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At least 649 records · Page 36

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DOE OSTI2017

Computational Studies of Gas Phase Reactions of Zirconium Tetrachloride (ZrCl{sub 4}) and Metal Chloride Impurities

Zirconium-based cladding materials that surround used nuclear fuel (UNF) rods represent a significant fraction of the total amount of high level waste that must be disposed of in long term geological repositories. The decontamination, recovery and reuse of these materials would significantly reduce the high level waste associated with light water reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. One part in the strategy to recycle zirconium from used cladding materials involves developing a computational modeling (DFT) protocol to understand the reactions between ZrCl{sub 4} and metal chloride impurities that may occur in the gas phase during sublimation. Several of the metal chloride species present are known to form Lewis acid/base adducts in the gas phase and development of purification protocols require investigation into the properties of these ZrCl{sub 4} contaminates.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

Tritium Management Requirements and Approaches for UNF Reprocessing

Four radionuclides have been identified as being sufficiently volatile in reprocessing of nuclear fuel that their release to the environment needs to be controlled to meet U.S. regulatory requirements. These radionuclides are {sup 3}H, {sup 14}C, {sup 85}Kr, and {sup 129}I. While iodine has been the focus of a number of studies due to the high decontamination factor (DF) requirements on multiple escape pathways, it is clear from prior studies that the control of tritium will also be a significant issue for future reprocessing plants, especially if processing relatively short-cooled fuels (<10 yr post-reactor discharge). Tritium contained in a used nuclear fuel (UNF) matrix will be released into the liquid and off-gas streams during fuel reprocessing. The amounts released into the process streams are a function of the type and burnup of the fuel processed and the chemical processes employed within the reprocessing plant. Previous studies have examined the tritium capture requirements for the reprocessing facility assuming that all of the tritium contained in the fuel matrix is volatilized in the head-end operations; i.e., tritium pretreatment is employed and tritium is completely released from the cladding. This scenario tends to limit the release pathway to the headend off-gas stream. Previous studies by Jubin and Spencer examined the accumulation and distribution of tritium in an aqueous-based reprocessing plant.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

Examining the Effect of Plume Rise on Radiological Consequences of Nuclear Accidents

A nuclear accident could cause release of radioactive material outside containment. This material will eventually disperse into the surrounding environment, and could pose a serious threat to public safety, and environment. Mitigation of radiological consequences of such an accident is highly desirable, and since Fukushima accident, there has been a growing focus on nuclear utilities to develop capabilities for this purpose. Undoubtedly, suppression of radioactive material release and dispersion is the primary mean for mitigating radiological consequences nevertheless alternative methods should also be explored to broaden the spectrum of choices for actual circumstances. As we know that, dispersion of radioactive material and subsequent radiological consequences are affected by plume rise. Plume rise is an important factor in determining ground level contamination since it can increase effective release height appreciably provided that effluent discharge speed and temperature is high enough. Under most circumstances, one can expect reduction in radiological consequences due to lower levels of radiation dose and ground contamination in the presence of adequate plume rise. Nevertheless, the effect of plume rise is usually ignored in radiological consequence studies for the sake of conservatism, and lack of information. However, this particular attribute of plume rise interested us to investigate the effect of plume rise in the scope of consequence mitigation and how this advantage could be utilized during an accident progression to minimize the impact of radioactivity release to the environment. In this work, we examine the effect of plume rise on radiological consequences of a nuclear accident for plume rise contributions much larger ({approx}500 m) than usually achievable in normal circumstances. The effect of plume rise on radiological consequences is quantified in this study as decontamination credit (DCC) achievable corresponding to maximum annual dose. This analysis is performed for a number of release heights and atmospheric conditions. We discuss available results in the scope of radiological consequence mitigation, devising a strategy for utilizing plume rise phenomenon with the help of an external propelling device like a jet engine for radiological consequence management. This study is continuation of our efforts for devising systems and strategies to mitigate consequences of radioactivity release accidents like Fukushima. We have proposed several ideas for suppressing/preventing the dispersion of released radioactive material to the environment using offsite equipment.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2015

Development of criticality risk evaluation method for fuel debris in Fukushima Dai-ichi NPS - 14373

