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At least 55 records · Page 3

Separation of dilute plutonium(IV) from nitric acid solutions via Reillex HPQ anion exchange resin

Anion exchange is a common method for the separation of plutonium (Pu) in aqueous systems, providing high recovery and decontamination from impurities. Reillex HPQ anion exchange resin has been used around the Department of Energy complex in this application for decades but has typically been used for Pu feed concentrations greater than 1 g/L. It is desirable to recover Pu at more dilute concentrations from a dissolved used fuel or target element, for example. In this work, the performance of Reillex HPQ anion exchange resin was characterized with feed solutions of ca. 0.24 g/L Pu. A significant reduction in the performance of the resin was realized with this dilute concentration relative to a feed solution of 2.35 g/L Pu with similar feed flow rates and the same resin column, likely due to the increased driving force for mass transfer with a higher feed concentration. The maximum capacity of Reillex HPQ resin for Pu can be improved by reducing the flow rate and increasing the feed Pu concentration. Furthermore, the breakthrough point of Pu can be improved in the same manner and by increasing the resin bed height. Diffusion of Pu into the resin was illustrated to be the rate limiting step.

Plutonium separations

Closure Report for Corrective Action Unit 366: Area 11 Plutonium Valley Dispersion Sites, Nevada National Security Site, Nevada with ROTC 1

This Closure Report presents information supporting closure of Corrective Action Unit (CAU) 366, Area 11 Plutonium Valley Dispersion Sites, and provides documentation supporting the completed corrective actions and confirmation that closure objectives for CAU 366 were met. CAU 366 consists of the following six Corrective Action Sites (CASs), located in Area 11 of the Nevada National Security Site: • CAS 11-08-01, Contaminated Waste Dump #1 • CAS 11-08-02, Contaminated Waste Dump #2 • CAS 11-23-01, Radioactively Contaminated Area A • CAS 11-23-02, Radioactively Contaminated Area B • CAS 11-23-03, Radioactively Contaminated Area C • CAS 11-23-04, Radioactively Contaminated Area D

54 ENVIRONMENTAL SCIENCES

Integral Experiment Execution of Thermal or Epithermal eXperiments using Plutonium with Polyethylene and Iron, IER 519, TEX-Hanford (-Iron), CED-3b

This report documents the execution of experiments and measurements for IER 519, Thermal/Epithermal eXperiments (TEX) for Hanford applications, using plutonium Zero Power Physics Reactor (ZPPR) plates moderated by interstitial polyethylene and iron (Fe) absorber plates. Initial hand stack, mass, and dimensional measurements were performed in July 2025. The experiments were completed over three weeks from December 2025 to January 2026 at the National Criticality Experiments Research Center (NCERC) at the Nevada National Security Sites (NNSS). All photos and critical data were provided by NCERC and experimenters in LANL’s NEN-2.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Scanning tunneling spectroscopy of surface-oxidized Gallium-stabilized δ -phase plutonium

Here, the first contiguous experimental scanning tunneling spectroscopy (STS) measurements of the electronic structure of a plutonium (Pu) surface are presented and compared to current theoretical results. The experiments took place under UHV conditions, for which Pu is known to retain a native surface oxide. The STS data shows that no band gap is observable at room temperature. Theoretical calculations predict that bulk Pu oxides are semiconductors, but the spectral results for the cleaned Pu surface native oxide under UHV conditions could be better characterized as that of a semimetal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Structural and Spectroscopic Characterization of Plutonium and Other Tetravalent Metals Complexed to a Keggin Ion

Here, we report the isolation of the first plutonium(IV) complex with a Keggin ion chelator: Cs 20 [Pu(PW 11 O 39 ) 2 ] 2 ·13H 2 O. Single crystal XRD and solid-state UV–vis absorbance analysis demonstrate the stabilization of Pu 4+ by the Keggin ligand. The unit cell contains two [Pu(PW 11 O 39 ) 2 ] 10– complexes (Pu(PW 11 ) 2 ) bridged by Cs + . Raman and 31 P NMR spectra of Pu(PW 11 ) 2 are consistent with the analogous Zr 4+ , Hf 4+ , Ce 4+ , and Th 4+ complexes. The Pu–O bond distances at the two Pu sites are 2.35(3) and 2.34(3) Å, matching the value extrapolated from the bonding trend built with the other 8-coordinated tetravalent cations. However, the long-range arrangement of the Pu(PW 11 ) 2 complexes within the lattice is unique in the series of M IV (PW 11 ) 2 compounds: pairs of Pu(PW 11 ) 2 are organized perpendicular to each other. Based on solution-state UV–visible absorbance, small-angle X-ray scattering (SAXS), and 31 P NMR, the tetravalent cations quantitatively form the 1:2 species in solution ([Pu(PW 11 O 39 ) 2 ] 10– (aq) ) and no 1:1 species ([Pu(PW 11 O 39 )(H 2 O) x ] 3– (aq) ). Finally, a linear correlation exists between the metal–oxygen distances in the M IV (PW 11 ) 2 compounds and the corresponding metal dioxides, allowing for extrapolation for Pa 4+ , Am 4+ , and Bk 4+ . The results indicate that our microscale POM approach represents a viable pathway to probe properties of rare actinide ions in discrete molecules, beyond the traditional oxide extended solids.

