Fragmentation by β-Decay in Tritium-Labelled Compounds, (II)

The behaviors of CH₃He⁺ and C₂H₅He⁺ formed by the decay of CH₃T and C₂H₅T were studied theoretically using the STO-3G molecular orbital method and was compared with that of HHe⁺ in the decay of HT. It was clearly shown that the ground state daughter ions CH₃He⁺ and C₂H₅He⁺ dissociate instantly to give CH₃ ⁺ and C₂H₅ ⁺ because their potential energy curves are repulsive, whereas the daughter ion HHe⁺ in the ground state does not dissociate. The transition probability to the ground state ions of CH₃He⁺ and of C₂H₅He⁺ are computed to be 66.5 and 64.8%, respectively. These values are in fairly good accordance with those obtained experimentally.     

Activation cross sections of the Yb(p,xn)Lu reaction for indirect production of the therapeutic radionuclide Yb

Activation cross sections of the ^natYb(p,xn)¹⁶⁹Lu reaction have been measured for the first time up to 70 MeV to investigate the production possibility of the radionuclide ¹⁶⁹Yb through decay of its parent ¹⁶⁹Lu. The cross sections were measured using the stacked foil irradiation technique and gamma spectrometry. The experimental data were compared with the results of the ALICE-IPPE theoretical model code. Different production routes were compared for the internal radiotherapy related radioisotope ¹⁶⁹Yb. Above 30 MeV proton energy the integral yield of the ^natYb(p,xn)¹⁶⁹Lu reaction is higher than that of the earlier investigated ¹⁶⁹Tm(p,n)¹⁶⁹Yb, ¹⁶⁹Tm(d,2n)¹⁶⁹Yb, ^natEr(α,xn)¹⁶⁹Yb, ^natYb(α,x)¹⁶⁹Lu and ^natHf(p,x)¹⁶⁹Lu reactions at the equivalent particle energies.     

Cyclotron production of the Ag, Pd, Rh radionuclides by Pd(p,x) nuclear processes

Production cross-sections of the ^105g+m,106mAg, ^100,101Pd, and ^{100g+m,101m,105g+m}Rh radionuclides through proton-induced reactions on natural palladium were measured up to 40 MeV by using a stacked-foil activation technique combined with high-resolution γ-ray spectrometry. The production cross-sections of ¹⁰¹Pd and ^{100g+m,105g+m}Rh radionuclides have been reported here for the first time from the ^natPd(p,x) nuclear processes. The present results are compared with the available literature values as well as the theoretical data calculated by the TALYS and the ALICE-IPPE computer codes. A quantitative comparison of the present results with the theoretical data has also been done with several deviation factor definitions. Optimal production pathways of the therapeutic ^105gRh radionuclide with minimal contamination using cyclotrons are discussed elaborately.     

Evaluation of 17O(n,a)14C Cross Section

The ¹⁷O(n, a)¹⁴C cross section has been evaluated for incident neutron energies from 10^?5eV to 20MeV for accurate calculation on the ¹⁴C production in nuclear reactors. Evaluation was based on the single-level Breit-Wigner formula for the thermal to resonance energy regions. In the higher energy region, a multi-step evaporation model code PEGASUS was used, and the results were normalized using the ¹⁶O(n, a) cross section ratio of JENDL-3 evaluation to PEGASUS calculation. Results are given in tabular and graphical forms, and also as one-group cross sections using typical BWR, PWR and FBR spectra of ORIGEN-2.     

Determination of the 129I transmutation rate and 129I(n, 2n)128I correction using gas mass spectrometry

Two groups of ¹²⁹I and ¹²⁷I targets were analyzed using a gas quadrupole mass spectrometer (QMS) to determine the transmutation rates via the melting method. Sodium iodide was chosen to make the target. The iodine composition in the ¹²⁹I targets is 82.7% ¹²⁹I and 17.3% ¹²⁷I. The transmutation rate of the ¹²⁹I(n, γ)¹³⁰I reaction was determined by measuring the ¹³⁰Xe with QMS. An equivalent corrective method was brought out to correct the ¹²⁹I(n, 2n)¹²⁸I branch which is interfered with by the ¹²⁷I(n, γ)¹²⁸I reaction. And the correction formula was deduced in theory. For very little ¹²⁸Xe from the ¹²⁹I(n, 2n)¹²⁸I reaction, the equivalent corrective method could not be suitable here. However, it is suitable for the mass of ¹²⁸Xe from ¹²⁹I(n,2n)¹²⁸I reaction that reaches the accurately detective level of the mass spectrometry.     

