• Title/Summary/Keyword: actinide

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Effect of pH, Redox Potential (Eh) and Carbonate Concentration on Actinides Solubility in a Deep Groundwater of Korea

  • Keum Dong-Kwon;Lee Han-Soo;Lee Chang-Woo
    • Nuclear Engineering and Technology
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    • v.36 no.2
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    • pp.196-202
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    • 2004
  • KAERI (Korea Atomic Energy Research Institute) is at present preparing a preliminary performance assessment to set up the HLW disposal concept of Korea. The solubility of the radionuclides contained in HLW is necessary as a source term in order to predict their potential migration in both the near and far fields. The solubility of actinides (Th, Am, U, Np and Pu) for a reference deep groundwater of Korea has been calculated using a geochemical code with thermodynamic data selected by a peer review of existing thermodynamic databases and literature. The solubilities from the experimental study and/or field observations from natural analogue studies are compared. The sensitivity of solubility to the variability of three main parameters of groundwater (pH, Eh, and carbonate concentration) is also investigated. The results of the sensitivity analysis show that the solubility of actinides strongly depends on the parameters considered. Within the range of parameter values studied (pH=7 to 10, Eh=-0.4 to -0.1V, and carbonate concentration=1.E-5 to 1.E-2 mol/L), the solubility of each actinide exists between 1.4E-10 and 1.6E-6 mol/L for Am, 4.9E-9 and 2.8E-6 mol/L for Th, 3.2E-9 and 5.7E-4 mol/L for U, 1.1E-9 and 1.0E-7 mol/L for Np, and 4.0E-11 and 2.8E-6 mol/L for Pu, respectively.

Analytical Solutions for a Three-Member Decay Chain of Radionuclides Transport in a Single Fractured Porous Rock (단일균열 다공성암반에서 방사성핵종의 수송에 대한 3단계 붕괴사슬의 해석해)

  • Yu, Young-Woo;Chung, Chang-Hyun;Kim, Chang-Lak
    • Nuclear Engineering and Technology
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    • v.26 no.4
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    • pp.453-460
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    • 1994
  • The migration equation is modified for a three-member decay chain in the fracture and porous matrix Analytical solutions are obtained by utilizing Laplace transform the initial conditions of Delta function and Bateman equation. The concentrations for each nuclide of Np$^{237}$ -U$^{233}$ -Th$^{229}$ and U$^{234}$ -Th$^{230}$ -Ra$^{226}$ chains selected from the 4n+1 and 4n+2 chains are plotted by utilizing analytical solutions in the fracture. Retardation coefficient of the nuclides are obtained using those of the granite. The results indicate that the daughter nuclides such as U$^{233}$ , Th$^{229}$ , Th$^{230}$ and Ra$^{226}$ become important at the far field from the repository though there is very small initial inventory in the waste solid or spent fuel, for they are produced by the mother nuclides decayed in the fracture and porous matrix.

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The conversion of ammonium uranate prepared via sol-gel synthesis into uranium oxides

  • Schreinemachers, Christian;Leinders, Gregory;Modolo, Giuseppe;Verwerft, Marc;Binnemans, Koen;Cardinaels, Thomas
    • Nuclear Engineering and Technology
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    • v.52 no.5
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    • pp.1013-1021
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    • 2020
  • A combination of simultaneous thermal analysis, evolved gas analysis and non-ambient XRD techniques was used to characterise and investigate the conversion reactions of ammonium uranates into uranium oxides. Two solid phases of the ternary system NH3 - UO3 - H2O were synthesised under specified conditions. Microspheres prepared by the sol-gel method via internal gelation were identified as 3UO3·2NH3·4H2O, whereas the product of a typical ammonium diuranate precipitation reaction was associated to the composition 3UO3·NH3·5H2O. The thermal decomposition profile of both compounds in air feature distinct reaction steps towards the conversion to U3O8, owing to the successive release of water and ammonia molecules. Both compounds are converted into α-U3O8 above 550 ℃, but the crystallographic transition occurs differently. In compound 3UO3·NH3·5H2O (ADU) the transformation occurs via the crystalline β-UO3 phase, whereas in compound 3UO3·2NH3·4H2O (microspheres) an amorphous UO3 intermediate was observed. The new insights obtained on these uranate systems improve the information base for designing and synthesising minor actinide-containing target materials in future applications.

