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DOE OSTI2014

Development of iron phosphate ceramic waste form to immobilize radioactive waste solution

The objective of this research was to develop an iron phosphate ceramic (IPC) waste form using converter slag obtained as a by-product of the steel industry as a source of iron instead of conventional iron oxide. Both synthetic off-gas scrubber solution containing technetium-99 (or Re as a surrogate) and LiCl-KCl eutectic salt, a final waste solution from pyrochemical processing of spent nuclear fuel, were used as radioactive waste streams. The IPC waste form was characterized for compressive strength, reduction capacity, chemical durability, and contaminant leachability. Compressive strengths of the IPC waste form prepared with different types of waste solutions were 16 MPa and 19 MPa for LiCl-KCl eutectic salt and the off-gas scrubber simulant, respectively, which meet the minimum compressive strength of 3.45 MPa (500 psi) for waste forms to be accepted into the radioactive waste repository. The reduction capacity of converter slag, a main dry ingredient used to prepare the IPC waste form, was 4,136 meq/kg by the Ce(IV) method, which is much higher than those of the conventional Fe oxides used for the IPC waste form and the blast furnace slag materials. Average leachability indexes of Tc, Li, and K for the IPC waste form were higher than 6.0, and the IPC waste form demonstrated stable durability even after 63-day leaching. In addition, the Toxicity Characteristic Leach Procedure measurements of converter slag and the IPC waste form with LiCl-KCl eutectic salt met the universal treatment standard of the leachability limit for metals regulated by the Resource Conservation and Recovery Act. This study confirms the possibility of development of the IPC waste form using converter slag, showing its immobilization capability for radionuclides in both LiCl-KCl eutectic salt and off-gas scrubber solutions with significant cost savings.

converter slag↗

DOE OSTI2015

Transforming growth factor-beta1 promotes the migration and invasion of sphere-forming stem-like cell subpopulations in esophageal cancer

Esophageal cancer is one of the most lethal solid malignancies. Mounting evidence demonstrates that cancer stem cells (CSCs) are able to cause tumor initiation, metastasis and responsible for chemotherapy and radiotherapy failures. As CSCs are thought to be the main reason of therapeutic failure, these cells must be effectively targeted to elicit long-lasting therapeutic responses. We aimed to enrich and identify the esophageal cancer cell subpopulation with stem-like properties and help to develop new target therapy strategies for CSCs. Here, we found esophageal cancer cells KYSE70 and TE1 could form spheres in ultra low attachment surface culture and be serially passaged. Sphere-forming cells could redifferentiate and acquire morphology comparable to parental cells, when return to adherent culture. The sphere-forming cells possessed the key criteria that define CSCs: persistent self-renewal, overexpression of stemness genes (SOX2, ALDH1A1 and KLF4), reduced expression of differentiation marker CK4, chemoresistance, strong invasion and enhanced tumorigenic potential. SB525334, transforming growth factor-beta 1(TGF-β1) inhibitor, significantly inhibited migration and invasion of sphere-forming stem-like cells and had no effect on sphere-forming ability. In conclusion, esophageal cancer sphere-forming cells from KYSE70 and TE1 cultured in ultra low attachment surface possess cancer stem cell properties, providing a model for CSCs targeted therapy. TGF-β1 promotes the migration and invasion of sphere-forming stem-like cells, which may guide future studies on therapeutic strategies targeting these cells. - Highlights: • Esophageal cancer sphere-forming cells possess cancer stem cell properties. • Sphere-forming cells enhance TGF-β1 pathway activity. • TGF-β 1 inhibitor suppresses the migration and invasion of sphere-forming cells.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2017

Analysis of nucleon electromagnetic form factors from light-front holographic QCD: The spacelike region

We present a comprehensive analysis of the space-like nucleon electromagnetic form factors and their flavor decomposition within the framework of light-front holographic QCD. We show that the inclusion of the higher Fock components $|{qqqq\bar{q}}$ has a significant effect on the spin-flip elastic Pauli form factor and almost zero effect on the spin-conserving Dirac form factor. We present light-front holographic QCD results for the proton and neutron form factors at any momentum transfer range, including asymptotic predictions, and show that our results agree with the available experimental data with high accuracy. In order to correctly describe the Pauli form factor we need an admixture of a five quark state of about 30$\%$ in the proton and about 40$\%$ in the neutron. We also extract the nucleon charge and magnetic radii and perform a flavor decomposition of the nucleon electromagnetic form factors. The free parameters needed to describe the experimental nucleon form factors are very few: two parameters for the probabilities of higher Fock states for the spin-flip form factor and a phenomenological parameter $r$, required to account for possible SU(6) spin-flavor symmetry breaking effects in the neutron, whereas the Pauli form factors are normalized to the experimental values of the anomalous magnetic moments. As a result, the covariant spin structure for the Dirac and Pauli nucleon form factors prescribed by AdS$_5$ semiclassical gravity incorporates the correct twist scaling behavior from hard scattering and also leads to vector dominance at low energy.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2017

