Search results for: plutonium

Authors: M. Bouhoun Ali, A. Y. Badjah Hadj Ahmed, M. Attou, A. Elias, M. A. Didi

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In this paper, the solvent extraction of uranium(VI), plutonium(IV) and thorium(IV) from aqueous solutions using 1-hydroxyhexadecylidene-1,1-diphosphonic acid (HHDPA) in treated kerosene has been investigated. The HHDPA was previously synthesized and characterized by FT-IR, 1H NMR, 31P NMR spectroscopy and elemental analysis. The effects contact time, initial pH, initial metal concentration, aqueous/organic phase ratio, extractant concentration and temperature on the extraction process have been studied. An empirical modelling was performed by using a 25 full factorial design, and regression equation for extraction metals was determined from the data. The conventional log-log analysis of the extraction data reveals that ratios of extractant to extracted U(VI), Pu(IV) and Th(IV) are 1:1, 1:2 and 1:2, respectively. Thermodynamic parameters showed that the extraction process was exothermic heat and spontaneous. The obtained optimal parameters were applied to real effluents containing uranium(VI), plutonium(IV) and thorium(IV) ions.

Keywords: solvent extraction, uranium, plutonium, thorium, 1-hydroxyhexadecylidene-1-1-diphosphonic acid, aqueous solution

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Authors: H. Shamoradifar, B. Teimuri, P. Parvaresh, S. Mohammadi

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One of the main characteristics of Heavy Water Moderated Reactors is their high production of plutonium. This article demonstrates the possibility of reduction of plutonium and other actinides in Heavy Water Research Reactor. Among the many ways for reducing plutonium production in a heavy water reactor, in this research, changing the fuel from natural Uranium fuel to Thorium-Uranium mixed fuel was focused. The main fissile nucleus in Thorium-Uranium fuels is U-233 which would be produced after neutron absorption by Th-232, so the Thorium-Uranium fuels have some known advantages compared to the Uranium fuels. Due to this fact, four Thorium-Uranium fuels with different compositions ratios were chosen in our simulations; a) 10% UO₂-90% THO₂ (enriched= 20%); b) 15% UO₂-85% THO₂ (enriched= 10%); c) 30% UO₂-70% THO₂ (enriched= 5%); d) 35% UO₂-65% THO₂ (enriched= 3.7%). The natural Uranium Oxide (UO₂) is considered as the reference fuel, in other words all of the calculated data are compared with the related data from Uranium fuel. Neutronic parameters were calculated and used as the comparison parameters. All calculations were performed by Monte Carol (MCNPX2.6) steady state reaction rate calculation linked to a deterministic depletion calculation (CINDER90). The obtained computational data showed that Thorium-Uranium fuels with four different fissile compositions ratios can satisfy the safety and operating requirements for Heavy Water Research Reactor. Furthermore, Thorium-Uranium fuels have a very good proliferation resistance and consume less fissile material than uranium fuels at the same reactor operation time. Using mixed Thorium-Uranium fuels reduced the long-lived α emitter, high radiotoxic wastes and the radio toxicity level of spent fuel.

Keywords: Heavy Water Reactor, Burn up, Minor Actinides, Neutronic Calculation

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Authors: C. G. Mendez-Garcia, E. T. Romero-Guzman, H. Hernandez-Mendoza, C. Solis, E. Chavez-Lomeli, E. Chamizo, R. Garcia-Tenorio

