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Peer Review Comments on the Authorized Limits Technical Document (OREM-19-2573) for Disposal of Waste Containing Residual Radioactive Material at the U.S. Department of Energy Industrial Landfill IV, Y-12 National Security Complex, Oak Ridge, Tennessee

Argonne National Laboratory is assigned responsibility by DOE/EM-4 to conduct a peer review of the proposed Authorized Limits (ALs) for disposal of waste containing residual radioactive material at the U.S. Department of Energy (DOE) Industrial Landfill IV, Y-12 National Security Complex, Oak Ridge, Tennessee. The ALs document package (Document Number OREM-19-2573, dated May 2020) was sent to Argonne by DOE on June 1, 2020 (Oak Ridge 2020a). Argonne started the review immediately and held several BlueJeans meetings with Oak Ridge and DOE to discuss review comments. The first BlueJeans meeting was June 17, 2020. Oak Ridge presented a briefing of the AL package, followed by discussion of the assumptions, methodology, and parameters used in the analysis. A follow-up BlueJeans meeting was held on June 24, 2020, at which Argonne presented both general and specific review comments in PowerPoint slides. This set of slides - Review Comments on the “Authorized Limits for Disposal of Waste Containing Residual Radioactive Material at DOE Industrial Landfill IV, Y-12 National Security Complex, Oak Ridge, Tennessee” - was then emailed to Oak Ridge and DOE after the BlueJeans meeting on June 24, 2020. A PDF version of this slide set is included as Appendix A.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Segmented Gamma Scanner for Radioactive Waste Assessment: A User Guide

Radioactive waste assessment is important for ensuring nuclear material security at various types of facilities, such as enrichment, fuel fabrication, and reprocessing plants. The waste generated at such nuclear facilities is stored in standard containers and is required to be characterized for material-accounting purposes. The segmented gamma scanner system is a popular, nondestructive analysis measurement system used for characterizing nuclear material, including radioactive waste. This document provides guidance on how to achieve effective performance from a segmented gamma scanner system for accurately quantifying fission products, activation products, and transuranic wastes.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the Idaho National Laboratory Classified Mockup Low-Level Waste at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation (UDQE) assesses whether the Idaho National Laboratory (INL) Classified Mockup Low-Level Waste (LLW) (INEL208599QR0, Revision 0 [INL 2020]) is suitable for shallow land burial (SLB) at the Area 5 Radioactive Waste Management Site (RWMS) on the Nevada National Security Site (NNSS). Disposal of the INL Classified Mockup LLW meets all performance objectives of U.S. Department of Energy (DOE) Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P (DOE 1999). The INL Classified Mockup LLW stream is recommended for acceptance without conditions.

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Fiscal Year 2020 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada

U.S. Department of Energy Standard DOE-STD-5002-2017, “Disposal Authorization Statement and Tank Closure Documentation,” requires preparation of an Annual Summary Report comparing low-level radioactive waste disposal facilities operations with the Disposal Authorization Statement (DAS) and its supporting technical documents including the performance assessment (PA) and the composite analysis (CA). The fiscal year (FY) 2020 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) was prepared by reviewing planned and discovered changes, waste receipts, monitoring results, research and development (R&D) results, and the status of DAS conditions and issues to assess the validity of the DASs, PAs, and CAs.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the Idaho National Laboratory Routinely Generated Remote Handled Low-Level Waste at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation assesses whether the Idaho National Laboratory Routinely Generated Remote Handled Low-Level Waste (NEID09MFCRLLW, Revision 7) is suitable for shallow land burial at the Area 5 Radioactive Waste Management Site on the Nevada National Security Site. Disposal of the INL Routinely Generated Remote Handled LLW meets all performance objectives of DOE Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P. The INL Routinely Generated Remote Handled LLW is recommended for acceptance without conditions.

