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Preparative scale separation of thulium from erbium for neutron capture cross section measurements - Part: Preparative scale
Here, this paper discusses the development of a separation method for isolation of Tm-171 from a half-gram irradiated erbium target in support of stockpile stewardship and astrophysics research. The developed procedure is based on cation exchange separation using alpha-hydroxyisobutyric acid (α-HIBA) as chelating agent. It is able to achieve either a decontamination factor of 1.4(4) × 10 5 with 68.9(3) % recovery or 95.4(3) % recovery with a decontamination factor of 5.82(7) × 10 3 for a mock 500-mg target containing 17.9 mg thulium in a single pass-through at room temperature.
The simultaneous removal of technetium and iodine from Hanford tank waste
The simultaneous removal of radionuclides technetium-99 and iodine-129 from an actual decontaminated Hanford tank waste sample (a mixture of decontaminated waste from tanks 241-AP-105 and 241-AP-107) was demonstrated for the first time in this work. A series of commercially available ion exchange resins were evaluated in batch contact tests in the tank waste, and all showed removal of both Tc and I. The highest Tc removal was observed for Purolite A530e while the highest iodine removal was observed for ResinTech SIR-110-MP. Batch tests in simulated tank waste with these two resins showed that the SIR-110-HP-MP had consistently higher K d for both pertechnetate and iodide and much higher K d than previous works on Tc removal from Hanford waste. As such, the SIR-110-MP was evaluated in a dual -column (lead/lag) test processing 5.2L of the tank waste mixture showing 60% breakthrough of Tc on the lead column and no significant breakthrough on the lag after 625 bed volumes (BV, 6 mL size) while significant iodine breakthrough (>50%) occurred after 28 BV. The limited iodine uptake was attributed to the column conditions generating mass transfer limitations. A fraction of the Tc and I was not captured by the resin (<10%) in either the batch tests or column tests. The iodine fraction was identified to be an iodide, likely organo-iodide. The fraction of the Tc was identified as a non-pertechnetate species, which is the first time non-pertechnetate has been identified in AP-105 and AP-107 tanks, although the exact species is still unknown.
TiO{sub 2}-based photocatalytic disinfection of microbes in aqueous media: A review
The TiO{sub 2} based photocatalyst has great potential for the disinfection/inactivation of harmful pathogens (such as E.coli in aqueous media) along with its well-known usefulness on various chemical pollutants. The disinfection property of TiO{sub 2} is primarily attributed to surface generation of reactive oxygen species (ROS) as well as free metal ions formation. Furthermore, its disinfection capacity and overall performance can be significantly improved through modifications of the TiO{sub 2} material. In this review, we provide a brief survey on the effect of various TiO{sub 2} materials in the disinfection of a wide range of environmentally harmful microbial pathogens (e.g., bacteria, fungi, algae, and viruses) in aqueous media. The influencing factors (such as reactor design, water chemistry, and TiO{sub 2} modifications) of such processes are discussed along with the mechanisms of such disinfection. It is believed that the combined application of disinfection and decontamination will greatly enhance the utilization of TiO{sub 2} photocatalyst as a potential alternative to conventional methods of water purification. - Highlights: • The advent of industrialization jeopardized the quality of drinking water. • TiO{sub 2} photocatalysis holds promise both in the degradation of pollutants and for disinfection. • The applicability of TiO{sub 2}-based decontamination is explored for microbial disinfection. • Here we provide a comprehensive review on titania-based photocatalysts for disinfection.
Logistics simulation of a remediation effort for a hypothetical radiological contamination scenario
To mitigate the effects following a large-scale nuclear or radiological material release in an urban environment and to expedite recovery, the Integrated Wash-Aid Treatment Emergency Reuse System (IWATERS) was developed. IWATERS consists of three operations: washing contaminated surfaces with an ionic wash solution, collecting, and treating the contaminated wash solution on-site to remove contaminants, and reusing the treated solution throughout operations to preserve the clean water resource. This study develops a framework to simulate the logistics of IWATERS deployment, thereby gaining an understanding of the timeline for decontamination operations. For this purpose, the Analysis of Mobility Platform and GoldSim were leveraged for a hypothetical contamination scenario covering 65,200 m 2 of an urban center. The framework reveals that remediation progress is limited by several resources, notably the availability of vermiculite, a reactive clay that is required to treat the contaminated wash solution. Further, this study also presents how the simulation approach can be used to characterize alternatives to reduce the influence of limited resources on operational progress. Overall, this work lays the foundation for evaluating different decontamination methods through detailed logistics simulation, i.e., by refining simulation assumptions and expanding the range of scenarios the simulation can depict.