and nuclear chemistry

Insights for controlling plutonium behavior in hydrochloric acid solutions

Cyclic voltammetry, UV-vis, and X-ray absorption spectroscopy were used to demonstrate that aqueous plutonium coordination chemistry and electron transfer reactivity can be controlled by judicious manipulation of hydrochloric acid concentrations.

Wang, Yufei [Los Alamos National Laboratory, Los A

Effects cascade debris and helium bubbles on the strength of aged plutonium

The radioactive decay of aging Pu is dominated by α-decay. This persistent α-decay produces crystalline defects in the form of dislocation loops and helium bubbles that evolve with time. Comparable defects are produced in other metallic alloys when subject to neutron irradiation, and these defects are known to modify the plastic deformation of irradiated materials. Models have been developed for these irradiated materials and validated against experimental confirmations of yield strength and the concomitant microstructural evolution. In this paper, we deploy those previously developed models and apply their mechanics to plutonium aging.

Chemical elements

Implementation of stacked ensemble machine learning for the detection of surrogate plutonium contamination in soil via LIBS

Supervised machine learning methods have demonstrated increased utility for the quantification of lanthanide and actinide elements in atomic spectroscopy applications. This study implements laser-induced breakdown spectroscopy (LIBS) for the identification of plutonium surrogate material (CeO 2 ) in soil matrices by training supervised machine learning methods on the recorded spectral data. A bagged ensemble using Random Forest yields the highest sensitivity predictions with a detection limit of 0.015 wt.% CeO 2 . However, high precision in Ce content prediction required the use of a stacked ensemble regression, which provided the superlative Ce quantification model with an error of 0.107% and a detection limit of 0.022 wt.%. Furthermore, the high performance of the stacked ensemble demonstrates its potential to enhance the accuracy and sensitivity of nuclear contaminant detection using field-deployable spectroscopic analyzers in real-world scenarios.

47 OTHER INSTRUMENTATION

Plutonium Retention by Crystalline Silicotitanate under Hyperalkaline Conditions Relevant to Tank-Side Cesium-Removal at the Hanford Site

Crystalline silicotitanate (CST) is used in Hanford’s Tank-Side Cesium-Removal (TSCR) process to selectively remove Cs-137 from highly caustic, nitrate-rich tank supernatants. Recent testing with actual waste samples suggests that CST can also retain measurable plutonium (Pu), which could affect radiological classification and disposal pathways for spent CST. To quantify this behavior, Pu partitioning to CST was studied under Hanford-relevant conditions using batch-contact experiments in a representative simulant (2 M NaNO3, 0.7 M NaOH). Isotherm data were measured and distribution ratios calculated, with Cs+ uptake used as benchmark. Under low-carbonate conditions, Pu was retained strongly by CST in systems initially contacted with either PuO2 nanoparticles (Pu(IV)) or aqueous Pu(VI), with distribution ratios of ~2,200–3,700 mL/g, generally exceeding those for Cs+ (~400–1,000 mL/g). Increasing carbonate concentration strongly reduced PuO2 nanoparticle retention; at [Na2CO3] = 1 M, distribution ratios decreased by up to one order of magnitude to roughly 100–300 mL/g. Electron microscopy suggests that Pu retention involves a combination of mechanisms such as PuO2 NP aggregation induced by CST leachate components, and association with CST bead surfaces.

Neumann, J.