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Assessing the Potential for Inadvertent Human Intrusion at the Area 3 and Area 5 Radioactive Waste Management Sites on the Nevada National Security Site, Nye County, Nevada

This paper recommends an approach to inadvertent human intrusion (IHI) at the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) on the Nevada National Security Site (NNSS). IHI analysis uses the consequences of an individual inadvertently contacting buried waste to set waste concentration limits for near-surface disposal of low-level radioactive waste (LLW). Regulatory agencies are increasingly applying risk-informed decision-making to LLW waste management (NRC 2006). Risk-informed decision-making combines scientific risk assessment with stakeholder values and perceptions to determine a level of acceptable risk. Risk considers not only the consequences of an event, but also its probability of occurring.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the TRU Waste Processing Center Mixed Low Level Waste at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation (UDQE) assesses whether the U.S. Department of Energy (DOE), National Nuclear Security Administration (NNSA) Transuranic (TRU) Waste Processing Center Mixed Low Level Waste (MLLW), FWORCHMLLW103, Revision 13 [TWPC 2021]), is suitable for shallow land burial (SLB) at the Area 5 Radioactive Waste Management Site (RWMS) on the Nevada National Security Site (NNSS). Disposal of the TRU Waste Processing Center MLLW meets all performance objectives of DOE Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P (DOE 1999). The TRU Waste Processing Center MLLW waste stream is recommended for acceptance without conditions.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the Idaho National Laboratory Classified Mockup Low-Level Waste, Revision 1, at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation (UDQE) assesses whether the Idaho National Laboratory (INL) Classified Mockup Low-Level Waste (LLW) (INEL208599QR0, Revision 1 [INL 2021]) is suitable for shallow land burial (SLB) at the Area 5 Radioactive Waste Management Site (RWMS) on the Nevada National Security Site (NNSS). Disposal of the INL Classified Mockup LLW meets all performance objectives of U.S. Department of Energy (DOE) Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P (DOE 1999). The INL Classified Mockup LLW stream is recommended for acceptance without conditions.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the Princeton Plasma Physics Laboratory Torus Cleanup System Molecular Sieve Dryer Bed at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation (UDQE) assesses whether the Princeton Plasma Physics Laboratory (PPPL) Torus Cleanup System Molecular Sieve Dryer Bed (MSDB), PERM000000043, Revision 0 (Perma-Fix [PERM] 2021), is suitable for shallow land burial (SLB) at the Area 5 Radioactive Waste Management Site (RWMS) on the Nevada National Security Site (NNSS). Disposal of the PPPL Torus Cleanup System MSDB meets all performance objectives of DOE Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P (DOE 1999). The PPPL Torus Cleanup System MSDB waste stream is recommended for acceptance without conditions.

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UNREVIEWED DISPOSAL QUESTION EVALUATION: Disposal of the Transuranic Waste Processing Center Low-Level Waste at the Area 5 Radioactive Waste Management Site, Nevada National Security Site, Nye County, Nevada

This Unreviewed Disposal Question Evaluation (UDQE) assesses whether the Transuranic Waste Processing Center (TWPC) Low-Level Waste (LLW), FWORCHLLW0102, Revision 12 (TWPC 2021), is suitable for shallow land burial (SLB) at the Area 5 Radioactive Waste Management Site (RWMS) on the Nevada National Security Site (NNSS). Disposal of the TWPC LLW meets all performance objectives of DOE Manual DOE M 435.1-1, Radioactive Waste Management Manual, Chapter IV, Section P (DOE 1999). The TWPC LLW waste stream is recommended for acceptance without conditions.

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Radioactive Source Localization via Bayesian Particle Filter

