Measurements of gamma-ray emission probabilities of 241, 243Am and 239Np

Gamma-ray emission probabilities of ^{241, 243}Am and ²³⁹Np have been precisely measured with gamma- and alpha-ray spectroscopic methods. The activities of the samples were determined by measuring alpha particles using a Si semiconductor detector. Gamma rays emitted from the samples were measured with a planar type High-Purity Germanium (HPGe) detector. An efficiency curve of the HPGe detector was derived with uncertainties from 0.7% to 2.5% by combining measured efficiencies and Monte Carlo simulation. The gamma-ray emission probabilities for the major gamma rays of these nuclides were determined with uncertainties less than 1.2%.     

Comparative study on the extraction of trivalent americium and europium by CMPO in imidazolium-based ionic liquids and dodecane

The extraction of Am³⁺ and Eu³⁺ by octyl(phenyl)-N,N-diisobutyl carbamoylmethylphosphine oxide (CMPO) in eight imidazolium-based ionic liquids and in n-dodecane was studied and compared. Slope analysis indicates that the ligand/metal ratio in the extracted complexes in ionic liquids is much larger than that in n-dodecane. Nitric acid has different impacts on the extraction, depending greatly on the nature of the ionic liquids. A mixed-extraction mechanism, namely cation exchange plus the formation of neutral complexes (solvation), was proposed for the extraction in the ionic liquid systems. In addition, temperature was found to have a remarkable influence on the extraction. Highly exothermic enthalpy changes were obtained for the extraction in ionic liquid systems. This work provides further insight into the particular role played by the unique properties of ionic liquids in the extraction of metal ions from nitric acid media.     

Magnetic Properties of Uranium Carbides after Neutron Irradiation

Fundamental investigations on valence control and solvent extraction of americium were carried out to develop a method for americium separation from reprocessing solution. In order to adjust americium valency from III to IV and VI, (NH₄)₁₀P₂W ₁₇O₆₁ synthesized was used as complexant stabilizing Am(IV). Oxidation behavior of americium was investigated as a function of (NH₄)₁₀P₂W ₁₇O₆₁ americium ratio. Using 0.1M (NH₄)₂S₂O₈ and 0.01M AgNO₃ as oxidation reagent, Am(IV) was obtained quantitatively at the ratio of 15. On decreasing the ratio to 0.6, 92% of americium was adjusted to Am(VI). The concentration of (NH₄)₂S₂O₈ could be reduced to 1/15 compared to the previously reported method in which no complexant was used. Americium(IV) was also prepared by reacting O₃ and AgNO₃ but no Am(VI) was obtained even at low (NH₄)₁₀P₂W ₁₇O₆₁ to americium ratio.

Americium(VI) could be extracted by tri-n-butyl phosphate stably without influence of (NH₄)₁₀P₂W ₁₇O₆₁. The distribution coefficient of Am(VI) was 4 between 100% tri-n-butyl phosphate and 1 M nitric acid, and separation factor from Nd(III) was 50.

With regard to the americium separation method which implemented valence control followed by extraction, adding (NH₄)₁₀P₂W ₁₇O₆₁ led to minimization of waste volume and improvement of extraction efficiency.     

Extraction of Trivalent Rare Earths and Minor Actinides from Nitric Acid with N,N,N’,N’-Tetradodecyldiglycolamide (TDdDGA) by Using Mixer-Settler Extractors in a Hot Cell

Single-stage batch experiments to reveal the extraction properties of N,N,N’,N’-tetradodecyldiglycolamide (TDdDGA) for Y, La, Eu, Nd, and Am in nitric acid were carried out. The distribution ratios of Y, Eu, Nd, and Am exceeded 10 when the nitric acid concentration was 1–2 mol/dm³ (M), and the distribution ratio of La was 5.5 when the nitric acid concentration was 2 M. A continuous counter-current experiment using 0.1 M TDdDGA diluted with n-dodecane was performed using mixer-settler extractors installed in a hot cell. Nitric acid with a concentration of 2.1 M containing minor actinides (MAs: Am and Cm), rare earths (REs: Y, La, Nd, and Eu), and other fission products (Sr, Cs, Zr, Mo, Ru, Rh, and Pd) was fed to the extractor. TDdDGA effectively extracted MAs and REs from the feed, while other fission products were barely extracted. The extracted MAs and REs were back-extracted by bringing them in contact with 0.02 M nitric acid, and they were collected as the MA–RE fraction. The results indicated that more than 98% of Am and Cm in the feed were recovered in the MA–RE fraction. The proportions of Y, La, Nd, and Eu in the MA–RE fraction were 94.0%, 99.9%, 99.9%, and 86.9%, respectively.     

