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Modeling of the AGR 3/4 PIE Experiments

TRISO Fuel Accident Scenarios Transport of Fission Products (FP) through modern nuclear-grade graphites is not well established The AGR 3/4 experimental results need to be modeled to extract FP transport characteristics A finite element model using graphite diffusivities from IAEA TECDOC-978 is compared against measured results

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Enhancing Post-Irradiation Examination (PIE) Efficiency with High-Throughput Experiments

Nuclear materials testing is essential for understanding changes in reactor environments, but traditional methods are costly and time-consuming. High-Throughput Experimentation (HTE) enables rapid screening and optimization of material properties by significantly increasing the number of specimens in the experiment. In this work, HTE methods were employed to irradiate novel materials at the Advanced Test Reactor (ATR) at Idaho National Laboratory. A total of 367 sub-sized tensile specimens were irradiated using the standard capsule design. To facilitate HTE, automated systems such as the Automated Mechanical Testing System were implemented for mechanical testing within hot cell environments, thereby reducing the need for manual interaction with hot cell manipulators and significantly lowering both the cost and duration of experiments. Digital image correlation (DIC) was used to measure displacement during mechanical testing, providing precise, non-contact measurement capabilities. The methodologies developed in this research will support the advancement of HTE techniques for future nuclear materials testing experiments at ATR. This approach allows for more efficient and cost-effective evaluation of new materials, ultimately leading to improved reactor performance, enhanced safety, and extended longevity within the nuclear industry.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

Critical Assessment of Photoionization Efficiency Measurements for Characterization of Soot-Precursor Species

We present a critical evaluation of photoionization efficiency (PIE) measurements coupled with aerosol mass spectrometry for the identification of condensed soot-precursor species extracted from a premixed atmospheric-pressure ethylene/oxygen/nitrogen flame. Definitive identification of isomers by any means is complicated by the large number of potential isomers at masses likely to comprise particles at flame temperatures. This problem is compounded using PIE measurements by the similarity in ionization energies and PIE-curve shapes among many of these isomers. Nevertheless, PIE analysis can provide important chemical information. For example, our PIE curves show that neither pyrene nor fluoranthene alone can describe the signal from C 16 H 10 isomers and that coronene alone cannot describe the PIE signal from C 24 H 12 species. A linear combination of the reference PIE curves for pyrene and fluoranthene yields good agreement with flame-PIE curves measured at 202 u, which is consistent with pyrene and fluoranthene being the two major C 16 H 10 isomers in the flame samples, but does not provide definite proof. The suggested ratio between fluoranthene and pyrene depends on the sampling conditions. We calculated the values of the adiabatic-ionization energy (AIE) of 24 C 16 H 10 isomers. Despite the small number of isomers considered, the calculations show that the differences in AIEs between several of the isomers can be smaller than the average thermal energy at room temperature. The calculations also show that PIE analysis can sometimes be used to separate hydrocarbon species into those that contain mainly aromatic rings and those that contain significant aliphatic content for species sizes investigated in this study. Our calculations suggest an inverse relationship between AIE and the number of aromatic rings. We have demonstrated that further characterization of precursors can be facilitated by measurements that test species volatility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improved sample utilization in thermal ionization mass spectrometry isotope ratio measurements: refined development of porous ion emitters for nuclear forensic applications

