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Ebert, W. L.

Publications and source records attributed to Ebert, W. L..

At least 19 records

Simplifying Ceramic Waste Form Processing

The glass-bonded sodalite ceramic waste form (CWF) was developed in the 1990s to immobilize chloride salt-bearing waste streams generated during treatment of spent sodium-bonded nuclear fuel. This was necessary because chloride salts are essentially insoluble in borosilicate glasses (on the order of 1%). In the CWF, synthetic sodalite (Na 8 [Al 6 Si 6 O 24 ]Cl 2 ) is generated by the reaction of zeolite 4A and NaCl during processing to sequester the chlorine. The resulting sodalite crystals become microencapsulated in borosilicate glass. Based on the current understanding of the reactions involved and advancements in pyroprocessing operations in which the waste salt is generated, the processes developed for producing fullsize CWF materials with waste salt may be unnecessarily complicated. Aspects of processing that could be simplified and initial studies to justify further engineering development are recommended.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effects of open circuit immersion and vertex potential on potentiodynamic polarization scans of metallic biomaterials

Abstract Electrodes made of commercially pure titanium (CP-Ti) and a CoCrMo alloy are immersed at an open circuit in a phosphate buffer saline electrolyte at room temperature for different durations prior to electrochemical analyses. Open circuit potential measurements, electrochemical impedance spectroscopy measurements, and cyclic potentiodynamic polarization (CPP) scans are used to assess the impact of the immersion time on derived property values. Stable passivation layers formed on both materials during immersion. The corrosion potentials determined from the anodic legs of CPP scans become more cathodic, and the corrosion currents decrease to lower values after longer immersion times. Measured currents indicate the layers formed on CP-Ti stabilize during forward anodic scans and persist to the vertex potential, whereas passivation breakdown occurs during anodic scans with CoCrMo with active corrosion at voltages up to the vertex potential. The characteristics of the return cathodic legs of CPP scans represent the surface conditions at the vertex potential: characteristic corrosion property values derived from the test responses represent passive surfaces on CP-Ti and leached surfaces on CoCrMo rather than intrinsic properties of those materials.

36 MATERIALS SCIENCE↗

Corrosion rates measured under potentiostatic conditions to represent performance of a cermet nuclear waste form

Electrochemical tests were conducted to assess the corrosion performance of a developmental multiphase cermet nuclear waste form in different conditions. Corrosion currents were monitored as the surface equilibrated in an acidic brine solution during potentiostatic tests at different imposed potentials. Electrochemical impedance spectroscopy was used to quantify differences in the electrical properties of surfaces stabilised at different potentials. The passivating oxides that will stabilise the surface under disposal conditions are formed and maintained during testing. The measured corrosion currents were two orders of magnitude lower for passivated surfaces than for polished surfaces over a wide range of redox conditions. The electrochemical results were correlated with microscopic analyses of the corroded surfaces and physical models of the surface passivation and degradation processes are proposed. The measured corrosion rates are suitable for the long-term performance modeling of cermet nuclear waste forms.

Gattu, V. K.↗

Technology Development Roadmap for Volatile Radionuclide Capture and Immobilization

An "Off-Gas and Waste Forms Strategy Workshop" was held in Washington, D.C. on January 31, and February 1, 2023, to review the current state of the art (baseline) technologies for capturing and immobilizing these volatile radionuclides in waste forms (WFs). The discussions in that workshop were used to develop a roadmap for future research and development to mature technologies that are presently not ready for use in a commercial reprocessing facility and develop and demonstrate technologies that provide more safety, more simplicity, or lower costs compared to the current baseline.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Thermophysical Property Measurements of NaCl-UCl3

Describe the research (summary of Scope of Work and principal objectives of the CRADA): Argonne produced and measured thermochemical and thermophysical properties of eutectic NaCl-UCl 3 salt at several temperatures in the range of interest. (Note measurements made with UCl 3 instead of PuCl 3 at participant’s request.)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Data Quality of Salt Property Measurements

