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At least 289 records · Page 16

Investigation of Luminescent Ceria as a Plutonium Oxide Simulant. Final Report

Plutonium oxide powders from various production lines at Los Alamos National Laboratory are stored and transported in specially designed “SAVY-4000”, “Hagan”, or other containment systems. Cerium oxide powder has been used as a less-hazardous simulant powder for testing accidental release from these containers under various operational scenarios. This work investigates the development and use of fluorescent cerium oxide powders as a more easily detectable, and potentially quantifiable, simulant powder for plutonium oxide container systems

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tribological Behavior of Structural Materials in High Temperature Helium Gas-Cooled Reactor Environments

The High-Temperature Gas-cooled Reactor (HTGR) is a Generation IV concept designed to produce electricity and hydrogen at high efficiencies via high operating temperatures (700 °C or higher). Helium, the primary coolant for HTGRs, contains impurities (e.g., CO, H2O and CH4) that can induce corrosion reactions at high temperatures such as oxidation and (de)carburization, which in turn can affect the tribological behavior of components. Incoloy® 800HT (Ni-Fe-Cr austenitic solid-solution alloy) and Inconel® 617 (Ni-Cr-Co-Mo solid-solution alloy) are two high-temperature superalloys currently selected as candidate structural materials for the HTGR. The objective of this study is to evaluate the high-temperature tribological performance of these two candidate alloys after conditioning them in HTGR environments. Four regimes of corrosion were considered: a non-conditioned regime (Regime I), an oxidizing regime (Regime II), a carburizing and oxidizing regime (Regime III), and a carburizing regime (Regime IV). To simulate oxidation in HTGR, samples were conditioned for 22 days at elevated temperatures in a once-through helium loop with 4 ppmv H2O. Carburization of the samples was achieved by the commercial process, Kolsterising®. In addition, two surface treatments – shot peening and aluminization – were considered as potential routes of improving the alloys’ wear resistance. Surface-treated samples were tested both before and after conditioning in Regime II. Tribological testing of the samples was performed via a pin-on-disk tribometer at elevated temperatures in ambient environment – 650 and 750°C for 800HT; 850 and 900°C for 617 – with applied loads of 1N, 2N and 5N. The wear behavior of the alloys was assessed via wear volume and friction coefficient measurements, supported by morphological, structural and compositional analyses of the wear tracks. Conditioning the samples in Regime II led to the formation of a chromium oxide on both alloys. This protective scale increased the wear resistance compared to that of as-received samples (Regime I) due to the formation of a compacted ‘glaze’ oxide layer during sliding, rendering the wear track nearly undistinguishable from the unworn background and resulting in wear volumes below the detection limits of the measurement technique. The variability of the friction coefficients of the conditioned samples was also considerably reduced compared to that of the as-received samples due to the glaze layer. Additionally, the initial friction coefficients of the samples conditioned in Regime II were reduced by 45% and 54% compared to those of as-received samples for alloys 800HT and 617, respectively. Carburizing the samples (Regime IV) hardened the surfaces of both alloys and promoted the formation of an iron oxide on 800HT during tribological testing, thereby increasing the wear resistance and decreasing the initial friction coefficient by a factor of two compared to those of as-received 800HT. Alloy 617 exhibited an enhanced wear resistance but similar initial friction coefficient compared to those of as-received samples due to the increased surface hardness. The Mn-Cr oxide developed during Regime III conditioning of 800HT did not develop a glaze layer during tribotesting, even at lower loads. Thus, it was not as protective as the oxide produced during conditioning of Regime II samples, leading to lower wear resistance of 800HT in Regime III compared to that measured in the Regime II condition. 800HT benefited from the aluminization surface treatment, particularly before conditioning in Regime II, due to the promotion of a wear-resistant aluminum oxide layer during testing and the increase in surface hardness due to the presence of a FeAl intermetallic phase. The presence of this phase caused an order-of-magnitude reduction in wear volumes compared to those of as-received 800HT. Aluminization of 617 decreased its wear resistance, particularly after conditioning in Regime II, due to significant wear of the aluminum oxide via a ceramic wear mechanism. This aluminum oxide was removed during sliding, causing the wear volumes to increase by a factor of five compared to those of 617 conditioned in Regime II. Shot-peened 800HT exhibited a tribological behavior similar to that of as-received 800HT, despite an enhancement in the rate of chromium oxide formation. Shot-peened 800HT conditioned in Regime II showed lower wear resistance compared to that of 800HT conditioned in Regime II due to the poor adhesion between the oxide and the underlying metal, preventing the formation of the glaze layer during sliding. Shot peening of 617 increased its wear resistance at higher load, reducing worn volumes by 60% compared to that measured with as-received 617. Tribotesting of shot-peened 617 in Regime II revealed that the glaze-oxide layer was formed at every load, resulting in negligible wear, similar to what was observed from testing 617 after conditioning in Regime II. Overall, alloy 617 exhibited tribologically superior behavior compared to that of alloy 800HT, as demonstrated by its lower friction coefficients and its order-of-magnitude lower wear volumes when measurable.