Alternative High-Performance Ceramic Waste Forms

This final report (M5NU-12-NY-AU # 0202-0410) summarizes the results of the project titled “Alternative High-Performance Ceramic Waste Forms,” funded in FY12 by the Nuclear Energy University Program (NEUP Project # 12-3809) being led by Alfred University in collaboration with Savannah River National Laboratory (SRNL). The overall focus of the project is to advance fundamental understanding of crystalline ceramic waste forms and to demonstrate their viability as alternative waste forms to borosilicate glasses. We processed single- and multiphase hollandite waste forms based on simulated waste streams compositions provided by SRNL based on the advanced fuel cycle initiative (AFCI) aqueous separation process developed in the Fuel Cycle Research and Development (FCR&D). For multiphase simulated waste forms, oxide and carbonate precursors were mixed together via ball milling with deionized water using zirconia media in a polyethylene jar for 2 h. The slurry was dried overnight and then separated from the media. The blended powders were then subjected to melting or spark plasma sintering (SPS) processes. Microstructural evolution and phase assemblages of these samples were studied using x-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersion analysis of x-rays (EDAX), wavelength dispersive spectrometry (WDS), transmission electron spectroscopy (TEM), selective area x-ray diffraction (SAXD), and electron backscatter diffraction (EBSD). These results showed that the processing methods have significant effect on the microstructure and thus the performance of these waste forms. The Ce substitution into zirconolite and pyrochlore materials was investigated using a combination of experimental (in situ XRD and x-ray absorption near edge structure (XANES)) and modeling techniques to study these single phases independently. In zirconolite materials, a transition from the 2M to the 4M polymorph was observed with increasing Ce content. The resulting powders were consolidated via SPS. Ce was reduced to the trivalent oxidation state and the zirconolite was converted into undesirable perovskite. The zirconolite polymorphs found in the synthesized powders were recovered after a post-SPS heat treatment in air. These results demonstrated the potential of processing in controlling the phase assemblage in these waste forms. Hollandites with Cr 3+ trivalent cations were identified as potential hosts for Cs immobilization and are being investigated for Cs retention properties. Series of compositions Ba 1.15-x Cs 2x Cr 2.3 Ti 5.7 O 16 , with increasing Cs loadings, were prepared by sol-gel process and characterized for structural parameters. Structural characterization was performed by a combination of powder XRD and neutron powder diffraction. Phase pure hollandite adapting monoclinic symmetry (I2/m) was observed for 0 ≤ x ≤ 0.55. These results were used to develop a new structural model to interpret Cs immobilization in these hollandites. Performance of these waste forms were evaluated for chemical durability and radiation resistance. Product consistency testing (PCT) and vapor hydration testing (VHT) were used for testing of chemical durability. Radiation resistance was tested using He + ions to simulate $\alpha$ particles and heavy ions such as Au 3+ to simulate a recoil. These results showed that these waste forms were chemically durable. The waste forms also amorphized to various degrees on exposure to simulated radiation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1978

Survival and reversion of a stable L form in soil

The stable L form of Agromyces ramosus reverted to a bacterial form when incubated in sterilized soil. The cellular and colonial morphology of this bacterial form resembled that of the original parent bacterial form. The two forms differed, however, in that the revertant maintained its bacterial form when transferred onto a low-salt (NaCl) medium but was virtually completely induced into the L-form state on a high-salt medium. The original parent bacterial form was not sensitive to salt. The possibility is discussed that an L-form - bacterial-form cycle for this bacterium might occur naturally in soil. This cycle would be mediated by fluctuations in local salt concentrations in the soil.