Automated Inspection of Criticality Control Overpacks for Surplus Plutonium Disposition: Qualification Update – 25313

In an effort to reduce the amount of nuclear waste in South Carolina, the Department of Energy (DOE) tasked the Savannah River Site (SRS) with diluting and disposing of the amount of plutonium in the state. This process involves the movement and shipment of over 100,000 criticality control overpacks (CCOs) throughout the project lifespan, lending itself to the use of automation to reduce worker radiation exposure and more efficiently utilize human capital. Due to the large scope, this overarching process was broken down into several different “automation projects” to be developed. The first opportunity pursued was the receipt and inspection of empty CCO drums coming into SRS, identified as Automation Project 1 (AP1), and is the focus of this paper. AP1 was developed to unpack incoming CCOs and inspect them for unwanted foreign objects and any damage to the drum or its contents. This process is accomplished by the combination of an automated guided vehicle (AGV) that delivers CCOs to a robotic arm which uses a suite of custom tools to disassemble a CCO, inspect the inside and outside of the CCO and its inner criticality control container (CCC), reassemble the CCC and CCO, and apply a tamper indicating device (TID) to the inspected drum. In past years, the robotic work cell had been developed in a small-scale testing facility for proof-of-concept. This year, major improvements were made to the robotic work cell to perform the process, including integration into the final facility where CCOs will be inspected. Other technical improvements include the implementation of sensor feedback and safety relays into the control system to allow the state of the work cell to be better tracked, and additional development of the TID application process to complete the robotic inspection. Further enhancements were made to the robotic vision processes and robot pathing, as well as development on a computer vision inspection process to detect inspection criteria anomalies in CCOs. In addition to developmental improvements, the work cell underwent a six-month testing period to ensure the project requirements were met. Results of this testing period demonstrate the work cell’s capability to meet project throughput goals at an acceptable level, successfully document the status of each CCO inspected, and reduce the toll on technical operations’ human power by two thirds. At the time of this paper, the work cell is capable of autonomously handling up to eight CCOs with an AGV, delivering CCOs to and from the robot work cell, and having a robotic arm perform a full receipt and inspection procedure on each CCO. Moving forward, repeatability will be improved so that these CCOs can be run back-to-back seamlessly, as well as improving the system to handle more significant edge cases and failure modes.

Spivey, Nicholas

Custom Equipment Development for Processing of Surplus Plutonium

Facilities and Material • Location: Savannah River Site K-Area, South Carolina • Plutonium designated as surplus is blended with adulterant material, re-packaged and shipped to WIPP in New Mexico • Currently one operational glovebox for downblending, facility modifications and construction of three additional glovebox lines in progress • Current operations are highly manual requiring full PPE and reader/worker steps

Krementz, Daniel [Savannah River National Laborato

Neutron radiation characteristics of plutonium dioxide fuel

The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, (alpha, n) reactions with low Z impurities in the fuel, and (alpha, n) reactions with O-18. For spontaneous fission neutrons a value of (1.95 + or - 0.07) X 1,000 n/s/g PuO2 is obtained. The neutron yield from (alpha, n) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha-particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.14 + or - 0.26) X 10,000 n/s/g PuO2. The neutron yield from (alpha, n) reactions with low Z impurities in the fuel is presented in tabular form for one part part per million of each impurity. The total neutron yield due to the combined effects of all the impurities depends upon the fractional weight concentration of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

Taherzadeh, M.

Emitted radiation characteristics of plutonium dioxide radioisotope thermoelectric generators

The nuclear and emitted radiation characteristics of the radioisotope elements and impurities in commercial grade plutonium dioxide are presented in detail. The development of the methods of analysis are presented. Radioisotope thermoelectric generators (RTG) of 1575, 3468 and 5679 thermal watts are characterized with respect to neutron and gamma photon source strength as well as spatial and number flux distribution. The results are presented as a function of detector position and light element contamination concentration for fuel age ranging from 'fresh' to 18 years. The data may be used to obtain results for given O-18 and Pu-236 concentrations. The neutron and gamma photon flux and dose calculations compare favorably with reported experimental values for SNAP-27.

Gingo, P. J.

Neutron Radiation Characteristics of Plutonium Dioxide Fuel

The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, reactions with low Z impurities in the fuel, and reactions with O-18. For spontaneous fission neutrons a value of (1.95 plus or minus 0.07) X 1,000 n/s/q PuO2 is obtained. The neutron yield from (alpha, neutron) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.42 plus or minus 0.32) X 10,000 n/s/q PuO2. The neutron yield from (alpha, neutron) reactions with low Z impurities in the fuel is presented in tabular form for one part per million of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

Taherzadeh, M.