36 MATERIALS SCIENCE↗

Catalyst Deactivation Modes of PdO/γ-Al 2 O 3 Catalysts for Lean Methane Oxidation

PdO/γ-Al 2 O 3 catalysts are one of the most active catalytic components for the complete oxidation of methane. Under reaction conditions, especially in a wet feed, the catalysts suffer severe performance degradation. This study establishes a series of testing protocols to systematically investigate the causes of catalyst deactivation under methane oxidation reaction conditions. Four distinct catalyst deactivation modes are identified. Two of the deactivation modes are directly related to H 2 O, either from the feed gas or as a part of the reaction products, with one (Mode 2) being attributed to the formation of surface hydroxyl groups and the other (Mode 3) to the competitive adsorption of H 2 O on the catalysts. The impact of the two deactivation modes is acute and severe but reversible. In contrast, the other two deactivation modes are gradual and persistent but irreversible. Both modes are induced by CH 4 oxidation reaction, with the impact of a wet feed (Mode 4) being substantially more severe than that of a dry feed (Mode 1). The major cause of the irreversible catalyst deactivation is attributed to surface reconstruction of PdO nanoparticles, which behaves as a passivation layer lowering the number of coordinately unsaturated Pd sites for CH 4 activation. Although the passivation layer is relatively stable against thermal or hydrothermal treatment, it is not completely inert. Formation and partial regeneration of the passivation layer is a highly dynamic process and heavily depends on the reaction temperature: a lower reaction temperature (≤ 450 ℃) can lead to quicker catalyst deactivation; but a higher reaction temperature (between 500 – 550 ℃) can result in a greater extent of catalyst deactivation.

PdO/γ-Al2O3↗

Arsenic stabilization performance of a novel starch-modified Fe-Mn binary oxide colloid

Arsenic (As) is an environmentally hazardous contaminant and can be a serious threat to human health. In China, remediation needs for a large number of As-contaminated sites renders a strong demand for efficient remedial reagents and cost effective approaches. In this study, a novel starch-modified Fe-Mn binary oxide (SFM), an amorphous colloidal material, has been synthesized as a remedial reagent and its As stabilization performance has been evaluated. A set of laboratory batch experiments were carried out by directly adding SFM of different dosages into three contaminated soils. Results demonstrated that SFM could transform As in soil from non-specifically and specifically sorbed fractions to the more stable form bounded to amorphous iron hydrous oxides, thus reducing the As concentration in TCLP leachates by 42.0-93.2%. Results from adsorption tests and microscopic analysis indicated that the interactions between SFM and As are mainly controlled by adsorption, oxidation, and precipitation processes. SFM has abundant surface hydroxyl groups, with excellent adsorption properties for both As(V) and As(III), with the maximum adsorption capacities of 160.63 and 284.64 mg/g respectively at pH 7.0. The adsorption process closely fitted pseudo second-order kinetics and Freundlich isotherm model. SFM could increase soil Eh and oxidize As(III) to As(V), which facilitated the As stabilization in soilColloidal iron-based material directly used for stabilization in As contaminated soils is reported here for the first time. Starch modification improves both the reactivity and mobility of SFM in soil. Our findings propose an efficient and convenient reagent for As remediation in soil.