Decay Heat Evaluation of Spent Fuel Assemblies in SFP of Kori Unit-1

  • Kim, Kiyoung;Kim, Yongdeog;Chung, Sunghwan
    • Proceedings of the Korean Radioactive Waste Society Conference
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    • 2018.11a
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    • pp.104-104
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    • 2018
  • Kori Unit 1 is the first permanent shutdown nuclear power plant in Korea and it is on June 18th, 2017. Spent fuel assemblies began to be discharged from the reactor core to the spent fuel pool(SFP) within one week after shutdown of Kori unit 1 and the campaign was completed on June 27th, 2017. The total number of spent nuclear fuel assemblies in SFP of Kori Unit-1 is 485 and their discharging date is different respectively. So, decay heat was evaluated considering the actual enrichment, operation history and cooling time of the spent fuel assemblies stored in SFP of the Kori Unit-1. The code used in the evaluation is the ORIGEN-based CAREPOOL system developed by KHNP. Decay heat calculation of PWR fuel is based on ANSI/ANS 5.1-2005, "Decay heat power in light water reactors" and ISO-10645, "Nuclear energy - Light water reactors - Calculation of the decay heat power in nuclear fuels. Also, we considered the contribution of fission products, actinide nuclides, neutron capture and radioactive material in decay heat calculation. CAREPOOL system calculates the individual and total decay heat of all of the spent fuel assemblies in SFP of Kori Unit-1. As a result, the total decay heat generated in SFP on June 28th, 2017 when the spent fuel assemblies were discharged from the reactor core, is estimated to be about 4,185.8 kw and to be about 609.5 kw on September 1st, 2018. It was also estimated that 119.6 kw is generated in 2050 when it is 32 years after the permanent shutdown. Figure 1 shows the trend of total decay heat in SFP of Kori Unit-1.

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A first-principles theoretical investigation of the structural, electronic and magnetic properties of cubic thorium carbonitrides ThCxN(1-x)

  • Siddique, Muhammad;Rahman, Amin Ur;Iqbal, Azmat;Azam, Sikander
    • Nuclear Engineering and Technology
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    • v.51 no.5
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    • pp.1373-1380
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    • 2019
  • Besides promising implications as fertile nuclear materials, thorium carbonitrides are of great interest owing to their peculiar physical and chemical properties, such as high density, high melting point, good thermal conductivity. This paper reports first-principles simulation results on the structural, electronic and magnetic properties of cubic thorium carbonitrides $ThC_xN_{(1-x)}$ (X = 0.03125, 0.0625, 0.09375, 0.125, 0.15625) employing formalism of density-functional-theory. For the simulation of physical properties, we incorporated full-potential linearized augmented plane-wave (FPLAPW) method while the exchange-correlation potential terms in Kohn-Sham Equation (KSE) are treated within Generalized-Gradient-Approximation (GGA) in conjunction with Perdew-Bruke-Ernzerhof (PBE) correction. The structural parameters were calculated by fitting total energy into the Murnaghan's equation of state. The lattice constants, bulk moduli, total energy, electronic band structure and spin magnetic moments of the compounds show dependence on the C/N concentration ratio. The electronic and magnetic properties have revealed non-magnetic but metallic character of the compounds. The main contribution to density of states at the Fermi level stems from the comparable spectral intensity of Th (6d+5f) and (C+N) 2p states. In comparison with spin magnetic moments of ThSb and ThBi calculated earlier with LDA+U approach, we observed an enhancement in the spin magnetic moments after carbon-doping into ThN monopnictide.

