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At least 199 records · Page 11

Additive manufacturing: a challenge to nuclear nonproliferation

Additive manufacturing (AM) is a rapidly developing technology that allows industries to automate and simplify the production of highly complicated items. Recently, there are concerns that AM techniques have the potential to be utilized in the fields of nuclear weapons and nuclear enrichment technology. Presently, there are very few international or domestic export controls that apply to AM's role in the nuclear industry, constituting an unmanaged proliferation pathway. Pre-existing export controls focus on general concepts and processes and do not consider specific nuances of various techniques that are categorized as additive manufacturing. To introduce legislation and controls that will be effective in monitoring proliferation pathways, one must investigate and characterize AM techniques and their nuclear applications. This paper categorizes and ranks 33 AM techniques based on their potential impact on the nuclear fuel cycle and the development of nuclear weapons. Through this method of characterization and categorization, export controls would address specific AM nuclear proliferation risks without disrupting the entire industry and fuel cycle. Additionally, legislation employing this method would identify loopholes in export controls using a holistic approach to managing and monitoring proliferation pathways.

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Alpha/beta-gated gamma–gamma spectroscopy of mixed fission products for trace analysis

This experiment demonstrated that some hard-to-detect fission products can be quantified directly from mixed fission product samples using advanced radio-emission spectroscopy techniques. A gamma/gamma coincidence detector was combined with a custom liquid scintillation counter to evaluate the benefits of alpha and beta coincident and anti-coincident analysis of mixed fission product samples. Reduction factors in the minimum detectable activity (MDA) relative to traditional gamma counting were quantified for a set of radionuclides. For isotopes like 91Y, 144Ce, 147Nd, and 153Sm MDA reductions of factors of 1-2 were observed using optimized beta thresholds. Using beta anti-coincidence counting reductions of factors 3-5 were observed for isotopes like 89Sr, 95mNb, 115Cd, and 137Cs and factors of 5-7 for isotopes like 235U using alpha coincidence counting. The selectivity of gamma/gamma coincidence and reduction in backgrounds using beta gating were also demonstrated with 136Cs and 153Sm. The improvements observed in the detection sensitivity of fission products and actinides achieved by combining time-correlated radiation signatures is significant and of value to applications such as nuclear fission physics, environmental monitoring for nuclear waste, reactor accidental releases, and nuclear forensics.

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Exploring rapid chemical separations of Sc-47 produced from photonuclear reactions on natural vanadium targets

Scandium-47 ( 47 Sc) production via bremsstrahlung irradiation of natural vanadium targets offers significant advantages for producing high purity 47 Sc; this work evaluates several rapid dissolution and chemical separation techniques for recovering high purity 47 Sc from irradiated vanadium. Here, techniques developed are combined into a simple, gram-scale, semi-automated target processing system that enables 47 Sc recovery from irradiated vanadium targets with chemical yields as high as 93 ± 3% and 47 Sc/V separation factors of 6 ± 3 ·10 11 within 90 min total processing times. Future research into H 2 O 2 resistant separation techniques and their applicability for direct process coupling to chelation are recommended.

07 ISOTOPE AND RADIATION SOURCES↗

Demonstration of 151 Sm analysis using Trinity nuclear debris samples

Here, the long-lived fission product 151 Sm (T 1/2 ≈ 90 y) present in archived dissolved Trinity nuclear test debris samples was analyzed using liquid scintillation counting and the results were compared to the expected values based upon historical analysis results. The measured 151 Sm activities were found to agree with the expected values within experimental error. This demonstration validates the use of this technique in situations where the sample is too old for traditional shorter half-life radioactive fission product signatures such as 99 Mo (T 1/2 = 2.75 d), 97 Zr (T 1/2 = 16.7 h), 147 Nd (T 1/2 = 10.98 d), and 153 Sm (T 1/2 = 46.3 h), or too dilute for determining fissions through stable isotope ratio measurements.

151Sm↗

Neptunium redox speciation and determination of its total concentration in dissolved fuel simulant solutions by spectrophotometry

Here, two new approaches to measure Np concentration in dissolved used nuclear fuel simulant (aqueous feed for PUREX process) by spectrophotometry are developed. The first approach is based on chemical reduction of Np in the feed to its tetravalent state using ascorbic acid with simultaneous conversion of Pu(IV) to Pu(III). Interfering effects from light absorbing fission and corrosion products are accounted for by measuring optical absorbance spectrum of aqueous raffinate after extraction of U, Np, and Pu by tributyl phosphate in dodecane. The second approach uses no chemical treatment at all and relies on spontaneous valency adjustment of Np to Np(V) by dilution of the feed with water to reduce its acidity to low decimolar range of nitric acid concentration. Results of Np determination in the feed by spectrophotometry are in good agreement with its concentration measured by ICP-MS.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Retention of radionuclides in sol–gel surrogate nuclear explosive debris

Sol–gel vitrification can be used to rapidly produce solid, vitreous materials to support nuclear forensics research. Here, this work investigates three sol–gel synthetic approaches’ ability to retain fission products within the glass as a function of drying temperature. Eight of the ten fission products studied were quantitatively retained (less than 5% losses) at temperatures up to 600 °C for glasses prepared using an acidic catalyst and at temperatures up to 300 °C for glasses prepared using a basic catalyst. Both systems show partial loss of ruthenium and complete loss of iodine at temperatures above 300 and 100 °C, respectively.