Yan, Xiulan↗

Re-Assembly and Test of a COMB Dipole Magnet With STAR Wires

Rare-Earth Barium Copper Oxide (REBCO) coated conductors are an attractive option for application in high field accelerator magnets due to their high critical field and the convenience of fabrication without heat treatment compared to some other superconductors. A small REBCO accelerator magnet was previously fabricated and tested in liquid nitrogen, demonstrating over 90% critical current retention in the coils. This paper describes the magnet re-assembly with a different support structure and its test in liquid helium at 1.8–4.5 K. The magnet quench history along with the instrumentation data is presented and discussed.

43 PARTICLE ACCELERATORS↗

Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite

Abstract Reduced silver mordenite has been considered as a sorbent for the capture of organic iodides, especially methyl iodide, from off-gases produced by aqueous used nuclear fuel reprocessing operations. The adsorption capacity of this material has been unpredictable especially when NO x and water are present. Previous work has found that a catalytic decomposition reaction is occurring on the surface but few determinations have been made of the kinetics of this reaction. The work presented tested the adsorption behavior and apparent catalytic reaction rate in humid conditions and compared those to dry conditions testing. Both experiments observed a first order reaction with rate constants of 0.0847 L/g sorbent/s and 0.1202 L/g sorbent/s respectively. Such a reduction in apparent rate constant is possibly due to either water obstructing methyl iodide adsorption or product desorption limitation. Changes in the adsorption profile were also apparent between these two, with the humid conditions experiment reaching saturation sooner than the dry conditions experiment. Additionally, an experiment into the effects of sorbent storage in a controlled laboratory environment was performed. The performance of the sorbent materials that were stored with silver in the zerovalent state was slightly inferior to those materials that were stored in ionic form (Ag + ) and reduced to zerovalent silver immediately prior to subjecting them to sorption test. The materials stored with silver in the ionic form (and reduced just prior to application) behaved essentially similarly to the freshly synthesized (and reduced) sorbents in the sorption tests. This suggests that zerovalent silver experiences some oxidation resulting in deactivation of some sites.

Goettsche, Heinrik↗

Simultaneous immobilization of aqueous co-contaminants using a bismuth layered material

The remediation of co-located contaminants in the vadose zone can be challenging due to accessibility and different responses of different contaminants to remedial actions. At the Hanford Site (WA, USA), multiple contaminants are present in the vadose zone and groundwater, including I, Tc, U, Cr, and NO3. We used a bismuth layered oxide in a series of batch experiments to test aqueous removal of multiple contaminants, including Tc, Cr, and U, as well as potentially competing anions, including NO3 and I. The results demonstrated successful removal of all four contaminants (>98% removal from the aqueous phase after 30 days) when tested individually. When contaminants were combined, a slight decrease in Tc removal occurred (-6%). The addition of sediment decreased the removal for Tc and I, but U and Cr removal was unaffected. Competition with anions released from the sediment likely caused the decreased removal of Tc and I and indicated that bismuth is less selective for these two contaminants. The results of these batch tests demonstrated that the bismuth based oxy-hydroxide material is a promising material for sequestering multiple contaminants in situ.