Characterization and thermophysical properties of Zr0.8Nd0.2O1.9-MgO composite

  • Nandi, Chiranjit;Kaity, Santu;Jain, Dheeraj;Grover, V.;Prakash, Amrit;Behere, P.G.
    • Nuclear Engineering and Technology
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    • v.53 no.2
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    • pp.603-610
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    • 2021
  • The major drawback of zirconia-based materials, in view of their applications as targets for minor actinide transmutation, is their poor thermal conductivity. The addition of MgO, which has high thermal conductivity, to zirconia-based materials is expected to improve their thermal conductivity. On these grounds, the present study aims at phase characterization and thermophysical property evaluation of neodymium-substituted zirconia (Zr0.8Nd0.2O1.9; using Nd2O3 as a surrogate for Am2O3) and its composites with MgO. The composite was prepared by a solid-state reaction of Zr0.8Nd0.2O1.9 (synthesized by gel combustion) and commercial MgO powders at 1773 K. Phase characterization was carried out by X-ray diffraction and the microstructural investigation was performed using a scanning electron microscope equipped with energy dispersive spectroscopy. The linear thermal expansion coefficient of Zr0.8Nd0.2O1.9 increases upon composite formation with MgO, which is attributed to a higher thermal expansivity of MgO. Similarly, specific heat also increases with the addition of MgO to Zr0.8Nd0.2O1.9. Thermal conductivity was calculated from measured thermal diffusivity, temperature-dependent density and specific heat values. Thermal conductivity of Zr0.8Nd0.2O1.9-MgO (50 wt%) composite is more than that of typical UO2 fuel, supporting the potential of Zr0.8Nd0.2O1.9-MgO composites as target materials for minor actinides transmutation.

Synthesis of Fe­Garnet for tile Immobilization of High Level Radioactive Waste (고준위 방사성폐기물의 고정화를 위한 Fe­석류석 합성 연구)

  • ;;;Yudintsev, S. V.
    • Journal of the Mineralogical Society of Korea
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    • v.16 no.4
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    • pp.307-320
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    • 2003
  • Garnet has been considered as a possible matrix for the immobilization of radioactive actinides. It is expected that Fe­based garnet be able to have the high substitution ability of actinide elements because ionic radius of Fe in tetrahedral site is larger than that of Si of Si­based garnet. Accordingly, we synthesized Fe­garnet with the batch composition of $Ca_{2,5}$C $e_{0.5}$Z $r_2$F $e_3$ $O_{12}$ and $Ca_2$CeZrFeF $e_3$ $O_{12}$ and studied their phase relations and properties. Mixed samples were fabricated in pellet forms under the pressure of 400 kg/$\textrm{cm}^2$ and were sintered in the temperature range of 1100∼140$0^{\circ}C$ in atmospheric conditions. Phase identification and chemical composition of synthesized samples were analyzed by XRD and SEM/EDS. In results, where the compounds were sintered at 130$0^{\circ}C$, we optimally obtained Fe­garnets as the main phase, even though some minor phases like perovskite were included. The compositions of Fe­garnets synthesized from the batch compositions of $Ca_{2,5}$C $e_{0.5}$Z $r_2$F $e_3$ $O_{12}$ and $Ca_2$CeZrFeF $e_3$ $O_{12}$, are $Ca_{2.5­3.2}$C $e_{0.3­0.7}$Z $r_{1.8­2.8}$F $e_{1.9­3.2}$ $O_{12}$ and $Ca_{2.2­2.5}$C $e_{0.8­1.0}$Z $r_{1.3­1.6}$ F $e_{0.4­.07}$ F $e_{3­3.2}$ $O_{12}$, respectively. Ca contents were exceeded and Ce contents were exceeded or depleted in 8­coodinated site, comparing to the initial batch composition. These results were caused by the compensation of the difference of ionic radius between Ca and Ce.

Quantitative Evaluation of Criticality According to the Major Influence of Applied with Burnup Credit on Dual-purpose Metal Cask (국내 금속겸용용기의 연소도 이득효과 적용 시 주요영향인자에 따른 정량적 핵임계 평가)

