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At least 973 records · Page 54

Chromatographic separation of radioactive noble gases from xenon

The Large Underground Xenon (LUX) experiment operates at the Sanford Underground Research Facility to detect nuclear recoils from the hypothetical Weakly Interacting Massive Particles (WIMPs) on a liquid xenon target. Liquid xenon typically contains trace amounts of the noble radioactive isotopes 85 Kr and 39 Ar that are not removed by the in situ gas purification system. The decays of these isotopes at concentrations typical of research-grade xenon would be a dominant background for a WIMP search exmperiment. To remove these impurities from the liquid xenon, a chromatographic separation system based on adsorption on activated charcoal was built. 400 kg of xenon was processed, reducing the average concentration of krypton from 130 ppb to 3.5 ppt as measured by a cold-trap assisted mass spectroscopy system. Finally, a 50 kg batch spiked to 0.001 g/g of krypton was processed twice and reduced to an upper limit of 0.2 ppt.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Response of bentonite microbial communities to stresses relevant to geodisposal of radioactive waste

Microbes have been isolated previously from bentonite materials that may be used as barriers for the disposal of radioactive waste. Actively respiring microbes in such barrier materials, within a repository environment, have the potential to adversely affect waste container corrosion rates. Additionally, they could potentially alter the properties of the bentonite barrier itself. This is of significance, since the integrity of the waste container and properties of the bentonite barrier are required to fulfil defined safety functions. Furthermore to help identify the critical factors that affect microbial activity in bentonite materials, this study examines the impact of a range of parameters that could affect microbial metabolism in a geodisposal environment. Several bentonites from different sources (bentonite mined from locations in Spain and the USA, along with commercially-sourced bentonite) were subjected to increased pressure (74 MPa, 30 s), heat (90 °C, 24 h), and irradiation (1000 Gy, 24.17 Gy min –1 ), before incubation in growth media selective for sulfate-reducing bacteria (SRB) or iron-reducing bacteria (IRB).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the long-term migration of uranyl in bentonite barrier for high-level radioactive waste repositories: The effect of different host rocks

Repositories for high level radioactive waste hosted in argillite or granite with bentonite backfill are the two disposal concepts that been extensively studied. A general perception is that granite has very low sorption capacity and therefore is disadvantageous in retarding the migration of radionuclides in comparison with argillite. However, when there is bentonite backfill, does the sorption capacity of granite really matter for the migration of radionuclides? How different host rocks would affect the migration of U(VI) through the bentonite backfill of an engineered barrier system (EBS), and which properties of the host rocks cause those differences in migration, given that migration of radionuclides is a critical measure in assessing the performance of a repository? Here we present two coupled thermal, hydrological, and chemical models for the transport of U(VI), each with an identical setup except for the type of host rock (argillite vs granite rock). Comparisons between our models show that the different host rocks exert their influence on migration of U(VI) via regulating the chemical conditions in the bentonite, which affect the concentration of U(VI) at the source and the adsorption of U(VI) in the bentonite. The key chemical conditions are pH, Ca + , and HCO 3 - concentration in pore-water, which are strongly affected by soluble carbonate minerals. Our models also show the occurrence of illitization (dissolution of smectite and precipitation of illite) in the bentonite, which affects the migration of U(VI) through changing pH and the quantity of adsorbents. Although generalization of current model results for granite and argillite should be done carefully, the simulations highlight the importance of pore-water chemistry in host rock, as well as bentonite-host rock interactions, when assessing the performance of a repository. In comparison to properties such as thermal conductivity, permeability, and adsorption capacity, properties that have been studied intensively, the pore-water chemistry of host rocks deserve equal or even more attention because of its strong influence on radionuclide migration.