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Plutonium is present in different concentrations in the environment and biological samples related to nuclear weapons testing, nuclear waste recycling and accidental discharges of nuclear plants. This radioisotope is considered the most radiotoxic substance, particularly when it enters the human body through inhalation of powders insoluble or aerosols. This is the main reason of the determination of the concentration of this radioisotope in the atmosphere. Besides that, the isotopic ratio of ²⁴⁰Pu/²³⁹Pu provides information about the origin of the source. PM₂.₅ sampling was carried out in the Metropolitan Zone of the Valley of Mexico (MZVM) from February 18th to March 17th in 2015 on quartz filter. There have been significant developments recently due to the establishment of new methods for sample preparation and accurate measurement to detect ultra trace levels as the plutonium is found in the environment. The accelerator mass spectrometry (AMS) is a technique that allows measuring levels of detection around of femtograms (10-15 g). The AMS determinations include the chemical isolation of Pu. The Pu separation involved an acidic digestion and a radiochemical purification using an anion exchange resin. Finally, the source is prepared, when Pu is pressed in the corresponding cathodes. According to the author's knowledge on these aerosols showed variations on the ²³⁵U/²³⁸U ratio of the natural value, suggesting that could be an anthropogenic source altering it. The determination of the concentration of the isotopes of Pu can be a useful tool in order the clarify this presence in the atmosphere. The first results showed a mean value of activity concentration of ²³⁹Pu of 280 nBq m⁻³ thus the ²⁴⁰Pu/²³⁹Pu was 0.025 corresponding to the weapon production source; these results corroborate that there is an anthropogenic influence that is increasing the concentration of radioactive material in PM₂.₅. According to the author's knowledge in Total Suspended Particles (TSP) have been reported activity concentrations of ²³⁹⁺²⁴⁰Pu around few tens of nBq m⁻³ and 0.17 of ²⁴⁰Pu/²³⁹Pu ratios. The preliminary results in MZVM show high activity concentrations of isotopes of Pu (40 and 700 nBq m⁻³) and low ²⁴⁰Pu/²³⁹Pu ratio than reported. These results are in the order of the activity concentrations of Pu in weapons-grade of high purity.

Keywords: aerosols, fallout, mass spectrometry, radiochemistry, tracer, ²⁴⁰Pu/²³⁹Pu ratio

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Authors: M. Guler, E. Guler

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We report some elastic parameters of cubic fluorite type neptunium dioxide (NpO2) with a recent EAM type interatomic potential through geometry optimization calculations. Typical cubic elastic constants, bulk modulus, shear modulus, young modulus and other relevant elastic parameters were also calculated during research. After calculations, we have compared our results with the available theoretical data. Our results agree well with the previous theoretical findings of the considered quantities of NpO2.

Keywords: NpO2, elastic properties, bulk modulus, mechanical properties

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Authors: E. Güler, M. Güler

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We report some elastic quantities of cubic fluorite type plutonium dioxide (PuO2) with a recent EAM type interatomic potential through geometry optimization calculations. Typical cubic elastic constants, bulk modulus, shear modulus, young modulus and other related elastic quantities were calculated during present research. After present calculations, we have compared our results with the existing theoretical data of literature. Our results are consistent with previous theoretical findings of the considered parameters of PuO2.

Keywords: PuO2, elastic properties, bulk modulus, mechanical properties

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Authors: Mohamad Saab, Florent Real, Francois Virot, Laurent Cantrel, Valerie Vallet

