the Third Quarter Calendar Year 2018 (CY18) sample of Tank 50 salt solution are presented in tabulated form. The information from this characterization will be used by Savannah River Remediation (SRR) for the transfer of aqueous waste from Tank 50 to the Saltstone Production Facility, where the waste will be treated and disposed in the Saltstone Disposal Facility. This Technical Report compares results, where applicable, to Saltstone Production Facility (SPF) Waste Acceptance Criteria (WAC) limits and targets. The chemical and radionuclide contaminant results from the characterization of the Third Quarter CY18 sampling of Tank 50 were requested by SRR personnel via a Task Technical Request (TTR) and details of the testing are presented in the Savannah River National Laboratory (SRNL) Task Technical and Quality Assurance Plan (TTQAP). This Technical Report is part of Deliverable 2 relating to Task 1 from the SRR request. Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals will be documented at a later time per the TTQAP for the Tank 50 Saltstone task.

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DOE OSTI2025

Conceptual Model Testing Related to SDU 6 Drainwell Observations

From its inception in the early 1950s through the end of the Cold War in the early 1990s, the Savannah River Site (SRS) produced nuclear materials for national defense in five reactors. Additionally, irradiated reactor fuel and target tubes were dissolved in nitric acid to recover plutonium and uranium using the PUREX (Plutonium Uranium Reduction EXtraction) process. Liquid waste from these chemical separations processes was then stored onsite in 51 underground tanks. Eight waste storage tanks have been operationally closed (i.e. cleaned and grouted) and the remaining tanks hold a mixture of liquids, insoluble solids, and precipitated salts (SRMC-LWP-2022-00001), the latter generated by evaporating water from the liquid waste. Waste is currently being retrieved from tanks and separated into 1) high-radioactivity, low-volume, and 2) low-radioactivity, high-volume components, principally through the Salt Waste Processing Facility (SWPF) (SRMC-LWP-2023-00001). The former waste stream is vitrified in the Defense Waste Processing Facility (DWPF), stored onsite, and destined for offsite disposal in a deep geologic repository. The latter stream is mixed with dry cementitious materials in the Saltstone Production Facility (SPF) and the wet slurry placed in onsite Saltstone Disposal Units (SDUs) within the Saltstone Disposal Facility (SDF), where it hardens into a cement waste form termed saltstone. A low-infiltration surface cover system will be placed over the SDF at closure, where SDUs will then be in the subsurface post-closure (SRR-CWDA-2019-00001).

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DOE OSTI2013

Development of a Performance and Processing Property Acceptance Region for Cementitious Low-Level Waste Forms at Savannah River Site - 13174

The Saltstone Production and Disposal Facilities (SPF and SDF) at the Savannah River Site (SRS) have been treating decontaminated salt solution, a low-level aqueous waste stream (LLW) since facility commissioning in 1990. In 2012, the Saltstone Facilities implemented a new Performance Assessment (PA) that incorporates an alternate design for the disposal facility to ensure that the performance objectives of DOE Order 435.1 and the National Defense Authorization Act (NDAA) of Fiscal Year 2005 Section 3116 are met. The PA performs long term modeling of the waste form, disposal facility, and disposal site hydrogeology to determine the transport history of radionuclides disposed in the LLW. Saltstone has been successfully used to dispose of LLW in a grout waste form for 15 years. Numerous waste form property assumptions directly impact the fate and transport modeling performed in the PA. The extent of process variability and consequence on performance properties are critical to meeting the assumptions of the PA. The SPF has ensured performance property acceptability by way of implementing control strategies that ensure the process operates within the analyzed limits of variability, but efforts continue to improve the understanding of facility performance in relation to the PA analysis. A similar understanding of the impact of variability on processing parameters is important from the standpoint of the operability of the production facility. The fresh grout slurry properties (particularly slurry rheology and the rate of hydration and structure formation) of the waste form directly impact the pressure and flow rates that can be reliably processed. It is thus equally important to quantify the impact of variability on processing parameters to ensure that the design basis assumptions for the production facility are maintained. Savannah River Remediation (SRR) has been pursuing a process that will ultimately establish a property acceptance region (PAR) to incorporate elements important to both processability and long-term performance properties. This process involves characterization of both emplaced product samples from the disposal facility and laboratory-simulated samples to demonstrate the effectiveness of the lab simulation. With that basis confirmed, a comprehensive variability study using non-radioactive simulants will define the acceptable PAR, or 'operating window' for Saltstone production and disposal. This same process will be used in the future to evaluate new waste streams for disposal or changes to the existing process flowsheet. (authors)

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DOE OSTI2020

Modeling Interfaces to Support Low-Level Waste Disposal System Performance Assessments - 20366

In low-level waste (LLW) disposal sites, interfaces between cementitious materials, used as waste forms and/or engineered barriers, and the surrounding soil or backfill material are often encountered. Reactions across these interfaces may lead to chemical and structural alteration of the cementitious and backfill materials that may ultimately affect long-term performance. For example, the ingress of carbon dioxide from soil gas into a waste tank concrete shell at the Hanford Site or Savannah River Site (SRS) or a low-level waste disposal vault at SRS leads to carbonation of cement hydration products (e.g. portlandite, calcium-silicate hydrate or C-S-H, and ettringite). The result of carbonation is a decrease in pH in the cement paste portion of the tank wall or vault concrete structure that could ultimately lead to de-passivation of the embedded structural steel and, eventually, to cracking. Cracking can lead to increased ingress of water into the structure, corresponding increased release of constituents of concern, and to subsequent increased transport of these constituents to the surrounding environment. The mobility of trace constituents (e.g., radionuclides of concern) in waste forms may increase in response to changes in pH, pore structure, and mineralogical gradients. Depletion of portlandite results in subsequent decalcification of C-S-H that leads to changes in the cement strength and may lead to structural failure. At the boundary between waste forms and concrete vaults, the migration of sulfate ions from the salt waste form (e.g., the saltstone waste form used for LLW disposal at the Savannah River Site in Saltstone Disposal Units, or SDUs) into the barrier or vault concrete has been predicted to result in expansive mineral phase formation (or 'sulfate attack'). Expansive mineral formation could result in cracking and potential loss of structural integrity in the vault concrete. In the performance assessment (PA) for the SRS SDUs, prediction of both the carbonation and sulfate attack fronts are critical to assessing the long-term performance of these LLW disposal vaults. A general purpose geochemical reactive transport model has been developed in LeachXS/ORCHESTRA to evaluate typical interfaces for LLW disposal environments, including SDUs at SRS. The model may be used to predict the long-term performance of interfaces between cementitious materials and saltstone or backfill materials with respect to primary phases by considering mass transport, cement chemistry, geochemical speciation, and multi-ionic diffusion over interfaces between different materials. The present study compares the performance and interactions between vault concrete and saltstone waste form for a representative SDU scenario. The materials were characterized using pH-dependence leaching test (EPA 1313) and semi-dynamic transport tests (EPA 1315) with test results used to parameterize the interface model. The development of a credible inter model provides an important basis for supporting future PAs where carbonation and sulfate attack are important aging and degradation mechanisms. (authors)

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