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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A History of Hanford Tank Waste, Implications for Waste Treatment and Disposal

More than 40 years of plutonium processing have left almost 56 million gallons of mixed radioactive waste sequestered in 177 underground tanks on the Hanford Site. Three different processing technologies were employed for plutonium purification in addition to uranium scavenging and fission product removal from the tank waste. All of these chemical processes have contributed to a complex waste stream that varies from tank to tank that presents downstream processing challenges to render the waste into a safe form for long-term storage. The current disposition pathway for Hanford tank waste is vitrification. To maximize waste loading and minimize the number of high-level waste canisters stored in a geologic repository, pretreatment of the waste is required. Both pretreatment and vitrification operations are impacted by the waste composition.

Separations, filtration, ion exchange↗
DOE OSTI2015

On the valence fluctuation in the early actinide metals

In this study, recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f 3 and f 4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f 6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Detection of Breeding Blankets Using Antineutrinos

The Plutonium Management and Disposition Agreement between the United States and Russia makes arrangements for the disposal of 34 metric tons of excess weapon-grade plutonium. Under this agreement Russia plans to dispose of its excess stocks by processing the plutonium into fuel for fast breeder reactors. To meet the disposition requirements this fuel would be burned while the fast reactors are run as burners, i.e., without a natural uranium blanket that can be used to breed plutonium surrounding the core. Here, we discuss the potential application of antineutrino monitoring to the verification of the presence of a breeding blanket. We found that a 36 kg antineutrino detector, exploiting coherent elastic neutrino-nucleus scattering and made of silicon could determine the presence of a breeding blanket at a liquid sodium cooled fast reactor at the 95 percent confidence level within 90 days.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2014

Joint US/Russian Studies of Population Exposures Resulting from Nuclear Production Activities in the Southern Urals

Beginning in 1948, the Soviet Union initiated a program for production of nuclear materials for a weapons program. The first facility for production of plutonium was constructed in the central portion of the country east of the southern Ural Mountains, about halfway between the major industrial cities of Ekaterinburg and Chelyabinsk. The facility now known as the Mayak Production Association and its associated town, now known as Ozersk, were built to irradiate uranium in reactors, separate the resulting plutonium in reprocessing plants, and prepare plutonium metal. The rush to production, coupled with inexperience in handling radioactive materials, lead to large radiation exposures, not only to the workers in the facilities, but also to the surrounding public. Fuel processing started with no controls on releases, and fuel dissolution and accidents in reactors resulted in release of about 37 PBq (1015 Bq) of 131I between 1948 and 1967. Designed disposals of low- and intermediate-level liquid radioactive wastes, and accidental releases via cooling water from tank farms of high-level liquid radioactive wastes, into the small Techa River caused significant contamination and exposures to residents of numerous small riverside villages downstream of the site. Discovery of the magnitude of the aquatic contamination in late 1951 caused revisions to the waste handling regimes, but not before over 200 PBq of radionuclides (with large contributions of 90Sr and 137Cs) were released. Liquid wastes were diverted to tiny Lake Karachay (which today holds over 4 EBq); cooling water was stopped in the tank farms. In 1957, one of the tanks in the tank farm overheated and exploded; over 70 PBq, disproportionately 90Sr, was blown over a large area to the northeast of the site; a large area was contaminated and many villages evacuated. This area today is known as the East Urals Radioactive Trace (EURT). Each of these releases was significant; together they have created a group of cohorts unrivaled in the world for their chronic, low-dose-rate radiation exposure. The 26,000 workers at Mayak were highly exposed to external gamma and inhaled plutonium. A cohort of individuals raised as children in Ozersk is under evaluation for their exposures to radioiodine. The Techa River Cohort consists of over 30,000 people who were born before the start of exposure in 1949 and lived along the Techa River. The Techa River Offspring Cohort consists of about 21,000 persons born to one or more exposed parents of this group - many of whom also lived along the contaminated river. The EURT Cohort consists of about 18,000 people who were evacuated from the EURT soon after the 1957 explosion and another 8000 who remained. These groups together are the focus of dose reconstruction and epidemiological studies funded by the US, Russia, and the European Union to address the question “Are doses delivered at low dose rates as effective in producing health effects as the same doses delivered at high dose rates?”

