Studies on the Characteristic of Titanium–Tritium Reaction

The p–c–T curves of tritium absorption and desorption of titanium were measured using the method of step equilibrium by stepping up the tritium quantity on an experimental apparatus of metal hydride. The p–c–T curves for tritium have one plateau at temperature below 300°C and two plateaus at temperature above 300°C. The thermodynamic parameters of the different phases were determined according to the van’t Hoff equation. The hysteresis effect was not observed in reversible process of tritium absorption and desorption of titanium on our experimental condition. The tritium absorption behavior of titanium in the temperature ranging from 550°C to 750°C and desorption behavior of titanium in the temperature ranging from 350°C to 550°C have been investigated in a constant volume system. A method of the reaction rate analysis was proposed and examined for determining the rate constant. The apparent activation energy obtained by this analysis for the absorption and the desorption were 155.5 ± 3.2 kJ mol⁻¹ and 62.1 ± 1.6 kJ mol⁻¹ respectively.     

Detritiation of Glovebox Atmosphere by Using Compact Tritium Removal Equipment

A compact tritium removal equipment (TRE), assembled in a console with casters, has been developed for detritiation of air in a glovebox used for handling of several curies of tritium. The TRE was designed to remove gaseous tritium in the form of T₂, HT and CH₃T through oxidation with precious metal/alumina catalysts followed by adsorption on zeolite pellets.

From the detritiation experiments with hydrogen tritide (HT, 2–20 mCi), the TRE was confirmed to have sufficient performance for the practical use. The tritium concentration in the test gas (total volume –32l; 1%H₂, 5%O₂, 94%N₂) decreased from 0.64 to 6.4 ×10-⁷ Ci.m³ within 155 min when the TRE was operated under the recirculation mode with the flow rate of 200 l-h¹ at the catalyst temperature of 200°C. In addition, the HT-to-HTO fractional conversion was determined at various catalyst temperatures (25–200°C) and flow rates (100–360 lh-¹).     

Kinetic estimation of hydrogen isotope exchange reaction between tritiated-water (HTO) vapor and each amino acid in a heterogeneous system

The hydrogen isotope exchange reaction between HTO vapor and each amino acid has been observed in order to establish a method of estimation of the internal exposure of organically bound tritium in a heterogeneous system at 25～70°C. Rate constants (k) for the amino acids have been obtained by applying the A″-McKay plot method. Using these k values, Arrhenius plots for both the COOH and NH₂ groups are drawn, and linearity was obtained over the range of 25～70°C. Comparing the rate constants, the following four statements can be made regarding the T-for-H exchange reaction. (1) The reactivity of the functional groups in amino acids increases with increasing temperature. (2) Applying Taft's equation, the ratio of polar effect to steric effect is 2:8 in the COOH group and 9:1 in the NH₂ group at 25°C. (3) The A″-McKay plot method is useful for studying the reactivity of materials, not only with one (or the same kind of) functional group(s) but also with two different kinds of functional groups. (4) The method used in this work may be useful to investigate the behavior of organically bound tritium, quantitatively.     

Production of 40 TBq Tritium Using Neutron-Irradiated 6Li-Al Alloy

A facility was reconstructed for producing tritium in 40 TBq per batch. Gaseous tritium was extracted from neutron-irradiated ⁶Li-Al alloy targets by heating at 700°C under vacuum and collected in uranium. The recovery yield of tritium was about 100% and the isotopic purity of the product was about 95%. Through the production run, no leakage of tritium from the facility was observed.     

Development of Deuterium-Tritium Loading Vessel for Laser Fusion Target

Tritium permeation at 350°C through stainless steel wall of a vessel filled with deuterium-tritium gas of 6.1 × 10⁶ Pa pressure was practically suppressed by Au plating of 20μm thick applied to the outside surface. The apparent diffusivity of hydrogen through plated Au layer, derived from the experimental data, was 2 x 10^?11 cm²/s for 470°C, which is 10^?5–10^?6 times smaller than what would be expected from values reported for wrought Au, and the apparent solubility was very significantly higher than similarly expected level. Gas analysis of the Au layer indicated that the effective suppression of tritium permeation is attributable to trapping of hydrogen by C contained in the Au as impurity. Adequate tightness against tritium leakage has been achieved by Au plating on a vessel used for loading glass microspheres with deuterium-tritium gas, intended for laser fusion targets.     