The precise and accurate determination of isotopic composition in nuclear forensic samples is vital for assessing origin, intended use and process history. Thermal ionization mass spectrometry (TIMS) is widely accepted as the gold standard for high performance isotopic measurements and has long served as the workhorse in the isotopic ratio determination of nuclear materials. Nuclear forensic and safeguard specialists have relied heavily on such methods for both routine and atypical e orts. Despite widespread use, TIMS methods for the assay of actinide systems continue to be hindered by poor ionization e ciency, often less than tenths of a percent; the majority of a sample is not measured. This represents a growing challenge in addressing nextgeneration nuclear detection needs by limiting the ability to analyze ultratrace quantities of high priority elements that could potentially provide critical nuclear forensic signatures. Porous ion emitter (PIE) thermal ion sources were developed in response to the growing need for new TIMS ion source strategies for improved ionization e ciency, PIEs have proven to be simple to implement, straightforward approach to boosting ion yield. This work serves to expand the use of PIE techniques for the analysis of trace quantities of plutonium and americium. PIEs exhibited superior plutonium and americium ion yields when compared to direct lament loading and the resin bead technique, one of the most e cient methods for actinide analysis, at similar mass loading levels. Initial attempts at altering PIE composition for the analysis of plutonium proved to enhance sample utilization even further. Preliminary investigations of the instrumental fractionation behavior of plutonium and uranium analyzed via PIE methods were conducted. Data collected during these initial trial indicate that PIEs fractionate in a consistent, reproducible manner; a necessity for high precision isotope ratio measurements. Ultimately, PIEs methods were applied for the age determination of various uranium isotopic standards. PIEs did not exhibit signi cant advantages for the determination of model ages when compared to traditional laments; however, this trial was able to provide valuable insight for guiding future investigations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An Eco-friendly Porous Poly(imide-ether)s for the Efficient Removal of Methylene Blue: Adsorption Kinetics, Isotherm, Thermodynamics and Reuse Performances

Poly(imide-ether)s (PIEs), which is porous in nature, was synthesized using aromatic diamines and dianhydrides via the solution polycondenzation reaction. In the process, PIEs was used as an adsorbent for the removal of basic dye [Methylene blue (MB)] from the aqueous solution. The structure and the thermal stability of PIEs were characterized by FT-IR, {sup 1}H-NMR, XRD and TG analysis, and the adsorption behaviour of the PIEs was confirmed using UV/Visible, FT-IR and SEM with EDX analysis. Batch adsorption experiments were carried out and their parameters (pH 6.95), initial MB concentration (200 mg/L), adsorbent dosage (50 mg), contact time (120 min) and temperature (28 °C) were optimized. The batch adsorption experimental data of the effect of contact time, initial MB concentration and temperature were evaluated using the adsorption kinetics (Pseudo-first order, Pseudo-second order, Elovich and Intra-particle diffusion kinetic), isotherm (Langmuir, Freundlich, Redlich–Peterson and Sips isotherms) and thermodynamic models respectively. In the study, adsorption of MB onto PIEs followed Pseudo-second kinetics and found to be the best fitting model based on the obtained experimental data. The homogeneity and heterogeneity surface nature of PIEs were elucidated with two and three isotherm parameters respectively. The adsorption thermodynamic study indicates that the adsorption of MB onto PIEs was endothermic and spontaneous in nature. The adsorbed PIEs solid waste was utilized to prepare the polymer composite, and its property was characterized. Graphical Abstract: .

54 ENVIRONMENTAL SCIENCES↗

Enhanced ionization efficiency in TIMS analyses of plutonium and americium using porous ion emitters

Investigations of enhanced sample utilization in thermal ionization mass spectrometry (TIMS) using porous ion emitter (PIE) techniques for the analyses of trace quantities of americium and plutonium were performed. Repeat ionization efficiency (i.e., the ratio of ions detected to atoms loaded on the filament) measurements were conducted on sample sizes ranging from 10–100 pg for americium and 1–100 pg for plutonium using PIE and traditional (i.e., a single, zone-refined rhenium, flat filament ribbon with a carbon ionization enhancer) TIMS filament sources. When compared to traditional filaments, PIEs exhibited an average boost in ionization efficiency of ~550% for plutonium and ~1100% for americium. A maximum average efficiency of 1.09% was observed at a 1 pg plutonium sample loading using PIEs. Supplementary trials were conducted using newly developed platinum PIEs to analyze 10 pg mass loadings of plutonium. As a result, platinum PIEs exhibited an additional ~134% boost in ion yield over standard PIEs and ~736% over traditional filaments at the same sample loading level.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Limits on Achievable Dimensional and Photon Efficiencies with Intensity-Modulation and Photon-Counting Due to Non-Ideal Photon-Counter Behavior

