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At least 685 records · Page 38

Fuel Cycle Considerations for Uranium, Plutonium and Minor Actinide Partitioning and Transmutation

This paper is written in memorial of the authors' past collaborations with Max Salvatores in the area of advanced nuclear fuel cycle evaluation. In this regard, a summary is provided of the results from two international studies led by Max Salvatores in which the authors participated: (1) the expert group on Homogeneous versus Heterogeneous Recycling of Transuranics in Fast Nuclear Reactors, and (2) the expert group on Potential Benefits and Impacts of Advanced Nuclear Fuel Cycles with Actinide Partitioning and Transmutation. Both of these studies presented the authors with the opportunity to contribute the results of past and ongoing research in the U.S., facilitating engagement and discussion on these subjects with researchers from other countries and organizations, resulting in the creation of broad international views on the relative benefits and challenges of transuranic recycle (NEA, 2012a; NEA, 2012b), a testament to the leadership and capabilities of Max Salvatores. Published by Elsevier Ltd.

Taiwo, Temitope↗

Epsilon Metal: A Waste Form for Noble Metals from Used Nuclear Fuel

Epsilon metal (e-metal) is the metallic phase that forms as inclusions at the grain boundaries in the UO2 fuel during reactor operation. This metal is composed of Pd, Mo, Rh, Ru, and Tc. These metallic inclusions are insoluble in strong acid and remnants of these metallic inclusions have been found in the UO2 matrix that remains from the natural reactors in Gabon that were active 1.8 billion years ago, therefore e-metal should be an excellent waste form for the immobilization of the long-lived isotopes 107Pd (6.5 ? 106 a) and 99Tc (2.13 ? 105 a), with 99Tc being the isotope of interest for repository performance. Therefore, the chemical durability of this potential waste form is assessed in this study. Typically, corrosion rates for metallic materials are measured electrochemically because they are quick, inexpensive, and can reveal the mechanism by which a metal corrodes, at least initially. However, in a repository the waste form would be subjected to slowly flowing water without an applied electrical potential over long time periods. Therefore, the corrosion rates of e-metal specimens were measured with both electrochemical tests and the single-pass flow-through test (SPFT). Potentiodynamic and potentiostatic polarization results suggest that a thin passive film exists on the alloy surface, which seems to be responsible for its high corrosion resistance. Additionally, X-Ray photoelectron spectroscopic results suggest that Pd oxides are significantly enriched in the passive film Results from the SPFT show that the dissolution rates were weakly dependent on pH. Only Mo and Re were found in solution and were used for the calculation of the dissolution rates. In general, the electrochemically determined corrosion rates agree reasonably well with the initial dissolution rate measured with the SPFT test, but they are about one or two orders of magnitude higher than the steady state rates. The causes for this discrepancy are discussed.

epsilon-metal, nuclear waste form, corrosion, sing↗

Defect cluster and nonequilibrium gas bubble associated growth in irradiated UMo fuels – a cluster dynamics and phase field model

Irradiation examination shows that gas bubble swelling kinetics is much faster after irradiation-induced recrystallization than that prior recrystallization in UMo fuels. It implies that gas bubbles in coarse grains and small recrystallized grains have different growth behavior. In this work, a phase-field model of gas bubble evolution integrating microstructure dependent cluster dynamics has been developed, for the first time, to study the gas bubble swelling behavior in the recrystallization zone of UMo fuels. Generation, diffusion, reaction, sink, emission and clustering of vacancies and interstitials are described by the cluster dynamics model while a phase-field model is used to describe the evolution of non-equilibrium gas bubbles including nucleation and growth. With the coupled model, the effect of defect generation rate, clustering rate, interstitial emission and sink rates on grain boundaries on the gas bubble evolution are systematically simulated. A set of model parameters (defect generation rate, clustering rate, interstitial emission and sink rates) is determined by comparing measured and simulated gas bubble swelling kinetics. The results demonstrate that interstitial clustering is one of the important physical mechanisms which results in a fast gas bubble swelling kinetics in the recrystallization zone. The developed model can also be extended to study the associated growth of defect and second phase precipitates often observed in irradiated materials.