Horwitz, A. H.↗

DOE OSTI2021

Bed form-induced hyporheic exchange and geochemical hotspots

Small-scale bed form topographies control hyporheic exchange and biogeochemical processes within aquatic sediments, which ultimately affect water quality and nutrient cycling at the watershed scale. The impact of three-dimensional and small-scale bed form topographies on hyporheic exchange and solute mixing is investigated in the present work. The effect of bed form morphologies on the development of zones of enhanced reaction rates (i.e., hotspots) is also studied. A computational fluid dynamics model to simulate river flow over bed forms is combined with a subsurface flow and multicomponent reactive solute transport model. A wide variety of bed form topographies are generated using geometric models by varying parameters controlling curvature as well as bed form wavelength and amplitude. The results in this research suggest that out-of-phase bed forms generate more complex hyporheic flow patterns which reduce the efficiency of solute transformations. Higher phase shifts in bed form shapes result in overall higher average velocity, larger zones of enhanced pressure and reaction rates, and higher amounts of solute exchange. Moreover, the bed form shapes control the reaction process for a wide range of sediment conductivities. Here this study advances the understanding of the effects of complex and small scale morphological features on hyporheic exchange processes including the rate and spatio-temporal distribution of reaction hotspots.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Coupling of Nuclear Waste Form Corrosion and Radionuclide Transports in Presence of Relevant Repository Sediments

Assessments of waste form and disposal options start with the degradation of the waste forms and consequent mobilization of radionuclides. Long-term static tests, single-pass flow-through tests, and the pressurized unsaturated flow test are often employed to study the durability of potential waste forms and to help create models that predict their durability throughout the lifespan of the disposal site. These tests involve the corrosion of the material in the presence of various leachants, with different experimental designs yielding desired information about the behavior of the material. Though these tests have proved instrumental in elucidating various mechanisms responsible for material corrosion, the chemical environment to which the material is subject is often not representative of a potential radioactive waste repository where factors such as pH and leachant composition will be controlled by the near-field environment. Near-field materials include, but are not limited to, the original engineered barriers, their resulting corrosion products, backfill materials, and the natural host rock. For an accurate performance assessment of a nuclear waste repository, realistic waste corrosion experimental data ought to be modeled to allow for a better understanding of waste form corrosion mechanisms and the effect of immediate geochemical environment on these mechanisms. Additionally, the migration of radionuclides in the resulting chemical environment during and after waste form corrosion must be quantified and mechanisms responsible for migrations understood. The goal of this research was to understand the mechanisms responsible for waste form corrosion in the presence of relevant repository sediments to allow for accurate radionuclide migration quantifications. The rationale for this work is that a better understanding of waste form corrosion in relevant systems will enable increased reliance on waste form performance in repository environments and potentially decrease the need for expensive engineered barriers.Our current work aims are 1) quantifying and understanding the processes associated with glass alteration in contact with Fe-bearing materials; 2) quantifying and understanding the processes associated with glass alteration in presence of MgO (example of engineered barrier used in WIPP); 3) identifying glass alteration suppressants and the processes involved to reach glass alteration suppression; 4) quantifying and understanding the processes associated with Saltstone and Cast Stone (SRS and Hanford cementitious waste forms) in various representative groundwaters; 5) investigating positron annihilation as a new tool for the study of glass alteration; and 6) quantifying and understanding the processes associated with glass alteration under gamma irradiation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2022

Friction Stir Welded Aluminum-Lithium (Al-Li) 2050 Blanks for Spin Forming

Spin forming is a metalworking process used to produce axially-symmetric parts by the application of lateral pressure from a forming tool to a circular blank mounted on a revolving, heated mandrel. This process enables production of cones, domes, or caps that can incorporate features such as flat bulkheads. Friction stir welded (FSW) Al-Li 2195 blanks have been spin formed for single-piece, launch vehicle domes up to 5 m in diameter. Al-Li 2050 plate has the advantage of availability up to 165 mm thick,whereas 2195 plate is traditionally only available up to 57 mm thick. Increased plate thickness enables greater design flexibility for machining of taller structural elements, such as stiffeners. However, 2050 is only available in plate widths up to ~3.9 m. This study demonstrated the capability of making custom 2050 blanks for spin forming large (>7.8 m in diameter), single-piece, light-weight flight articles (e.g., lunar habitats and landers) by FSW two (or more) plates together. Spin forming of welded 2050 blanks has not been attempted before this investigation. The objective was to evaluate the mechanical properties of 2050 parent material and FSW regions after spin forming and subsequent T6 heat treatment. A 3 m diameter x 38 mm thick 2050 blank was fabricated from two 1.5 m wide pieces by FSW and subsequently spin formed into a cone article. Additionally, three 1.2 m diameter x 8.1 mm thick 2050 blanks were produced by FSW and spin formed into subscale cone articles with varying strain input. Mechanical properties are reported for spin formed 2050-T6 parent material and FSW regions on the articles. Abnormal grain growth (AGG) in the FSW during heat treatment was expected based on prior experience with 2195. Implementation of an AGG suppression strategy during heat treatment reduced AGG in the FSW regions and improved ductility.