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2024

Development of spectroscopic tools for nuclear forensics signatures development

The Savannah River National Laboratory (SRNL) has been developing advanced spectroscopic tools for the characterization of plutonium-bearing compounds with the intent to develop material and process signatures for nuclear forensics. Plutonium in a production, refining, or finishing facility will exist in many forms including oxide precursors (PuF4, PuF3, Pu oxalate, etc.), oxide, and metal. The ability to identify plutonium in each of these chemical forms and determine their processing history is crucial for the development of spectroscopic signatures. This presentation will focus on our work to develop and apply spectroscopic tools at SRNL using doubled-walled cells (DWC) to characterize the thermal decomposition of oxalates, calcination chemistry, alpha-decay-induced chemistry, age dating since last calcination, and other signatures related to plutonium processing.

Villa-Aleman, Eliel↗
DOE OSTI2012

Central plateau remediation optimization study

The Central Plateau is a 195-km2 (75 mi 2 ) area located in the center of the 1,517 km2 (586 mi 2 ) Hanford Site in south central Washington State (Figure ES-1). The Hanford Site was established in 1943 and was originally designed, built, and operated to produce plutonium for nuclear weapons. During World War II, plutonium production reactors were constructed along the Columbia River. Separations facilities (canyon buildings) were constructed in the Central Plateau to chemically extract plutonium from irradiated fuel. While plutonium production continued at the Hanford Site through the 1980s, additional mission activities, such as energy research/development and isotope separation, began in the 1950s. The Hanford Site mission, managed by the US Department of Energy (DOE) is now focused on treatment of wastes generated during past operations, and the cleanup of excess facilities and environmental contamination to mitigate impacts to human health and the environment. On the Central Plateau, there are hundreds of currently active and excess facilities and more than 1,000 soil waste sites and pipelines that will require remediation as part of final cleanup.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

The Deployable Fast-Neutron Coded-Aperture Imager: Demonstration of Locating One or More Sources in Three Dimensions

This brief report describes commissioning measurements performed using a newly constructed fast neutron coded-aperture imager intended for performing quantitative measurements of plutonium holdup at fuel cycle facilities. The present report was prepared in fulfillment of milestone M3FT-13OR0402054, “Imager commissioning and 3D source configuration measurements” of Fuel Cycle R&D Material Protection, Accounting, and Control Technology (MPACT) work package FT-13OR040205, “Fast Neutron Imaging to Quantify Nuclear Materials - ORNL.” In addition to representing the first measurements made with the new device, these measurements also demonstrate for the first time the ability to localize one or more neutron sources in three dimensions by combining imaging data from multiple measurements in which the imager was positioned at different locations. The development and use of fast-neutron imaging technology are motivated by a desire to locate and quantify plutonium holdup in scenarios where contact measurements with non-imaging detectors may be impractical or their results ambiguous because of surrounding material or nearby sources. Considering the goal of quantitative measurements, fast neutrons (as opposed to the more numerous gamma rays) are preferred in many situations because of their ability to penetrate equipment and nuclear material that are essentially opaque to gamma radiation. However, there are many challenges associated with constructing a practical imager for fast neutrons. For example, the ability of fast neutrons to penetrate material also leads to challenges in constructing a fast-neutron imager that is sufficiently compact to be suitable for use in a facility while remaining sufficiently sensitive to neutron emanations from plutonium or other actinides. Moreover, use of the imager in a production environment favors mechanically robust detectors that do not contain flammable liquid, unlike the organic liquid scintillators that are typically used to achieve fast-neutron detection. Last of all, a single-sided measurement geometry, as is typically used in imaging applications, necessitates accurate measurement of the location of a deposit of plutonium holdup in three dimensions in order to correctly infer the source strength. In response to these challenges, Oak Ridge National Laboratory (ORNL) has built a fast-neutron imager that has a compact footprint and whose segmented neutron detectors are built from the first cast plate of the recently developed plastic scintillator with pulse shape discrimination properties developed by Lawrence Livermore National Laboratory and commercially available from Eljen Technologies as experimental scintillator EJ-299-34. This report presents a description and preliminary analysis of mock holdup measurements intended to determine the three-dimensional location of one or more neutron sources placed in prototypical equipment from a set of imaging measurements that scanned the extent of the equipment.