58 GEOSCIENCES↗

Neutron diffraction illustrates residual stress behavior of welded alloys used as radioactive confinement boundary

Corrosion-resistant welded alloys are frequently used as a leak-tight boundary in critical applications that require confinement of hazardous and/or radioactive substances, including an increasing population of spent nuclear fuel (SNF) canisters. The behavior of residual stresses generated as a result of irregular elastic–plastic deformation during processes such as welding is one of today's key issues to a full understanding of the aging mechanisms that may compromise the confinement boundary. Whether such processes and any subsequent weld repairs, not subjected to post-weld heat treatment, would negatively affect the initial material by introducing through-thickness tensile stresses remains an open question. Here we report the first residual stress measurements using neutron diffraction on the welded joints of a SNF canister. We found significant tensile residual stresses in the as welded sample, indicating that initiation and through-thickness growth of cracks may be possible. Following repair, we observed a stress redistribution and introduction of beneficial compressive stresses. We anticipate our results will improve understanding of confinement susceptibility to aging and guide improvements in repair techniques.

36 MATERIALS SCIENCE↗

Patient Positioning Based on a Radioactive Tracer Implanted in Patients With Localized Prostate Cancer: A Performance and Safety Evaluation

Purpose: To evaluate the performance and safety of a radiation therapy positioning system (RealEye) based on tracking a radioactive marker (Tracer) implanted in patients with localized prostate cancer. Methods and Materials: We performed a single-arm multi-institutional trial in 20 patients. The iridium-192 ({sup 192}Ir)-containing Tracer was implanted in the patient together with 4 standard gold seed fiducials. Patient prostate-related symptoms were evaluated with the International Prostate Symptom Score (IPSS) questionnaire. Computed tomography (CT) was performed for treatment planning, during treatment, and after treatment to evaluate the migration stability of the Tracer. At 5 treatment sessions, cone beam CT was performed to test the positioning accuracy of the RealEye. Results: The Tracer was successfully implanted in all patients. No device or procedure-related adverse events occurred. Changes in IPSS scores were limited. The difference between the mean change in Tracer-fiducial distance and the mean change in fiducial-fiducial distance was -0.39 mm (95% confidence interval [CI] upper boundary, -0.22 mm). The adjusted mean difference between Tracer position according to RealEye and the Tracer position on the CBCT for all patients was 1.34 mm (95% CI upper boundary, 1.41 mm). Conclusions: Implantation of the Tracer is feasible and safe. Migration stability of the Tracer is good. Prostate patients can be positioned and monitored accurately by using RealEye.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Multi-Sampling Ionization Chamber (MUSIC) for measurements of fusion reactions with radioactive beams

A detection technique for high-efficiency measurements of fusion reactions with low-intensity radioactive beams was developed. The technique is based on a Multi-Sampling Ionization Chamber (MUSIC) operating as an active target and detection system, where the ionization gas acts as both target and counting gas. In this way, we can sample an excitation function in an energy range determined by the gas pressure, without changing the beam energy. The detector provides internal normalization to the incident beam and drastically reduces the measuring time. In the first experiment we tested the performance of the technique by measuring the 10,13,15 C+ 12 C fusion reactions at energies around the Coulomb barrier.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Trace radioactive impurities in final construction materials for EXO-200

Here, we report results from a systematic measurement campaign conducted to identify low radioactivity materials for the construction of the EXO-200 double beta decay experiment. Partial results from this campaign have already been reported in a 2008 paper by the EXO collaboration. Here we release the remaining data, collected since 2007, to the public. The data reported were obtained using a variety of analytic techniques. The measurement sensitivities are among the best in the field. We concluded the construction of the EXO-200 detector and Phase-I data was taken from 2011 to 2014. The detector’s extremely low background implicitly verifies the measurements and the analysis assumptions made during construction and reported in this paper.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Design of SECAR a recoil mass separator for astrophysical capture reactions with radioactive beams