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.
Capture and Decomposition of the Nerve Agent Simulant, DMCP, Using the Zeolitic Imidazolate Framework (ZIF-8)
Understanding mechanisms of decontamination of chemical warfare agents (CWA) is an area of intense research aimed at developing new filtration materials to protect soldiers and civilians in case of state-sponsored or terrorist attack. In this study, we employed complementary structural, chemical, and dynamic probes and in situ data collection, to elucidate the complex chemistry, capture, and decomposition of the CWA simulant, dimethyl chlorophosphonate (DMCP). Our work reveals key details of the reactive adsorption of DMCP and demonstrates the versatility of zeolitic imidazolate framework (ZIF-8) as a plausible material for CWA capture and decomposition. Here, the in situ synchrotron-based powder X-ray diffraction (PXRD) and pair distribution function (PDF) studies, combined with Fourier transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), zinc K-edge X-ray absorption near edge structure (XANES), and Raman spectroscopies, showed that the unique structure, chemical state, and topology of ZIF-8 enable accessibility, adsorption, and hydrolysis of DMCP into the pores and revealed the importance of linker chemistry and Zn 2+ sites for nerve agent decomposition. DMCP decontamination and decomposition product(s) formation were observed by thermogravimetric analysis, FT-IR spectroscopy, and phosphorus (P) K-edge XANES studies. Differential PDF analysis indicated that the average structure of ZIF-8 (at the 30 Å scale) remains unchanged after DMCP dosing and provided information on the dynamics of interactions of DMCP with the ZIF-8 framework. Using in situ PXRD and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), we showed that nearly 90% regeneration of the ZIF-8 structure and complete liberation of DMCP and decomposition products occur upon heating.
Metal-Organic Framework- and Polyoxometalate-Based Sorbents for the Uptake and Destruction of Chemical Warfare Agents
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In Situ Probes of Capture and Decomposition of Chemical Warfare Agent Simulants by Zr-Based Metal Organic Frameworks
Zr-based metal organic frameworks (MOFs) have been recently shown to be among the fastest catalysts of nerve-agent hydrolysis in solution. We report a detailed study of the adsorption and decomposition of a nerve-agent simulant, dimethyl methylphosphonate (DMMP), on UiO-66, UiO-67, MOF-808, and NU-1000 using synchrotron-based X-ray powder diffraction, X-ray absorption, and infrared spectroscopy, which reveals key aspects of the reaction mechanism. The diffraction measurements indicate that all four MOFs adsorb DMMP (introduced at atmospheric pressures through a flow of helium or air) within the pore space. In addition, the combination of X-ray absorption and infrared spectra suggests direct coordination of DMMP to the Zr6 cores of all MOFs, which ultimately leads to decomposition to phosphonate products. These experimental probes into the mechanism of adsorption and decomposition of chemical warfare agent simulants on Zr-based MOFs open new opportunities in rational design of new and superior decontamination materials.
Anion-adaptive crystalline cationic material for 99 TcO 4 - trapping
Efficient anion recognition is of great significance for radioactive 99 TcO 4 - decontamination, but it remains a challenge for traditional sorbents. Herein, we put forward a tactic using soft crystalline cationic material with anion-adaptive dynamics for 99 TcO 4 - sequestration. A cucurbit[8]uril-based supramolecular metal-organic material is produced through a multi-component assembly strategy and used as a sorbent for effective trapping of TcO 4 - . Excellent separation of TcO 4 - /ReO 4 - is demonstrated by fast removal kinetics, good sorption capacity and high distribution coefficient. Remarkably, the most superior selectivity among metal-organic materials reported so far, together with good hydrolytic stability, indicates potential for efficient TcO 4 - removal. The structure incorporating ReO 4 - reveals that the supramolecular framework undergoes adaptive reconstruction facilitating the effective accommodation of TcO 4 - /ReO 4 - . The results highlight opportunities for development of soft anion-adaptive sorbents for highly selective anion decontamination.