In the event of a misplaced radioactive source or other emergency situation, measuring a radiation field, mapping its distribution, and determining a source location are essential tasks to ameliorating the situation. However, radiation fields may be extremely hazardous to human surveyors and minimizing received radiation doses is just as essential. Robots appear to be a potential solution to these problems. Beyond simply measuring radiation, the robot's computer processing capabilities offer a way to apply complex data analysis methods to radiation measurements in real-time. Methods which predict likely source locations can then feed this information into other processes, potentially improving path planning and enabling more efficient measurements. Given a robot mounted with a gamma-ray detector, can we: develop a methodology to account for detector performance across a wide range of source angles, distances, and photon energies? operate an autonomously navigating robot to effectively survey and characterize an area of interest? implement a data analysis method, conventionally used in measurements of motion, for source localization purposes? An open-source TurtleBot 3 robot, running Robot Operating System (ROS) on Ubuntu 16.04 LTS, was fitted with a Kromek GR1{sup R} Cadmium Zinc Telluride (CZT) solid-state gamma-ray detector. As a part of ROS, the packages OpenSlam, gmapping, and amcl were used to perform Simultaneous Localization and Mapping (SLAM), determining the robot's position and mapping the surrounding area. Data was acquired via Lidar mounted on top the TurtleBot 3. Detector Calibration Fit: The equation was fit to 365 counts of various energies, distances, and angles. A MATLAB{sup R} program was written to simulate measurements taken a robot on a random walk, with count data and positions discretized into finite element pixels. Using this program, a sample of 100 runs was performed on a map with a simulated source at the center, with a total of 200 of 2 pixels each. Similarly, multiple runs of the filter were performed on recorded robot measurement data. In both simulation and real tests, when corrected for errors (particles placed outside of bounds or on the robot, and simulation-specific errors), corresponding t-tests of predicted x and y-coordinates were within a 95% confidence interval of the actual position. For the real trial, these positions are slightly skewed right in the x-axis as the robot remained mainly to the left side of the source within the sample area. These simulations demonstrate potential validity for the usage of a particle filter as method of radioactive source localization. In the future, true real-time implementation and data fusion may further augment the performance of the robot to localize lost sources. Additionally, identification of multiple sources, determination of source types, and usage of a collimator are areas to potentially be explored.

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National nuclear forensics libraries: a case study on benefits and possibilities for identification of sealed radioactive sources

A National Nuclear Forensic Library (NNFL) is a useful nuclear forensics tool which consists of information and subject matter expertise on radioactive and nuclear (RN) materials produced, used or stored within a State. If RN material is found out of regulatory control the NNFL can be used as part of a nuclear forensics investigation to help identify whether or not the material is consistent with a country’s national holdings. In previous work, a number of signatures which can be useful to identify sealed sources of 241 Am were investigated. To validate the measurement results, an official query concerning information about two of the previously investigated 241 Am sources was sent to the United States Department of State, the international point-of-contact (POC) for the U.S. NNFL. The aim of this work is to show how data obtained in a characterization of a radioactive source can be used in conjunction with an NNFL to investigate the history of a source out of regulatory control.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Analysis of Glycolate in Radioactive Waste by Ion Chromatography (IC) and Proton Nuclear Magnetic Resonance (H NMR)

Here, in preparation for implementing the Nitric-Glycolic (NG) acid flowsheet for the Savannah River Site (SRS) Liquid Waste System (LWS), analytical methods for determining glycolate at low concentration, below 20 mg/L in radioactive samples, were developed to support system management and safety. To accommodate the wide range of LWS matrix conditions, two alternative methods were developed, refined, and demonstrated for glycolate analysis in radioactive waste samples: ion chromatography (IC) and a proton nuclear magnetic resonance (H NMR). Investigators validated IC and H NMR methods for glycolate analysis, defined the range of applicability, and demonstrated key supporting analytical protocols. The deployed IC method is applicable in low to moderate ionic strength samples and requires sample pretreatment using a Dionex OnGuard II H + cartridge. The deployed H NMR method is more labor intensive but provides options for a broader range of matrices. Based on the results, high quality glycolate analysis of the Defense Waste Processing Facility (DWPF) condensate in Tank 22 is feasible by IC down to approximately 12 mg/L. Using H NMR, glycolate may be determined to 8 mg/L or lower depending on the run time with the potential for broader applicability of the method to higher ionic strength conditions in other tanks of the SRS LWS.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Development, feasibility, and uncertainty of radioactive 22 Na tracer dilution and gamma spectroscopy for mass determination of molten salt for pyroprocessing spent nuclear fuels

Accurate knowledge of the total mass of molten salts both for pyroprocessing spent nuclear fuels and for molten salt reactors is necessary for safeguards purposes. However, it is challenging to know or measure the total mass of molten salt due to the complicated shapes as well as the compositional—and thus density—changes that occur over time during operation. Here, we investigated radioactive tracer dilution (RTD) as a potential safeguards technique for application to the total mass measurement of LiCl–KCl–UCl 3 salt used for uranium electrorefining, with a focus on the feasibility, uncertainty, and fission product effect of RTD for salt mass measurement. To this end, experimental-scale RTD tests (600–700 g of total mass) were initially carried out by adding 22 Na tracer salt into LiCl–KCl salt containing 0, 5, and 28wt% radioactive salts from an electrorefiner (ER) for refining uranium. Upon the completion of the experimental-scale RTD tests, we performed a scale-up RTD test by directly adding 22 Na tracer salts to the ER, which uses about 12 kg of LiCl–KCl–UCl 3 salt during normal operation. This paper reports the main features of RTD for total mass measurement of molten salt and summarizes the results of the experimental-scale and scale-up RTD tests.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron Capture Cross Sections of Radioactive Nuclei