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Improvements in iridium target chemistry

Abstract We developed and optimized the dissolution and separation chemistry of iridium (Ir) from irradiated Ir pellets and prepared Ir counting samples for analysis by a silicon drift detector. Previous Ir chemistry techniques used on the irradiated Ir pellets are tedious, lengthy, and require extra safety precautions and planning due to the use of perchloric acid in the dissolution step. The dissolution and separations method described in this paper are safer, eliminating the use of perchloric acid, more efficient, and can successfully replace the previous procedure.

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A chromatography chemistry for purifying $\mathrm{Pa}$ from $\mathrm{U-Nb}$ metal alloys

Here we present a chromatography chemistry for purifying protactinium from uranium metal alloys containing weight-percent concentrations of niobium. Niobium is precipitated in 9 M HCl without the co-precipitation of Pa as demonstrated by gamma-ray spectrometry. Protactinium is further purified using Bio-Rad™ anion resin AG® 1-X8 and 9 M HCl + 0.0128 M HF. A Pa/Nb separation factor of 85,000 and a 90% Pa recovery is demonstrated, which is amenable to 231 Pa concentration determination by isotope dilution and 231 Pa/ 235 U model age calculation for nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Evaluation of two extraction chromatography resins for scandium and titanium separation for medical isotope production

Scandium-47 ( 47 Sc) can be used in nuclear medicine as a therapeutic-diagnostic, or "theragnostic," radioactive medical isotope for cancer detection and treatment. The 47 Sc isotope can be produced through the photonuclear reaction 48 Ti(γ,p) 47 Sc by irradiating enriched 48 Ti target material. The enriched target material necessary for production is costly; 48 TiO 2 costs ~ $\$$1550/g, and targets can be > 50 g ($\$$77,500) to produce medically relevant amounts of 47 Sc. In order to keep costs low, a highly efficient separation of scandium from bulk titanium is desired, along with efficient methods for recycling the target material. Here this research is focused on evaluating efficient methods for the separation of scandium from bulk quantities of titanium using commercially available diglycolamide-based and hydroxamate-based extraction chromatography resins (DGA resin and ZR resin, respectively). The sorption of 47 Sc and Ti on these resins were investigated at varying concentrations of HNO 3 , HCl, H 2 SO 4 , and HF to explore how they might be used in a large-scale production/processing setting.

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Extraction of selenium and arsenic with TOA-impregnated XAD-2 resin from HCl

Here the uptake of 75 Se and 73 As on trioctylamine-impregnated resin from HCl solutions was studied with batch uptake, kinetics, and column studies. Selenium-75 extracts well (D w ~ 900) at high HCl concentrations (≥ 10 M) with and no extraction of 73 As at any HCl concentration. The uptake kinetics were slow with low extraction (D w < 100) for time periods ≤ 15 min and no clear equilibrium achieved even after 24 h. Column studies were performed to characterize the separation of 75 Se and 73 As; 75Se is retained from conc. HCl while arsenic is eluted with high yields and high radiopurity.

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Results from a controlled depleted uranium metal casting experiment designed to investigate nuclear Forensic Radiochronometry Signatures

The accurate interpretation of uranium metal 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry model ages requires an understanding of how uranium parent nuclides and decay progeny ( 230 Th and 231 Pa) behave during uranium metal casting. In order to directly measure the spatial distribution of 230 Th and 231 Pa in uranium metal before and after vacuum induction melting (VIM), Los Alamos National Laboratory identified uranium metal feedstock, characterized the metal feedstock, conducted a controlled casting experiment of an approximately 120 kg uranium metal rod, and characterized the cast metal. Herein this study presents radiochronometry results and quantified 230 Th and 231 Pa VIM separation factors from bulk uranium.