Lawter, Amanda R.↗

Post-irradiation examinations of annular mixed oxide fuels with average burnup 4 and 5% FIMA

In this paper, we present post-irradiation examination results on two type of annular mixed oxide fuel pins irradiated in the Fast Flux Test Facility (FFTF) sodium cooled reactor to an average burnup between 4% and 5% fission of initial heavy atom (FIMA). The pins differed only from the initial Pu content, which was 22 wt% and 26 wt%, respectively. The overall performance of the pins was excellent, in line with previous historical results. The pins with higher Pu content experienced higher irradiation temperatures which influenced the fission gas release, fuel swelling, and Cs distribution compared to the other pins. All the post-irradiation examinations results are discussed against the irradiation parameters. In particular, the pins with higher initial Pu content, i.e., 26 wt%, experienced higher power that resulted in enhanced fission gas release compared to the other two pins with 22 wt% initial Pu content. For the pins with higher fission gas release, onset of Cs redistribution was observed. The two pins that had lower initial Pu content and burnup showed a Cs axial distribution similar to the as-produced one.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Exploring sodium dynamics in the dilute oxygen regime of mixed oxy-sulfide NaPSiSO glasses

All-solid-state‑sodium batteries have great potential to lower the cost of grid-scale energy storage systems. However, they require a low cost, high conductivity solid electrolyte to become a reality. The electrochemical properties of mixed oxy-sulfide glasses NaPSiSO exceed those of either the pure sulfide or the pure oxide glass alone. In this work, we have tested models of sodium ion dynamics in the NaPSiSO series: zNa 2 S+(1-z)[(1-y)[(1-x)SiS 2 + xPS 5/2 ] + yNaPO 3 ] where 0.57 ≤ z ≤ 0.588, 0 ≤ x ≤ 0.35, and 0.15 ≤ y ≤ 0.35 using 23 Na nuclear magnetic resonance to directly probe the local fields and their fluctuations at the nuclear sites. We determined the distribution of activation energies in these materials arising from distributions of local environments and provided quantitative information about the connectivity of the ionic pathways through which the sodium ions move. We found that the sodium ion conduction dynamics were described as an ionic percolation through a Gaussian distribution of energy barriers and that the composition dependence of the ionic conductivity in the dilute oxygen regime is well-described by the Nernst-Einstein relation modified for percolation.

25 ENERGY STORAGE↗

Aliovalent gallium dopants remove Ti 3+ defects and improve photocatalytic and photoelectrochemical water oxidation properties of LaTiO 2 N

LaTiO 2 N is a promising semiconductor for the water splitting reaction due to its 2.1 eV band gap and stability against corrosion. However, its solar energy conversion is limited by Ti 3+ recombination defects introduced during ammonolysis. Here we show for the first time that Ti 3+ defects in LaTiO 2 N can be suppressed with incorporation of 2, 5, and 10% aliovalent gallium (Ga 3+ ) dopants during synthesis via the layered La 2 Ti 2 O 7 intermediate. Electron paramagnetic resonance (EPR) spectroscopy on the solid powders confirms a reduction in the Ti 3+ donor density from 2.97 × 10 17 cm −3 for the non-doped material to ∼6.24 × 10 16 cm −3 for 5% Ga-doped LaTiO 2 N. The remaining Ti 3+ defects are concentrated near the LaTiO 2 N surface, according to X-ray photoelectron spectroscopy. The defect reduction shifts the optical absorption edge from 2.02 to 2.09 eV and eliminates a broad absorption band at 1050 nm from the optical absorption spectra. It also removes a 1.0–1.7 eV sub-band gap photovoltage signal from surface photovoltage spectra. This suggests that empty Ti 3+ d-orbitals are located 1.0–1.7 eV above the LaTiO 2 N valence band edge. Removing these recombination states with increasing Ga 3+ content enhances the photoconversion efficiency of LaTiO 2 N during water oxidation. The optimized 2 wt% CoO x -loaded 5% Ga-doped LaTi O2 N material has a 16% AQE (400 nm) for O 2 production from aqueous silver nitrate solution and a ∼2.1 mA cm −2 water oxidation photocurrent at 1.23 V under 100 mW cm −2 Xe arc lamp illumination. The water oxidation photocurrent is stable during a 50 min test, and the Faraday efficiency for O 2 generation is 97%, confirming short-term corrosion stability of LaTiO 2 N. Altogether, these results provide a better understanding of the distribution, concentration, and impact of Ti 3+ defects on the optical, photovoltage, and photoelectrochemical properties of LaTiO 2 N. In combination with other defect control strategies, aliovalent Ga 3+ doping can help bring the solar energy conversion efficiency of LaTiO 2 N closer to the theoretical limit.