A recoil mass separator SECAR has been designed for the purpose of studying low-energy (p,γ) and (α,γ) reactions in inverse kinematics with radioactive beams for masses up to about A = 65. Their reaction rates are of importance for our understanding of the energy production and nucleosynthesis during explosive hydrogen and helium burning. The radiative capture reactions take place in a windowless hydrogen or He gas target at the entrance of the separator, which consists of four Sections . The first Section selects the charge state of the recoils. The second and third Sections contain Wien Filters providing high mass resolving power to separate efficiently the intense beam from the few reaction products. In the following fourth Section , the reaction products are guided into a detector system capable of position, angle and time-of-flight measurements. In order to accept the complete kinematic cone of recoil particles including multiple scattering in the target in the center of mass energy range of 0.2 MeV to 3.0 MeV, the system must have a large polar angle acceptance of ± 25 mrad. This requires a careful minimization of higher order aberrations. Furthermore, the present system will be installed at the NSCL ReA3 accelerator and will be used with the much higher beam intensities of the FRIB facility when it becomes available.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Production and characterization of thin, self-supporting Si foils for use as targets in radioactive beam experiments

Development of thin, self-supporting silicon foils (both natural and isotopically-enriched) for use as targets in reaction studies with radioactive beams is detailed. Foils with a thickness of ~220 μg/cm 2 were produced using vapor deposition and were floated onto aluminum frames with 10–15 mm diameter holes. During their production, the foil thickness was measured using a quartz crystal monitor. Subsequently, the foil thickness was characterized by particle energy loss measurements and Rutherford backscattering (RBS). These measurements demonstrated that the thickness could be determined to within a 0.5% uncertainty. The elemental purity of the foils was assessed using RBS and X-ray photoelectron spectroscopy. Lastly, this analysis demonstrated that the foils have 87%–90% silicon abundance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A novel approach for critical heat flux enhancement during severe accident mitigation with removal of radioactive materials from the coolant

In this paper, a new system, which consists of mature and proven technologies, is suggested for simultaneous objectives in nuclear power plants: CHF enhancement and effective decontamination. It consists of multifunctional magnetic nanoparticles and a collector part. CHF enhancement for severe accident mitigation strategies like IVR-ERVC and core catcher is expected along with an efficient decontamination process of target radioactive nuclides, and through the collector part, where external magnetic fields are applied, working fluid can be effectively purified. The multifunctional magnetic nanoparticle possesses potentials to severe accident scenarios based on its distinct characteristics. Also, a nanofluid system is strongly affected by environments and state of the immersed particles; the CHF enhancement can be stably achieved in real applications with proper consideration and optimization.

Kam, Dong Hoon↗

Decay spectroscopy at the two-proton drip line: Radioactivity of the new nuclides 160 Os and 156 W

The radioactivity of $^{160}_{76}$Os 84 and $^{156}_{74}$W 82 that lie at the two-proton drip line has been measured in an experiment performed at the Accelerator Laboratory of the University of Jyväskylä. The 160 Os nuclei were produced using fusion-evaporation reactions induced by a beam of 310 MeV 58 Ni ions bombarding a 106 Cd target. The 160 Os ions were separated in flight using the recoil separator MARA and implanted into a double-sided silicon strip detector, which was used to measure their decays. The α decays of the ground state of 160 Os (Ε α = 7092(15) keV, t 1/2 = 97$^{+97}_{-32}$ μs) and its isomeric state (Ε α = 8890(10) keV, t 1/2 = 41$^{+15}_{-9}$ μs) were measured, allowing the excitation energy of the isomer to be determined as 1844(18) keV. These α-decay properties and the excitation energy of the isomer are compared with systematics. The α decays were correlated with subsequent decays to investigate the β decays of the ground state of 156 W, revealing that unlike its isotones, both low-lying isomers were populated in its daughter nuclide, 156 Ta. An improved value for the half-life of the proton-decaying high-spin isomeric state in $^{156}_{73}$Ta 83 of 333$^{+25}_{-22}$ ms was obtained in a separate experiment using the same experimental systems with a 102 Pd target. This result was employed to improve the precision of the half-life determined for 156 W, which was measured as 157$^{+57}_{-34}$ ms.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

In vivo transport of three radioactive [ 18 F]-fluorinated deoxysucrose analogs by the maize sucrose transporter ZmSUT1