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Preliminary investigation of an uncertainty budget for uranium isotope ratio analysis using a liquid sampling—atmospheric pressure glow discharge—orbitrap mass spectrometer system

The liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source has proven to be an effective analysis tool for making uranium isotope ratio measurements when coupled to high-resolution mass spectrometers, such as the Orbitrap. While previous studies have shown the capabilities of the LS-APGD for isotope ratio determination, a systematic evaluation of the measurement uncertainty of the technique has not been conducted. To this end, the International Standards Organizations (ISO) guidelines to the expression of uncertainty in measurement (GUM analysis) have been applied to generate an uncertainty budget. For this work, a preliminary assessment derived from the GUM analysis was performed. The uncertainty in the instrument blank determination has been identified as a primary factor contributing to measurement uncertainty for the LS-APGD-Orbitrap method. These findings for the specific test case of uranium isotopic analysis will be invaluable in applications across the breadth of isotope ratio mass spectrometry performed on this unique instrumental platform.

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Behavior of selenium and arsenic in $\mathrm{HCl}$ and $\mathrm{HNO}$ 3 on $\mathrm{TRU, TEVA, DGA,}$ and $\mathrm{Pb}$ extraction chromatography resins

The uptake behavior of 73 As and 75 Se was studied in HCl and HNO 3 -H 2 O 2 solutions on commercial extraction chromatography resins (TEVA, TRU, DGA, and Pb resin). There was no uptake of 73 As or 75 Se from HNO 3 media. From HCl, there was 75 Se uptake at high concentrations on all the resins and no uptake of 73 As. Separations of 75 Se and 73 As on these resins have high yields and high radiopurity for 73 As, but limited recovery of 75 Se. TRU and TEVA resin may have potential for use in isotope generators as 75 Se can be retained for at least 26 days with repeated elutions.

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Determination of distribution coefficients of 41 elements in nitric and hydrochloric acids for actinide resin

The distribution coefficients of 41 elements were determined on Eichrom’s Actinide resin in HCl and HNO 3 solutions of molarities between 0.01 M and 9 M. Herein a separation scheme for these 41 elements was designed utilizing these distribution coefficients that combines the Actinide resin with Eichrom’s TRU resin. Overall, these values improve the ability to create separations targeting specific analytes utilizing Actinide resin.

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An introduction to the significance of sample size in particle analyses for nuclear forensics and radiological investigations

Particulate isotopic analysis in nuclear forensics has developed rapidly during the past two decades due to technical advances in determining the isotopic composition of individual particles. This paper introduces basic statistical concepts that can be applied by analysts to understand the importance of statistical adequacy when interpretating particle data. While these basic statistical methods provide a useful point-of-entry to particle data analysis, more sophisticated statistical and modeling approaches are needed to extract maximal information from such datasets in the future.

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Impact of lowering potassium contamination in liquid scintillation cocktails for ultra-sensitive radiation detection

Intrinsic 40 K radioactive backgrounds from impurities of natural K in liquid scintillation cocktails have previously been demonstrated to limit their use in ultra-sensitive applications. Here, this work explores two methodologies in parallel for the reduction of 40 K backgrounds in the cocktails, and lays the groundwork for use in ultra-sensitive applications. In one method, alternative low-K liquid scintillation matrix constituents were identified and in the other, a simple purification method for single components and finished cocktails was developed. Both methods were verified via ICP-MS analysis. Liquid scintillation counting of selected purified cocktails demonstrated background reduction, improved stability, and enhanced performance. The best performing purified cocktail was also counted on a custom-built ultra-low background liquid scintillation counter, with results below the detector background.

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Uptake behavior of arsenic and selenium with sulfur-based extraction chromatography resins in HCl and HNO 3 media

Here, the uptake behavior of 73 As and 75 Se was studied in HCl and HNO3 media with CL resin, ethanethiol resin and dimethyl sulfide resin. In HCl solutions, there was high extraction of selenium on CL resin and ethanethiol resin but lower uptake on dimethyl sulfide resin; arsenic was only extracted by CL resin. From HNO 3 , selenium was extracted only by ethanethiol resin and CL resin and there was no uptake of arsenic on any resin. While the sulfur-based resins have high selenium uptake and selectivity, column separations are challenging due to the chemical instability of these resins.

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Removal of fission product tellurium and iodine from recently irradiated HEU using copper metal

Gamma detection of select fission products or activation products such as 153 Sm and 239 Np in a fission sample is difficult due to gamma interferences from radiotellurium and radioiodine. To aid in the detection of these difficult-to-detect nuclides, the radiotellurium and radioiodine were removed using Cu metal turnings. This method is highly effective at the removal of the interfering radionuclides removing > 98% of the radiotellurium and radioiodine. A mechanistic study was conducted. Determining the deposition mechanism, using a number of techniques including XANES and electrochemistry providing an understanding of the electrochemical path for the Te deposition. Initial work focused on the use of stable Te, further expanding into activated TeO 2 , and a fresh fission sample. Importantly, this method presents a rapid method for the direct detection of select fission products that could have a significant impact on nuclear related fields including nuclear forensics.

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