An ideal intensity-modulated photon-counting channel can achieve unbounded photon information efficiencies (PIEs). However, a number of limitations of a physical system limit the practically achievable PIE. In this paper, we discuss several of these limitations and illustrate their impact on the channel. We show that, for the Poisson channel, noise does not strictly bound PIE, although there is an effective limit, as the dimensional information efficiency goes as e[overline] e PIE beyond a threshold PIE. Since the Holevo limit is bounded in the presence of noise, this illustrates that the Poisson approximation is invalid at large PIE for any number of noise modes. We show that a finite transmitter extinction ratio bounds the achievable PIE to a maximum that is logarithmic in the extinction ratio. We show how detector jitter limits the ability to mitigate noise in the PPM signaling framework. We illustrate a method to model detector blocking when the number of detectors is large, and illustrate mitigation of blocking with spatial spreading and altering. Finally, we illustrate the design of a high photon efficiency system using state-of-the-art photo-detectors and taking all these effects into account.

quantum limited communications↗

Post Irradiation Examination Results of Irradiated Yttrium Hydride

Department of Energy’s (DOE’s) Microreactor program (MRP) aims to provide the fundamental data to enable the development of microreactors. As such, material property data of critical materials for microreactor technologies are researched. Because substoichiometric yttrium dihydride (YHx, where x<2) is considered as a potential solid neutron moderator, its material property data has been combined in the Advanced Moderator Material Handbook which includes thermodynamic and thermophysical properties of YHx with the exception of irradiated material’s properties due to limited PIE. To fill the knowledge gap for the irradiated YHx, specimens and irradiation capsules were prepared at Los Alamos National Laboratory (LANL). Specimens were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory’s (INL’s). post-irradiation examination (PIE) was performed at INL’s Materials and Fuels Complex (MFC). This report compiles the PIE results of irradiated YHx specimens through fiscal years 2022 and 2023 (FY22-23) . The PIE data will directly be incorporated into the newer version of the Advanced Moderator Material Handbook. The main takeaways include that (i) the geometrical stability and mechanical integrity of YHx was intact with couple exceptions after high-temperature irradiations (600-800°C), (ii) hydrogen content variation due to manufacturing or irradiation in YHx caused visible surface discoloration, that is also related to the microstructural changes, (iii) qualitative comparisons of PIE methods implied that H retention was significantly higher at 600°C as compared to 800°C, (iv) thermal properties included signatures correlated with the H loss or re-gain, (v) importance of manufacturing readiness and initial as-manufactured specimens history was emphasized, (vi) the needs of targeted irradiations focusing on temperature and time parameters and very targeted PIE were specified.

08 HYDROGEN↗

Status Report on Fast Flux Test Facility Mechanistic Fuel Failure Experiment Analysis with BISON for Post Irradiation Examination Support

The renewed interest in metallic U-Zr nuclear fuel alloy has led to a drive for deeper understanding of the mechanisms driving the phenomena observed under irradiation conditions. The Department of Energy Advanced Fuel Campaign has developed infrastructure to support metallic fuel development, including Post Irradiation Examination (PIE) of legacy Fast Flux Test Facility (FFTF) Mechanistic Fuel Failure (MFF) experiments. The PIE performed on legacy FFTF MFF experiments gives insight on metallic fuel performance and can address the lack of knowledge and scarcity of reliable data identified in several studies over recent years. Unfortunately, PIE efforts can cost significant time and resources which can impede the progress of metallic U-Zr fuel development. Metallic U-Zr fuel performance modeling can be used to inform PIE efforts on regions of interest for relevant investigations and can help understand phenomena observed in PIE. This report demonstrates the current progress of FFTF MFF fuel performance simulations using the BISON fuel performance code and discusses the support provided by simulation to PIE efforts. Progress in temperature, profilometry, fission gas release, plenum pressure, and zirconium redistribution simulation results have been demonstrated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Report on the Incorporation of Post-Irradiation Examination Results of Yttrium Hydride for Advanced Moderator Handbook