Sucrose transporter (SUT) proteins translocate sucrose across cell membranes; however, mechanistic aspects of sucrose binding by SUTs are not well resolved. Specific hydroxyl groups in sucrose participate in hydrogen bonding with SUT proteins. We previously reported that substituting a radioactive fluorine-18 [ 18 F] at the C-60 position within the fructosyl moiety of sucrose did not affect sucrose transport by the maize (Zea mays) ZmSUT1 protein. To determine how 18 F substitution of hydroxyl groups at two other positions within sucrose, the C-10 in the fructosyl moiety or the C-6 in the glucosyl moiety, impact sucrose transport, we synthesized 10-[F 18 ]fluoro-10-deoxysucrose and 6-[F 18 ]fluoro-6-deoxysucrose ([ 18 F] FDS) analogs. In this work, each [ 18 F]FDS derivative was independently introduced into wild-type or sut1 mutant plants, which are defective in sucrose phloem loading. All three (10-, 60-, and 6-) [ 18 F]FDS derivatives were efficiently and equally translocated, similarly to carbon-14 [ 14 C]-labeled sucrose. Hence, individually replacing the hydroxyl groups at these positions within sucrose does not interfere with substrate recognition, binding, or membrane transport processes, and hydroxyl groups at these three positions are not essential for hydrogen bonding between sucrose and ZmSUT1. [ 18 F]FDS imaging afforded several advantages compared to [ 14 C]-sucrose detection. We calculated that 10-[ 18 F]FDS was transported at approximately a rate of 0.90 ± 0.15 m.h-1 in wild-type leaves, and at 0.68 ± 0.25 m.h-1 in sut1 mutant leaves. Collectively, our data indicated that [ 18 F]FDS analogs are valuable tools to probe sucrose-SUT interactions and to monitor sucrose transport in plants.

59 BASIC BIOLOGICAL SCIENCES↗

Monte Carlo investigation of a high-efficiency, two-plane Compton camera for long-range localization of radioactive materials

Compton cameras have become an instrument of interest for long-range localization of radioactive materials in nuclear-nonproliferation applications. In this work, a specialized simulation tool was developed for the optimization of a Compton camera through realistic Monte Carlo simulations. This tool can be used for Compton cameras with different geometries. The MCNPX-PoliMi code was used to simulate Compton scatters and photoelectric absorptions in the camera's detectors. The imaging capability is derived from the physics of Compton scattering and the full-energy information obtained in photoelectric absorptions. The simulated system is a 1 1 m2 Compton camera consisting of two planar arrays of photon detectors. Several scintillators were evaluated: LaBr3, CaF2, and NaI(Tl) (all inorganic scintillators), and C9H10 (plastic organic scintillator). The investigation was carried out with a 137Cs source. A minimum detectable activity (MDA) was defined and used to assess the performance of cameras based on different detectors. The simulation results show that C9H10 is a reliable, low-cost, scatter-plane material, increasing the MDA by ~0.2 mCi when compared to a CaF2 scatter plane. On the other hand, the intrinsic background of LaBr3 undermines its above-average energy resolution as the MDA increased by ~0.5 mCi when compared to a NaI(Tl) absorption plane.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Trisodium Phosphate Phases and Solubility in Alkaline Solutions Relevant to Radioactive Waste Processing

The U.S. Department of Energy’s Hanford Site faces significant challenges in managing millions of gallons of legacy radioactive waste, where phosphate precipitation can obstruct pipelines during retrieval and processing. To resolve long-standing inconsistencies in reported solubility and clarify factors governing trisodium phosphate hydrates, we examined the Na3PO4:NaOH:H2O system. Powder and single-crystal X-ray diffraction revealed that commercial precursors undergo transformations that produce multiple hydrates, including three previously unreported phases comprising an ordered polymorph of Na3(PO4)·12H2O·1/6NaOH, Na3PO4·5H2O, and Na3PO4·9H2O. Computational modeling indicated that the ordered dodecahydrate is more stable than its disordered counterpart, suggesting kinetic persistence of structural disorder. Solubility measurements were conducted with solutions prepared either from anhydrous Na3PO4 or from Na3(PO4)·12H2O·1/6NaOH and revealed that release of interstitial NaOH from the hydrate precursor elevated solution alkalinity, thereby significantly reducing phosphate solubility relative to solutions prepared with anhydrous Na3PO4 across 20–44 °C. These results begin to reconcile inconsistencies in prior solubility data and clarify how phase composition dictates phosphate precipitation under alkaline conditions.

