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At least 91 records · Page 5

Evaluation of chromatographic resins for high efficacy separation of radium from chemical analogues

The separation of Radium (Ra) from interfering chemical analogues is of major importance for both the accurate measurement of Ra-226 in environmental samples and the preparation of radium targets destined for medical isotope production. The adsorption behavior of Ra, Barium (Ba), and Strontium (Sr) was investigated on multiple crown-ether-based proprietary extraction chromatographic resins developed by TrisKem Int. Among these, the TK101 resin, characterized by a novel room-temperature ionic liquid (RTIL) dual extractant–solvent system, demonstrated enhanced affinity and selectivity, particularly at low acid concentrations, achieving a D w of 3477 ± 73 for Ra in 0.04 M HNO₃, whereas the maximum Ra D w obtained with the traditional Sr resin in 8 M HNO 3 was only 12.33 ± 0.4. In 0.04 M HNO 3 , a Ra distribution ratio (D w ) of 776 was achieved within 1 min, indicating rapid uptake kinetics. The adsorption capacities were estimated at 19.6 ± 0.1 mg/g for Ba and 12.0 ± 0.2 mg/g for Sr. However, competing alkali metals significantly reduced alkaline earth metal uptake, indicating that the TK101 resin is best suited for radium purification following a preconcentration step to minimize matrix effects in high salinity samples. Dynamic column studies confirmed the strong chromatographic performance of the TK101 resin, with no significant Ba or Sr breakthrough in the Ra fraction and a Ra recovery of 87 ± 2.8%. These results demonstrate the potential of the TK101 resin for selective radium separation in analytical and radiochemical applications.

and nuclear chemistry↗

Gas-solid reaction pathway for chlorination of rare earth and actinide metals using hydrogen and chlorine gas

Hydriding and chlorination of buttons of metallic cerium have been tested as a head-end step to separating metal impurities from actinides. The objective here was to achieve complete conversion to chlorides while maintaining high surface area via small particles and open porosity. Hydriding by reaction with 100% H 2 gas at 573 K was successful at reducing cm-scale metal buttons into small particles/fragments. This step was followed by reaction with flowing 99.5% anhydrous Cl 2 gas at temperatures ranging from 423 to 573 K for 60 min. In experiments reported here, up to 92% conversion to cerium chloride was achieved from reacting with the anhydrous chlorine gas. The final chloride product has high porosity coupled with small particle sizes (microns to 1600 μm), which makes it suitable for subsequent purification processes. Higher chlorine concentrations in the gas favor higher conversion to chloride. The optimal temperature to achieve high chlorination is 523 K. Oxygen is a minor impurity in the chlorine gas which appears to prevent complete chlorination from being achieved.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Actinide complexes with Wells–Dawson polyoxometalates (part 1): americium and curium

We report the first trivalent actinide complexes with a Wells–Dawson polyoxometalate. Americium(III) forms two distinct phases: triclinic K 17 Am(P 2 W 17 O 61 ) 2 ·42.5H 2 O and monoclinic K 17 Am(P 2 W 17 O 61 ) 2 ·12H 2 O. Curium(III) crystallizes as monoclinic K 17 Cm(P 2 W 17 O 61 ) 2 ·8H 2 O. XRD-quality single crystals were obtained from just ∼330 nanograms of actinides. This work establishes clear structure–property relationships that will guide investigations on scarce f-elements.

and nuclear chemistry↗

Actinide complexes with Wells–Dawson polyoxometalates (part 2): californium

We report the first example of a polyoxometalate (POM) compound containing californium. Using a Wells–Dawson POM ligand, K 17 Cf(P 2 W 17 O 61 ) 2 ·2H 2 O was synthesized and characterized. Californium is the heaviest element ever crystalized with a POM. Significant solubility differences among the POM's f-element complexes were observed, enabling selective precipitation with separation factors rivaling liquid–liquid extraction.

and nuclear chemistry↗

Hauser-Feshbach Analysis of Fast Neutron-Induced Reactions on Chlorine

Neutron-induced reactions on 35Cl have recently been measured and analyzed in a Hauser-Feshbach framework at Los Alamos National Laboratory. Particular focus has been applied to the “fast” energy range above 100 keV, where these reactions become important for applications like CLYC (Cs 2 LiYCl 6 :Ce) detector characterization and the development of molten chloride fast reactors. However, challenges to applying a purely statistical analysis to this mass range have presented themselves in the form of cross section fluctuations and deviations due to low-mass structure. In this paper, these challenges and their current solutions will be highlighted, as well as preliminary extensions of the analysis to neighboring isotopes and future plans to extend the measurements down to thermal energies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

