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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Summary of SRNL Support to the DOE-ORP Enhanced Waste Glass Program for FY23

In fiscal year 2023 (FY23) Savannah River National Laboratory (SRNL) continued tasked work for the Office of River Protection (ORP) to expand glass compositional regions accessible for low-activity waste (LAW) and high-activity waste (HLW) vitrification processing. Experimental work continued in four primary technical areas focused on processing and performance of glasses relevant to the Hanford missions. The data and results from this work will be used to expand and validate the glass models being developed at Pacific Northwest National Laboratory (PNNL) for waste processing and acceptance. This report summarizes the activities and deliverables associated with work performed in FY23.

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DOE OSTI2023

Optimization Efforts at DWPF to Ensure Waste Tank Closure by 2037 – 24404

At the Savannah River Site (SRS) in Aiken, South Carolina, the Defense Waste Processing Facility (DWPF) produces a glass-form product by processing high-level liquid waste (HLW) with borosilicate glass in a high-heated Melter, then putting the vitrified waste into stainless-steel canisters. Since 1996, DWPF has performed this vitrification process for the liquid waste mission at the SRS; the overall objective for this mission is to reduce the volume in the upstream waste tanks, so those tanks can be emptied and operationally closed. This mission seeks to eliminate the single biggest environmental risk in the state of South Carolina, which requires a robust processing strategy within the DWPF, along with optimal interface between the other facilities in the liquid waste organization (LWO). As of the end of July 2023, DWPF has safely remediated 63.7 MCi of HLW, and filled 4,319 canisters (We project that about 4,000 more canisters are needed to be filled to reach the closure goal.)

Armstead, III, Frank L.↗
DOE OSTI2020

Spent Crystalline Silicotitanate Storage Study

Washington River Protection Solutions is working to support initial production of immobilized low-activity waste (LAW) by feeding Hanford tank supernate from tank farms to the Hanford Waste Treatment and Immobilization Plant (WTP) LAW Facility. This goal incorporates the design of a Tank-Side Cesium Removal (TSCR) system, which filters tank waste supernate to remove suspended solids and then removes Cs by processing it through crystalline silicotitanate (CST) ion exchange media manufactured by Honeywell UOP, LLC. The 137 Cs-depleted product is intended to be sent to the WTP for vitrification. The Cs-loaded CST columns will be stored indefinitely, with a goal of eventual CST removal and treatment. Thus, the spent CST needs to be recoverable. The testing described herein looks to potential upset process conditions where CST storage may be required before various rinse steps are completed. This study evaluated upset conditions at three sequential processing steps envisioned for TSCR (feed, 0.1 M NaOH rinse, water rinse), and in-column drying with compressed air (normal end step) to assess impacts on the nature of the CST bed. Testing was conducted at the small scale (12-mL bed volume); simulated AP-105 tank waste was used as the feed. Following process disruption, the CST bed was dried in place at 70 °C. Post-dried CST bed physical properties (angle of repose, penetration depth, particle morphological changes) were measured to evaluate how CST moved and flowed. The testing is intended to provide a preliminary assessment of issues that may arise from desiccation of CST with the indicated salt solutions in place. Since these were small-scale tests, the processing conditions will not match full scale conditions exactly; however, the tests do provide insight into the impact of stopping processing at an earlier step than normal. Except for the feed that was dried in-place, all other process stop-conditions showed the CST bed flowed well after drying. At this small scale, CST beds would not present an issue for retrievability. The feed that was dried in place had solidified into a rock-hard monolith with no movement possible. Samples had to be chipped from the surface.

