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DOE OSTI2020

Product consistency test results for the LAW Phase 4 gases

In this report, the Savannah River National Laboratory provides chemical analysis of Product Consistency Test (PCT) leachates from a series of simulated nuclear waste glasses fabricated at the Pacific Northwest National Laboratory (PNNL). The series included quenched and canister-centerline cooled (CCC) versions of the glasses. The resulting data will be used in the development of enhanced property/composition models for waste vitrification at Hanford. For some of the glass leachates, minor scatter among the triplicate values of some analytes were observed. For other leachates, there were more significant differences among the triplicate values. A review of the PCT data noted that there was little difference between the normalized values based on targeted or measured glass composition. Several of the study glasses have normalized concentration of element “i” (NCi) values that are greater than the Hanford Tank Waste Treatment and Immobilization Plant immobilized low-activity waste constraint of 4 g/L for boron (B), sodium (Na), and silicon (Si). The results of these glasses will help ensure the ability of advanced glass performance models to appropriately predict acceptable compositions. For the study glasses with NCi values exceeding 4 g/L, the CCC heat treatment samples had generally lower NCi values than quenched samples. The samples of the Environmental Assessment (EA) reference glass included with each PCT set had generally consistent NCi values. The release rates for boron (B), potassium (K), lithium (Li), sodium (Na), and silicon (Si) were highly correlated for the study glasses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Crystalline Silicotitanate Batch Contact Testing with Ba, Ca, Pb, and Sr

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 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. Processing of actual tank waste supernate showed effectively complete uptake of Sr and Ba by CST and significant uptake of Ca. Further, Campbell et al. (2019) analyzed CST post-column testing and found significant (>1E-2 mmoles/g) uptake of Ca and Pb along with some Ba, Cd, Fe, Sr, and U. This led to concern that selected metals, particularly the +2 cations, Ca, Sr, Ba, and Pb may be consuming Cs exchange sites and possibly reducing CST capacity for Cs. Exchange of +2 cations was assumed to be associated with the M(OH) + species for the metal (M) ion in the caustic solution. A series of batch contact testing was conducted to evaluate the exchange behavior of Ba, Ca, Pb, and Sr onto CST. The Cs exchange behavior was also tested as a benchmark for direct comparisons. The CST was provided in the sodium form by Honeywell UOP, as IONSIV TM R9140-B, Lot 2002009604, 18 x 50 mesh. A <30-mesh aliquot was collected to match the sieve fraction expected for use in upcoming small column test configurations. Kinetic exchange rate and isotherms were measured at metal concentrations benchmarked from the AP-107 tank waste feed composition and as limited by the metal solubility in the alkaline solution. Two simplified matrices were tested: 1) 1.0 M NaOH/4.6 M NaNO 3 and 2) 0.1 M NaOH/5.5 M NaNO 3 ; these matrices represented the expected 5.6 M Na concentration of process feed and served to address the hydroxide concentration effect on exchange behavior.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Spent Crystalline Silicotitanate Storage Study—Post AP-105DF Processing

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Spent Crystalline Silicotitanate Storage Study—Post AP-105DF Processing

A Tank-Side Cesium Removal (TSCR) system is under development by Washington River Protection Solutions 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. Tank waste supernate will be filtered to remove suspended solids and then Cs will be removed by processing it through crystalline silicotitanate (CST) ion exchange media manufactured by Honeywell UOP, LLC. 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 after undetermined storage time. Previous testing with AP-105 simulant showed that rinsing the CST bed with 3 bed volumes (1.4 apparatus volumes [AVs]) of 0.1 M NaOH resulted in a dried bed that maintained flow characteristics indicative of ease of recovery. This study explored the intermediate conditions (between feed dried in place and the 1.4 AVs of 0.1 M NaOH rinse) to evaluate CST bed properties after: 1) stoppage with feed in place; 2) stoppage after draining feed; 3) stoppage after 0.7 AV of 0.1 M NaOH rinse through column; 4) stoppage after 1.5 AVs of 0.1 M NaOH rinse through column. Post processing, each column was heated at 50 °C for 19 days under pseudo-storage conditions to simulate the expected dried and stored CST bed conditions. Testing was conducted at the small scale (12-mL bed volume); actual, Cs-depleted, AP-105 tank waste was used as the feed. Post-dried CST bed physical properties (angle of repose and penetration depth) were measured to evaluate how CST moved and flowed. All process stop-conditions resulted in a solidified CST bed except for the final condition, 1.5 AVs of 0.1 M NaOH rinse. At this small scale, the three CST beds presented an issue for retrievability after the short storage period (19 days at 50 °C). The latter case confirmed the results from simulant testing. The testing was intended to provide a preliminary assessment of issues that may arise from desiccation of CST during storage with the indicated salt solutions in place. Since these were small-scale tests, the processing system did not scale to full scale conditions exactly; however, the tests did provide insight into the impact on the dried and stored CST bed after stopping processing at an earlier step (upset condition) than normal. These results indicate that if an upset condition occurs at TSCR, a dilute hydroxide rinse should be considered before the CST dries from internal heating.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Combined Technologies for In Situ Remediation of Tc-99 and U in Subsurface Sediments