Spin forming↗

DOE OSTI2016

A Degradation Model and Testing Protocol for Metallic Waste Forms

Metallic waste forms developed to immobilize high-level radioactive wastes generated in advanced (closed) fuel cycles are being evaluated as part of the US DOE Fuel Cycle Research and Development program. The electrometallurgical reprocessing of used metallic fuels to recover U and Pu generates two waste streams: salt waste comprised of electro-refiner salt contaminated with oxidized fission products and metallic waste comprised of activated cladding and metallic fission products that were not oxidized under the processing conditions. Metallic waste forms can be made by directly melting the cladding and fuel wastes with small amounts of trim metals to form a multiphase alloy material in which radionuclides and other waste constituents are immobilized within chemically durable intermetallic and iron-based solid solution phases. Some components of the waste streams serve as important constituents of phases comprising the waste form, such as Mo and Zr, which form Fe{sub 2}Mo and Fe{sub 2}Zr intermetallic phases. Other waste constituents are accommodated as substitutional contaminants, such as Tc within the Fe{sub 2}Mo intermetallic and U/TRU within the Fe{sub 2}Zr intermetallic. Sufficient amounts of these host phases must be available to accommodate all radionuclides in the waste stream. The compositional flexibility of the host phases to incorporate waste components is being utilized to formulate metal waste forms that will accommodate variations in waste streams compositions that will occur over long-term fuel reprocessing operations. Small amounts of trim metals can be added to tailor the phase assembly to match the waste stream composition and facilitate waste form processing. For example, additional Zr may be added during waste form production to ensure all U/TRU is sequestered in a durable Fe{sub 2}Zr host phase and trim Cr, Mo, and Ni can be added to supplement the amounts provided by the steel cladding to improve the durability of a metallic waste form. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Stringy canonical forms

Canonical forms of positive geometries play an important role in revealing hidden structures of scattering amplitudes, from amplituhedra to associahedra. In this paper, we introduce “stringy canonical forms”, which provide a natural definition and extension of canonical forms for general polytopes, deformed by a parameter α'. They are defined by real or complex integrals regulated with polynomials with exponents, and are meromorphic functions of the exponents, sharing various properties of string amplitudes. As α'→ 0, they reduce to the usual canonical form of a polytope given by the Minkowski sum of the Newton polytopes of the regulating polynomials, or equivalently the volume of the dual of this polytope, naturally determined by tropical functions. At finite α', they have simple poles corresponding to the facets of the polytope, with the residue on the pole given by the stringy canonical form of the facet. There is the remarkable connection between the α'→ 0 limit of tree-level string amplitudes, and scattering equations that appear when studying the α'→ ∞ limit. We show that there is a simple conceptual understanding of this phenomenon for any stringy canonical form: the saddle-point equations provide a diffeomorphism from the integration domain to the interior of the polytope, and thus the canonical form can be obtained as a pushforward via summing over saddle points. When the stringy canonical form is applied to the ABHY associahedron in kinematic space, it produces the usual Koba-Nielsen string integral, giving a direct path from particle to string amplitudes without an a priori reference to the string worldsheet. We also discuss a number of other examples, including stringy canonical forms for finite-type cluster algebras (with type A corresponding to usual string amplitudes), and other natural integrals over the positive Grassmannian.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Preparation and characterization of multiphase ceramic designer waste forms