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DOE OSTI2024

Full Scale HEPA Filter Encapsulation in Ultra-High-Performance Grout - Proof of Concept

The Hanford Tank Waste Treatment and Immobilization Plant (WTP) currently being constructed to treat radioactive waste, includes vitrification facilities for both the high-level waste (HLW) and low activity waste (LAW) fractions. Operation of the WTP will produce contaminated high-efficiency particulate air filters (HEPA), as part of the solid secondary waste (SSW) stream. The HEPA filters receive off-gas from the vessel vent header and primary off-gas treatment system in LAW Facility and remove particulate contaminants including 99 Tc and 129 I salts. The current disposal method for HEPA filters is encapsulation in metal containers using cementitious material (CM) and disposal in the Integrated Disposal Facility (IDF). Results from the 2017 IDF Performance Assessment (PA) WRPS (2018) demonstrated that while compliance is maintained for the 1000 year compliance period mandated by DOE O 435.1 and its accompanying manual, release of constituents from the HEPA filters result in exceedance of the performance objective imposed as the groundwater regulatory limit at later times. For example, at about 1500 years post-closure, solid secondary waste (SSW), including HEPA filters is predicted to become a dominant contributor to 99 Tc release and over the 10,000-year sensitivity analysis period, SSW is the dominant contributor of 129 I release to the groundwater. The estimated release could potentially be reduced if the HEPA filters are not compacted and waste containers could be distributed throughout a large space, thereby diluting the contaminant release. Additionally, a better cementitious material could be used to encapsulate the HEPA filters. One alternative method for disposal of contaminated HEPA filters is encapsulation of the filters in ultra high-performance grout (UHPG). UHPG is a variation of ultra-high-performance concrete (UHPC) is commonly used in the prestressed concrete industry for large structural members. Recent studies of UHPG show it has excellent properties for containing radionuclides such as 99 Tc and 129 I Nichols and Kaplan (2021). This report presents the results of the first attempt to encapsulate a clean, full-size HEPA filter in UHPG and evaluate the effectiveness of the immobilization process and final waste form. A full-scale proof-of-concept simulated waste form was prepared by encapsulating a HEPA filter in a 110-gallon stainless steel (SS) drum using UHPG. A change from Type I/II PC to Type 1L PLC was made after American Rock Products informed the team that they would no longer be using Type I/II by the end of 2024 and the northwest was phasing out Type I/II PC overall. Type I/II PC used in previous studies of UHPG for encapsulation (Nichols and Kaplan 2021). After the UHPG was cured both the scaled mockup and the full-scale simulated waste forms were sectioned for visual examination. UHPG completely encapsulated the filters and bonded to the external surfaces of materials comprising the filters. No cracks were observed in the sectioned waste forms.

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DOE OSTI2024

Regulatory Spike Testing of RPP-WTP LAW and HLW Glasses for Compliance with Land Disposal Restrictions, VSL-03R3760-1, Rev. 1

The United States Department of Energy’s (DOE’s) Hanford site is the current location of storage of about 50 million gallons of mixed waste. This waste is stored in underground tanks at the Hanford site and is both a listed and characteristic waste, as defined in 40 CFR Part 261, and a dangerous waste according to Chapter 173-303 of the Washington Administrative Code (WAC). The waste is also subject to the Land Disposal Restrictions (LDR) (40 CFR Part 268 and WAC 173-303-140). The River Protection Project - Waste Treatment Plant (RPP-WTP) will provide DOE with a means for treating this waste by vitrification (for subsequent disposal). The tank waste will be partitioned into low and high activity fractions, which will then be vitrified respectively into Immobilized Low Activity Waste (ILAW) and Immobilized High Level Waste (IHLW) products. The ILAW product will be disposed of in an engineered facility on the Hanford site while the IHLW product will be directed to the national deep geological disposal facility for high level nuclear waste. The ILAW and IHLW products must meet a variety of requirements with respect to protection of the environment.

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DOE OSTI2024

Ion Exchange Processing of AN-107 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System