A Nuclear Magnetic Resonance Study on Ligand Exchange Reactions in La(III), Nd(III), and U(VI) Nitrato Complexes with n-Octyl(pheny1)-N,N-Diisobutylcarbamoylmethylphosphine Oxide in Non-aqueous Solvents

The exchange reactions of n-octyl(pheny1)-N, N-diisobutylcarbamoylmethylphosphine oxide (CMPO) in La(III), Nd(III), and U(VI) nitrate complexes with CMPO (La(III)-, Nd(III)-, and U(VI)-CMPO complexes) have been studied in CD₃COCD₃ by means of ³¹P NMR method. The number of CMPO coordinated to the first coordination sphere of La(III) ion was directly determined to be 3 by the area integrations of ³¹P NMR signals of free and coordinated CMPO molecules. The same coordination number of 3 was also obtained for the U(VI)-CMPO complex. The coordination number was not determined for the Nd(III)-CMPO complex, because of its paramagnetic behavior. The exchange rate constants of CMPO in La(III)- and U(VI)- CMPO complexes were obtained by the two-site exchange model. Paramagnetic line broadening was observed in the Nd(III)-CMPO complex and the rate constant for the exchange of CMPO was determined by the line-broadening method. The exchange rates of CMPO in La(III)- and Nd(III)-CMPO complexes depend on the free CMPO concentration ([CMPO]), while that in U(VI)-CMPO complex is independent of [CMPO]. The dissociative (D) and dissociative interchange (I_d ) mechanisms were proposed for the exchange reactions in the La(III)- and Nd(III)-CMPO complexes, and dissociative (D) or I_d mechanism was proposed for the U(VI)-CMPO complex. The dissociative rate constants (s^?1) at 25°C and activation parameters ΔH^# (kJ·mol^?1) and ΔS^# (J·K^?1·mol^?1) are 4.76x10³, 28.7±0.1, ?78.4±0.2 for La(III)-CMPO complex, 4.72x10³, 42.6±0.4, ?31.7±1.3 for Nd(III)-CMPO complex, and 3.20x10³, 46.9±0.6, ?20.5±2.2 for U(VI)-CMPO complex, respectively.     

New Phase Transitions in Non-Stoichiometric U3O8-x at High Temperatures, (I)

The phase equilibrium of non-stoichiometric U₃O_8-x has been studied by thermogravimetry in the range 765°≦T≦995°C and 10^?4≦Po₂≦1 atm. The results suggest the presence of six phases within U₃O_8-x the phase, separated by second (or higher) order transitions. The relative partial molar free energies, enthalpies and entropies within an each of the six phases, as well as the standard free energies, enthalpies and entropies for the phase changes are calculated and compared with previous works.     

New Phase Transitions in Non-Stoichiometric U3O8-x at High Temperatures, (II)

Electrical conductivity and X-ray diffraction studies on non-stoichiometric U₃O_8-x phase were carried out simultaneously in the range 765°≦T≦995°C and 10^?4≦Po₂≦1 atm. The plot of logσ vs. logPo₂ showed many refractions which corresponded with the phase transitions determined by thermogravimetry reported in the preceding paper. Based on the data of both electrical conductivity and thermogravimetry, the non-stoichiometric defect structures of various U₃O_8-x phases are interpreted as consisting of singly charged oxygen interstitials (O_l′) and doubly charged oxygen vacancies (Vo^.)? Some of the X-ray diffraction lines were found to undergo splitting with decreasing oxygen partial pressure. These splits are qualitatively discussed in reference to the out-of-step structure model. The mechanism of electrical conduction in the high temperature hexagonal U₃O_8-x phases is surmised to be the hopping of small polarons.     

Interaction of energetic clusters (Au3, Au400 and C60) with organic material and adsorbed gold nanoparticles

Using molecular dynamics simulations (MD), this contribution compares the interaction of three energetic clusters (Au₃, Au₄₀₀ and C₆₀) with a hybrid surface of crystalline polyethylene (PE) covered by a layer of gold nanoparticles. This model system mimics the situation encountered in metal-assisted secondary ion mass spectrometry. The chosen impact points are representative of the PE surface, the metal particles and the frontier between the metal and the polymer. The simulations show the differences between the impact over the Au nanoparticle and the polymer surface, in terms of projectile penetration, crater formation and sputtering yield of PE and gold species. For C₆₀ and Au₃ projectiles, a simple correlation is found between the quantity of energy deposited in the top polymeric layers and the quantity of sputtered polymer material, including all the impact points. The results obtained with Au₄₀₀ do not fit on this line, indicating that other physical parameters are prevalent. The mechanistic view of the interaction provided by the MD helps explain the differences. In short, while C₆₀ and Au₃ quickly break apart, creating energetic recoils and severing many bonds in the surface, Au₄₀₀, with the largest total momentum by far (∼10 times larger than the others) and the lowest energy per atom (25 eV), tends to act and implant in the solid as a single entity, pushing the polymeric material downwards and breaking few bonds in the surface.     