New Capability at ORNL: High Precision Uranium Titration

Destructive analytical measurements establish a nuclear facility’s nuclear material inventory and inventory differences for Nuclear Material Accountancy and Control. A nuclear laboratory’s ability to perform accurate high-precision analytical measurements is key for tracking large inventories within a facility’s material balance areas and during production to track material movement through dynamic processes. For uranium, these measurements are made by using several established high-precision measurement protocols. These include isotope dilution mass spectrometry, gravimetry, and potentiometric titrations. Whatever measurement technique a nuclear lab chooses to use, reference materials (RMs) with certified attributes and accompanying uncertainties are used to calibrate measurement systems, and are the cornerstone for accurate results. In addition to calibration, RMs provide for metrological traceability, are used for method development and validation, and thus provide critical evaluations of the appropriateness and performance of analytical processes used. Evaluations may include validation that a method is fit-for-purpose, quantification of systematic and random biases, and the evaluation of long-term and short-term performance metrics. High-precision measurement techniques require that measured attributes be certified to a high degree of precision in the RMs used—ultimately, to a higher degree than that of the measurement technique itself. The US authority on the production of special nuclear material Certified Reference Materials is the NBL Program Office (NBLPO), formally known as New Brunswick Laboratory (NBL). The NBLPO is responsible for the sales and distribution of existing NBL certified reference materials (CRMs) and for the production of the next generation of nuclear RMs. To accomplish its mission, NBLPO is establishing key base capabilities within the DOE laboratory complex that formerly existed at the NBL laboratory. The Nuclear Analytical Chemistry (NAC) section within the Chemical Sciences Division (CSD) at Oak Ridge National Laboratory (ORNL) is currently working with NBLPO to set up laboratory and measurement capabilities to provide measurements and capabilities for production and/or recertification of existing and future CRMs for uranium assay. The NBL-developed high-precision titration (HPT) method is a critically-evaluated, extremely precise and accurate primary method utilized for the determination of uranium content in a variety of uranium materials. The HPT method, combined with detailed balance weighing protocols, provides for an analytical methodology that is unsurpassed in precision and one in which all sources of error have been evaluated, a requirement of CRM certification. HPT capability within the United States was lost with the closure of the labs at NBL. The NAC has been collaborating with NBLPO to stand up and demonstrate the capability to perform uranium assay via HPT at ORNL. HPT can produce results with an expanded uncertainty of approximately 0.01% for pure uranium compounds, with typical precisions of <0.006%. The major tasks required to stand up the method at ORNL were the refurbishment of a dedicated lab and equipment setup, procedure development, analyst training, establishing method-specific quality assurance, and qualification of an analyst to perform the method. This report summarizes these tasks, outlines the documents drafted, and gives the outcome of the qualification titrations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Production of NBL PO plutonium isotopic standards CRM 136A, CRM 137A, and CRM 138A

Lawrence Livermore National Laboratory (LLNL) produced approximately 1 mg units of purified Pu from the parent New Brunswick Laboratory (NBL) certified reference materials (CRM) 137, 136 and 138 isotopic standards for the NBL Program Office (NBL PO) as detailed in the revised project plan. As stated in the plan, three representative units of each material were dispensed at the same time to be characterized at LLNL and provide informational values for the quantity of Pu and progeny nuclides in each unit. NBL PO intends to collect and evaluate isotopic measurement data from multiple laboratories and certify these materials as new isotopic standards C137A, C136A, and C138A, respectively. Soon after production eleven units of each analytical standard were shipped to other analytical laboratories for the certification effort, and 121, 119, and 119 units of C137A, C136A and C138A, respectively were shipped to Mickey Finch at Y12 NBL distribution center in November 2024 (30-gallon drum, TID 003777 PRL 7000005043). Residual purified Pu from the effort is being stored indefinitely in B332 at LLNL. Detailed methods can be found in the production plan, and this report describes and documents aspects of the production effort that are not in or were modified from the original production plan.

and nuclear chemistry↗

Joint Sample Analyses of Nuclear Forensic Materials Provided by the Republic of Kazakhstan: U. S. Laboratory Results

This document serves as an interim report to summarize sample analyses performed by Lawrence Livermore National Laboratory (LLNL) and Los Alamos National Laboratory (LANL) on a series of five nuclear forensics samples provided by the Institute of Nuclear Physics (INP) in the Republic of Kazakhstan. The sample set contains four uranium oxide powders and one low-enriched uranium fuel pellet. The samples were provided as part of a broader collaboration that involved a set of joint sample analyses conducted by INP and the US National Laboratories. The joint analyses are being conducted using well-developed analytical plans. These activities are designed to support the advancement of nuclear forensic science and capacity building in all three institutes in both countries. This report builds upon an earlier preliminary summary of the joint interactions and will be augmented by a final report. The final report will summarize the results and value of all sample analyses performed at the three institutes (INP, LLNL, and LANL). The final report will also provide an intercomparison of the results, analytical methods and best practices employed, as well as outline future collaborative nuclear forensics activities that are being developed in the Kazakhstan region.