The Hanford Site stores an estimated 56 million gallons of mixed radioactive and chemically hazardous waste in large underground tanks. In support of the Direct Feed Low-Activity Waste (DFLAW) Program for expediting Hanford tank waste supernate treatment, laboratory-scale ion exchange processing using prototypic unit operations was conducted on AN-107 tank waste at the Pacific Northwest National Laboratory Radiochemical Processing Laboratory. This report describes the small-scale ion exchange testing with 13.7 L of diluted and filtered supernate from Tank 241-AN-107 (hereafter referred to as AN-107) at 16 °C (62 °F). One of the waste acceptance criteria (WAC) for the Waste Treatment Plant (WTP) Low-Activity Waste Facility is that the waste must contain less than 3.18×10 -5 Ci 137 Cs per mole of Na. For the AN-107 tank waste to meet this criterion, only 0.147% of the influent 137 Cs concentration may be delivered to the WTP; this requires a Cs decontamination factor of 678. Testing with AN-107 matched current Tank Side Cesium Removal (TSCR) facility prototypic operations where a lead-lag configuration was used until the lag column reached the WAC limit, then a polish column was brought online for continued processing in a lead-lag-polish column configuration. Feed was processed at 1.9 bed volumes (BVs) per hour; the flowrate, in terms of contact time with the crystalline silicotitanate (CST) bed, matched the expected flowrate at TSCR. The Cs-decontaminated product was retained for vitrification testing (to be reported separately). The lead column reached 40% Cs breakthrough after processing ~1700 BVs of feed; the 50% Cs breakthrough was extrapolated from the breakthrough data to occur at 1873 BVs. Testing compared to previous AP-101 and AP-107 testing at 16 °C showed ~300 BV increases in volume processed to reach the WAC limit for both lead and lag columns. The increase in capacity was determined to be due to the significantly lower K concentration in the AN-107 compared to the other tank waste matrices. A comparison in breakthrough curves for the three tests indicated slightly slower kinetic behavior in the AN-107, with variations in feed matrices (high organic complexants) likely responsible for the deviation. The Cs effluent from the lag column reached the WAC limit after processing 1097 BVs. Anticipating this breakthrough point, the polish column was preemptively installed around 900 BVs. Cs breakthrough from the lag column began at 500 BVs, reaching 3.06×10 0 µCi/mL, or 2.6 % Cs breakthrough, after processing all 1700 BVs of feed. Table S.1 and Figure S.1 summarize the observed column performance and relevant Cs loading characteristics.

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DOE OSTI2024

DuraMelter 100 Sub-Envelope Changeover Testing Using LAW SubEnvelopes A1 and C1 Feeds in Support of the LAW Pilot Melter (Final Report)

The primary goal of the testing described in this report was to develop and recommend a compliant HLW glass formulation to support the actual waste testing of AZ-101 Envelope D waste (blended with actual pretreatment products including Cs- and Tc-eluates from pretreatment of AP-101 and AZ-101 LAW). Testing of actual waste will be performed at Battelle, Pacific Northwest Division. The test objective was met by the development and recommendation of the glass formulation HLW98-95; the formulation has been transmitted to the WTP to support vitrification of HLW AZ-101 actual waste.

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DOE OSTI2024

Compositional Variation Tests on DuraMelter 100 with LAW Sub-Envelope C1 Feed (LAWC22) Glass in Support of the LAW Pilot Melter (Final Report)

The Vitreous State Laboratory at The Catholic University of America (VSL) is developing and testing glass formulations for RPP-WTP waste envelopes to provide data to meet the RPP-WTP contract requirements and to support system design activities. That work is based upon small-scale batch melts (“crucible melts”) using waste envelope simulants. Selected formulations have also been tested in small-scale continuously-fed joule-heated melters (DM10 and DM100 systems) and, ultimately, in the LAW Pilot Melter. Such melter tests provide information on key process factors such as feed processing behavior, dynamic effects during processing, sulfate incorporation, processing rates, off-gas amounts and compositions, foaming control, etc., that cannot be reliably obtained from crucible melts. This sequential scale-up approach in the vitrification testing program ensures that maximum benefit is obtained from the more costly pilot-scale tests and that the most effective use is made of that resource. The principal objective of the work described in this report was to collect the necessary small-scale melter test data with a LAW Sub-Envelope C1 waste simulant in order to support the next series of tests with the same melter feed on the LAW Pilot Melter. This work was conducted under a corresponding Test Specification and Test Plan.

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DOE OSTI2024

Summary of SRNL Support Activities to the DOE-ORP Enhanced Waste Glass Program for Fiscal Year 2024

In fiscal year 2024 (FY24) Savannah River National Laboratory (SRNL) continued tasked work for the Office of River Protection (ORP) to expand glass compositional regions accessible for low-activity waste (LAW) and high-activity waste (HLW) vitrification processing. Experimental work continued in four primary technical areas focused on processing and performance of glasses relevant to the Hanford missions. The data and results from this work will be used to expand and validate the glass models being developed at Pacific Northwest National Laboratory (PNNL) for waste processing and acceptance. This report summarizes the activities and deliverables associated with work performed in FY24.