Separation of Actinides and Fission Products Using Titanium-Based Materials

Separation of minor actinides such as americium and curium from lanthanides and other fission products is important for the development of efficient nuclear fuel reprocessing methods. This article describes findings from initial investigations into the use of titanium-based materials for the separation of actinides including americium, plutonium, neptunium, and uranium from fission products including lanthanides, strontium, and cesium. Two types of materials were studied; the first was sodium titanates (ST) that have a layered structure and the second was titanosilicates that have a 3-dimensional tunnel structure. Testing indicated that the layered sodium titanates and tunnel-structured titanosilicate materials exhibit a strong affinity for Am, lanthanides, Sr, and Cs at pH 3 and a significantly reduced affinity for Am and the lanthanides at a higher acid concentration (pH 1). Testing also indicated that the ST material exhibited high affinity for actinides in a pH 3 solution. The addition of complexing agents significantly decreased the sorption of Am and lanthanides.     

A New Method for Partitioning of Trivalent Actinides from High-Level Liquid Waste

The extraction behavior of Am(III) and Eu(III) in a solution of tetra-bis(2-ethylhexyl)diglycolamide (TEHDGA) and bis(2-ethylhexyl)phosphoric acid (HDEHP) in n-dodecane (n-DD) was studied from nitric acid medium. The distribution ratio of Am(III) and Eu(III) in TEHDGA-HDEHP/n-DD was measured as a function of various parameters such as concentrations of nitric acid, TEHDGA, HDEHP, and nitrate ion. The data were compared with those obtained in individual solvents namely 0.1 M TEHDGA/n-DD and 0.25 M HDEHP/n-DD. The synergistic extraction of Am(III) and Eu(III) observed in a solution of 0.1 M TEHDGA – 0.25 M HDEHP/n-DD was attributed to the involvement of both TEHDGA and HDEHP for extraction. Slope analysis of the extraction data indicated the predominant participation of HDEHP for extraction at low acidities and TEHDGA and nitrate ion at higher acidity. The stripping behavior of Am(III) and Eu(III) from the extracted organic phase was investigated using citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). A suitable aqueous formulation was developed to separate Am(III) alone from chemically similar Eu(III) present in loaded organic phase, to facilitate a single-step separation of trivalent actinides from the high-level liquid waste (HLLW).     

Extraction of Trivalent Europium and Americium from Nitric Acid Solution with Bisdiglycolamides

Two bisdiglycolamides (BisDGAs) of N,N,N′′′,N′′′-tetrabutyl-N?,N′′-ethidene bisdiglycolamide (TBE-BisDGA) and N,N,N′′′,N′′′-tetrabutyl-N?,N′′-m-xylylene bisdiglycolamide (TBX-BisDGA) were synthesized. Their extraction behaviors of Eu(III) and Am(III), as well as nitric acid were investigated from nitric acid medium by using n-octanol as diluent. Nitric acid is extracted as the form of HNO₃·(BisDGAs)_0.6 by BisDGAs and the conditional acid uptake constants of TBE-BisDGA and TBX-BisDGA were 0.26 and 0.10, respectively. The distribution ratios of Eu(III) and Am(III) increased with the increase of nitric acid and extractant concentration, whilst decreased with temperature rise. TBX-BisDGA had a stronger extraction power for Eu(III) and Am(III) than TBE-BisDGA. Both of the extractants displayed a higher affinity toward Eu(III) than Am(III). In the examination of the acidity range from 0.5 to 5.0 M, a maximum separation factor SF_{Eu(III)/Am(III)} can reach 8.0 at 3.0 M HNO₃ for TBX-BisDGA; and 10 at 4.0 M HNO₃ for TBE-BisDGA, respectively. Slope analyses showed that Eu(III) and Am(III) are extracted as di-solvated species by TBX-BisDGA or TBE-BisDGA. The extraction mechanism was described and the apparent extraction equilibrium constant as well as Gibbs free energy change, enthalpy change and entropy change were presented. In addition, their Eu(III) complexes were analyzed by using infrared spectra.     