In this study, combinations of chemical remedies were tested in bench-scale batch experiments to evaluate a two-step reduction-sequestration approach to effectively stabilize high concentrations of inorganic contaminant mixtures. Bench tests simulated contaminant and geochemical conditions of a perched aquifer located within the Central Plateau at the Hanford Site, located in southeastern Washington State (USA). Pairwise combinations of a reductant [e.g., zero valent iron, sulfur modified iron (SMI), or calcium polysulfide] and a sequestering agent [e.g., calcite, apatite, or dilute alkaline solution (e.g., NaOH)] were evaluated for immobilization and stabilization of technetium (Tc) (50,000 pCi/L), uranium (U) (150 mg/L), and nitrate (NO 3 ) (200 mg/L) in high ionic strength groundwater. The results of these batch studies demonstrated that reduction by SMI and sequestration in apatite or calcite are the most effective combination for these contaminant mixtures and conditions. Aqueous concentrations of Tc and U decreased by 95.6% ± 2.5% and 101.1% ± 5.2%, respectively, with SMI-apatite and 98.3% ± 0.0% and 101.2% ± 5.2%, respectively, with SMI-calcite. Sequential extractions showed that sequestered contaminants had limited capacity for re-oxidation; in fact, less than 10% of immobilized Tc and U was recovered by selective extraction of mineral phases most susceptible to oxidation. In addition, X-ray absorption near edge structure analysis of the sediment samples treated with SMI-calcite showed the presence of only U(IV), while both U(IV) and U(VI) were present in the SMI apatite combination [ratio of 0.43 U(IV):0.59 U(VI)].This study describes preliminary results that a two-step approach for stabilizing contaminant mixtures of long-lived radionuclides can be effective at reducing contaminant fluxes to groundwater from vadose and perched water zones.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

An Intensified Electro-Catalytic Process for Production of Formic Acid from Power Plant CO 2 Emissions (Final Technical Report)

The goal of this project was to develop and test a novel electro-catalytic method for the production of high-value formic acid from coal-derived CO 2 as a strategy to offset the cost of CO 2 capture. Formic acid is currently produced from the conversion of higher-order carbon products such as methane and/or methanol. This electro-catalytic CO 2 reduction process utilizes a highly selective catalyst in a flow-through reactor design to maximize the formic acid production rate. The specific objectives of this proposed study were to; 1) produce and screen highly selective engineered CO 2 reducing catalysts capable of exclusively producing formic acid; 2) immobilize the catalyst within a flow process to continually produce formic acid and increase catalyst lifetime; and 3) assess the stability of the electrocatalyst during long-term operation. The project involved the development and testing of an engineered catalyst to selectively reduce CO 2 directly and exclusively to formic acid. After the best-performing catalyst was selected, it was immobilized and tested inside a flow-through reactor at UK CAER using realistic conditions expected from CO 2 produced during coal combustion and separated by a CO 2 capture plant.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2022

Colloid-Facilitated Actinide Transport in a Cementitious-Impacted SRS Groundwater

The objective of this report is to provide a literature review relevant to the question of whether colloid facilitated transport of plutonium is enhanced in a cementitious groundwater system on the Savannah River Site (SRS). Contaminant transport is commonly described as taking place in a system with a mobile aqueous phase and an immobile solid phase. There has been an increasing awareness of a third phase, a mobile solid phase, also referred to as a mobile colloidal phase. Mobile colloids consist of organic and/or inorganic submicron-particles that move with groundwater flow. When radionuclides are associated with the mobile colloids, the net effect is that radionuclides can move faster through the subsurface system than would be predicted by transport models that do not include mobile colloids. It is important to distinguish between subsurface colloids and subsurface mobile colloids. The subsurface environment includes an enormous reservoir of colloids, but only a tiny fraction, if any, are mobile. Mobile colloid formation is commonly described as involving a three-step process: genesis, stabilization, and transport. It was concluded that there is a strong likelihood that submicron colloids of plutonium exist near the source term, (i.e., the genesis step is likely completed). While such particles have not been directly detected, it is highly likely that plutonium could either attach to submicron particles in the sediment or that submicron plutonium fragments exist at the source. However, the tendency for these plutonium colloids to move in the SRS subsurface is extremely low, especially in engineered cementitious environments where the ionic strength of the solution and the elevated concentrations of divalent cations greatly curtails colloid suspension stability (i.e., the stabilization step is likely not completed). Together these data strongly indicate that plutonium-bearing colloids would likely exist in the near field of a tank closure facility, but the colloids would be unlikely to be mobile, thereby providing a vector for enhanced transport. Under cementitious leachate impacted groundwater conditions, it is reasonable to assume plutonium transport occurs primarily as a two-phase system, a mobile aqueous phase and an immobile solid phase.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Preliminary IHLW Formulation Algorithm Description