Alternative methods to calculate neutron capture cross sections on radioactive nuclei are reported using the theory of Inclusive Non-Elastic Breakup (INEB) developed by Hussein and McVoy. The statistical coupled-channels theory proposed in Ref. [2] is further extended in the realm of random matrices. The case of reactions with the projectile and the target being twocluster nuclei is also analyzed and applications are made for scattering from a deuteron target. An extension of the theory to a three-cluster projectile incident on a two-cluster target is also discussed. The theoretical developments described here should open new possibilities to obtain information on the neutron capture cross sections of radioactive nuclei using indirect methods.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Simulation of radioactive plume transport in the atmosphere including dynamics of particle aggregation and breakup

Accurate prediction of the atmospheric transport of debris particles relies heavily on our knowledge of the size distribution of the particles within a debris cloud. Assuming a fixed particle size during simulations is not always viable since the size distribution of the debris can change during transport. Various microphysical processes, such as aggregation and breakup, influence debris particles and dictate any changes to the size distribution. To track those changes that can occur, a population balance model can be adopted and instituted within a model framework. Nonetheless, many of the models that simulate the transport of radioactive debris following a device-driven fission incident have historically neglected to consider these processes. As such, this work describes our effort to develop a modeling framework capable of simulating the transport and deposition of a radioactive plume generated from a fission incident with a dynamic population balance including particle aggregation and breakup. Herein the impact of aggregation and breakup, individually and collectively, on the particle size distribution is explored using the developed framework. When simulating aggregation, for example, six mechanisms, including Brownian coagulation, the convective enhancement to Brownian coagulation, van der Waals-viscous force correction for Brownian coagulation, gravitational collection, turbulent inertial motion, and turbulent shear, are considered. Brownian coagulation and its corrections have, as one would expect, a large impact on relatively small aggregates. Aggregates with a diameter that is less than or equal to 1.0 μm, for instance, comprise 50.6 vol % of all aggregates in the absence of aggregation and 31.2 vol % when Brownian coagulation and its corrections are considered. Gravitational collection and, to a much lesser extent, turbulent shear and turbulent inertial motion are, conversely, of great importance to relatively large aggregates (i.e., diameter greater than 3.0 μm). Additionally, the individual effects of atmospheric and particle parameters, such as wind speed and particle density, are examined. Of the parameters examined, turbulent energy dissipation and aggregate fractal dimension (i.e., aggregate shape with lower values representing more irregular particles) were of substantial importance since both terms directly impact aggregate stability and, by extension, the breakup rate. Large-scale transport and deposition simulations in a dry atmosphere are also presented and discussed as a proof of concept.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Strategy to safely enable X-ray computed tomography examination of highly radioactive tristructural isotropic nuclear fuel

Nondestructive post-irradiation examination of nuclear fuels and materials is useful in collecting data to inform commercial licensing of new nuclear concepts. This work details the planning, shielding design, and workflow of an X-ray computed tomography examination of an irradiated AGR-5/6/7 fuel compact with a dose rate of 1318 R/hr on contact from both β and ɤ-ray radiation with 120 R/hr of the dose rate coming exclusively from ɤ-rays. Post-irradiation examination of highly radioactive samples can help reduce the timeframe from conceptualization of novel nuclear concepts to their commercial implementation as not only is less time spent waiting for experiments to decay away to acceptable levels for examinations, but data from these experiments can more quickly inform model efforts and subsequent experiments. While this work represents the hottest radiological sample that has been openly transported and examined at Idaho National Laboratory’s Irradiated Materials Characterization Laboratory to date, it is anticipated that this work and its lessons learned will facilitate future examinations of similar or even more radioactive specimens.

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