After the accident of Fukushima Dai-ichi Nuclear Power Station, there has been still damaged nuclear fuel in the reactor buildings, which is called 'fuel debris' and contains an amount of fissile materials show that it is currently subcritical, which must be kept until finishing retrieval work. In the latest plan, retrieving fuel debris is to start in 2025. The International Research Institute for Nuclear Decommissioning, IRID, has been developing the technology for decontamination in reactor building. A developed method will be reviewed and granted by the Nuclear Regulatory Authority in Japan, NRA, before the start of the retrieving. Criticality risk information will be needed for decision making on following two subcriticality issues, -Criticality control of fuel debris to keep is subcritical until the end of retrieval work. -Safe operation for retrieving fuel debris to keep it subcritical. Because fuel debris has been out of criticality control and the key condition for its current subcriticality is unknown, it is important to obtain criticality risk information as soon as possible. Applying conventional Probabilistic Safety Assessment, PSA, to fuel debris is difficult, because it is based on the probability of becoming out of criticality control due to troubles such as equipment failure, operation mistake and so on. A new method, which has been developed by Japan Atomic Energy Agency to technically support the NRA, is designed to estimate criticality risk based on a probability distribution of k{sub eff} due to uncertainty of composition and geometry of fuel debris, which method will provide risk information for the two subcriticality issues as well as for the tolerance level of criticality risk if it is unavoidable. Developed method contains four steps: two steps of analysis of criticality risk and two steps of quantification of the risk. A procedure of risk quantification has been defined, in which systematic analysis of criticality risk can be done by making 'status matrix'. A trial analysis by using the procedure shows that some events which can initiate criticality are able to be supposed to happen during maintenance period until the beginning of retrieving fuel debris, and that analysis also indicates countermeasures should be considered as soon as possible in order to reduce criticality risk for public and workers. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Synergistic degradation performance of UV / TiO 2 photocatalysis and biotrickling filtration inoculated with Aspergillus sp. S1 for gaseous m ‐xylene

Abstract Background Biotricking filtration (BTF) based on absorption and biodegradation of waste gas by microorganisms in a biofilm can be used to degrade with difficulty hydrophobic volatile pollutants. Photocatalysis is a promising technology for the abatement of gaseous contaminants because of its nonselective oxidation of volatile organic compounds; however, photocatalysis technology has the limitations of high energy consumption and low mineralization efficiency. This study, therefore, aimed to investigate the synergistic effects of UV/TiO 2 photocatalysis (PCO) pretreatment and BTF in treating gaseous m ‐xylene. Results BTF incubated with a mold, Aspergillus sp. S1, was acclimated with m ‐xylene as the sole carbon source. A combined system of PCO with BTF was developed to remove gaseous m ‐xylene. The results showed that the startup period was shortened by 3 days in the PCO‐BTF combined system compared to that with BTF alone. The removal efficiency reached 73% and 91% for the BTF and PCO‐BTF systems respectively when the empty bed residence time was extended to 90 s. In addition, PCO‐BTF could withstand transient shock loading of m ‐xylene of 5000 mg m −3 and gradually restore its decontamination performance. Conclusions PCO pretreatment was effective in the enhancement of the removal capacity of BTF for m ‐xylene. The PCO‐BTF system proposed in this study provides an attractive alternative to abate hydrophobic volatile pollutants. The integration of PCO essentially prompted the capability of Aspergillus sp. S1 in the BTF unit, which paves the way for the treatment of gaseous waste at an industrial scale. © 2022 Society of Chemical Industry (SCI).

Du, Qingping↗

DOE OSTI2018

Decommissioning of Research Building B at VNIINM: Main Results

Research building B at the Bochvar High-Technology Research Institute for Inorganic Materials (VNIINM) located within the city limits of a dense residential development was decommissioned in 2013–2015. Radioactively contaminated equipment and utility services were disassembled and removed, building structures were decontaminated, the framework was dismantled, the grounds of the development site were restored, and radioactive waste was transferred to specialized organizations. The framework was liquidated in strict accord with the norms and regulations governing the use of atomic energy.