Trend in criticality calculation results of borated-water-moderation experimental cores relating to 10B(n, α) cross section

ABSTRACT

In connection with the accuracy of the ¹⁰B(n, α) cross section in the thermal- and epithermal-neutron energy regions, criticality calculation results were examined for six benchmark sets of light-water-moderation critical experiments of UO₂ and MOX fuel lattice cores with un-borated and borated water. Two of the benchmark sets were those implemented in the Tank-Type Critical Assembly (TCA). The others were taken from the International Handbook of Evaluated Criticality Safety Benchmark Experiments (ICSBEP), and the International Handbook of Evaluated Reactor Physics Benchmark Experiments (IRPhEP). The enrichments of the UO₂ fuel range from 1.9 wt% to 2.6 wt%, and the Pu contents of the MOX fuel do from 2.0 to 6.6 wt%. The boron concentrations in water are up to 1511 ppm. The effective neutron multiplication factors (k_eff ) were taken from the published documents. They were calculated with continuous-energy Monte Carlo calculation codes in combination with JENDL-4.0, and other evaluated nuclear data libraries. It was confirmed that the k_eff values of the critical cores increased with the boron concentrations, which indicates that the ¹⁰B(n, α) cross section in the thermal- and epithermal-neutron energy regions should be larger than those in JENDL-4.0 and other libraries.     

Recent Results in JT-60 Advanced Experiment JT-60 Team,JAERI (Presented by Naoyuki MIYA)

Major efforts in the recent JT-60 experiments have been concentrated on the improved confinement of plasmas with profile control and on the steady state operation study. Peaked density profiles were produced with the successive pellet injection. The energy confinement time was improved by 40% as large as that with the gas fuelled discharges. The fusion products n _e(0)τET _i(0)reached 1.2 × 10²⁰m^?3·s·keV, which was twice that of gas fuelled discharges. High-β_p, plasmas were obtained in low-I _p discharges with improved confinement and a high ion temperature T _i, (0) of 12 keV. The bootstrap current reached 80% of the total plasma current at β_p=3.2. The new concept of a steady-state tokamak power reactor has been proposed on the basis of this result. The maximum current drive efficiency ηCD of 3.4 × 10₁₉m^?2·MA/MW was obtained in the LH current drive experiments. Helium ash exhaust experiments using He-beam injection into H⁺ plasmas showed promising results for α-particle exhaust in a fusion power reactor.     

Structural and Electrochemical Studies on Uranium(VI) Nitrato Complex with n-Octyl(phenyl)-N,N-Diisobutylcarbamoylmethylphosphine Oxide in Non-aqueous Solvents

The structure of uranyl nitrato complex with CMPO [n-Octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide] in solid state and in non-aqueous solvents without containing free CR/IPO has been studied by using IR spectrophotometer, ¹³C- and ³¹P-NMR. The carbonyl(vcO) and phosphoryl(vpO) stretching bands of coordinated CMPO were observed at lower wavenumber than the corresponding bands of free CMPO in both the states. The ¹³C and ³¹P peaks assigned to the carbonyl carbon and phosphoryl phosphine of coordinated CMPO was detected in the lower field than that of free CMPO. From these results, it was concluded that the uranyl nitrato complex with CMPO in both the states has the structure with two nitrate and one CMPO coordinated as bidentate in the equatorial plane of uranyl ion, i.e., UO₂(NO₃)₂·CMPO. Furthermore, the electrochemical studies of UO₂(NO₃)₂·CMPO complex in CH₃CN have been carried out using cyclic and normal pulse voltammetric methods. It was found that the UO₂(NO₃)₂·CMPO complex is reduced to U(V) complex at around ?1.22V vs. Fc/Fc⁺ (ferrocene/ferrocenium) and that the resulting reductant is oxidized to U(VI) at around +0.04V vs. Fc/Fc⁺.