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DOE OSTI2024

Compositional Variation Tests on DuraMelter 100 with LAW Sub-Envelope B1 Feed in Support of the LAW Pilot Melter, VSL-02R62N0-5, Rev. 0 (May 2003)

The principal objective of the DM100 tests was to demonstrate the robustness of the vitrification process with respect to feed and glass compositional changes resulting from variations in the simulant-to-additive ratio. The DM100-WV unit was selected for these tests; this melter was used for all of the Part B 1 tests on LAW Envelopes A, B, and C sulfate incorporation that were used to support the subsequent tests on the Pilot Melter as well as for the more recent LAW Sub-Envelope Al, A2, A3 and Cl tests. The same melter was selected for the present tests in order to maintain comparisons between the data sets. In addition, the somewhat smaller glass volume for the same melt surface area as compared to the DM100-BL melter means that more glass turnovers are achieved for a given test duration. The DM100 tests used nominal feed and feed with a 15% surplus in waste simulant. Previous Pilot Melter tests on Envelope A with 10% variations (but with sulfate removal) showed significant impacts on glass production rates that were ultimately corrected by adjustments in the sugar additions. Consequently, robustness with respect to throughput as well as sulfate tolerance are important motivations for these tests.

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DOE OSTI2024

Regulatory Testing of RPP-WTP HLW Glasses to Support Delisting Compliance, VSL-04R4780-1, Rev. 0 (Sep 2004)

The primary goal of the testing described in this report was to collect data to demonstrate compliance of the immobilized high-level waste (IHLW) glasses with delisting requirements. The collected data will be used to support a petition to delist the IHLW glasses destined for the national disposal facility. The Delisting Data Quality Objectives (DQO) (Cook and Blumenkranz 2003) identified a list of (16) inorganic constituents of potential concern (COPCs) and their associated limits for delisting. These COPCs can be divided into three groups, Cases 1, 2, and 3, based on their Toxicity Characteristic Leaching Procedure (TCLP) responses versus their respective delisting limits. To briefly summarize, Case 1 COPCs are those that, when loaded at their highest expected concentration in Waste Treatment Plant (WTP) glasses, are not expected to leach at their respective delisting limits when the glasses are exposed to the TCLP. Case 2 COPCs may reach the delisting limits in TCLP leachates of WTP glasses if loaded to concentrations near their maximum expected concentrations in glass. Finally, Case 3 COPCs are components that are likely to be present in concentrations sufficient to exceed their respective delisting limits in TCLP leachates of some possible glasses. The test objective was to show that, for (i) the expected range of inorganic contents in the waste feed to the Hanford WTP high level waste (HLW) vitrification facility, (ii) the expected range of glass product compositions, and (iii) the Case 1 and Case 2 COPCs identified by the DQO, the IHLW glasses meet all the relevant requirements for delisting. For Case 3 COPCs (i.e., Cd), the testing was to demonstrate the relationship between glass composition and TCLP cadmium (Cd) release, and then employ the results to develop TCLP-composition response models. During WTP operations, TCLP-composition models can be used to predict, within the required statistical uncertainties, TCLP responses of IHLW production glasses that are within the compositional region used to develop the model.

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DOE OSTI2024

Organic Evaporation, Oxidation, and Hydrolysis Testing in Support of Hanford Sample-and-Send