Department of Energy’s (DOE’s) Microreactor program (MRP) aims to provide the fundamental data to enable the development of microreactors. As such, material property data of critical materials for microreactor technologies are researched. Because substoichiometric yttrium dihydride (YHx, where x<2) is considered as a potential solid neutron moderator, its material property data has been combined in the Advanced Moderator Material Handbook which includes thermodynamic and thermophysical properties of YHx with the exception of irradiated material’s properties due to limited PIE. To fill the knowledge gap for the irradiated YHx, specimens and irradiation capsules were prepared at Los Alamos National Laboratory (LANL). Specimens were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory’s (INL’s). post-irradiation examination (PIE) was performed at INL’s Materials and Fuels Complex (MFC). This report compiles the PIE results of irradiated YHx specimens through fiscal years 2022 and 2023 (FY22-23) . The PIE data will directly be incorporated into the newer version of the Advanced Moderator Material Handbook. The main takeaways include that (i) the geometrical stability and mechanical integrity of YHx was intact with couple exceptions after high-temperature irradiations (600-800°C), (ii) hydrogen content variation due to manufacturing or irradiation in YHx caused visible surface discoloration, that is also related to the microstructural changes, (iii) qualitative comparisons of PIE methods implied that H retention was significantly higher at 600°C as compared to 800°C, (iv) thermal properties included signatures correlated with the H loss or re-gain, (v) importance of manufacturing readiness and initial as-manufactured specimens history was emphasized, (vi) the needs of targeted irradiations focusing on temperature and time parameters and very targeted PIE were specified.

08 HYDROGEN↗

Recent Metallic Fuel Data Recovery in FIPD

The Metallic Fuels Irradiation and Physics Database (FIPD) [1] is an organized collection of metallic fuel test pin data (U-xPu-yZr, = 0 ~ 28; y = 2 ~ 10) and documentation available to industry. FIPD mainly contains three types of data: (1) Fuel pin fabrication data, including fuel slug diameter, fuel slug length, cladding diameter, smear density, etc. (2) Fuel pin operation conditions, including axial distributions for power, temperatures, fluences, burnup, and isotopic densities, etc. and (3) Fuel pin post-irradiation examination (PIE) data, including fission gas release and gas chemistry, profilometry, and neutron radiography, etc. The operating conditions for pins with PIE data available in FIPD span significant ranges across key parameters. The fuel peak burnup extends from less than 5% up to 20 at%. The cladding peak temperature varies from about 490°C to 660°C. Finally, the cladding peak DPA shows a wide range from less than 5 to 120. These broad ranges reflect the diverse testing conditions and operational parameters captured in the available PIE data. More detail about FIPD can be found in ref. [2]. The database development is an ongoing effort covering metallic fuel experiments from the Experimental Breeder Reactor II (EBR-II) and the Fast Flux Test Facility (FFTF). As reported in the ref. [3, 4], most of the PIE data generated during the IFR program [5] has been collected, reviewed, processed, and integrated into FIPD. The most recently added PIE data can be found in ref. [4], which shows the collection of over 95% of the PIE data by the time of this paper. The recent improvements to the database are summarized in this paper.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nondestructive and destructive assay for forensics characterization of weapons-grade plutonium produced in LEU irradiated in a thermal neutron spectrum