Abstract The long-term performance, or resistance to elemental release, is the defining characteristic of a nuclear waste form. In the case of multiphase ceramic waste forms, correlating the long-term performance of multiphase ceramic waste forms in the environment to accelerated chemical durability testing in the laboratory is non-trivial owing to their complex microstructures. The fabrication method, which in turn affects the microstructure, is further compounding when comparing multiphase ceramic waste forms. In this work, we propose a “designer waste form” prepared via spark plasma sintering to limit interaction between phases and grain growth during consolidation, leading to monolithic high-density waste forms, which can be used as reference materials for comparing the chemical durability of multiphase waste forms. Designer waste forms containing varying amounts of hollandite in the presence of zirconolite and pyrochlore in a fixed ratio were synthesized. The product consistency test (PCT) and vapor hydration test (VHT) were used to assess the leaching behavior. Samples were unaffected by the VHT after 1500 h. As measured by the PCT, the fractional Cs release decreased as the amount of hollandite increased. Elemental release from the zirconolite and pyrochlore phases did not appear to significantly contribute to the elemental release from the hollandite phase in the designer waste forms.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Structural evidence for the partially oxidized dipyrromethene and dipyrromethanone forms of the cofactor of porphobilinogen deaminase: structures of the Bacillus megaterium enzyme at near-atomic resolution

The enzyme porphobilinogen deaminase (PBGD; hydroxymethylbilane synthase; EC 2.5.1.61) catalyses a key early step in the biosynthesis of tetrapyrroles in which four molecules of the monopyrrole porphobilinogen are condensed to form a linear tetrapyrrole. Two near-atomic resolution structures of PBGD from B. megaterium are reported that demonstrate the time-dependent accumulation of partially oxidized forms of the cofactor, including one that possesses a tetrahedral C atom in the terminal pyrrole ring. The enzyme porphobilinogen deaminase (PBGD; hydroxymethylbilane synthase; EC 2.5.1.61) catalyses an early step of the tetrapyrrole-biosynthesis pathway in which four molecules of the monopyrrole porphobilinogen are condensed to form a linear tetrapyrrole. The enzyme possesses a dipyrromethane cofactor, which is covalently linked by a thioether bridge to an invariant cysteine residue (Cys241 in the Bacillus megaterium enzyme). The cofactor is extended during the reaction by the sequential addition of the four substrate molecules, which are released as a linear tetrapyrrole product. Expression in Escherichia coli of a His-tagged form of B. megaterium PBGD has permitted the X-ray analysis of the enzyme from this species at high resolution, showing that the cofactor becomes progressively oxidized to the dipyrromethene and dipyrromethanone forms. In previously solved PBGD structures, the oxidized cofactor is in the dipyromethenone form, in which both pyrrole rings are approximately coplanar. In contrast, the oxidized cofactor in the B. megaterium enzyme appears to be in the dipyrromethanone form, in which the C atom at the bridging α-position of the outer pyrrole ring is very clearly in a tetrahedral configuration. It is suggested that the pink colour of the freshly purified protein is owing to the presence of the dipyrromethene form of the cofactor which, in the structure reported here, adopts the same conformation as the fully reduced dipyrromethane form.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2009

Discrimination of Spore-Forming Bacilli Using spoIVA

A method of discriminating between spore-forming and non-spore-forming bacteria is based on a combination of simultaneous sporulation-specific and non-sporulation-specific quantitative polymerase chain reactions (Q-PCRs). The method was invented partly in response to the observation that for the purposes of preventing or reducing biological contamination affecting many human endeavors, ultimately, only the spore-forming portions of bacterial populations are the ones that are problematic (or, at least, more problematic than are the non-spore-forming portions). In some environments, spore-forming bacteria constitute small fractions of the total bacterial populations. The use of sporulation-specific primers in Q-PCR affords the ability to assess the spore-forming fraction of a bacterial population present in an environment of interest. This assessment can provide a more thorough and accurate understanding of the bacterial contamination in the environment, thereby making it possible to focus contamination- testing, contamination-prevention, sterilization, and decontamination resources more economically and efficiently. The method includes the use of sporulation-specific primers in the form of designed, optimized deoxyribonucleic acid (DNA) oligonucleotides specific for the bacterial spoIVA gene (see table). [In "spoIVA," "IV" signifies Roman numeral four and the entire quoted name refers to gene A for the fourth stage of sporulation.] These primers are mixed into a PCR cocktail with a given sample of bacterial cells. A control PCR cocktail into which are mixed universal 16S rRNA primers is also prepared. ["16S rRNA" denotes a ribosomal ribonucleic acid (rRNA) sequence that is common to all organisms.] Following several cycles of heating and cooling according to the PCR protocol to amplify amounts of DNA molecules, the amplification products can be analyzed to determine the types of bacterial cells present within the samples. If the amplification product is strong, relative to the product of a control PCR sequence, then it is concluded that the bacterial population in the sample consists predominantly of spore-forming cells. If the amplification product is weak or nonexistent, then it is concluded that the bacterial population in the sample consists predominantly or entirely of non-spore-forming cells.