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All spent nuclear fuel reprocessing plants use the PUREX process (Plutonium Uranium Refining by Extraction), which is a liquid-liquid extraction method. The organic extracting solvent is a mixture of tri-n-butyl phosphate (TBP) and hydrocarbon solvent such as hydrogenated tetra-propylene (TPH). By chemical complexation, uranium and plutonium (from spent fuel dissolved in nitric acid solution), are separated from fission products and minor actinides. During a normal extraction operation, uranium is extracted in the organic phase as the UO₂(NO₃)₂(TBP)₂ complex. The TBP solvent can form an explosive mixture called red oil when it comes in contact with nitric acid. The formation of this unstable organic phase originates from the reaction between TBP and its degradation products on the one hand, and nitric acid, its derivatives and heavy metal nitrate complexes on the other hand. The decomposition of the red oil can lead to violent explosive thermal runaway. These hazards are at the origin of several accidents such as the two in the United States in 1953 and 1975 (Savannah River) and, more recently, the one in Russia in 1993 (Tomsk). This raises the question of the exothermicity of reactions that involve TBP and all other degradation products, and calls for a better knowledge of the underlying chemical phenomena. A simulation tool (Alambic) is currently being developed at IRSN that integrates thermal and kinetic functions related to the deterioration of uranyl nitrates in organic and aqueous phases, but not of the n-butyl phosphate. To include them in the modeling scheme, there is an urgent need to obtain the thermodynamic and kinetic functions governing the deterioration processes in liquid phase. However, little is known about the thermodynamic properties, like standard enthalpies of formation, of the n-butyl phosphate molecules and of the UO₂(NO₃)₂(TBP)₂ UO₂(NO₃)₂(HDBP)(TBP) and UO₂(NO₃)₂(HDBP)₂ complexes. In this work, we propose to estimate the thermodynamic properties with Quantum Methods (QM). Thus, in the first part of our project, we focused on the mono, di, and tri-butyl complexes. Quantum chemical calculations have been performed to study several reactions leading to the formation of mono-(H₂MBP), di-(HDBP), and TBP in gas and liquid phases. In the gas phase, the optimal structures of all species were optimized using the B3LYP density functional. Triple-ζ def2-TZVP basis sets were used for all atoms. All geometries were optimized in the gas-phase, and the corresponding harmonic frequencies were used without scaling to compute the vibrational partition functions at 298.15 K and 0.1 Mpa. Accurate single point energies were calculated using the efficient localized LCCSD(T) method to the complete basis set limit. Whenever species in the liquid phase are considered, solvent effects are included with the COSMO-RS continuum model. The standard enthalpies of formation of TBP, HDBP, and H2MBP are finally predicted with an uncertainty of about 15 kJ mol⁻¹. In the second part of this project, we have investigated the fundamental properties of three organic species that mostly contribute to the thermal runaway: UO₂(NO₃)₂(TBP)₂, UO₂(NO₃)₂(HDBP)(TBP), and UO₂(NO₃)₂(HDBP)₂ using the same quantum chemical methods that were used for TBP and its derivatives in both the gas and the liquid phase. We will discuss the structures and thermodynamic properties of all these species.

Keywords: PUREX process, red oils, quantum chemical methods, hydrolysis

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Authors: Hendrik Bernard Van Der Walt, Frik Van Niekerk

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Fuel models render a reduction in BOL when thorium is added to a reactor core. Thorium emulates the role of a fertile poison, and is beneficial for reducing beginning of cycle (BOC) excess reactivity. In spite of the build-up of 233U over the duration of a fuel cycle, the effects of fuel reloading have a significant impact on fuel viability, especially in the case of heterogeneous thorium-based fuels. The most common practice of compensating for the reduction of BOC reactivity is the addition of fissile isotopes (uranium fuel with increased enrichment or plutonium). This study introduces a heterogeneous thorium-based fuel with minimal fissile isotope additions. A pseudo reloading scheme was developed for numerical simulations of an infinite reactor based on the North-Anna 1 reactor operating in Virginia, USA. Use of this reloading pattern allows new thorium-based fuel to be loaded into the reactor model as part of a phasing in strategy at the end of any conventional reactor cycle. Results demonstrate the effects of thorium-based fuel on fuel cycle characteristics such as fuel cycle length, neutron economy and material matrix. Application of the above mentioned approach delivered promising results and presents a heterogeneous thorium-based fuel which could replace conventional fuel of typical, currently operating (or future) reactors without the need for expensive reactor redesign or fuel recycling strategies.