Graham, Trenton R. (ORCID:0000000189078004)↗

Atom-at-a-Time Radioactive Molecule Identification: Looking toward Studies of Superheavy Elements

The chemical behavior of superheavy elements (SHEs, Z > 103) remains poorly understood. Their chemical properties are expected to deviate from established trends, challenging the predictive power of the periodic table. To investigate these elements experimentally, they must first be synthesized through nuclear reactions and then quickly subjected to chemical studies before they decay. Given the low production rates of these reactions and the need for measurements on an atom-at-a-time basis, innovative techniques are needed. Here, to address these challenges, a novel gas-phase chemistry method has been developed at Lawrence Berkeley National Laboratory, utilizing the Berkeley Gas-filled Separator and FIONA. This technique enables the production, identification, and study of molecular species formed by SHEs. As a proof of concept, we present measurements on the formation and identification of 151,152 HoO + molecules, demonstrating the capability to study the production of radioactive molecules under controlled conditions and directly identify them via their mass-to-charge ratio. These measurements validate the effectiveness of this technique for low-statistics SHE studies, highlighting the potential of this approach to ignite the next generation of experimental SHE chemistry research, offering a path to re-evaluate SHE placement on the periodic table.

Chemistry↗

Conjugates of Magnetic Nanoparticle -- Actinide Specific Chelator for Radioactive Waste Separation

A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed.

99 GENERAL AND MISCELLANEOUS↗

Selective Binding and Light-Driven Release of Fluorous PF 6 – and Radioactive 99 TcO 4 – Anions for All-to-Nothing Liquid–Liquid Extraction

The removal of anions from aqueous media using molecular receptors in liquid–liquid extraction is a long-standing strategy to clean up contaminated water sources. Therein, high selectivity is needed to remove specific ions from mixtures of other ions, and high affinity provides extractions at low concentrations. However, the high affinity creates a conundrum by impeding the release of the ions in any stripping steps needed for further processing. To circumvent this problem, light-responsive receptors have been proposed as candidates for turning off the binding, but they are currently untested in liquid–liquid extraction. We tested the feasibility of light-driven release using a cyanostar macrocycle. We demonstrate the selective extraction of PF$^{–}_{6}$ anions over large excesses of competing anions (Cl – , NO$^{–}_{3}$, SO$^{2–}_{4}$) followed by photodriven release for quantitative isolation of the target. Release relies on photoisomerization of the macrocycle’s five stilbenes generating distorted isomers to turn off binding. With modest reversibility, only a single-shot release was demonstrated, akin to photodriven uncaging. These methods were extended to the capture and photodriven release of ReO$^{–}_{4}$ and radioactive 99 TcO$^{–}_{4}$ anions at ∼90% efficiency. Extraction was demonstrated down to the highly dilute 4 ppb levels of the 99 TcO$^{–}_{4}$ anion. Furthermore, this proof-of-concept demonstration verifies the use of a large change in affinity for the all-to-nothing capture and release of target anions between liquid phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage

The incorporation of supramolecular macrocycles into porous organic polymers may endow the material with enhanced uptake of specific guests through host–guest interactions. Here we report a solvent and catalyst-free mechanochemical synthesis of pillar[5]quinone (P5Q) derived multi-microporous organic polymers with hydrophenazine linkages (MHP-P5Q), which show a unique 3-step N 2 adsorption isotherm. In comparison with analogous microporous hydrophenazine-linked organic polymers (MHPs) obtained using simple twofold benzoquinones, MHP-P5Q is demonstrated to have a superior performance in radioactive iodomethane (CH 3 I) capture and storage. Mechanistic studies show that the rigid pillar[5]arene cavity has additional binding sites though host–guest interactions as well as the halogen bond (-I···N = C-) and chemical adsorption in the multi-microporous MHP-P5Q mainly account for the rapid and high-capacity adsorption and long-term storage of CH 3 I.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