Venkateswaran, Kasthuri↗

NASA NTRS2026

Fatigue Life of Flow-Formed Aluminum 2195 and 6061 Alloys

The successful design and fabrication of metallic cryotanks for commercial aviation applications require lightweight, durable materials capable of withstanding high pressures and cryogenic temperatures through tens of thousands of thermomechanical refueling cycles. Flow forming is an advanced manufacturing technique that offers high-rate production and scalability for fabricating integrally stiffened cylinders suitable for cryotank applications. This work establishes the durability of flow-formed aluminum alloys by characterizing their fatigue life performance under conditions that mimic cryotank refueling cycles. Residual stresses in flow-formed aluminum-lithium (Al-Li) 2195-T6 cylinders were assessed using the contour method and found to be minimal. Fatigue life testing was conducted on flow-formed Al-Li 2195-T6 at room temperature and cryogenic temperatures (-321°F [-196°C]), with wrought Al-Li 2195-T6 serving as a baseline for comparison. Results showed that flow-formed materials exhibited fatigue performance comparable to or better than wrought materials, with no statistically significant differences observed between different specimen orientations relative to processing directions. Fractography revealed reduced delaminations in the flow-formed Al-Li 2195 samples as compared to wrought, indicating potential improvement to the microstructure that could result in improved service properties. Texture analysis using electron backscattered diffraction (EBSD) indicated recrystallization during heat treatment, potentially contributing to reduced delamination susceptibility. These findings demonstrating flow-formed material durability coupled with the high manufacturing efficiency of flow forming, makes flow forming an attractive process to produce aircraft cryotanks.

EBF3↗

DOE OSTI2017

Liquid secondary waste: Waste form formulation and qualification

The Hanford Site Effluent Treatment Facility (ETF) currently treats aqueous waste streams generated during site cleanup activities. When the Hanford Tank Waste Treatment and Immobilization Plant (WTP) begins operations, including Direct Feed Low Activity Waste (DFLAW) vitrification, a liquid secondary waste (LSW) stream from the WTP will need to be treated. The volume of effluent for treatment at the ETF will increase significantly. The powdered salt waste form produced by the ETF will be replaced by a stabilized solidified waste form for disposal in Hanford’s Integrated Disposal Facility (IDF). Washington River Protection Solutions is implementing a Secondary Liquid Waste Immobilization Technology Development Plan to address the technology needs for a waste form and solidification process to treat the increased volume of waste planned for disposal at the IDF. Waste form testing to support this plan is composed of work in the near term to provide data as input to a performance assessment (PA) for Hanford’s IDF. In 2015, three Hanford Liquid Secondary Waste simulants were developed based on existing and projected waste streams. Using these waste simulants, fourteen mixes of Hanford Liquid Secondary Waste were prepared and tested varying the waste simulant, the water-to-dry materials ratio, and the dry materials blend composition.1 In FY16, testing was performed using a simulant of the EMF process condensate blended with the caustic scrubber—from the Low Activity Waste (LAW) melter—, processed through the ETF. The initial EMF-16 simulant will be based on modeling efforts performed to determine the mass balance of the ETF for the DFLAW.2 The compressive strength of all of the mixes exceeded the target of 3.4 MPa (500 psi) to meet the requirements identified as potential IDF Waste Acceptance Criteria in Table 1 of the Secondary Liquid Waste Immobilization Technology Development Plan.3 The hydraulic properties of the waste forms tested (hydraulic conductivity and water characteristic curves) were comparable to the properties measured on the Savannah River Site (SRS) Saltstone waste form. Future testing should include efforts to first; 1) determine the rate and amount of ammonia released during each unit operation of the treatment process to determine if additional ammonia management is required, then; 2) reduce the ammonia content of the ETF concentrated brine prior to solidification, making the waste more amenable to grouting, or 3) manage the release of ammonia during production and ongoing release during storage of the waste form, or 4) develop a lower pH process/waste form thereby precluding ammonia release.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Immobilization of cesium and iodine into Cs 3 Bi 2 I 9 perovskite-silica composites and core-shell waste forms with high waste loadings and chemical durability