Hu, Shenyang↗

Nondestructive measurements of residual 235 U mass of Israeli Research Reactor-1 fuel using the Advanced Experimental Fuel Counter

In 2018, a measurement campaign took place with participants from Los Alamos National Laboratory (LANL), the Nuclear Research Centre-Negev (NRCN) and Soreq Nuclear Research Center (SNRC) at the Israeli Research Reactor-1 (IRR-1) in which 14 of the reactor’s used fuel assemblies (FAs) with varied amount of depletion were measured with the nondestructive assay instrument Advanced Experimental Fuel Counter (AEFC). Designed for safeguards purposes, the AEFC measures both neutrons emitted from the FA (passive neutrons) and fission neutrons induced by an external neutron source (in this experiment, 252 Cf). Signals recorded with the AEFC include total neutron count rates (Singles), time-correlated neutron count rates (Doubles), and total gamma-ray count rates. The 235 U content of the FAs was previously assessed by two independent methods: (1) measurement of the transparency of the FA to low-energy gamma rays from an activated rhenium source (rhenium gamma transmission, or the RGT method) and (2) calculation of the 30-year burnup history of the core using detailed three-dimensional Monte-Carlo core depletion calculations. The results from the FAs that had been measured via the RGT method were used to construct the calibration curves, which translate the AEFC count rates to 235 U mass. Then, the calibration was evaluated using AEFC measurements of six additional FAs that were not measured via the RGT method. From the results, it was determined the Doubles calibration curve was more reliable than that of the Singles and follows a simple second-order polynomial fit for the whole range of residual 235 U mass content, albeit with larger statistical uncertainty. Detailed uncertainties quantification was conducted for both the AEFC Singles and Doubles. This includes the analysis of statistical uncertainties, calibration uncertainty, and random uncertainties due to the sensitivity of the AEFC to several sources of uncertainty, namely the FA position, FA orientation, interrogation source position, and ambient pool temperature. Finally, an overall total uncertainty of 6 g of 235 U is estimated for the Singles and Doubles, which is mainly due to calibration uncertainty (for the Singles) and statistical uncertainty (for the Doubles), and which constitutes 3%–6% of the 235 U total mass in the FAs, depending on their level of depletion.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Laser ablation spectrometry for studies of uranium plasmas, reactor monitoring, and spent fuel safety

Nuclear security is one of the defining challenges of our time. Nuclear threats range from deliberate dispersal of radioactive material to contaminate the vital infrastructure to diversion and smuggling of special nuclear material for clandestine nuclear programs and nuclear terrorism, respectively. There is an associated need to develop and sustain the nuclear forensics capabilities, which requires the understanding of complex processes that occur in plasmas of nuclear materials. The area of nuclear safety has seen a resurgence of public interest, and there is a concomitant need to safely store used nuclear fuel and detect structural material failure in nuclear power systems, especially in innovative reactor designs envisioned for future adoption. Laser-produced plasmas are complicated extreme environments that can generate intense and rich, highly specific signatures of nuclear and radiological materials, which can then be explored in a wide range of applications. They include interdiction and rapid detection of nuclear materials, including their isotopic composition, detection over long distances, laboratory simulation of weapons effects, monitoring the condition of structural materials in dry cask storage containers, and novel instrumentation for nuclear power systems. We present a compilation of recent representative examples of the application of laser spectroscopy, and laser-induced breakdown spectroscopy in particular, to nuclear safety and security problems. A case is made that spectroscopic techniques based on laser-produced plasmas offer complementary, and sometimes unique, capabilities that motivate the continued exploration of their efficient production and understanding of the signatures they produce