42 ENGINEERING↗

DOE OSTI2018

Association of Vampirovibrio chlorellavorus with decline and death of Chlorella sorokiniana in outdoor reactors

The outdoor ARID raceway was established for optimizing the cultivation of microalgae for biofuel production. During the summers of 2014 and 2015, discoloration was observed in cultures of Chlorella sorokiniana , which shifted from a vibrant green color to yellow, followed by cell clumping, decline in density, and rapid death, resulting in 40–60% reduced biomass production. To investigate, total DNA was purified from the raceway samples and subjected to polymerase chain reaction (PCR) amplification using degenerate primers that amplify the 16S rRNA gene of eubacteria. BLASTn analysis of the cloned amplicon sequences revealed the presence of the Gram-negative, predatory bacterium, Vampirovibrio chlorellavorus . Scanning electron microscopic examination showed an abundance of coccoid cells, 0.3–0.6 μm in diameter, some of which were attached to C. sorokiniana cells. PCR amplification indicated the presence of V. chlorellavorus in raceway vessels, water lines, connective tubing, and in early, scaled-up DOE1412 cultures used to inoculate the raceway. Based on PCR detection, the decontamination of the equipment and water line with "Wal-Clean" more effectively eliminated V. chlorellavorus and delayed the onset of attack, compared to the chlorine disinfectant, trichloromelamine (TCM). Total DNA was isolated from soil samples collected monthly from the nearby Rillito River during 2014–2015 and subjected to PCR amplification using primers designed to amplify the 16S rRNA and 18S rRNA gene of V. chlorellavorus and C. sorokiniana , respectively. Results indicated that V. chlorellavorus and Chlorella spp. were present in most of the riverbed samples nearly year round, suggesting a possible naturally occurring reservoir of the predatory bacterium.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2018

Isolation of Au and Pt radionuclides from deuteron-irradiated platinum using TBP resin

A separation procedure was developed and implemented for the isolation of gold (Au) and platinum (Pt) radionuclides from deuteron irradiated Pt using tri-butyl phosphate (TBP) resin. Results of the procedure demonstrated a Pt recovery of 98 ± 2% and a Au recovery of 92±7%, in their respective fractions (n=4, ±1s). The decontamination factors were 2900 ± 500 for Au removal from the Pt fraction and 830±30 for Pt removal from the Au fraction (n=4, ±1s).

radiochemical separation, deuteron, Tributyl phosp↗

DOE OSTI2020

Molar Absorptivities of U(VI), U(IV), and Pu(III) in Nitric Acid Solutions of Various Concentrations Relevant to Developing Nuclear Fuel Recycling Flowsheets

Testing of a co-decontamination (CoDCon) tributyl phosphate (TBP) based solvent extraction flowsheet is being performed to optimize conditions for achieving a target U/Pu ratio in the Pu-containing product. The flowsheet is designed to directly produce a mixture of U and Pu with a U/Pu mass ratio of 7/3. The system is monitored in real time using optical spectroscopy, which allows for control of the U/Pu ratio in the aqueous U/Pu nitrate product. On-line spectrophotometric monitoring of the aqueous stream at the reductive stripping step involves determination of U(VI), U(IV) and Pu(III) concentrations and relies on molar absorptivities of these species in nitric acid at a number of wavelengths corresponding to their peaks’ maxima. The magnitudes of these molar absorptivities are a sensitive function of nitric acid concentration and have to be determined as precisely as possible using an off-line spectrophotometry under well controlled conditions. This step (called training set acquisition) is typically performed not in a high contamination area of radiological glovebox where flow-through cells and other on-line equipment are installed but in a less aggressive environment of a radiological fume hood with much better control of stock solutions quality, dilution factors, optical absorbance scale calibration, etc. This is followed by the calibration transfer between the off-line instrument and the instrument deployed during extraction and stripping runs. This paper reports values of molar absorptivities of U(VI), U(IV), and Pu(III) in nitric acid solution of 0.5 M to 4 M concentration and compares them with available technical literature data. Results of off-line spectrophotometric analysis of selected aqueous grab samples from one of CoDCon runs show satisfactory agreement with total uranium and plutonium concentrations determined in the same samples by ICP-MS.

Sinkov, Sergey I.↗

DOE OSTI2022

Column separation of tetravalent cerium fission products from trivalent rare earth radio-isotopes

Rapid and efficient isolation of individual rare earth element (REE) radioisotopes from complex mixtures is necessary to support the fields of nuclear forensics, medical isotope production and nuclear physics measurements. The separations must be robust and generate sufficiently high purity samples for subsequent radiological analysis. Current methodologies utilize a laborious two step Ce(IV)-iodate precipitation followed by Ce(IV)-nitrate di-(2-ethylhexyl)phosphoric acid/n-heptane extraction. This work reports an alternative method to isolate Ce fission product isotopes equilibrated with milligrams of cold carrier, from the remaining REE’s using a Ce(IV)/LN-resin (Eichrom Technologies) based separation. Optimization of Ce(IV) loading, REE(III) elution volume and subsequent Ce(III) stripping step utilized 166m Ho tracer. Mixed fission product experiments provided a further test of this LN-resin method, with analysis of purified 141/144 Ce, 147 Nd and 91 Y. Overall, while decontamination factors were lower for the LN-resin method, (vs. the combined precipitation/extraction) the simplicity of the technique and the satisfactory fission product analysis results point to the efficacy of this method.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Pore-Scale Modeling of Electrokinetics in Geomaterials