This report documents the initial algorithm that could be used by the Waste Treatment and Immobilization Plant (WTP) in batching high-level waste (HLW) and glass-forming chemicals (GFCs) in the HLW melter feed preparation vessel (MFPV) (HFP-VSL-00001 and -00005). Not all Hanford tank waste can be accommodated by the models developed for this report and significant expansion of the model boundaries could be achievable to reduce the WTP mission life and total canister production count. The immobilized HLW (IHLW) must meet a series of constraints to be acceptable for disposal in the Monitored Geologic Repository, which are contained in the Specification 1 of the Contract (DOE 2000), the Waste Acceptance Product Specifications (WAPS, DOE 1996), and the Waste Acceptance System Requirements Document (WASRD, DOE 2007). The IHLW Waste Form Compliance Plan (WCP, 24590-HLW-PL-RT-07-0001, Rev 3) specifies that the formulation algorithm will be developed and used to comply with the constraints associated with glass composition and properties. This report is not an engineering calculation, does not provide design input, and is not an engineering study. Algorithm inputs include the chemical analyses of the blended HLW in the HLW blend vessel (HBV) (HLP-VSL-00028, the volume and composition of the MFPV heel, the volume and composition of the MFPV after waste addition, the volume and composition of MFPV batch after GFC addition, the compositions of individual GFCs, and the mass of glass in each canister. In addition to these inputs, uncertainties in the HLW composition and processing parameters are included in the algorithm. Using the above inputs, the algorithm calculates the following outputs: 1) the volume of HLW to be transferred from the HBV to the MFPV, 2) the mass of each GFC for addition to the MFPV, 3) the composition of the glass that will be produced along with uncertainties, and 4) the predicted properties, with associated uncertainties, of the resulting IHLW. The algorithm uses the property-composition models to calculate properties with associated uncertainties and compares them with various constraints to ensure that a processable feed is formulated and a compliant IHLW is produced. The GFC additions are determined using an optimization approach to provide high confidence that the HLW glass will meet all product quality requirements and key processing constraints. For most HLW batches there are many possible glass compositions that meet all constraints. In these cases, the glass composition is optimized for a series of target component concentrations and target property values. The algorithm also incorporates process measurement and product quality uncertainties, based on the work of Piepel et al. (2005). Estimates of the various process and measurement uncertainties that affect glass compositions and predicted glass properties have been previously reported (Piepel et al. 2005, 2006) and the impacts of these estimated uncertainties on the IHLW composition envelope that meets product quality and processing-related properties with sufficient confidence were evaluated. The details of work performed to date to develop this initial GFC addition and batching algorithm are summarized in Sections 4 and 5. An example data set is used to illustrate the calculations of the algorithm summarized in Section 6. Finally, in Section 7, there is a statement of the required work to achieve a final operational IHLW formulation control algorithm. This report is not an engineering calculation, does not provide design input, and is not an engineering study.

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DOE OSTI2022

Fabrication of Biofunctionalized PVA/PEI Nanofibers for Rare Earth Element Extraction from Coal Mine Tailings

The need for rare earth elements (REEs) for new technology is becoming increasingly stiff with demand at a record high. Biological ligands like lanmodulin and lanthanide binding tags (LBT) have gained noticeable attention for their selective extraction of valuable lanthanide metals in aqueous solution. Building on previous work using microbeads as the extraction media, we propose that nanofibers can improve extraction capabilities. Nanofibers could provide more efficient flow and higher extraction yields due to their high surface area to volume ratio. Relying on thiolmaleimide click chemistry as the biological ligand immobilization route, electrospinning as the nanofiber manufacturing method, and numerous characterization techniques, we produced electrospinning polymer solutions and nanofibers with a maximum neodymium adsorbent capacity of 12.1 μmol/g of extraction media immobilized with LBT. Although the prior work produced an extraction media with an equivalent capacity of ~40 μmol/g, the electrospinning process is much more economical and scalable. This work paves the way for an industrially relevant, environmentally-friendly REE extraction material. Further work is required to produce higher quality nanofibers, to investigate common ion interference with REE adsorbance, and to scale production up to a relevant scale.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2023