Hausladen, Paul↗
DOE OSTI2013

Multi-Collector Inductively Coupled Plasma Mass Spectrometer – Operational Performance Report

The INL made an assessment of the commercially available inductively coupled plasma mass spectrometers (ICPMS) for actinide analysis; emphasizing low detection limits for plutonium. INL scientists subsequently determined if plutonium was present on a swipe, at a 10 million atom decision level. This report describes the evaluation of ICPMS instruments and the operational testing of a new process for the dissolution, separation and analysis via ICPMS of swipes for plutonium and uranium. The swipe dissolution, plutonium and uranium isolation, separation and purification are wet chemistry methods following established procedures. The ICPMS is a commercially available multi-collector magnetic sector mass spectrometer that utilizes five ion counting detectors operating simultaneously. The instrument includes a sample introduction system allowing for sample volumes of < 1 mL to be reproducibly injected into the instrument with minimal waste of the sample solution, while maximizing the useable signal. The performance of the instrument was measured using SRM 996 ( 244 Pu spike) at concentrations of 12 parts per quadrillion (ppq, fg/mL) and with SRM 4350B Columbia River Sediment samples spiked onto swipes at the 10 million atom level. The measured limit of detection (LOD, defined as 3s) for 239 Pu is 310,000 atoms based upon the instrument blank data. The limit of quantification (LOQ defined as 10 s) for 239 Pu is 105,000 atoms. The measured limit of detection for 239 Pu from the SRM 4350B spiked onto a swipe was 2.7 million atoms with the limit of quantification being 9.0 million atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Determining the Release of Radionuclides from Tank Waste Residual Solids: FY2015 Report

Methodology development for pore water leaching studies has been continued to support Savannah River Site High Level Waste tank closure efforts. For FY2015, the primary goal of this testing was the achievement of target pH and Eh values for pore water solutions representative of local groundwater in the presence of grout or grout-representative (CaCO 3 or FeS) solids as well as waste surrogate solids representative of residual solids expected to be present in a closed tank. For oxidizing conditions representative of a closed tank after aging, a focus was placed on using solid phases believed to be controlling pH and E h at equilibrium conditions. For three pore water conditions (shown below), the target pH values were achieved to within 0.5 pH units. Tank 18 residual surrogate solids leaching studies were conducted over an E h range of approximately 630 mV. Significantly higher Eh values were achieved for the oxidizing conditions (ORII and ORIII) than were previously observed. For the ORII condition, the target Eh value was nearly achieved (within 50 mV). However, E h values observed for the ORIII condition were approximately 160 mV less positive than the target. E h values observed for the RRII condition were approximately 370 mV less negative than the target. Achievement of more positive and more negative E h values is believed to require the addition of non-representative oxidants and reductants, respectively. Plutonium and uranium concentrations measured during Tank 18 residual surrogate solids leaching studies under these conditions (shown below) followed the general trends predicted for plutonium and uranium oxide phases, assuming equilibrium with dissolved oxygen. The highest plutonium and uranium concentrations were observed for the ORIII condition and the lowest concentrations were observed for the RRII condition. Based on these results, it is recommended that these test methodologies be used to conduct leaching studies with actual Tank 18 residual solids material. Actual waste testing will include leaching evaluations of technetium and neptunium, as well as plutonium and uranium.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Compilation of PRF Canyon Floor Pan Sample Analysis Results