Tritium Breeding Capability of Heliotron-H Fusion Reactor Blankets

Preparation and operation procedures of chromatographic column for hydrogen isotope separation have been examined. The best separation of isotopic molecular hydrogen was obtained when the stationary phase was activated at 230°C for 16 h and subsequently deactivated with CO₂ at ?7°C. The technique has been applied to analyzing commercially available tritium gases. Protium tritide (HT), DT, and tritiated-methane and -ethane were observed as impurities in all three samples analyzed. It was experimentally confirmed that most of the contaminant protium in the tritium gas came from the inner-surface of the storage vessel.     

Analysis of Tritium Behavior in Very High Temperature Gas-Cooled Reactor Coupled with Thermochemical Iodine-Sulfur Process for Hydrogen Production

The tritium concentration in the hydrogen product in Japan's future very high temperature gas-cooled reactor (VHTR) system coupled with a thermochemical water-splitting iodine-sulfur (IS) process (VHTRIS system), named GTHTR300C, was estimated by numerical analysis. The tritium concentration in the hydrogen product significantly depended on undetermined parameters, i.e., the permeabilities of a SO₃ decomposer and a H₂SO₄vaporizer made of SiC. Thus, the estimated tritium concentration in the hydrogen product for the conservative analytical condition ranged from 3.4 × 10^?3 Bq/cm³ at STP (38 Bq/g-H₂) to 0.18 Bq/cm³ at STP (2,000 Bq/g-H₂). By considering the tritium retained by core graphite and the reduction in permeation rate by an oxide film on the heat transfer tube of the IHX and the HI decomposer, the tritium concentration in the hydrogen product decreased to the range from 3.3 × 10^?5 Bq/cm³ at STP (0.36 Bq/g-H₂) to 5.6 × 10^?3 Bq/cm³ at STP (63 Bq/g-H₂), which were smaller than those for the conservative analytical condition by factors of about 3.2 × 10^?2 and 9.6 × 10^?3, respectively. The effectof the helium flow rate in the helium purification system on the tritium concentration in the hydrogen product was also evaluated.     

Studies on the Characteristic of Zirconium–Tritium Reaction

The p–c–T curves of tritium absorption and desorption of zirconium were measured using the method of step equilibrium by stepping up the tritium quantity on an experimental apparatus of metal hydride. The p–c–T curves for tritium have one plateau at temperature range from 450 to 500°C and two plateaus at temperature above 600°C. The thermodynamic parameters of the different phases were determined according to the van’t Hoff equation. The hysteresis effect was observed in reversible process of tritium absorption and desorption of zirconium on our experimental condition. The tritium absorption behavior by zirconium in the temperature range from 450 to 620°C and desorption behavior of zirconium in the temperature range from 775 to 875°C have been investigated. A method of the reaction rate analysis was proposed and examined for determining the rate constant. The apparent activation energy obtained by this analysis for the absorption and the desorption were (−16.8 ± 0.8) kJ·mol⁻¹ and (57.7 ± 1.6) kJ·mol⁻¹, respectively.     

Temperature dependence of He trapping in niobium

The total amount and the depth distributions of 9 and 15 keV implanted ³He ions trapped in polycrystalline niobium have been studied using the ³He(d,p)⁴He reaction. The implantation target temperature was varied from 20 to 1000° C and subsequent anneal studies were carried out for temperatures up to 1600° C. For implantation temperatures below 400° C all ²He particles coming to rest in the target are trapped. Between 500°C and 1000°C the trapping probability decreases gradually with increasing temperature to a few percent. A greater amount of helium is always retained upon annealing of a lower temperature implant to a particular temperature than is retained for implantation at that temperature.     