Wang, Li [University of California, Davis, CA (Uni↗

A high-efficiency cryogenic neutron spin flipper for IMAGINE-X at the high flux isotope reactor

The Laue neutron macromolecular crystallography beamline, IMAGINE, at the High Flux Isotope Reactor (HFIR) is undergoing a major upgrade to incorporate the dynamic nuclear polarization (DNP) technique. Upon completion, the new IMAGINE-X instrument is expected to enhance the signal-to-noise ratio of the diffraction data by an order of magnitude. To take full advantage of the benefits of DNP, both a highly polarized neutron beam and a high-efficiency neutron spin flipper are required. We have developed a compact cryogenic spin flipper utilizing the Meissner effect in high-Tc yttrium–barium–copper–oxide superconducting films. The flipper has been successfully tested at two HFIR neutron development beamlines, Larmor and Poplar, with neutron wavelengths of 5.3 and 2.4 Å respectively. At Larmor, a flipping efficiency of 0.995 ± 0.004 was achieved for 5.3 Å neutrons, and at Poplar, efficiency of up to 0.9987 ± 0.0004 was obtained for 2.4 Å neutrons. Both tests demonstrated the flipper’s excellent performance and suitability for integration into IMAGINE-X.

Fu, Sichao [Oak Ridge National Laboratory (ORNL), ↗

Summary Report For The Analysis Of The Sludge Batch 7b (Macrobatch 9) DWPF Pour Stream Glass Sample For Canister S04023 (Rev. 1)

In order to comply with the Defense Waste Processing Facility (DWPF) Waste Form Compliance Plan for Sluldge Batch 7b, Savannah River National Laboratory (SRNL) personnel characterized the Defense Waste Processing Facility (DWPF) pour stream (PS) glass sample collected while filling canister S04023. This report summarizes the results of the compositional analysis for reportable oxides and radionuclides and the normalized Product Consistency Test (PCT) results. The PCT responses indicate that the DWPF produced glass that is significantly more durable than the Environmental Assessment glass.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Summary Report for the Analysis of the Sludge Batch 7b (Macrobatch 9) DWPF Pour Stream Glass Sample for Canister S04023

In order to comply with the Defense Waste Processing Facility (DWPF) Waste Form Compliance Plan for Sludge Batch 7b, Savannah River National Laboratory (SRNL) personnel characterized the Defense Waste Processing Facility (DWPF) pour stream (PS) glass sample collected while filling canister S04023. This report summarizes the results of the compositional analysis for reportable oxides and radionuclides and the normalized Product Consistency Test (PCT) results. The PCT responses indicate that the DWPF produced glass that is significantly more durable than the Environmental Assessment glass. Results and further details are documented in SRNL-STI-2013-00462, Revision 1 “Analysis of the DWPF Sludge Batch 7b (Macrobatch 9) Pour Stream Glass Sample.”

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Atomic Layer Deposition for Improved Biomass Conversion Catalysts