Chromatographic Separation of Trivalent Actinides by Using Tertiary Pyridine Resin with Methanolic Nitric Acid Solutions

Chromatographic separation of trivalent actinides (Am, Cm and Cf) was performed by using a tertiary pyridine resin embedded in silica beads with methanolic nitric acid solutions. The trivalent actinides were eluted from the resin column in the reverse order of atomic numbers (Cf-Cm-Am). Higher concentration of methanol in the mixed solution accelerated both the adsorption of these elements on the resin and the separability for these elements. Americium was clearly separated from Cm and Cf by using a 1 cm-ø × 10 cm-height column with a 60vol% of methanol/40 vol% of concentrated nitric acid mixed solution at ambient temperature.     

Minor actinide transmutation in fast reactor metal fuels irradiated for 120 and 360 equivalent full-power days

An irradiation experiment on uranium–plutonium–zirconium (U–Pu–Zr) alloys containing 5 wt% or less minor actinides (MAs) and rare earths was carried out in the Phénix fast reactor. The isotope compositions of the fuel alloys irradiated for 120 and 360 equivalent full-power days (EFPDs) were chemically analyzed by inductively coupled plasma–mass spectrometry after 3.3–5.3 years of cooling. The results of chemical analysis indicated that the discharged burnups of the fuel alloys irradiated for 120 and 360 EFPDs were 2.1–2.5 and 5.3–6.4 at%, respectively. The changes in the isotopic abundances of plutonium, americium, and curium during the irradiation experiment were assessed to discuss the transmutation performance of MA nuclides added to U–Pu–Zr alloy fuel. Multigroup three-dimensional diffusion and burnup calculations accurately predicted the changes in these isotopic abundances after fuel fabrication. An evaluation of the MA transmutation ratio based on the results of chemical analysis revealed that the quantity of MA elements in the U–19Pu–10Zr–5MA (wt%) alloy decreased by about 20% during the irradiation experiment for 360 EFPDs.     

Frictional Pressure Drop for NaK-N2 Two-Phase Flow in Rectangular Cross Section Channel of Large Aspect Ratio

In this paper, the frictional pressure drop in an isothermal liquid metal-gas two-phase flow through a rectangular channel with large width-to-height ratio is treated semiempirically for a NaK-N₂ two-phase flow system.

The frictional pressure drop in the two-phase flow is compared with the following two reference values :

1. The frictional pressure drop in the liquid flowing alone in single phase with the same velocity as that of the liquid in the two-phase mixture.

2. The frictional pressure drop in the liquid flowing alone in single phase with the same mass flow rate as that of the liquid in the two-phase mixture.

The comparison with the former reference value is necessary for the prediction of friction loss in a liquid metal MHD generator channel whose medium would be two-phase mixture.

The semiempirical analysis was performed assuming the two-phase mixture to be a continuous medium with its properties, e.g. viscosity and density, defined by void fraction and the velocity determined by the total mass flow rate.

In the region of low slip and density ratio ρ_g/ρ_l the frictional pressure drop in the two-phase flow appeared to be smaller than that due to the liquid flowing alone with the same velocity as that of the liquid in the two-phase flow.

The experiments have been undertaken with the NaK-N₂ two-phase mixture flowing through a rectangular channel (4 × 60 mm²).

Data were taken over the following parameter range:

NaK velocity: 5～30 m/sec, Void fraction: 0～70%

Density ratio: 0.006～0.013, Quality: 0.07～1.10%.