Characterization and Recovery of Critical Metals from Municipal Solid Waste Incineration Ashes

The dependence on international supplies and lack of diverse supplies of critical materials (such as rare earth elements, REEs) have prompted the US to explore new sources and develop environmentally friendly technologies for critical metal extraction, processing, and manufacturing. Secondary wastes have been explored for the recovery of REEs. Municipal solid waste (MSW) is a large solid waste stream and may constitute the largest resource for REEs and other critical metals; yet its incineration ashes (MSWI ashes) have received limited attention in terms of critical metal recovery. On the other hand, management of MSWI ashes also presents significant challenges both operationally and financially, such as landfill costs, volume reduction, and contaminant immobilization. To address the challenges associated with the management of and resource recovery from MSWI ashes, this project developed a closed-loop, integrated, scalable, and environmentally friendly waste management and resource recovery system. This system is characterized with maximum recovery of REEs, production of additional salable products, minimal production of secondary waste, and high immobilization of heavy metal contaminants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Assessment of Amine-Based CO2BOLs for Direct Air Capture

Direct air capture (DAC) technologies extract CO 2 from the atmosphere for CO 2 storage, or utilization. Capturing CO 2 from the air is the most expensive application of carbon capture because CO 2 in the atmosphere is very dilute. There are limited number of CO 2 capture technologies for DAC application. This project aims at developing an energy efficient technology for DAC, leveraging two PNNL’s chemistries (solid and liquid CO 2 capture). Three CO 2 capture sorbents consisting of amine based CO 2 BOLs immobilized in mesoporous silica were designed, synthesized, and tested. These sorbents had ~ 19-23 wt.% amine loadings which is lower than typical amine-based silica sorbents. The surface area and pore volumes of these solid supported CO 2 BOLs are lower compared to those of the pristine silica support. The CO 2 capture performance of these materials was significantly lower than the typical silica supported amines due to low amine loading and higher molecular weight with low amine density. These results show that immobilize CO 2 BOLs in silica are not viable materials for removing CO 2 from ambient air. This project also designed, synthesized at tested liquid solvents for DAC application. Solvent properties that is vapor pressure, CO 2 uptake capacity, kinetics, and viscosity for three novel solvents were evaluated. The CO 2 uptake capacity for one of the most promising amine-based solvent BEPBEGDA was the highest at 13.2 wt% corresponding to 97 mol%. The vapor pressure of the BEPBEGDA solvents were very low at 80 °C compared to other solvents making them suitable for DAC application. The effect of humidity on the CO 2 capture performance of these solvents was evaluated which shows that presence of moisture doesn’t have a negative effect on the CO 2 uptake performance but makes it slightly better. The performances of these solvents were slightly below that of the 0.1M NaOH solution tested under similar conditions. Despite of the slightly lower CO 2 uptake, it is expected that these liquid solvents will have lower regeneration temperature and minimum evaporative losses due their low vapor pressure. Future work will focus on optimization of the liquid solvents for DAC application to improve both CO 2 capture efficiency and capacity without viscosity and vapor pressure increase. Testing of these solvents under DAC conditions using a gas liquid contactor that mimic industrial applications is needed. Solvent cost projection, techno-economic analysis and life cycle analysis are required to evaluate economic viability of this technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Mitigating cerium migration for perfluorosulfonic acid membranes using organic ligands

Improving the electrochemical stability of proton exchange membranes is a pressing priority for heavy-duty fuel cell vehicles. The lifetime of the most widely used perfluorosulfonic acid membranes is limited by reactive free radicals generated inside the system. Cerium has been found to reduce the chemical degradation of the membranes. However, cerium migration during fuel cell operation limits the chemical durability enhancement effect expected from the radical scavenging activity of cerium. Here we investigate a wide range of organic immobilizers for cerium, measuring their suitability concerning cerium retention, radical scavenging activity, and fuel cell performance. We report that partially fluorinated phosphonic acids enhance cerium retention up to 45 times and reduce fluoride emission rate by 38% compared to the commercial Nafion™ XL membrane pre-impregnated with cerium. The energetics of cerium-phosphonic acid complex systems by density functional theory calculations rationalizes effective cerium immobilization.