Data quality is a key element to assessing technical uncertainties in property values of salt mixtures that are pivotal in molten salt reactor (MSR) design and safety assessments under both normal operating conditions and accident scenarios. Key properties for the salt mixtures being evaluated for use in MSRs have not been measured and the few values for relevant salt compositions available in the literature are inconsistent and not suitable for use in licensing. The applications of established techniques commonly used for property measurements to molten salts are still experimental in nature and vetted consensus standards are not yet available. Work is in progress to develop and standardize methods through DOE and commercially funded projects. The quality of measured property values limits the current ability to reliably design equipment and model normal MSR operation and the effects of operational upsets. Insights from experimental measurements pertinent to reducing technical uncertainty for regulatory development are summarized in this report. Quality controls are recommended for key properties based on the mathematical calculations used to derive property values and methods used to measure experimental values and salt produced for use in the measurements.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Corrosion Behavior of Developmental Iron Phosphate Waste Forms: FY20 Status Report

Corrosion tests were performed to assess the dissolution behaviors of developmental iron phosphate materials that are being evaluated as an alternative to the glass-bonded sodalite ceramic waste form to immobilize salt wastes from electrochemical separation operations. Production of the iron phosphate waste form results in dehalogenation of the waste salt that increases potential waste loading. Ferric oxide is added to the waste form to increase the chemical durability. Tests conducted to optimize the amount of ferric oxide used to make the waste form are summarized in this report. Specimens prepared from materials made with between 17 and 34 mole % ferric oxide were subjected to two test methods to assess the effects of the iron content on the relative durability and retention of immobilized salt cations including cesium, strontium, and neodymium. Modified ASTM C1308 test results show the intrinsic durability was significantly higher for materials made with 27 mol % ferric oxide. Further additions generated iron-rich inclusion phases and did not improve durability. Modified ASTM C1285 test results show that solution feedback attenuates the dissolution rate similar to what is observed for borosilicate glasses within seven days. Analyses of test specimens after 42 days show no evidence that surface layers formed. Combined with previous studies addressing the salt loading, a composition region of the ammonium (di)hydrogen phosphate-waste salt-ferric oxide ternary has been defined for durable waste form compositions. Materials with that composition can be used to determine optimal processing conditions, assess long-term performance, and parameterize a degradation model.

Stariha, S. A.↗

The Precision of Product Consistency Tests with Environmental Assessment Glass

Several series of triplicate tests conducting following the ASTM C1285 product consistency test method have been performed using samples of Environmental Assessment glass in Teflon™ and steel test vessels. The results of tests with test parameters within the ranges specified in the PCT method A procedure were used to calculate repeatability and reproducibility precision statistics for tests in each type of vessel. These show the test response and test precision attained in tests conducted in Teflon™ and stainless steel test vessels are statistically indistinguishable.

36 MATERIALS SCIENCE↗

The Precision of Product Consistency Tests with Reference Glasses ARM-1 and SRM 623

An interlaboratory study (ILS) was conducted in 2014 to measure the precision with which the ASTM-International product consistency test method A (PCT-A) can be performed using properly prepared samples of reference glass ARM-1 or SRM 623 and test parameter values near the centers of ranges specified in procedure ASTM C1285. The ILS did not evaluate the full range of test parameter values allowed in the PCT-A method and the results do not represent the precision that should be expected if extreme values of the ranges are used. However, the precision measured in the ILS quantified the precision of tests conducted with mean parameters that were used to estimate the effects of individual parameters. Follow-on tests were conducted to assess the effects of several individual test parameter values on the test response and uncertainties in the derived glass dissolution rates. The effects of particle size distributions in glass samples prepared by wet- and dry-sieving methods, methods to remove fines, and the limiting parameter values for the water-to-glass (w/g) mass ratio and test duration allowed in PCT-A were measured. Test responses for all variations except test duration exceeded the precision measured in the ILS for conducting triplicate PCT-A tests within a single laboratory. The accuracy of glass dissolution rates derived from PCT results benefits from using a tighter control of these test variables than required in ASTM C1285. Comparison with previous analyses of the method shows how use of the relative standard deviation to represent the test precision can be misleading, and that the mean response and standard deviation should both be considered.