and nuclear chemistry↗

Analysis Report for Hydrolyzed UF 6 Samples

Under the auspices of the US Department of Energy/National Nuclear Security Agency’s Nuclear Reference Material Program (NRMP), the Material Signatures and Isotopic Standards (MSIS) group of Oak Ridge National Laboratory was tasked with analyzing two UF6 filled hoke tubes for uranium isotopic composition. This report documents the results of the measurements performed by the MSIS group’s International Organization for Standardization/International Electrotechnical Commission 17025:2017 accredited operating procedure CSD-AM-CIMS-IN20, Determination of Uranium and Plutonium Isotopic Composition using Thermal Ionization Mass Spectrometry, and in accordance with the quality assurance plan as described in QAP-X-96-CSD/RML-001, Nuclear Analytical Chemistry Laboratory Section Quality Assurance Plan.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

ORNL Report for Hydrolyzed UF 6 Samples 439451, 438792, 439144, 439616, and 439617

Under the auspices of the US Department of Energy/National Nuclear Security Agency’s Nuclear Reference Material Program (NRMP), the Material Signatures and Isotopic Standards (MSIS) group of Oak Ridge National Laboratory was tasked with analyzing five UF 6 filled P-10 tubes for uranium isotopic composition. This report documents the results of the measurements performed by the MSIS group’s International Organization for Standardization/International Electrotechnical Commission 17025:2017 accredited operating procedure CSD-AM-CIMS-IN20, Determination of Uranium and Plutonium Isotopic Composition using Thermal Ionization Mass Spectrometry, and in accordance with the quality assurance plan as described in QAP-X-96-CSD/RML-001, Nuclear Analytical Chemistry Laboratory Section Quality Assurance Plan.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Recent Advances toward Efficient Calculation of Higher Nuclear Derivatives in Quantum Chemistry

In this article, we provide an overview of state-of-the-art techniques that are being developed for efficient calculation of second and higher nuclear derivatives of quantum mechanical (QM) energy. Calculations of nuclear Hessians and anharmonic terms incur high costs and memory and scale poorly with system size. Three emerging classes of methods—machine learning (ML), automatic differentiation (AD), and matrix completion (MC)—have demonstrated promise in overcoming these challenges. We illustrate studies that employ unsupervised ML methods to reduce the need for multiple Hessian calculations in dynamics simulations and those that utilize supervised ML to construct approximate potential energy surfaces and estimate Hessians and anharmonic terms at reduced cost. By extension, if electronic structure operations could be written in a manner similar to functions underlying ML methods, rapid differentiation or AD routines can be employed to inexpensively calculate higher arbitrary-order derivatives. While ML approaches are typically black-box, we describe methods such as compressed sensing (CS) and MC, which explicitly leverage problem-specific mathematical properties of higher derivatives such as sparsity and low-rank, to complete higher derivative information using only a small, incomplete sample. The three classes of methods facilitate reliable predictions of observables ranging from infrared spectra to thermal conductivity and constitute a promising way forward in accurately capturing otherwise intractable higher-order responses of QM energy to nuclear perturbations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Interlaboratory comparison of secondary ion mass spectrometry analysis results from the 7th international technical nuclear forensics working group collaborative material exercise

A review and interlaboratory comparison of secondary ion mass spectrometry (SIMS) data obtained by laboratories participating in the International Technical Nuclear Forensics Working Group (ITWG) 7th Collaborative Material Exercise (CMX-7) has been conducted. The analyzed materials were two uranium compounds in powder form and two pieces of uranium metal. The instruments used in this comparison were a small-geometry (SG) SIMS, CAMECA IMS 7f from the Research Centre Rez, and a large-geometry (LG) SIMS, CAMECA IMS 1280 from Los Alamos National Laboratory. Despite the differences in instruments and analytical procedures, e.g., sample preparation, SIMS setups, and data post-processing, there was good agreement for the 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios in the analyzed materials. The main difference was in the precision, which was, as expected, higher for the LG-SIMS. In addition, a comparison between the laboratories was also made for the image processing algorithms applied to raw data acquired in automated particle measurement (APM) mode. In conclusion, the result of this comparison has led to identification of best practices for setting up parameters of the APM software.

and nuclear chemistry↗

Aqueous harvesting of 88 Zr at a radioactive-ion-beam facility for cross-section measurements