A solvent-free solid catalyst for the selective and color-indicating ambient-air removal of sulfur mustard
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Alkaline earth ion exchange study in pure silica LTA zeolites using periodic first-principles calculations
Experiments show that Zeolites, such as Linde Type A (LTA), are promising materials for radioactive decontamination processes. In this work, the thermodynamic properties associated with alkaline earth ion (Ca2+, Sr2+ and Ba2+) exchange in pure silica LTA was studied using periodic first-principles calculations. The adsorption energies of alkaline earth ions compared with that of Na+ were investigated. The driving force for the alkaline earth exchange and related isotherms were calculated, and analyzed as a function of the electron chemical potential. The results demonstrate that Na+ in a pure silica LTA can completely be removed by Ba2+ and almost completely be removed by Sr2+ from a stream, but cannot be effectively exchanged by Ca2+. We also showed that electron-donating dopants should suppress the Sr2+ and Ba2+ ion exchange, and that there is a substantial preference for incorporating Ba2+ over Sr2+. Lastly, the substantial difference between the adsorption energies of the ions in an assumed vacuum and those computed in water suggests that a solvation model is needed for accurate representation of ion adsorption in an LTA zeolite.
Dark Energy Survey Year 3 results: galaxy clustering and systematics treatment for lens galaxy samples
ABSTRACT In this work, we present the galaxy clustering measurements of the two DES lens galaxy samples: a magnitude-limited sample optimized for the measurement of cosmological parameters, maglim, and a sample of luminous red galaxies selected with the redmagic algorithm. maglim/redmagic sample contains over 10 million/2.5 million galaxies and is divided into six/five photometric redshift bins spanning the range z ∈ [0.20, 1.05]/z ∈ [0.15, 0.90]. Both samples cover 4143 $\deg ^2$ over which we perform our analysis blind, measuring the angular correlation function with an S/N ∼ 63 for both samples. In a companion paper, these measurements of galaxy clustering are combined with the correlation functions of cosmic shear and galaxy–galaxy lensing of each sample to place cosmological constraints with a 3 × 2pt analysis. We conduct a thorough study of the mitigation of systematic effects caused by the spatially varying survey properties and we correct the measurements to remove artificial clustering signals. We employ several decontamination methods with different configurations to ensure the robustness of our corrections and to determine the systematic uncertainty that needs to be considered for the final cosmology analyses. We validate our fiducial methodology using lognormal mocks, showing that our decontamination procedure induces biases no greater than 0.5σ in the (Ωm, b) plane, where b is the galaxy bias.
Simulations and Experimental Verifications of an Algorithm for Radiation Source Mapping and Navigational Path Generation
Accurate and efficient mapping and localization of both ionizing and non-ionizing radiation sources are important across many different fields. As such, a versatile mapping and navigational path generation algorithm, which can be applied to any point source measurements that follow an inverse-square characteristic, was developed using non-linear least squares methods. Forty thousand simulations were performed on the algorithm, which located sources successfully in a 10 m × 10 m × 10 m three-dimensional space with a success rate of over 80% across different noise functions, given a proportional constant of 10 to 1,000. The algorithm was also verified experimentally with small-scale radioactive decontamination of a 70 cm × 70 cm surface and localization of a lost Wi-Fi router in a 70 m × 70 m open field. One hundred twenty-one measurements were taken from each experiment, which were then fed into the algorithm for navigation. For the radioactive 137Cs source, the estimated locations were within 7 cm × 7 cm of the answer in 79.3% of the scenarios, while the Wi-Fi router was located to within 7 m × 7 m in 57.9% of the tests. In general, the method requires much less information and data than a geographically comprehensive survey and thus shows a lot of potential for practical applications, such as lost source retrieval with unmanned aerial vehicles, small-scale decontamination, mapping undocumented Wi-Fi routers or radio towers, and radiation simulation with radio signals. Here, the different failure modes, desirable features, and potential improvements were also identified but remain as future work.