A post-irradiation examination (PIE) of an enriched uranium sample was performed to advance a nuclear forensics methodology, based on intra-elemental nuclide ratios. The PIE was carried out on a few milligrams of low enriched uranium dioxide (LEUO 2 ) sample, irradiated to a burnup of 1 GWd/MTU. The PIE of the LEUO 2 sample provided the concentration of selected plutonium and fission product nuclides ( 239 Pu, 240 Pu, 241 Pu, 91 Y, 95 Zr, 95 Nb, 103 Ru, 133 Cs, 134 Cs, 135 Cs, 137 Cs, 136 Ba, 138 Ba, 140 Ba, 140 La, 141 Ce, 144 Ce, 149 Sm, 150 Sm, 152 Sm, 153 Eu, and 154 Eu). The PIE supported validation of the MCNP (Monte Carlo N-Particle neutronics simulation code) predicted concentration of these nuclides in the irradiated LEUO 2 sample. This study showed that most of the MCNP predicted nuclide concentrations were within 15% and several within 10% compared to the PIE results. Furthermore, gamma and mass spectrometry of nuclides in irradiated LEUO 2 enabled the determination of uranium burnup and time since irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Validation environment for AIPS/ALS: Implementation and results

The work is presented which was performed in porting the Fault Injection-based Automated Testing (FIAT) and Programming and Instrumentation Environments (PIE) validation tools, to the Advanced Information Processing System (AIPS) in the context of the Ada Language System (ALS) application, as well as an initial fault free validation of the available AIPS system. The PIE components implemented on AIPS provide the monitoring mechanisms required for validation. These mechanisms represent a substantial portion of the FIAT system. Moreover, these are required for the implementation of the FIAT environment on AIPS. Using these components, an initial fault free validation of the AIPS system was performed. The implementation is described of the FIAT/PIE system, configured for fault free validation of the AIPS fault tolerant computer system. The PIE components were modified to support the Ada language. A special purpose AIPS/Ada runtime monitoring and data collection was implemented. A number of initial Ada programs running on the PIE/AIPS system were implemented. The instrumentation of the Ada programs was accomplished automatically inside the PIE programming environment. PIE's on-line graphical views show vividly and accurately the performance characteristics of Ada programs, AIPS kernel and the application's interaction with the AIPS kernel. The data collection mechanisms were written in a high level language, Ada, and provide a high degree of flexibility for implementation under various system conditions.

Segall, Zary↗

Postirradiation Examination of the ATF-1 Experiments - 2019 Status

A collaborative effort of the Advanced Fuels Campaign together with industry consortia is focused on the development of enhanced accident tolerant fuels for Light Water Reactors (LWRs). The scoping studies, referred to as ATF-1 irradiations, are being performed in the Advanced Test Reactor of Idaho National Laboratory using drop-in style irradiations. The Post-Irradiation Examinations (PIEs) of ATF-1 began in 2017 and continued in 2019. This report describes the results of examinations on ATF-1 irradiations designed to test the performance of advanced iron-based cladding, including compatibility of FeCrAl with UO2, and ATF-1 irradiation of U3Si5. Two rodlets with commercial iron-based cladding and UO2 pellets have been irradiated to low burnup (i.e., < 20 GWd/tHM). The first rodlet had an Alloy33 cladding, while the other had a Kanthal APMT® cladding. The performed PIEs were focused on the determination of fuel microstructure, evaluation of fuel-cladding interaction and irradiation-induced variations of cladding mechanical properties. For both rodlets, no significant changes in the cladding hardness were measured, and the cladding hoop strain remained limited. Gamma tomography revealed no Cs axial migration as expected for LWR fuel, but significant cesium radial migration, which was induced by thermal migration consequent to high irradiation temperatures. Microstructure analyses revealed formation of secondary phases along the pellet rim of samples from both rodlets. No wastage or extensive chemical interaction between the fuel and the internal wall of the cladding was observed, suggesting that the secondary phases accumulated at the pellet rim might be due to formation of Cs-U-O compounds. However, further advanced PIEs are necessary to finally confirm this hypothesis. Optical microscopy analysis of the rodlet designed by Oak Ridge National Laboratory to evaluate the interaction between UO2 and various FeCrAl alloys revealed no extensive interaction in all the samples irradiated in the rodlet. Localized defects, namely circular pitting and cracks of a few tents of microns, were observed on the FeCrAl disc surfaces in some of the diffusion couples. These defects might be surface fabrication defects rather than irradiation-induced localized corrosion, but chemical analyses are needed to determine whether accumulation of corrosive fission products are causing enhanced interaction. Both non-destructive and destructive PIEs were collected on a rodlet containing U3Si5 fuel. The rodlet had extremely low fission gas release, similar to previously analyzed U3Si2 rodlets. Gamma tomography revealed thermo-migration of fission product ruthenium toward the center of the fuel pellet. The fuel microstructure resembles the as-fabricated microstructure, showing extensive microcracking related to the phase transition at 450°C. Two types of secondary phases were observed, which could either be due to segregation and precipitation of fission products or to UN impurities from fabrication. Finally, the current status of PIE on other ATF-1 irradiations will be discussed. These irradiations include UN-U3Si5 rodlets, UN-U3Si2 rodlets and an additional test with U3Si2 fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