Blistering of niobium due to 0.5 to 9 keV helium and hydrogen bombardment

Blistering of well-annealed niobium single crystals due to 0.5 to 9 keV helium and hydrogen ion bombardment at temperatures between ?110°C and 1000°C has been investigated by Rutherford backscattering (RIBS) in double alignment and with a scanning electron microscope (SEM). For He bombardment blistering was observed by RIBS in the temperature range investigated for all energies above 1 keV. The critical dose at which blisters first appear is about 1 to 2 × 10¹⁷ incident He ions per cm². It increases slightly with increasing ion energy and with decreasing target temperature. Blisters of 500 to 5000 Å in diameter were found. The depth at which the blisters develop increases from ≈ 180 Å for 1 keV to 1100 Å for 9 keV He ions. It is a factor of ≈ 3 larger than the theoretical mean range of the ions in amorphous material. Above ≈ 600°C grain boundaries develop extending also into the unbombarded region. For hydrogen bombardment no blistering could be observed at room temperature up to doses of 2 × 10¹⁹ ions per cm².     

Evaluation of tritium diffusion through the Neutral Beam Injector calorimeter panel

The Neutral Beam Test Facility (NBTF) to be realized in Padoa will test the Neutral Beam Injection (NBI), one of the Heating and Current Drive Systems foreseen for ITER. The NBI is based on the acceleration of hydrogen or deuterium negative ions up to 1 MeV. This work has been aimed at assessing the tritium release from the NBTF in order to provide data for the safety analysis. In particular, the diffusion of the tritium through the neutral beam target material (the CuCrZr alloy calorimeter panels) has been assessed by using literature data of the diffusion coefficient. The tritium generated inside the calorimeter panels moves into both the vacuum and water side: the tritium diffusion flux has been evaluated during the beam-on (200 °C) and the beam-off (20 °C) phases of the NBTF experiments consisting of an interim campaign and a final test. The penetration depth of the tritium through the 2 mm thick CuCrZr alloy material has been also evaluated by using a Monte-Carlo code. As main result, the assessed diffusion flux of tritium during both the beam-on and the beam-off phases are modest. In fact, at the end of the interim campaign (100 days), about the 96% of the all generated tritium (626.5 MBq) exits the calorimeter while the residual tritium inventory (25 MBq) leaves the copper alloy with a diffusion time of about 1 month. At the end of the final test (14 days) about the 99% of the total generated tritium (1.023 × 10⁴ MBq) leaves the copper alloy and the remaining tritium inventory (152.2 MBq) is released by about 32 days. In both the interim campaign and the final test, more than the 99% of the total tritium is transferred into the vacuum side of the calorimeter panel while negligible tritium amounts enter the cooling water system thus showing a very low impact on the environment.     

First wall surface problems for a D ↽ T tokamak reactor

The effects of deuterium, tritium, helium and neutron bombardment on surface degradation of the first wall of a 5000 MW_th D-T reactor have been analyzed. The effects of both sputtering and blistering have been analyzed and the results applied to 316 stainless steel wall operating at temperatures from 300 to 500°C. It has been calculated that the total wall erosion rate is 0.22 mm/year and that 14 MeV neutron sputtering accounts for two thirds of this number. Sputtering from all neutrons results in $\text{≈0.17}\text{mm/year}$ erosion. The calculated erosion rate is 2–3 times that which would be allowable for a 30 year first wall lifetime.     

Using the tritium plasma experiment to evaluate ITER PFC safety

The Tritium Plasma Experiment was assembled at Sandia National Laboratories, Livermore and is being moved to the Tritium Systems Test Assembly facility at Los Alamos National Laboratory to investigate interactions between dense plasmas at low energies and plasma-facing component materials. This apparatus has the unique capabilty of replicating plasma conditions in a tokamak divertor with particle flux densities of 2 × 10²³ ions/m².s and a plasma temperature of about 15 eV using a plasma that includes tritium. An experimental program has been initiated using the Tritium Plasma Experiment to examine safety issues related to tritium in plasma-facing components, particularly the ITER divertor. Those issues include tritium retention and release characteristics, tritium permeation rates and transient times to coolant streams, surface modification and erosion by the plasma, the effects of thermal loads and cycling, and particulate production. An industrial consortium led by McDonnell Douglas will design and fabricate the test fixtures.Prepared for the U.S. Department of Energy, Office of Energy Research under DOE Idaho Field Office Contract DE-AC07-76ID01570.     