The Hanford site has approximately 54 to 56 million gallons of radioactive mixed waste stored in 156 unretrieved underground storage tanks. The Hanford Waste Treatment and Immobilization Plant (WTP) is being built to treat and immobilize the tank waste. The baseline method for immobilization of Low Activity Waste (LAW) through the WTP is vitrification, but additional immobilization capacity is needed to supplement the initial LAW melters. An alternative cementitious waste form is being investigated for that future immobilization method. However, one impediment to a cementitious waste form is the presence of Land Disposal Restricted (LDR) organic chemicals in tank waste, which are regulated on a concentration based standard in the final waste form. Hence, if the quantity of organics in LAW is high enough, they must be destroyed or removed to make a waste form compatible with disposal in a mixed low level waste landfill. This work evaluates potential avenues for treatment of LDR organics to eliminate the impediment and permit possible use of a cementitious waste form. Vacuum evaporation testing to remove LDR organics consisted of preparing a non-radioactive LAW simulant, spiking that simulant with organic chemicals, and evaporating the mixture via differential distillation. The apparatus was a laboratory-scale vacuum evaporator operated at 60 ±5 torr absolute (vacuum evaporation). The LAW simulant represented the liquid expected to be retrieved from the Hanford tank farms at approximately 4.0 M [Na+] total sodium ion concentration. The concentration of the organic chemicals added was significantly higher than typically found in the tank waste samples since the higher levels were necessary to assist in analytical measurement and tracking of the spiked species.

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DOE OSTI2024

The Utility of Waste Tank Historical Reviews in Bulk Waste Removal Operations at the Savannah River Site – 25271

SRMC is actively working to remove, treat, and dispose radioactive waste generated by the separation facilities at SRS since their initial operations in the 1950s. The separation facilities at SRS have produced nuclear materials for a variety of purposes, particularly national defense, and continue to support the disposition of spent fuel through the Accelerated Basin Deinventory program. In almost 70 years of operation, nearly 625,000 m3 (165 million gallons) of radioactive waste have been generated and transferred to the tank farm facilities at SRS [1]. As a result of volume reduction (e.g., evaporation) and waste solidification (e.g., vitrification), approximately 127,000 m3 (33.5 million gallons) of material remain as of June 30, 2024 [2]. This liquid waste has since been stored in 51 large underground waste tanks present on the site. These waste tanks may contain up to 4,921 m3 (1.3 million gallons) of radioactive waste each in the form of saltcake or sludge. SRMC’s contract is to treat and dispose of this waste, clean the tanks, and operationally close them. To date, 8 of the 51 waste tanks have been operationally closed. Waste retrieval and tank closure activities are ongoing in an additional 17 tanks through either operations in the field or in design [3].

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DOE OSTI2025

Annual Status Report (FY 2024): Performance Assessment for the Integrated Disposal Facility

The purpose of this Annual Summary Report (ASR) for Fiscal Year (FY) 2024 is to evaluate the continued adequacy of the Integrated Disposal Facility (IDF) Performance Assessment (PA) and Disposal Authorization Statement (DAS). This report consolidates relevant monitoring data, modeling analyses, and regulatory reviews to demonstrate a reasonable expectation that the PA objectives and performance measures will be met, as required under DOE O 435.1. The ASR follows the guidance in DOE-STD-5002-2017, which provides a framework for maintaining the validity of the DAS through periodic assessment of facility performance and compliance with waste disposal requirements. The IDF is a near-surface disposal facility designed to receive and permanently dispose of low-level waste (LLW) and mixed low-level waste (MLLW) generated from Hanford Site operations. The facility consists of two double-lined disposal cells equipped with leak detection and leachates recovery systems to ensure environmental protection. Waste planned for disposal includes vitrified low-activity waste (LAW) and solid secondary waste (SSW) from the Hanford Waste Treatment and Immobilization Plant (WTP). At the end of FY 2024, the IDF had not yet received any waste, as it remains in a pre-operational state. Disposal activities will begin with the hot commissioning of the WTP LAW Vitrification Facility using the Direct-Feed Low-Activity Waste (DFLAW) approach in Calendar Year (CY) 2025. This ASR justifies the continued adequacy of the PA and DAS by reviewing key documents and data sources. these sources are listed in Table A-2 in Appendix A.4): The Operating Disposal Authorization Statement (ODAS) for the IDF (DOE-EM, 2021) remains in effect, with no outstanding conditions or key issues affecting its implementation. Based on the comprehensive review of PA analyses, monitoring data, and regulatory compliance activities, this ASR concludes that the IDF remains in compliance with DOE O 435.1, and there is reasonable assurance that the PA performance objectives will be met once disposal operations commence in CY 2025.