Cs$_3$Bi$_2$I$_9$, a defect perovskite derivative, is a potential host phase to immobilize iodine and cesium with high waste loadings. In this work, two strategies were explored to form Cs$_3$Bi$_2$I$_9$-silica composites and a core-shell structure in order to improve chemical durability of waste form materials meanwhile maintaining high waste loadings. Cs$_3$Bi$_2$I$_9$ loadings as high as 70 wt.% were incorporated into a silica matrix to form silica-ceramic composites, and 20 wt.% Cs$_3$Bi$_2$I$_9$ was encapsulated into silica to form a core–shell structure by low temperature spark plasma sintering. Chemical durability of the composite and core-shell waste forms was evaluated by semi-dynamic leaching experiments, and Cs and I were incongruently released from waste form matrices. A BiOI alteration layer formed, acting as a passivation layer to reduce the release of radionuclides. The long-term iodine release rate was low (30 mg m$^{-2}$ day$^{-1}$) for the 70 wt.%Cs$_3$Bi$_2$I$_9$–silica composite leached in deionized water at 90 °C, which can be further reduced to 5 × 10$^{-3}$ mg m$^{-2}$ day$^{-1}$ for the 20 wt.% core-shell structure. This work highlights a robust way to immobilize the highly mobile radionuclides with high waste loadings through encapsulation into durable matrices and a surface passivating mechanism that can greatly reduce the elemental transport from waste form materials and significantly enhance their chemical durability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Ripple Effects: Bed Form Morphodynamics Cascading Into Hyporheic Zone Biogeochemistry

The water quality and ecosystem health of river corridors depend on the biogeochemical processes occurring in the hyporheic zones (HZs) of the beds and banks of rivers. HZs in riverbeds often form because of bed forms. Despite widespread and persistent variation in river flow, how the discharge- and grain size-dependent geometry of bed forms and how bed form migration collectively and systematically affects hyporheic exchange flux, solute transport, and biogeochemical reaction rates are unknown. As such, we investigated these linked processes through morphodynamically consistent multiphysics numerical simulation experiments. Several realistic ripple geometries based on bed form stability criteria using mean river flow velocity and median sediment grain size were designed. Ripple migration rates were estimated based primarily on the river velocity. The ripple geometries and migration rates were used to drive hyporheic flow and reactive transport models which quantified HZ nitrogen transformation. Results from fixed bed form simulations were compared with matching migrating bed form scenarios. We found that the turnover exchange due to ripple migration has a large impact on reactant supply and reaction rates. The nitrate removal efficiency increased asymptotically with Damköhler number for both mobile and immobile ripples, but the immobile ripple always had a higher nitrate removal efficiency. Since moving ripples remove less nitrogen, and may even be net nitrifying at times, consideration for bed form morphodynamics may therefore lead to reduction of model-based estimates of denitrification. The connection between nitrate removal efficiency and Damköhler number can be integrated into frameworks for quantifying transient, network-scale, HZ nitrate dynamics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Unified model of nucleon elastic form factors and implications for neutrino-oscillation experiments

Precise knowledge of the nucleon’s axial-current form factors is crucial for modeling GeV-scale neutrino-nucleus interactions. Unfortunately, the axial form factor remains insufficiently constrained to meet the precision requirements of upcoming long-baseline neutrino-oscillation experiments. This work studies the nucleon’s axial and vector form factors using the light-front approach to build a quark-diquark model of the nucleon with an explicit pion cloud. The light-front wave functions in both the quark and pion-baryon Fock spaces are first calibrated to existing experimental information on the nucleon’s electromagnetic form factors and then used to predict the axial form factor. The resulting squared charge radius of the axial pseudovector form factor is predicted to be $r$$^{2}_{A}$ = 0.29 ± 0.03 fm 2 , where the small error accounts for the model’s parametric uncertainty. We use our form factor results to explore the (quasi)elastic scattering of neutrinos by (nuclei)nucleons, with the result that the widely implemented dipole ansatz is an inadequate approximation of the full form factor for modeling both processes. Here, the approximation leads to a 5%–10% overestimation of the total cross section, depending on the (anti)neutrino energy. We project overestimations of similar size in the flux-averaged cross sections for the upcoming DUNE long-baseline neutrino-oscillation experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