Heterogeneous catalysts are a key enabler of the transition towards a sustainable, bio-based economy for fuels and chemicals. However, the harsh conditions in many biomass conversion processes lead to nanoparticle sintering, support collapse, and metal leaching in conventional PGM catalysts. Next-generation catalysts must be developed to address these stability challenges. This presentation will discuss ongoing work between the Catalytic Carbon Transformation and Scale-Up Center at NREL and various industrial partners to develop scalable and cost-effective atomic layer deposition (ALD) coatings for improving the performance of biomass conversion catalysts. The substantial focus will be devoted to the benefits of TiO2 ALD coatings on supported Pd hydrogenation catalysts. Ten cycles of TiO2 ALD were found to dramatically improve the activity of a conventional Pd/Al2O3 catalyst towards aromatic hydrogenation, despite partial coverage of the Pd sites by the ALD layer. Subsequent advanced characterization and atomic-scale computational modeling revealed that the ALD coating weakened the adsorption strength of hydrogenation surface intermediates, leading to higher reaction rates. Reaction testing after exposure to sulfur impurities, high temperature oxidation, and hydrothermal treatment demonstrated the improved stability of the ALD-coated catalyst. Additionally, the ALD synthesis process was found to be scalable over two orders of magnitude with minimal deviation in synthesized catalyst properties. These results were contextualized with cost models of industrial ALD coating and aromatic hydrogenation processes to further refine the value proposition of ALD coatings. Given the demonstrated improvements in hydrogenation, TiO2 ALD coatings have also been applied to supported Pt catalysts for use in other biomass conversion reactions, such as hydrodeoxygenation for the production of sustainable aviation fuel (SAF) and the oxidation of glucose to bio-derived gluconic acid.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Atomic Layer Deposition for Improved Biomass Conversion Catalysts

Heterogeneous catalysts are a key enabler of the transition towards a sustainable, bio-based economy for fuels and chemicals. However, the harsh conditions in many biomass conversion processes lead to nanoparticle sintering, support collapse, and metal leaching in conventional PGM catalysts. Next-generation catalysts must be developed to address these stability challenges. This presentation will discuss ongoing work between the Catalytic Carbon Transformation & Scale-Up Center at NREL and various industrial partners to develop scalable, cost-effective atomic layer deposition (ALD) coatings for improving the performance of biomass conversion catalysts. Substantial focus will be devoted to the benefits of TiO2 ALD coatings on supported Pd hydrogenation catalysts. Ten cycles of TiO2 ALD were found to dramatically improve the activity of a conventional Pd/Al2O3 catalyst towards aromatic hydrogenation, despite partial coverage of the Pd sites by the ALD layer. Subsequent advanced characterization and atomic-scale computational modeling revealed that the ALD coating influenced the adsorption strength of hydrogenation surface intermediates in unexpected ways, leading to higher reaction rates. Reaction testing after exposure to sulfur impurities, high temperature oxidation, and hydrothermal treatment demonstrated the improved stability of the ALD-coated catalyst. Additionally, the ALD synthesis process was found to be scalable over two orders of magnitude with minimal deviation in synthesized catalyst properties. These results were contextualized with cost models of industrial ALD coating and aromatic hydrogenation processes to further refine the value proposition of ALD coatings. Given the demonstrated improvements in hydrogenation, TiO2 ALD coatings have also been applied to supported Pt catalysts for use in other biomass conversion reactions, such as hydrodeoxygenation for production of sustainable aviation fuel (SAF) and the oxidation of glucose for bio-derived gluconic acid. Recent findings from these experimental campaigns will also be shared. ALD technology holds great potential in the development of next-generation catalysts for biofuels and bioproducts and this work constitutes an important examination of the impact of ALD coatings in a variety of reaction environments.