Pore-scale finite-volume continuum models of electrokinetic processes are used to predict the Debye lengths, velocity, and potential profiles for two-dimensional arrays of circles, ellipses and squares with different orientations. The pore-scale continuum model solves the coupled Navier–Stokes, Poisson, and Nernst–Planck equations to characterize the electro-osmotic pressure and streaming potentials developed on the application of an external voltage and pressure difference, respectively. Here, this model is used to predict the macroscale permeabilities of geomaterials via the widely used Carmen–Kozeny equation and through the electrokinetic coupling coefficients. The permeability results for a two-dimensional X-ray tomography-derived sand microstructure are within the same order of magnitude as the experimentally calculated values. The effect of the particle aspect ratio and orientation on the electrokinetic coupling coefficients and subsequently the electrical and hydraulic tortuosity of the porous media has been determined. These calculations suggest a highly tortuous geomaterial can be efficient for applications like decontamination and desalination.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Minimizing energy demand and environmental impact for sustainable NH 3 and H 2 O 2 production—A perspective on contributions from thermal, electro-, and photo-catalysis

There is an urgent need to provide adequate and sustainable supplies of water and food to satisfy the demand of an increasing population. Catalysis plays important roles in meeting these needs by facilitating the synthesis of hydrogen peroxide that is used in water decontamination and chemicals production, and ammonia that is used as fertilizer. However, these chemicals are currently produced with processes that are either very energy-intensive or environmentally unfriendly. This article offers the perspectives of the challenges and opportunities in the production of these chemicals, focusing on the roles of catalysis in more sustainable, alternative production methods that minimize energy consumption and environmental impact. While not intended to be a comprehensive review, the article provides a critical review of selected literature relevant to its objectives, discusses areas needed for further research, and potential new directions inspired by new developments in related fields. For each chemical, production by thermal, electro-, and photo-excited processes are discussed. Problems that are common to these approaches and their differences are identified and possible solutions suggested.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Production and separation of carrier-free 7 Be

A high-purity carrier-free 7 Be was efficiently isolated following proton bombardment of a lithium hydroxide - aluminum target. The separation of beryllium from lithium and aluminum was achieved through a hydrochloric acid elution system utilizing cation exchange chromatography. The beryllium recovery, +99%, was assessed through gamma spectroscopy while the chemical purity was established by mass spectrometry. In conclusion, the decontamination factors of beryllium from lithium and aluminum were determined to be 6900 and 300, respectively.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2025

Separation of terbium from proton-irradiated gadolinium oxide targets – development of an effective, scalable and automatable process

This work reports an effective and scalable radiochemical separation process for isolating terbium from Gd 2 O 3 . The separation process uses three commercially available extraction chromatography resin columns, has been implemented on a computer-controlled chemistry module, and tested with 100 mg quantities of proton-irradiated nat Gd 2 O 3 . Here, the 4-hour separation procedure isolated radioterbium in 1.3 mL of 0.01 M HCl with 80 ±8% radiochemical yield and a Gd decontamination factor >(1.2 ± 0.3)·10 5 .

Adjacent lanthanide separation↗

DOE OSTI2013

Quantitative analysis of wet-heat inactivation in bovine spongiform encephalopathy