36 MATERIALS SCIENCE↗

Corrosion Tests with Developmental Iron Phosphate Glass Waste Forms

Corrosion tests are in progress to assess the dissolution behavior of developmental iron phosphate waste forms for salt waste from electrochemical separation operations. Specimens cut from materials made at PNNL to represent a range of waste salt loadings in prototype composition DPF-5 and a range of iron oxide loadings in prototype composition DPF-3 were subjected to modified ASTM C1308 tests to assess the compositional effects on the relative durabilities and retention of immobilized salt cations. The materials were composed of different amounts of glass and crystalline phases. The test results show both the intrinsic durability of the material and the salt cation retention decrease as the total amount of salt cations added to the material is increased. The results of ASTM C1220 and ASTM C1285 tests conducted with materials DPF5-280 and DPF5-336, which contained about 28% and 34% salt cations (on a mass oxide basis) and bounded the durabilities of the other materials, show that solution feedback does not attenuate the dissolution rate. This suggests the degradation of iron phosphate waste forms can be modelled by using a constant rate that probably depends on the composition and volume fraction of the glass phase. A reference composition should be formulated and used in tests to determine those dependencies. The ASTM C1220 and ASTM C1285 tests with DPF5-280 and DPF5-336 remain in progress to corrode the specimens enough to distinguish the relative extents of glass and crystalline phase corrosion by microscopic examinations. Those results are expected to provide insights regarding the relative dissolution rates of crystalline and glass phases and impact on durability to inform the formulation of the reference composition.

Ebert, W. L.↗

Analyses of iron phosphate glasses for dehalogenated salt waste

Specimens cut from series of glasses made at PNNL to represent a range of salt loadings in prototype composition DPF-5 and a range of iron oxide loadings in prototype composition DPF-3 were subjected to modified ASTM C1308 tests to assess the relative durabilities and retention of salt cations. Test results show both the intrinsic durability and salt cation retention decrease as the total amount of salt cations is increased, but waste forms made with up to 34 mass % salt waste loadings on a salt-cation basis are more durable than glass-bonded sodalite waste forms made with optimal salt waste loadings (about 6% on a salt-cation basis). Other tests are in progress to assess the effect of solution feedback on the long-term durability of these materials.

Ebert, W. L.↗

A U-bearing composite waste form for electrochemical processing wastes

Metallic/ceramic composite waste forms are being developed to immobilize combined metallic and oxide waste streams generated during electrochemical recycling of used nuclear fuel. Composites were made for corrosion testing by reacting HT9 steel to represent fuel cladding, Zr and Mo to simulate metallic fuel waste, and a mixture of ZrO2, Nd2O3, and UO2 to represent oxide wastes. More than half of the added UO2 was reduced to metal and formed Fe-Zr-U intermetallics and most of the remaining UO2 and all of the Nd2O3 reacted to form zirconates. Fe-Cr-Mo intermetallics were also formed. Microstructure characterization of the intermetallic and ceramic phases that were generated and tests conducted to evaluate their corrosion behaviors indicate composite waste forms can accommodate both metallic and oxidized waste streams in durable host phases. (c) 2018 Elsevier B.V. All rights reserved.

Chen, X. (ORCID:0000000332734431)↗

Effect of molybdenum additions on the microstructures and corrosion behaviours of 316L stainless steel-based alloys

Alloys were made by alloying 5, 10, 15, 17.5, and 20 wt % Mo with Type 316L stainless steel. Sigma phases containing 21–29 wt % Mo formed along the austenite grain boundaries with the addition of 5 wt % Mo and increased with additions up to 15 wt % Mo, but they decreased with further additions. Laves phases containing 33–40 wt % Mo co-precipitated at additions of 10 wt % Mo which increased with further Mo increases. The corrosion resistance, assessed by potentiodynamic polarisation in a 10 mM NaCl solution adjusted to pH 4, increased relative to Type 316L for alloys made with 5 and 10 wt % added Mo, but decreased with further additions due to preferential corrosion of the Laves phase. The alloy made with 10 wt % added Mo had the highest corrosion resistance due primarily to the high Mo content of the austenite.

36 MATERIALS SCIENCE↗

Electrochemical corrosion of a noble metal-bearing alloy-oxide composite

The effects of added Ru and Pd on the microstructure and electrochemical behaviour of a composite material made by melting those metals with AISI 410 stainless steel, Zr, Mo, and lanthanide oxides were assessed using electrochemical and microscopic methods Furthermore, the lanthanide oxides reacted with Zr to form durable lanthanide zirconates and Mo alloyed with steel to form FeMoCr intermetallics. The noble metals alloyed with the steel to provide solid solution strengthening and inhibit carbide/nitride formation. In a passive film formed during electrochemical tests in acidic NaCl solution, but became less effective as corrosion progressed and regions over the intermetallics eventually failed.

36 MATERIALS SCIENCE↗