2017 Year End Nuclear Science User Facilities (NSUF) Post-Irradiation Examination Summary Report

The Nuclear Science User Facilities (NSUF) are part of a growing number of Department of Energy (DOE) user facilities in the U.S., and is the only national designated nuclear energy user facility. Through a peer-reviewed proposal process, NSUF provides external research teams cost-free access to reactor, post-irradiation examination (PIE) and beamline capabilities at INL and a diverse mix of affiliated partner institutions at universities, national laboratories and industry facilities located across the country. In Fiscal Year 2017 (FY17), the NSUF sponsored planning, management and execution of PIE activities at Idaho National Laboratory (INL), the Center for Advanced Energy Studies (CAES), and other NSUF partner facilities. The individual projects associated with these PIE activities are a result from DOE awards under the following mechanisms: Consolidated Innovative Nuclear Research (CINR) awards that include full sample irradiation and PIE, PIE only (using samples from the NSUF Fuel and Materials Library) awards, or Rapid Turn-Around Experiments (RTE). An accounting of FY17 activities for each project is provided in this report.

36 MATERIALS SCIENCE↗

AGR-5/6/7 Irradiation Disassembly and Metrology First Look

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program was established to perform research and development on tristructural isotropic (TRISO)-coated particle fuel to support deployment of high-temperature gas-cooled reactors (HTGRs), which are graphite-moderated nuclear reactors cooled with helium. This work continues as part of the Advanced Reactor Technologies (ART) TRISO Fuel Program. The overarching program goal is to provide a baseline fuel qualification data set to support licensing, deployment, and operation of HTGRs in the United States. To achieve these goals, the program includes fuel fabrication, irradiations of TRISO fuels and high-temperature materials (e.g., graphite), safety testing and post-irradiation examination (PIE), fuel performance modeling, and fission product transport and source term determination. The ART AGR program has conducted four distinct fuel irradiation experiments in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). The first of these irradiation tests, designated AGR-1, began in ATR in December of 2006 and ended in November 2009. This experiment was primarily to act as a shakedown test of the multi-capsule test train design and to provide early data on fuel performance that would be used in fuel fabrication process development. AGR-1 fuel kernels were produced on an engineering scale, but the TRISO coatings and cylindrical fuel compacts were fabricated on a laboratory scale. The AGR-1 PIE was completed and the final report was published in 2015. The second irradiation test, AGR-2, started in ATR in June 2010 and ended in October 2013. The AGR-2 irradiation test was designed to provide fuel performance data for coated particles fabricated on an engineering-scale pilot line using a coater with an internal chamber diameter of 150 mm (6 in.). The final PIE report was published in 2021. AGR-3/4, a single irradiation that combined what were originally conceived as the third and fourth tests, was to support the refinement of fission product transport models and to assess the effects of sweep gas impurities on fuel performance and fission product transport. PIE of the AGR-3/4 experiment is still in progress as of this writing. The subject of this report is AGR-5/6/7, the final qualification test of AGR TRISO fuel made entirely at the engineering scale.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