Highlights: ► We quantitatively analyzed wet-heat inactivation of the BSE agent. ► Infectivity of the BSE macerate did not survive 155 °C wet-heat treatment. ► Once the sample was dehydrated, infectivity was observed even at 170 °C. ► A quantitative PMCA assay was used to evaluate the degree of BSE inactivation. - Abstract: The bovine spongiform encephalopathy (BSE) agent is resistant to conventional microbial inactivation procedures and thus threatens the safety of cattle products and by-products. To obtain information necessary to assess BSE inactivation, we performed quantitative analysis of wet-heat inactivation of infectivity in BSE-infected cattle spinal cords. Using a highly sensitive bioassay, we found that infectivity in BSE cattle macerates fell with increase in temperatures from 133 °C to 150 °C and was not detected in the samples subjected to temperatures above 155 °C. In dry cattle tissues, infectivity was detected even at 170 °C. Thus, BSE infectivity reduces with increase in wet-heat temperatures but is less affected when tissues are dehydrated prior to the wet-heat treatment. The results of the quantitative protein misfolding cyclic amplification assay also demonstrated that the level of the protease-resistant prion protein fell below the bioassay detection limit by wet-heat at 155 °C and higher and could help assess BSE inactivation. Our results show that BSE infectivity is strongly resistant to wet-heat inactivation and that it is necessary to pay attention to BSE decontamination in recycled cattle by-products.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2018

Non-thermal plasma reduces periodontitis-induced alveolar bone loss in rats

Periodontitis, a chronic infectious disease induced by microbial biofilm, is one of the most common diseases worldwide. Scaling and root planning (SRP) has always been recognized as the typical treatment. However, the therapeutic efficiency is often limited due to the intraoperative bleeding and the limitations of instruments. Non-thermal atmospheric plasma (NTP) appears to be a potential tool for periodontitis due to its promising biofilm degradation and decontamination effects. In this study, we investigated the role of NTP, as an adjuvant approach for the treatment of ligature-induced periodontitis in rats. Herein we showed that SRP or SRP-NTP application attenuated the periodontitis-induced alveolar bone loss, reflected by the increased BV/TV value and the decreased CEJ-AB distance, which might be related to the lower detection rate of periodontal pathogen in SRP and SRP-NTP groups. Besides, SRP-NTP rats showed less bone loss and lower CEJ-AB distance than that of SRP group at 30d post treatment, indicating a more comprehensive and long-lasting effect of SRP-NTP. A remarkable decrease of osteoclast number and lower expression of RANKL was also detected in SRP-NTP rats. In addition, expression of inflammatory-related cytokines such as TNF-α and IL-1β decreased significantly in SRP-NTP group, while IL-10 level increased substantially. These results together illustrated that a combination of SRP and NTP treatment was an effective way to prevent periodontitis progress, which reduced alveolar bone loss and promoted periodontium restoration in ligature-induced periodontitis rats. In conclusion, non-thermal plasma treatment may be considered as a feasible and effective supplementary approach to control periodontitis.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2015

Microwave processing of cement and concrete materials – towards an industrial reality?

Each year a substantial body of literature is published on the use of microwave to process cement and concrete materials. Yet to date, very few if any have lead the realisation of a commercial scale industrial system and is the context under which this review has been undertaken. The state-of the–art is evaluated for opportunities, and the key barriers to the development of new microwave-based processing techniques to enhance production, processing and recycling of cement and concrete materials. Applications reviewed include pyro-processing of cement clinker; accelerated curing, non-destructive testing and evaluation (NDT&E), and end-of-life processing including radionuclide decontamination.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes

We present that actinium-225 (t 1/2 = 9.92 d) is an α-emitting radionuclide with nuclear properties well-suited for use in targeted alpha therapy (TAT), a powerful treatment method for malignant tumors. Actinium-225 can also be utilized as a generator for 213 Bi (t 1/2 45.6 min), which is another valuable candidate for TAT. Actinium-225 can be produced via proton irradiation of thorium metal; however, long-lived 227 Ac (t 1/2 = 21.8 a, 99% β - , 1% α) is co-produced during this process and will impact the quality of the final product. Thus, accurate assays are needed to determine the 225 Ac/ 227 Ac ratio, which is dependent on beam energy, irradiation time and target design. Accurate actinium assays, in turn, require efficient separation of actinium isotopes from both the Th matrix and highly radioactive activation by-products, especially radiolanthanides formed from proton-induced fission. In this study, we introduce a novel, selective chromatographic technique for the recovery and purification of actinium isotopes from irradiated Th matrices. A two-step sequence of cation exchange and extraction chromatography was implemented. Radiolanthanides were quantitatively removed from Ac, and no non-Ac radionuclidic impurities were detected in the final Ac fraction. An 225 Ac spike added prior to separation was recovered at ≥98%, and Ac decontamination from Th was found to be ≥10 6 . Finally, the purified actinium fraction allowed for highly accurate 227 Ac determination at analytical scales, i.e., at 227 Ac activities of 1–100 kBq (27 nCi to 2.7 μCi).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