(020.3260) Isotope shifts, (140.3440) Laser-induce↗

A new neutron time-of-flight detector for fuel-areal-density measurements on OMEGA

A new neutron time-of-flight (nTOF) detector for fuel-areal-density measurements in cryogenic DT implosions was installed on the OMEGA Laser System. The nTOF detector has a cylindrical thin-wall, stainless-steel, 8-in.-diam, 4-in.-thick cavity filled with an oxygenated liquid xylene scintillator. Four gated photomultiplier tubes (PMTs) with different gains are used to measure primary DT and D{sub 2} neutrons, down-scattered neutrons in nT and nD kinematic edge regions, and to study tertiary neutrons in the same detector. The nTOF detector is located 13.4 m from target chamber center in a well-collimated line of sight. The design details of the nTOF detector, PMT optimization, and test results on OMEGA will be presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Effect of Ni content on the morphological evolution of Ni-YSZ solid oxide fuel cell electrodes

The coarsening of Ni in Ni–yttria-stabilized zirconia (YSZ) anodes is a potential cause of long term solid oxide fuel cells (SOFC) performance degradation. The specifics of the Ni-YSZ structure—including Ni/YSZ ratio, porosity, and particle size distributions—are normally selected to minimize anode polarization resistance, but they also impact long-term stability. A better understanding of how these factors influence long-term stability is important for designing more durable anodes. The effect of structural details, e.g., Ni-YSZ ratio, on Ni coarsening has not been quantified. Furthermore, prior measurements have been done by comparing evolved structures with control samples, such that sample-to-sample variations introduce errors. Here in this paper, we report a four dimensional (three spatial dimensions and time) study of Ni coarsening in Ni-YSZ anode functional layers with different Ni/YSZ ratios, using synchrotron x-ray nano-tomography. The continuous structural evolution was observed and analyzed at sub-100 nm resolution. It is shown quantitatively that increasing the Ni/YSZ ratio increases the Ni coarsening rate. This is due to both increased pore volume and a decrease in the YSZ volume fraction, such that there is more free volume and a less obtrusive YSZ network, both of which allow greater Ni coarsening. The results are shown to be in good agreement with a power-law coarsening model. In conclusion, the finding is critical for informing the design of SOFC electrode microstructures that limit coarsening and performance degradation.

36 MATERIALS SCIENCE↗

Thermal, mechanical, and electrical properties of LSCo/mullite composite contact materials for solid oxide fuel cells

Lanthanum strontium cobaltite (LSCo) is considered as a good candidate cathode contact material for solid oxide fuel cells, due to high electrical conductivity. However, LSCo has a very large coefficient of thermal expansion (CTE) than the cells and metallic interconnects. As a result, poor mechanical stability is expected during thermal cycling. To minimize the CTE mismatch, we investigate a composite approach involving mixing LSCo with an inert material of low CTE, such as mullite at volume fractions from 0.1 to 0.4. Composite’s CTE shows a decreasing trend with increasing mullite volume fractions, and is consistent with model predictions. X-ray powder diffraction analysis of sintered LSCo/mullite composites exhibits no presence of other phases for samples aged for 500h at 800oC, indicating chemical compatibility. Electrical conductivity by a 4-pt method shows a decreasing trend with increasing mullite content. Contact strength of as-sintered and thermally cycled samples show that only the composite with 0.4 volume fraction has a measurable strength; the other composites have no strength. Overall, the composite approach is demonstrated in the LSCo/mullite system to lower the CTE and hence achieve thermal cycle stability. The addition of the inert phase to the LSCo matrix; however, also reduces the electrical conductivity.