On September 28, 2015, debris collected from the PRF (236-Z) canyon floor, Pan J, was observed to exhibit chemical reaction. The material had been transferred from the floor pan to a collection tray inside the canyon the previous Friday. Work in the canyon was stopped to allow Industrial Hygiene to perform monitoring of the material reaction. Canyon floor debris that had been sealed out was sequestered at the facility, a recovery plan was developed, and drum inspections were initiated to verify no additional reactions had occurred. On October 13, in-process drums containing other Pan J material were inspected and showed some indication of chemical reaction, limited to discoloration and degradation of inner plastic bags. All Pan J material was sealed back into the canyon and returned to collection trays. Based on the high airborne levels in the canyon during physical debris removal, ETGS (Encapsulation Technology Glycerin Solution) was used as a fogging/lock-down agent. On October 15, subject matter experts confirmed a reaction had occurred between nitrates (both Plutonium Nitrate and Aluminum Nitrate Nonahydrate (ANN) are present) in the Pan J material and the ETGS fixative used to lower airborne radioactivity levels during debris removal. Management stopped the use of fogging/lock-down agents containing glycerin on bulk materials, declared a Management Concern, and initiated the Potential Inadequacy in the Safety Analysis determination process. Additional drum inspections and laboratory analysis of both reacted and unreacted material are planned. This report compiles the results of many different sample analyses conducted by the Pacific Northwest National Laboratory on samples collected from the Plutonium Reclamation Facility (PRF) floor pans by the CH2MHill’s Plateau Remediation Company (CHPRC). Revision 1 added Appendix G that reports the results of the Gas Generation Rate and methodology. The scope of analyses requested by CHPRC includes the determination of common anions, gamma spectrometry, metals, corrosivity, organics and alpha spectrometry (note: alpha spectrometry was cancelled during the performance of this work with concurrence from CHPRC). Results may help elucidate the components that led to the unexpected reaction in the canyon as well as inform the radiological and hazardous characteristics. The specific anions, gamma emitters, organics and metals requested by CHPRC are provided in the analytical reports sections. The individual analyses were conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.) developed by PNNL specifically for this project. The final reports for each analysis set are included in this compilation of the results. Each package was reviewed under the PFP Floor Pan Evaluation Project Quality Assurance Project Plan so no additional reviews were conducted in this compilation task. The Gas Generation Rates in Appendix G were conducted under the PNNL “How Do I…” quality assurance program and were NOT conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.).

36 MATERIALS SCIENCE↗
DOE OSTI2017

The Inglorious Death of Jumbo

In the summer of 1944, J. Robert Oppenheimer and Los Alamos faced a crisis. An isotopic impurity in Plutonium rendered the metal unusable in a gun-assembled atomic bomb (i.e., Little Boy). Making this situation worse was a shortage of Uranium. The combination of these two problems threatened the entire wartime project. The answer to this dilemma, in part, was to develop a novel assembly method for Plutonium using the supersonic shock waves created by several tons of high explosives to compress a ball of Plutonium into a supercritical state. Since this method, implosion, was not much more than a theoretical construct, the Trinity test was devised to proof test the process. Given the speculative nature of implosion, Trinity was a gamble of sorts. If the test failed (i.e., little or no nuclear yield), the blast of the high explosives would scatter the scarce and expensive Plutonium over the surrounding desert. Since the probability of failure remained high into the early summer of 1945, some method of containing a failed nuclear explosion was needed. Jumbo was the answer.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗
DOE OSTI2017

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↗
DOE OSTI2019

Pu Handbook Chapter 39: Thermophysical Property Measurements

The ability to carry out thermophysical property measurements on actinide materials is very important for complete characterization. This is especially true of plutonium and plutonium containing materials where many questions still remain surrounding its physics. Over the past decade, there have been numerous examples of interesting physical behavior in many of these flux grown crystals and prepared alloys including unconventional superconductivity, complex magnetism, paramagnetism, and radiation damage or aging studies. In all of these cases, data was obtained that include the measurement of magnetic susceptibility, heat capacity, or electrical resistivity as well as other property measurements. These have allowed more detailed study of the dual nature of the 5$f$ electrons of plutonium in a variety of crystal structures and coordination environments. The alpha-particle radioactivity of plutonium provides an additional challenge to collecting data from the materials in a safe and effective way. It is therefore very important that the experimentalist is able to obtain high quality data while keeping the measurement system as well as the sample holder free of any radioactive contamination that may spread during the measurement process. In this section, the most widely used techniques for characterization of the synthesized material will be described. These include the physical property methods of magnetic susceptibility, heat capacity, and electrical resistivity as well as a few others.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Physical Sciences Vistas Summer 2019

In support of the Laboratory’s mission to maintain the nation’s nuclear stockpile, Los Alamos researchers investigate every aspect of plutonium in every possible environment. This includes plutonium hydriding. In metals, hydriding occurs when hydrogen accumulates in the spaces between the metal atoms. This process changes the physical properties of plutonium metal, leading to embrittlement and a less functional material. The understanding of this process is of importance to many aspects of the Laboratory’s plutonium mission.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Who Invented the Christy Gadget