Keywords: nuclear fuel, nuclear characteristics, nuclear fuel cycle, thorium-based fuel, heterogeneous design, fuel reloading

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Authors: Muhammad Minhaj Khan, Jaemin Lee, Suhong Lee, Jinyoung Chung, Johoo Whang

Abstract:

The Republic of Korea has been facing strong storage crisis from nuclear waste generation as At Reactor (AR) temporary storage sites are about to reach saturation. Since the country is densely populated with a rate of 491.78 persons per square kilometer, Construction of High-level waste repository will not be a feasible option. In order to tackle the storage waste generation problem which is increasing at a rate of 350 tHM/Yr. and 380 tHM/Yr. in case of 20 PWRs and 4 PHWRs respectively, the study strongly focuses on the advancement of current nuclear power plants to GEN-IV sustainable and ecological nuclear systems by burning TRUs (Pu, MAs). First, Calculations has made to estimate the generation of SNF including Pu and MA from PWR and PHWR NPPS by using the IAEA code Nuclear Fuel Cycle Simulation System (NFCSS) for the period of 2016, 2030 (including the saturation period of each site from 2024~2028), 2089 and 2109 as the number of NPPS will increase due to high import cost of non-nuclear energy sources. 2ndly, in order to produce environmentally sustainable nuclear energy systems, 4 scenarios to burnout the Plutonium and MAs are analyzed with the concentration on burning of MA only, MA and Pu together by utilizing SFR, LFR and KALIMER-600 burner reactor after recycling the spent oxide fuel from PWR through pyro processing technology developed by Korea Atomic Energy Research Institute (KAERI) which shows promising and sustainable future benefits by minimizing the HLW generation with regard to waste amount, decay heat, and activity. Finally, With the concentration on front and back end fuel cycles for open and closed fuel cycles of PWR and Pyro-SFR respectively, an overall assessment has been made which evaluates the quantitative as well as economical combativeness of SFR metallic fuel against PWR once through nuclear fuel cycle.

Keywords: GEN IV nuclear fuel cycle, nuclear waste, waste sustainability, transmutation

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Authors: Z. M. Biyasheva, M. Zh. Tleubergenova, Y. A. Zaripova, A. L. Shakirov, V. V. Dyachkov

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In recent years, interest in ecogenetic and biomedical problems related to the effects on the population of radon and its daughter decay products has increased significantly. Of particular interest is the assessment of the consequence of irradiation at hazardous radon areas, which includes the Almaty region due to the large number of tectonic faults that enhance radon emanation. In connection with the foregoing, the purpose of this work was to study the genetic effects of exposure to supernormal radon doses on the alpha-radiation model. Irradiation does not affect the growth of the cell, but rather its ability to differentiate. In addition, irradiation can lead to somatic mutations, morphoses and modifications. These damages most likely occur from changes in the composition of the substances of the cell. Such changes are epigenetic since they affect the regulatory processes of ontogenesis. Variability in the expression of regulatory genes refers to conditional mutations that modify the formation of signs of intraspecific similarity. Characteristic features of these conditional mutations are the dominant type of their manifestation, phenotypic asymmetry and their instability in the generations. Currently, the terms “morphosis” and “modification” are used to describe epigenetic variability, which are maintained in Drosophila melanogaster cultures using linkaged X- chromosomes, and the mutant X-chromosome is transmitted along the paternal line. In this paper, we investigated the epigenetic effects of alpha particles, whose source in nature is mainly radon and its daughter decay products. In the experiment, an isotope of plutonium-238 (Pu²³⁸), generating radiation with an energy of about 5500 eV, was used as a source of alpha particles. In an experiment in the first generation (F₁), deformities or morphoses were found, which can be called "radiation syndromes" or mutations, the manifestation of which is similar to the pleiotropic action of genes. The proportion of morphoses in the experiment was 1.8%, and in control 0.4%. In this experiment, the morphoses in the flies of the first and second generation looked like black spots, or melanomas on different parts of the imago body; "generalized" melanomas; curled, curved wings; shortened wing; bubble on one wing; absence of one wing, deformation of thorax, interruption and violation of tergite patterns, disruption of distribution of ocular facets and bristles; absence of pigmentation of the second and third legs. Statistical analysis by the Chi-square method showed the reliability of the difference in experiment and control at P ≤ 0.01. On the basis of this, it can be considered that alpha particles, which in the environment are mainly generated by radon and its isotopes, have a mutagenic effect that manifests itself, mainly in the formation of morphoses or deformities.

Keywords: alpha-radiation, genotoxicity, morphoses, radioecology, radon

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