30 DIRECT ENERGY CONVERSION↗

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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Device and Method for Parallel Measurement of Phosphoproteome and Proteome from Single Cells

We present the development of an immobilized metal affinity chromatography (IMAC) chip designed to enable nanoscale phosphopeptide enrichment within microfabricated nanowells. This novel platform leverages surface chemistry to immobilize high-density Nickel-Nitrilotriacetic Acid (Ni-NTA) molecules on nanowells, followed by applying Fe 3+ . The nanowell surface serves as a capture media to enrich phosphopeptides based on IMAC. The system's efficiency was validated using ß-casein as a model protein, demonstrating the chip’s capability to significantly enrich phosphopeptides. Future applications of this technology are anticipated to enable the detection of over 100 phosphopeptides from individual cells and more than 500 phosphopeptides from pools of 100 cells, offering exciting potential for single-cell phosphoproteomics. We will next apply an integrated proteomics workflow to perform multi-omics measurements, including single-cell isolation, protein digestion, and phosphopeptide enrichment, followed by LC-MS analysis of both the global proteome and phosphoproteome. Future research will explore the use of this technology to study phosphorylation dynamics in cancer cells, enhancing our understanding of cellular signaling and disease mechanisms.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Portable fiber optic sensor for rare earth elements and other critical metals using photoluminescence methods

Rare earth elements and other metals are vital to a range of technologies that are used in the energy and defense sectors. However, monopolistic market conditions have caused significant concern over the stability of the critical metal supply chain, and this has spurred extensive efforts in many nations to produce these metals domestically, both from conventional sources such as mining and well as from unconventional sources such as coal and its utilization byproducts. Slow and expensive characterization methods pose a significant barrier for both metals prospecting and process monitoring. A promising solution to this challenge is the development of highly sensitive luminescent sensors for metals, which can offer low costs, portability, and sensitivity. Anionic zinc adeninate metal-organic frameworks (BioMOFs) are known to distinguishing and detect part-per-billion levels of terbium, europium, samarium, and dysprosium in water by sensitizing the narrow, element-specific emission bands from these lanthanides. Here, a BioMOF material is immobilized onto a large diameter, solarization-resistant fiber optic tip integrated with a portable, low-cost spectrometer for rare earth element sensing. Immobilizing the sensing material on fiber instead of dispersing the sensing material in solution offers several advantages: it facilitates solvent removal, which enhances luminescent signal from the sensitized lanthanides, and it also allows the BioMOF to be recycled for multiple uses. The sensing system was deployed on a simulated process stream and exhibited qualitative agreement with inductively-coupled plasma mass spectrometry for terbium and europium detection, highlighting the potential for the sensing system to be deployed for real-world applications. By using different sensing materials, the same portable sensor may be deployed to detect other energy relevant metals such as cobalt, providing a cost-effective and sensitive platform for critical metal characterization.

Crawford, Scott↗

DOE OSTI2024

ILAW Container Cost Reduction and Optimization Study

This study, performed on behalf of Washington River Protection Solutions (WRPS), examines the potential for making cost savings for the Immobilized Low Active Waste (ILAW) containers over the mission life of the Waste Treatment and Immobilization Plant (WTP). it builds on earlier study assessments 24590-LAW-RPT-M-01-001 Rev 0 ILAW Product Container Specifications Optimization Study and DOE/ORP-2013-02 Rev 0 Decision Analysis of Low-Active Waste Container Finishing Handling System Alternatives. The WTP design and installed equipment has evolved over an extended period ~20 years. Consequently, some of the existing requirements relating the ILAW containers may no longer be applicable under current mission plans where the glass filled containers are placed into the Integrated Disposal Facility (IDF) rather than stacked in an engineered purpose-built ventilated store as originally envisioned. The study team reviewed available WTP project reference documents to establish the functions the container must perform and assign requirements against each of these functions. With the assumptions that some of the existing WTP contract restrictions would not necessarily apply to the subsequent facility operations contract the container requirements were reviewed to identify those which were ‘hard constraints‘, imposed by regulatory requirements. Initially each of these hard constraints were reviewed, evaluated and documented to see if they precluded the use of an alternate less expensive material of construction, carbon steel, to the existing 304 L stainless steel in the current container specification. That review did not generate any fatal flaws for a change in material of construction to carbon steel allowing the study team to examine the impacts of material cost savings, potential changes to the design and requirements and impacts on interfaces of the containers with the existing WTP process equipment from container receipt, transfers, glass filling, cooling and export. In addition, a change in container target fill level was evaluated and qualitative, and quantitative where feasible, impacts to the container fabrication process assessed. Lastly, additional follow on development or testing activities to support the use of carbon steel were assessed and a recommended path forward with a ROM cost and timescale developed.

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