The Christy Gadget, named after its principal inventor, is the informal name for the device tested at Trinity on July 16th, 1945. In late 1944, Robert Christy proposed a novel invention that altered the design of the plutonium pit in Fat Man. While scientists originally intended to use a hollow sphere of plutonium, there was a substantial risk given a number of asymmetries that resulted from implosion. Christy proposed changing the design of the plutonium core to a solid sphere of plutonium with a modulated neutron source. The new model was adopted and used in the early implosion bombs. While there is little debate about the important role that Christy played in demonstrating its feasibility as a safe design, there is a debate as to who initially proposed the idea of the Christy Device. My project this summer outlines and resolves this dispute. While Christ does deserve the majority of the credit for the invention and design, I also acknowledge the important role Rudolf Peierls and John von Neumann played in its development.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Nuclear Criticality Safety Assessment of Criticality Control Containers without Moderation Control at the Waste Isolation Pilot Plant

The Waste Isolation Pilot Plant (WIPP) provides for safe, permanent disposal of government-owned transuranic (TRU) and TRU mixed wastes. Receipt and disposal of waste at the WIPP site began in March 1999. The Sandia report, Consideration of Nuclear Criticality When Disposing of Transuranic Waste at the Waste Isolation Pilot Plant, addressed potential nuclear criticality safety issues based on the projected inventory characteristics known at the time [1]. As designs for inventory, waste forms, and disposal packages have changed, new analyses have been performed, and updates have been made to address any potential effects to the WIPP safety basis. New analyses performed include Saylor 2017 [2] and Brickner 2019 [3], which address certain waste containers with specified loadings under post-closure conditions. Both examined several hypothetical scenarios and included analyses to bound (from a criticality potential standpoint) credible configurations that could occur at WIPP during the repository regulatory post-closure disposal time period for feature, event, and process (FEP) considerations—10,000 years. During this post-closure period at WIPP, the screening of FEPs is governed by the risk-based standards and implementing regulations of the US Environmental Protection Agency (EPA) (i.e., 40 CFR 191 and 40 CFR 194, respectively) [4,5]. An FEP screening can be based on either a low-consequence or low-probability rationale. A low-probability rationale includes either (a) a qualitative rationale that the FEP is not credible or (b) a quantitative demonstration that the probability is less than 10-4 in 104 years. In this evaluation, a qualitative lowprobability rationale of not credible is used by demonstrating that bounding configurations of the waste are not critical. The demonstration of subcriticality is through quantitative calculations, but a probability of criticality is not evaluated. Rather, the rationale for this evaluation is that bounding configurations with an effective neutron multiplication factor (keff) well below the upper subcriticality limit (USL) make criticality incredible. Reference [2] documented a nuclear criticality assessment of the WIPP repository for disposal of dilute surplus plutonium materials using the Dilute and Dispose Approach and packaging in criticality control overpacks (CCOs). The CCO is the waste disposal container recently designed to allow for up to 380 fissile gram equivalent (FGE) 239 Pu per drum, which is a higher fissile loading than typical waste containers. The CCO consists of a criticality control container (CCC) positioned by upper and lower plywood spacers within a standard 55 gal drum. The CCC is used to establish a geometry control for fissile materials during transportation and WIPP emplacement operations. The current WIPP waste acceptance criteria for CCO payloads limit beryllium to less than or equal to 1% by weight of the waste contents and require the waste form to be non-machine compacted. Reference [2] considered two scenario progressions—room closure from salt creep, hereafter referred to as the reconfigured dry scenario, and flooding with brine, hereafter referred to as the reconfigured wet scenario. The subsequent drying out of the reconfigured wet scenarios was also considered. For all scenarios, subcriticality was maintained when 50 g of B 4 C (acting as a neutron absorber) per CCC was intermixed within the plutonium disposition waste form. The analysis used a waste form description that limits the amount of moderation that could be present within the waste form (i.e., it limits the amount of water and polyethylene that could be present based on planned processing conditions). This analysis to evaluate increased limits on the amount of moderation that could be present was performed as a companion to Reference [2] to address concerns associated with verifying moisture and/or plastic contents of waste materials following packaging of dilute surplus plutonium in the CCO. To that end, this analysis used the models and methods from Reference [2] to evaluate a more generic base waste form consisting of water and polyethylene that is more similar (and nearly identical) to the generic waste forms utilized in other models/analyses supporting the TRU Package Transporter Model II (TRUPACTII) safety analysis [6] (all are without moderation controls). The waste form in this analysis uses a base mixture of 75% water and 25% polyethylene, the total amount of which is varied to determine the optimum moderation to fissile material (H/Pu) ratio. The fissile loading is maintained at up to 380 FGE 239 Pu (modeled as PuO 2 ) per CCO with an additional 545 g of beryllium (to bound the 1% by weight contents restriction) and 50 g of B 4 C intermixed per CCO. The beryllium content (1% by weight) is based on the total allowed waste weight (this does not include packaging and container weights). Figures ES-1 and ES-2 display summary results, showing that with this model including 50 g of B 4 C per CCO, the system keff remains under 0.85 for all moderator amounts and provides a significant margin against post-closure criticality under postulated bounding conditions for compaction. Figure ES-1 compares an infinite model with a room model at the initial emplacement spacing and under full radial compaction. Full radial compaction places each CCC in direct contact and does not credit any anticipated spacing associated with current post-closure geomechanical modeling of the repository [7]. The effects of variations in the H/Pu ratio were evaluated by varying the amount of the water/polyethylene component of the waste model, with fissile loading maintained at 380 239 Pu FGE. Similarly, Figure ES-2 illustrates how various amounts of B 4 C per CCO influence k eff at different radial compactions, all at the H/Pu ratio of 200 (in the room array model). Therefore, while the results from Saylor 2017 [2] modeled more realistic process limits associated with packaging of dilute surplus plutonium, this analysis demonstrates that limits on moderation (plastic and water content) are not necessary to ensure subcriticality in the WIPP repository, provided the requisite B 4 C absorber is present.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Gamma ray analysis of the K2 containers