Isotope harvesting is a method of collecting the long-lived radioisotopes that build up during the operation of ion-beam facilities in a way that is useful for subsequent research. As a demonstration of this method for the collection of a group IV metal at a fragmentation facility, the high-energy Zr 88 secondary beam produced from a 140-MeV/u Mo 92 primary beam at the National Superconducting Cyclotron Laboratory (NSCL) was stopped in a water target. The setup aimed to mimic the aqueous beam dump that will be implemented at the Facility for Rare Isotope Beams (FRIB). The collected Zr 88 and accompanying Y 88 decay daughter were radiochemically extracted from the solution and made into target samples suitable for neutron-capture cross-section measurements. These samples were then irradiated at two reactor facilities, and the Zr 88 average thermal-neutron-capture cross section ( σ T ) and resonance integral ( I ) were determined to be σ T = ( 8.04 ± 0.63 ) × 10 5 b and I = ( 2.53 ± 0.28 ) × 10 6 b. The σ T value agrees well with previous results and I , determined for the first time here, was found to be the largest measured resonance integral by two orders of magnitude. The Y 88 thermal-neutron-capture cross section was determined to be less than 1.8 × 10 4 b. This work demonstrates the steps needed to make cross-section measurements with samples produced via aqueous isotope harvesting.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Advancing nuclear forensics competencies at the National Nuclear Center of the Republic of Kazakhstan and conceptual development of a National Nuclear Forensics Library

Since 2021, the National Nuclear Center (NNC) of the Republic of Kazakhstan has been successfully developing a project dedicated to nuclear forensics. The relevance of this project is underscored by Kazakhstan’s leading position in the global uranium mining and export market. The country operates research reactors and is involved in the production of experimental nuclear fuel. The nuclear forensics project is being implemented in several key areas: the project will develop competencies in laboratory research of samples, interpretation of results, and develop a prototype concept for the National Nuclear Forensics Library. In implementing these challenges, the NNC experts draw on the experience of colleagues from world-leading scientific and research centers. Designing a prototype National Nuclear Forensics Library (NNFL) is a challenging project. In conclusion, the solution to this task is based on the IAEA’s approaches, recommendations, and the experience gained from the construction of similar systems in other countries.

and nuclear chemistry↗

Purification of legacy Ra-226 from ingrown Pb-210 using cation exchange chromatography

With the growing interest in using radium-226 (Ra-226) as a source material to produce essential radionuclides for targeted alpha therapies, the global demand for Ra-226 has surged, rendering its acquisition difficult. The shortage necessitates the exploration of alternative pathways to obtain this isotope beyond traditional commercial vendors. Legacy radium sources remain widespread due to Ra-226’s historical use but require the removal of ingrown daughter products to obtain a pure Ra-226 product. In conclusion, a straightforward and effective purification method for legacy Ra-226 ampoules has been developed using cation exchange chromatography, enabling the reliable conversion of legacy materials into high-purity Ra-226 solutions.

and nuclear chemistry↗

Sample screening of uranium ore concentrates using portable spectrophotometers: investigating the correlation between visible colors and chemical signatures

A research collaboration between the Japan Atomic Energy Agency and the Department of Energy’s National Nuclear Security Administration examined nuclear forensic signatures and analytical methods for tracing the origins of uranium ore concentrates (UOCs). Here, this study focuses on utilizing portable spectrophotometers capable of reflectance measurements in the visible light spectrum as a potential rapid screening tool for nuclear forensics analysis. Unlike laboratory-based near-infrared spectroscopy or digital image analysis, this research investigated the potential to correlate visible color measurements with key nuclear forensics signatures using seven types of UOC samples with known origins and three UOC certified reference materials. Results demonstrated that distinct color groups, quantified using CIELAB values, correlated with major uranium compounds. Furthermore, the findings indicated that trace elements can influence the UOC colors, providing additional insights into material characteristics. Although this approach requires further validation across a broader range of UOC species, this study demonstrated that simple colorimetric analysis using visible spectrophotometry, which does not require complex sample preparation or data processing, can serve as a practical and novel rapid tool for preliminary screening and attribution in nuclear forensics investigations.

and nuclear chemistry↗

In-situ anodic precipitation process for highly efficient separation of aluminum alloys

Electrorefining process has been widely used to separate and purify metals, but it is limited by deposition potential of the metal itself. Here we report in-situ anodic precipitation (IAP), a modified electrorefining process, to purify aluminium from contaminants that are more reactive. During IAP, the target metals that are more cathodic than aluminium are oxidized at the anode and forced to precipitate out in a low oxidation state. This strategy is fundamentally based on different solubilities of target metal chlorides in the NaAlCl4 molten salt rather than deposition potential of metals. The results suggest that IAP is able to efficiently and simply separate components of aluminum alloys with fast kinetics and high recovery yields, and it is also a valuable synthetic approach for metal chlorides in low oxidation states.

36 MATERIALS SCIENCE↗