  • Dho, Ho-seog;Kim, Tae-man;Cho, Chun-Hyung
    • Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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    • v.13 no.2
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    • pp.141-154
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    • 2015
  • In general, conventional criticality analysis for spent fuel transport/storage systems have been performed based on the assumption of fresh fuel concerning the potential uncertainties from number density calculations of actinide nuclides and fission products in spent fuel. However, these evaluation methods cause financial losses due to an excessive criticality margin. In order to overcome this disadvantage, many studies have recently been conducted to design and commercialize a transportation and storage cask applied to the Burnup Credit (BUC). This study conducted an assessment to ensure criticality safety for reactor operating parameters, axial burn-up profiles and misload accident conditions, which are the factors that are likely to affect criticality safety when the BUC is applied to the dual-purpose cask under development at the KOrea RADioactive waste agency (KORAD). As a result, it was found that criticality resulting from specific power, changed substantially and relied on conditions of low enrichment and high burn-up. Considering the end effect in the case of high burn-up produced a positive-definite result. In particular, the increment of maximum effective multiplication factors due to misloading was 0.18467, confirming that misload is a factor that must be taken into account when applying the BUC. The results of this study may therefore be utilized as references in developing technologies to apply the BUC to domestic models and operational procedures or preventing any misload accidents during the process of spent fuel loading.

Verification of MCNP/ORIGEN-2 Model and Preliminary Radiation Source Term Evaluation of Wolsung Unit 1 (월성 1호기 MCNP/ORIGEN-2 모델 검증 및 예비 선원항 계산)

  • Noh, Kyoungho;Hah, Chang Joo
    • Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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    • v.13 no.1
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    • pp.21-34
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    • 2015
  • Source term analysis should be carried out to prepare the decommissioning of the nuclear power plant. In the planning phase of decommissioning, the classification of decommissioning wastes and the cost evaluation are performed based on the results of source term analysis. In this study, the verification of MCNP/ORIGEN-2 model is carried out for preliminary source term calculation for Wolsung Unit 1. The inventories of actinide nuclides and fission products in fuel bundles with different burn-up were obtained by the depletion calculation of MCNPX code modelling the single channel. Two factors affecting the accuracy of source terms were investigated. First, the neutron spectrum effect on neutron induced activation calculation was reflected in one-group microscopic cross-sections of relevant radio-isotopes using the results of MCNP simulation, and the activation source terms calculated by ORIGEN-2 using the neutron spectrum corrected library were compared with the results of the original ORIGEN-2 library (CANDUNAU.LIB) in ORIGEN-2 code package. Second, operation history effect on activation calculation was also investigated. The source terms on both pressure tubes and calandria tubes replaced in 2010 and calandria tank were evaluated using MCNP/ORIGEN-2 with the neutron spectrum corrected library if the decommissioning wastes can be classified as a low level waste.

Evaluation of co- and Mutual Weparation for Actinide(III) and RE by a $(Zr-DEHPA)/n-dodecane-HNO_3$ Extraction System ($(Zr-DEHPA)/n-dodecane-HNO_3$ 금속함유 추출 계에 의한 악티나이드(III)및 RE의 공추출 및 상호 분리)

  • Lee, Eil-Hee;Lim, Jae-Kwan;Chung, Dong-Yong;Yang, Han-Beom;Kim, Kwang-Wook
    • Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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    • v.5 no.2
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    • pp.123-132
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    • 2007
  • This study was performed to evaluate the co- and mutual separation for Am, Cm and RE elements from the simulated multi-component solution equivalent to real HLW level by a Zr-DEHPA(di-(2-ethylhexyl) phosphoric acid containing Zirconium)/$NDD(n-dodecane)-HNO_3$ extraction system. Zr-DEHPA was self-synthesized and the optimal condition of (15g/L Zr-1M DEHPA)/NDD-1M $HNO_3$ was selected taking into consideration of prevention of the third phase, and effects of concentration of DEHPA, nitric acid and impregnant amount of Zr on the co-extraction of Am, Cm and RE. In that condition, the extraction yields were 81% (Am), 85% (Cm), more than 80% (RE elements), 98% (Mo), 85% (Fe), 98% (U), 73% (Np), and less than 5% (other elements) so that the system developed for the co-extraction of Am-Cm/RE was proved to be available. For that, however, U, Np, Mo and Fe was elucidated to have to be removed in advance, and Zr inducing the third phase formation was found to be practically excluded. The co-extracted Am-Cm/RE were sequentially separated in an order of Am-Cm (stripping agent : 0.05 M DTPA-1M Lactic acid of pH 3.6)${\rightarrow}RE$ (stripping agent : 5M $HNO_3$), and then their separation factors were evaluated. At above conditions, Am of 65.4%, Cm of 63.9%, RE (except for Y) of more than 85% were stripped.

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