Geometrical Interpretation of Mutual Relatonship between Ordinary Coherence and Noise Power Contribution Ratio

Angular neutron fluxes leaking from the surface of lithium-oxide and graphite slab assemblies have been measured with irradiation of D-T neutrons. The spectrum measurement was performed using the time-of-flight technique with an NE213 scintillation detector. The thicknesses of the slabs were 0.6 to 5 mean free path for 14.8 MeV neutrons, and the measured leaking angles of the angular fluxes were 0.0°, 12.2°, 24.9°, 41.8° and 66.8°. The experimental results have been compared with the results calculated by the continuous energy Monte Carlo transport code MCNP, using the data in the JENDL-3PR1, ?3PR2, and ENDF/B-V nuclear data files. The comparisons between the experimental and calculated results show that the data of ⁷Li in JENDL-3PR2 is improved for the secondary emission spectra of the 4.63 MeV level and (n, 2n) reactions; the angular distributions of 3rd-and 4th-level inelastic reactions of C in the JENDLs are questionable. The thickness dependences for high energy neutrons also suggest that the total cross section of ⁷Li and the elastic cross sections of C are slightly inadequate.     

The thermal neutron diffusion cooling coefficient in polyethylene

The diffusion cooling coefficient C for thermal neutrons in polyethylene at 20°C has been determined theoretically. Granada's Synthetic Model of the scattering law has been applied to describe the interaction of neutrons with polyethylene. Two approximations of the neutron energy distribution in finite homogeneous systems have been used. The result of the calculation using a rough approximation is C_B=2160 cm⁴ s⁻¹. According to a more advanced formalism which follows Nelkin's analysis of the neutron pulse decay in a finite medium, applying the diffusion theory with transport correction, the value obtained is C=2916 cm⁴ s⁻¹.     

Ratio of Permeabilities of Tritium to Protium through Palladium-Alloy Membrane

Experiments were performed to study the ratio of permeabilities of protium to tritium through Pd-Ag-Au alloy at the conditions of 350°C≦T≦550°C and p<1,000 mmHg.

The observed ratio was 2.12±0.03 at 350°C, and it was almost independent of temperature. It is remarkable that the obtained ratio of permeabilities is considerably larger than the square root of the atomic weight ratio?3.

The dependence of separation factor for the hydrogen isotopes on pressure and “cut” is also discussed.     

Tritium diffusion in zircaloy-2 in the temperature range −78 to 204° C

Tritium diffusion measurements in Zircaloy-2 were carried out over the temperature range ?78 to 204 °C by direct measurement of tritium diffusion gradients. The ⁶Li (n, α)³H reaction was used to inject tritium into the specimens and to produce initial tritium concentration in the range 0.0065 ppm to 0.013 ppm ³H by weight. Two diffusion components were identified from the concentration profiles: a surface trapping region approximately 5 μm thick and a normal diffusion profile characteristics of bulk diffusion. Surface release measurements of tritium verified the existence of a surface trapping layer. The bulk diffusion component was consistent with classical diffusion solutions and was given by: D = 0.00021_?0.00018^+0.005 exp?(8500 ± 200 cal/RT) cm² · sec^?1.The surface trapping was attributed to oxide films formed on the Zircaloy-2 at room temperature. The apparent diffusion coefficients for the surface region were consistent with: D = 4.0_?3.3^+19.7 × 10^?14 exp?(7200 ± 1500 cal/RT) cm² · sec^?1 over the temperature range 25 to 411°C.     

Triton Emission Spectra in Some Target Nuclei Irradiated by Ultra-Fast Neutrons

High-current proton accelerator technologies make use of spallation neutrons produced in (p,xn) and (n,xn) nuclear reactions on high-Z targets. The produced neutrons are moderated by heavy water. These moderated neutrons are subsequently captured on ³He to produce tritium via the (n,p) reaction. Tritium self-sufficiency must be maintained for a commercial power plant. So, working out the systematics of (n,t) reaction cross sections and triton emission differential data are important for the given reaction taking place on various nuclei at different energies. In this study, triton emission spectra by using ultra-fast neutrons (incident neutron energy >50 MeV), the (n,xt) reactions for some target nuclei as ¹⁶O, ²⁷Al, ⁵⁶Fe, ⁵⁹Co, ²⁰⁸Pb and ²⁰⁹Bi have been investigated. In the calculations, the pre-equilibrium and equilibrium effects have been used. The calculated results have been compared with the experimental data taken from the literature.