bioenergy↗

Atomic Layer Deposition for Improved Biomass Conversion Catalysts

Heterogeneous catalysts are a key enabler of the transition towards a sustainable, bio-based economy for fuels and chemicals. However, the harsh conditions in many biomass conversion processes lead to nanoparticle sintering, support collapse, and metal leaching in conventional PGM catalysts. Next-generation catalysts must be developed to address these stability challenges. This presentation will discuss ongoing work between the Catalytic Carbon Transformation and Scale-Up Center at NREL and various industrial partners to develop scalable and cost-effective atomic layer deposition (ALD) coatings for improving the performance of biomass conversion catalysts. The substantial focus will be devoted to the benefits of TiO2 ALD coatings on supported Pd hydrogenation catalysts. Ten cycles of TiO2 ALD were found to dramatically improve the activity of a conventional Pd/Al2O3 catalyst towards aromatic hydrogenation, despite partial coverage of the Pd sites by the ALD layer. Subsequent advanced characterization and atomic-scale computational modeling revealed that the ALD coating weakened the adsorption strength of hydrogenation surface intermediates, leading to higher reaction rates. Reaction testing after exposure to sulfur impurities, high temperature oxidation, and hydrothermal treatment demonstrated the improved stability of the ALD-coated catalyst. Additionally, the ALD synthesis process was found to be scalable over two orders of magnitude with minimal deviation in synthesized catalyst properties. These results were contextualized with cost models of industrial ALD coating and aromatic hydrogenation processes to further refine the value proposition of ALD coatings. Given the demonstrated improvements in hydrogenation, TiO2 ALD coatings have also been applied to supported Pt catalysts for use in other biomass conversion reactions, such as hydrodeoxygenation for the production of sustainable aviation fuel (SAF) and the oxidation of glucose to bio-derived gluconic acid. Recent findings from these experimental campaigns will also be shared. ALD technology holds great potential in the development of next-generation catalysts for biofuels and bioproducts, and this work constitutes an important examination of the impact of ALD coatings in a variety of reaction environments.

atomic layer deposition↗

GIF-VHTR Materials (Graphite) Project Plan: Progress since September 2021

¦1: Data, Design Methodology and Construction 1.1: Graphite Selection and Acquisition Strategy (Original tasks completed) 1.2: Graphite Properties (Virgin Materials) 1.3: Graphite Fracture Behaviour(Original tasks completed) 1.4: Graphite Oxidation Behaviour(Original tasks completed) 1.5: Graphite Component Testing 1.6: Graphite Irradiation Effects 1.7: Graphite Irradiation Induced Creep 1.8: Graphite Codes and Standards Development (ASME & ASTM) 1.9: Graphite BehaviourModels Development 1.10: Links to Existing Graphite Irradiation BehaviourDatabases 1.11: Materials Database ¦2: Operation and Inspection 2.1: Methodologies for determining requirements for inspection of graphite cores 2.2: Methodologies for ISI of graphite cores ¦3: Decommissioning and Disposal (New task added 2021) 3.1: Technical data for decommissioning and disposal issues

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electrochemical Manipulation and Radiolytic Evaluation of Organic Phase Neptunium

Presentation for Seed LDRD proposal presentation: This Seed LDRD research proposes to test an innovative approach to precisely control the oxidation state distribution of neptunium (Np) under used nuclear fuel (UNF) reprocessing conditions using novel electrochemical methods. Current UNF reprocessing technologies are not financially viable in the US, requiring significant scientific and technological innovation to improve cost efficiency. Reducing the number of process cycles is one avenue for increasing cost efficiency, of which resolving the challenge associated with isolating Np is critical. Under envisioned process conditions, Np is present in a mixture of extractable (Np(IV) and Np(VI)) and inextractable (Np(V)) oxidation states, the distribution of which is dependent on several factors, including ionizing radiation dose, that change throughout a reprocessing scheme. Consequently, Np unintentionally partitions into various UNF reprocessing phases and product streams, ultimately increasing the number of process cycles to isolate UNF components. Here, we propose to employ novel, high surface area, optically transparent, Ligand Modified tin-doped indium oxide Electrodes (LMES). These LMEs bind Np, and therefore enable concurrent generation and spectroscopic characterization of Np oxidation states in organic solutions. These proof-of-concept experiments will: (i) facilitate optimization of the proposed electrochemical system conditions for Np oxidation state manipulation; (ii) identify the accessible electrochemical window for Np complexes in the organic phase; (iii) report characteristic optical spectra for each accessible complexed Np oxidation state; and (iv) determine the lifetime and partitioning of a given atypical Np oxidation state in the organic phase in the presence and absence of ionizing radiation fields. The data gathered by this Seed LDRD will provide support for the design of an electrochemical process concept for the precise manipulation of Np oxidation states in UNF reprocessing solvent systems, with the intention of providing advanced control over Np mass transfer, and thus greater process efficiency and economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