Contact materials, LSCo, mullite, CTE, electrical ↗

Investigating instabilities in a Rotating Detonation Combustor Operating with Natural Gas-Hydrogen Fuel Blend – Effect of Air Preheat and Annulus Width

Propagation characteristics of a detonation wave in an air-breathing Rotating Detonation Combustor (RDC) using natural gas-hydrogen fuel blends is presented in this paper. Short duration (~up to 6s) experiments were performed on a 152.4mm OD uncooled RDC with two different annulus gap widths (5.08mm and 7.62mm) over a range of equivalence ratios (0.6–1.0) at varying inlet air temperatures (~65°C-204°C) and natural gas content (up to 15%) with pre-combustion operating pressure slightly above ambient.It was observed that the RDC, with an annulus gap width of 5.08mm, was inherently unstable when natural gas (NG) was added to the hydrogen fuel while operating at pre-combustion pressures near ambient and at an inlet air temperature of 65°C. Increasing the annulus gap width to 7.62mm improved the stability of the detonation wave at similar temperatures and pressure permitting operation with as much as 5% NG by volume. While observed speeds of the detonation waves were still below theoretical values, an increase in inlet air temperature reduced the variability in wave speed. The frequency analysis thus explored in this study is an effort to quantify detonation instability in an RDC under varying operational envelope. The data presented is relevant towards developing strategies to sustain a stable detonation wave in an RDC using natural gas for land based power generation.

Roy, Arnab↗

Characterization of a Sulfonated Poly(Ionic Liquid) Block Copolymer as an Ionomer for Proton Exchange Membrane Fuel Cells using Rotating Disk Electrode

Ionic liquid (IL) additives to both traditional and advanced oxygen reduction reaction (ORR) electrocatalysts have yielded remarkable improvements in catalyst performance and durability. However, incorporating ILs or IL-modified catalysts into the electrodes of a proton exchange membrane fuel cell (PEMFC) membrane electrode assembly (MEA) has proven to be challenging. Sulfonated poly(ionic liquid) block copolymers (S-PILBCP) present an opportunity to incorporate IL functionality directly into the ionomer, orthogonal to protonic conductivity. Here, we use a rotating disc electrode (RDE) to characterize the interface between a S-PILBCP and Pt catalyst in comparison to Nafion. Catalyst thin films prepared with S-PILBCP show an 80% improvement in the ORR activity over those containing Nafion. Thin films of S-PILBCP also show a significantly reduced degree of poisoning sulfonate adsorption on a Pt(111) surface in comparison to Nafion. Furthermore, these half-cell results provide useful insights that help to highlight the source of the impact of the S-PILBCP on PEMFC MEA performance.

25 ENERGY STORAGE↗

Optimizing the fuel efficiency of an opposed piston engine for electric power generation

This paper investigates the optimal crankshaft motion for an opposed piston (OP) engine in a novel hybrid architecture to maximize fuel efficiency. The OP engine was selected for this work due to its inherent thermodynamic benefits and the balanced nature of the engine which can achieve downsizing through reducing the number of cylinders rather than the individual cylinder volume. The typical geartrain required on an OP engine was exchanged for two electric motors, reducing friction loss and decoupling the crankshafts. Using the motors to control the crankshaft motion profiles, this architecture introduces capabilities to dynamically vary compression ratio, combustion volume, and scavenging dynamics. To leverage these opportunities, an optimization scheme was developed utilizing nonlinear optimization of a 0-D model to compute the crankshaft motion profile that maximizes the work generated by the system. This optimization was then iteratively coupled with a high fidelity model which supplies the cylinder flow boundary conditions. This iterative approach reduces the model complexity used in the optimal control problem (OCP) while capturing the gas exchange dynamics critical to the 2-stroke cycle of the OP engine. By using the rate of change of motor torque as the input to the OCP, the torque fluctuation in a single cycle can be limited to ensure tracking feasibility. The results show crankshaft velocity slows during the compression stroke and conversely accelerates during the expansion stroke, reducing the peak motor torque required for control and thus reducing the motor losses. The extended residence time at top dead center, however, leads to an increase in heat transfer, illustrating the trade-off between the work extraction efficiency and the indicated engine efficiency.

Engineering↗