Treatment of irradiated graphite from French Bugey reactor
In 2008, following the general French plan for nuclear waste management, Electricite de France attempted to find for irradiated graphite an alternative solution to direct storage at the low-activity long-life storage center in France managed by the national agency for wastes (ANDRA). EDF management requested that its engineering arm, EDF CIDEN, study the graphite treatment alternatives to direct storage. In mid-2008, this study revealed the potential advantage for EDF to use a steam reforming process known as Thermal Organic Reduction, 'THOR' (owned by Studsvik, Inc., USA), to treat or destroy the graphite matrix and limit the quantity of secondary waste to be stored. In late 2009, EDF began a test program with Studsvik to determine if the THOR steam reforming process could be used to destroy the graphite. The program also sought to determine if the graphite could be treated to release the bulk of activity while minimizing the gasification of the bulk mass of the graphite. In October 2009, tests with non-irradiated graphite were completed and demonstrated destruction of a graphite matrix by the THOR process at satisfactory rates. After gasifying the graphite, focus shifted to the effect of roasting graphite at high temperatures in inert gases with low concentrations of oxidizing gases to preferentially remove volatile radionuclides while minimizing the graphite mass loss to 5%. A radioactive graphite sleeve was imported from France to the US for these tests. Completed in April 2010, 'Phase I' of testing showed that the process removed >99% of H-3 and 46% of C-14 with <6% mass loss. Completed in September 2011, 'Phase II' testing achieved increased removals as high as 80% C-14. During Phase II, it was also discovered that roasting in a reducing atmosphere helped to limit the oxidation of the graphite. Future work seeks to explore the effects of reducing gases to limit the bulk oxidation of graphite. If the graphite could be decontaminated of long-lived radionuclides up to 95% for C-14 while minimizing mass loss to <5%, this would minimize the volume of any secondary waste streams and potentially lower the waste class of the larger bulk of graphite. Alternatively, if up to 95% decontamination of C-14 is achieved, the graphite may be completely gasified which could result in lower disposal. (authors)
Addressing the dynamic nature of reference data: a new nucleotide database for robust metagenomic classification
Accurate metagenomic classification relies on comprehensive, up-to-date, and validated reference databases. While the NCBI BLAST Nucleotide (nt) database, encompassing a vast collection of sequences from all domains of life, represents an invaluable resource, its massive size—currently exceeding 10 12 nucleotides—and exponential growth pose significant challenges for researchers seeking to maintain current nt-based indices for metagenomic classification. Recognizing that no current nt-based indices exist for the widely used Centrifuge classifier, and the last public version currently available was released in 2018, we addressed this critical gap by leveraging advanced high-performance computing resources. We present new Centrifuge-compatible nt databases, meticulously constructed using a novel pipeline incorporating different quality control measures, including reference decontamination and filtering. These measures demonstrably reduce spurious classifications, as shown through our reanalysis of published metagenomic data where Plasmodium annotations were dramatically reduced using our decontaminated database, highlighting how database quality can significantly impact research conclusions. Through temporal comparisons, we also reveal how our approach minimizes inconsistencies in taxonomic assignments stemming from asynchronous updates between public sequence and taxonomy databases. These discrepancies are particularly evident in taxa such as Listeria monocytogenes and Naegleria fowleri, where classification accuracy varied significantly across database versions. These new databases, made available as pre-built Centrifuge indexes, respond to the need for an open, robust, nt-based pipeline for taxonomic classification in metagenomics. Applications such as environmental metagenomics, forensics, and clinical metagenomics, which require comprehensive taxonomic coverage, will benefit from this resource. Our work highlights the importance of treating reference databases as dynamic entities, subject to ongoing quality control and validation akin to software development best practices. This approach is crucial for ensuring accuracy and reliability of metagenomic analysis, especially as databases continue to expand in size and complexity.
Experimental Ion Exchange Column with SuperLig®639 And Simulant Formulation
SuperLig®639 ion exchange resin was tested as a retrieval mechanism for pertechnetate, through decontamination of a perrhenate spiked 5M Simple Average Na + Mass Based Simulant. Testing included batch contacts and a three-column ion exchange campaign. A decontamination of perrhenate exceeding 99% from the liquid feed was demonstrated. Analysis of the first formulation of a SBS/WESP simulant found unexpectedly low concentrations of soluble aluminum. Follow-on work will complete the formulation.
Simulation of Sediment and Cesium Transport in the Ukedo River and the Ogi Dam Reservoir during a Rainfall Event using the TODAM Code
The accident at the Fukushima Daiichi Nuclear Power Plant in March 2011 caused widespread environmental contamination. Although decontamination activities have been performed in residential areas of the Fukushima area, decontamination of forests, rivers, and reservoirs is still controversial because of the economical, ecological, and technical difficulties. Thus, an evaluation of contaminant transport in such an environment is important for safety assessment and for implementation of possible countermeasures to reduce radiation exposure to the public.