The K2 containers contain PuO2 with 238 Pu being the most abundant isotope of all plutonium isotopes. The purpose of this analysis is to determine the light element impurities in the PuO2. These light elements can interact with the alpha particles from plutonium decay to release gamma rays, protons, and neutrons through the reactions (α,α’), (α,p), and (α,n) respectively. The gamma rays released by the interactions can be measured and compared with the gamma rays released by the plutonium. The ratios of the gamma rays from the interactions and the plutonium gamma rays allow for the determination of the impurities in the items. The elements that can be detected are Lithium (Z=3), Beryllium (Z=4), Boron (Z=5), Fluorine (Z=9), Sodium (Z=11), Magnesium (Z=12), Aluminum (Z=13), Silicon (Z=14), Phosphorous (Z=15), Chlorine (Z=17), and Potassium (Z=19).

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Analysis of Tank 38H (HTF-38-22-91, -92) and Tank 43H (HTF-43-22-93, -94) Samples for Support of the Enrichment Control and Corrosion Control Programs

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The results indicate the concentrations of most soluble species in the Tank 38H surface sample increased slightly from the previous surface sample. The Tank 38H sub-surface sample shows changes in concentration for soluble species in the solution with some increasing and some decreasing. The current Tank 38H sub-surface sample contains more sludge solids than the previous sample based on visual appearance. The small differences in the concentrations of major components between the Tank 38H surface and sub-surface samples indicate only minimal stratification of solution species within the tank. The Tank 43H surface and sub-surface samples are similar in composition to the previous samples. The similar solution compositions measured in the Tank 43H surface and sub-surface samples indicate a minimal stratification within the tank. The total uranium and plutonium in the current Tank 38H surface sample remains similar to the previous analysis. The Tank 38H sub-surface sample shows an increase in uranium and plutonium concentrations compared to the previous sample likely because of an increase in sludge solids in the current sample. The total uranium concentration in the two Tank 43H samples is essentially unchanged from previous sample results. The plutonium concentration in the Tank 43H surface sample is similar to the previous sample results while the plutonium in the Tank 43H sub-surface sample increased relative to the previous analysis. The sum of the major cations versus the sum of the major anions shows a difference of <10% for both samples from Tank 38H and for both samples from Tank 43H providing an indication of good data quality for the non-radioactive analytes in the samples. The silicon concentrations measured in the Tank 38H sub-surface sample increased compared with the previous sample results likely due to the presence of more sludge solids in the current sample. The Tank 38H surface sample silicon concentrations is similar to the previous sample results. The Tank 43H surface and sub-surface sample silicon concentrations both increased compared to the previous sample results. The samples analyzed from Tanks 38H and 43H show silicon concentrations ranging from 61.5 to 97.3 mg/L.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