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DOE OSTI2025

FY24 Development of Improved Grout Waste Forms for Alternative Low Activity Waste Treatment

Since the WTP Low Activity Waste (LAW) Vitrification Facility was not designed to process the entire inventory of Hanford LAW, up to half of the retrieved Hanford LAW will require supplemental immobilization. Immobilizing LAW in a cementitious waste form known as Cast Stone has been investigated as a possible candidate supplemental immobilization technology. In FY21, Washington River Protection Solutions, LLC (WRPS) tasked Atkins and the Vitreous State Laboratory (VSL) of The Catholic University of America (CUA) to perform testing to evaluate methods for reducing the release of COCs, particularly nitrate, 99Tc, and 129I, from cementitious waste forms made from aqueous LAW derived from Hanford Tank Waste. FY22 work built on the FY21 results and further developed formulations while targeting higher waste loadings. The objective of this work was to perform laboratory-scale testing to further refine the most promising formulation(s) that were identified in the FY23 work. The goal of the refinement was to further reduce the release rates for 99Tc, Cr, 129I, and nitrate while maintaining workability of the fresh grout, and to increase waste loading.

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DOE OSTI2025

FY22 Development of Improved Grout Waste Forms for Supplemental Low Activity Waste Treatment

About 54 to 56 million gallons of radioactive mixed waste is currently stored in underground tanks at the United States Department of Energy’s (DOE’s) Hanford site in the State of Washington. This waste will be separated into low- and high activity waste fractions, which will then be vitrified respectively into Immobilized Low Activity Waste (ILAW) and Immobilized High Level Waste (IHLW) products for subsequent disposal. The ILAW product will be disposed of in an engineered facility at the Hanford site while the IHLW product is designed for acceptance into a national deep geological disposal facility for high level nuclear waste. Treatment of the tank waste will take place in the Hanford Tank Waste Treatment and Immobilization Plant (WTP), which is under construction. However, since the WTP Low Activity Waste (LAW) Vitrification Facility was not designed to process the entire inventory of Hanford LAW, up to half of the retrieved Hanford LAW will require supplemental immobilization. Immobilizing LAW in a cementitious waste form known as Cast Stone has been investigated as a possible candidate supplemental immobilization technology

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DOE OSTI2025

FY25 Organic Evaporation Testing in Support of Hanford Sample-and-Send

The Hanford Waste Treatment and Immobilization Plant (WTP) is being built to treat and immobilize the approximately 56 million gallons of radioactive mixed waste stored in 156 underground storage tanks. The baseline method for immobilization of Low-Activity Waste (LAW) is vitrification, but additional immobilization capacity is needed to supplement the initial LAW melters. Additionally, efforts are being undertaken to accelerate the disposition of Pre-Treated Waste (PTW) in Hanford’s West Area. An alternative cementitious waste form is being investigated as an alternative immobilization method. However, one impediment to a cementitious waste form is the presence of Land Disposal Restricted (LDR) organic chemicals in tank waste, which are regulated on a concentration-based standard in the final waste form. Hence, if the quantity of organics in PTW and LAW is high enough, treatment may be needed to destroy or remove said organics to make a waste form compatible with disposal in a mixed low level waste landfill. This work evaluates evaporation as a potential avenue for treatment of LDR organics to eliminate the impediment and permit possible use of a cementitious waste form.

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DOE OSTI2025

Affinity of LDR Organics to Cementitious Materials and Activated Carbon

The Hanford site stores approximately 56 million gallons of radioactive and hazardous waste in underground storage tanks. The current low-activity waste (LAW) vitrification facility does not have the capacity to immobilize all of the LAW. Therefore, cementitious waste forms are being evaluated as a cost-effective supplemental waste treatment, focusing on the solidification/immobilization of Land Disposal Restricted (LDR) organics, which is currently not recognized by the Environmental Protection Agency (EPA) as a standard treatment method (40 CFR 268.42). Previous efforts by the EPA and waste management agencies have highlighted the potential for cementitious materials to retain certain organic species through physical (encapsulation) and chemical (sorption) interactions.

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