Atmospheric discharge of 14C from the Tokai reprocessing plant: comprehensive chronology and environmental impact assessment

Quantitative evaluation of the atmospheric discharge of radiocarbon (¹⁴C) is of primary importance for accurately assessing the radioecological impact of the operation of the Tokai reprocessing plant (TRP). However, monitoring the atmospheric ¹⁴C discharge was not conducted at the TRP prior to October 1991. The main purpose of this study was to establish the chronology of atmospheric ¹⁴C discharges for the entire operation period (1977–2014). We found a strong correlation between the ¹⁴C discharge and spent fuel reprocessing data obtained after October 1991; we used this correlation to estimate the monthly ¹⁴C discharges in the 1977–1991 period. The total amount of atmospheric ¹⁴C discharge was estimated at 7741 ± 217 GBq for the entire period, with the largest annual discharge of 978 GBq in 1992. Tree-ring ¹⁴C analysis and model calculations using the established discharges were conducted to assess the excess ¹⁴C concentrations around the TRP in the past. The results suggested that the excess ¹⁴C concentrations were <45 Bq kg^?1 C and the annual effective dose via the atmosphere–rice ingestion pathway was as low as 1.2 μSv y^?1, indicating no significant radioecological impact of atmospheric ¹⁴C discharges from the TRP.     

Atmospheric 85Kr and 133Xe activity concentrations at locations across Japan following the Fukushima Dai-ichi Nuclear Power Plant accident

Atmospheric ⁸⁵Kr and ¹³³Xe activity concentrations were determined from weekly air samples collected at Sapporo, Akita and Chiba, Japan, throughout 2011. The results demonstrated that the Fukushima Dai-ichi Nuclear Power Plant accident in early March 2011 resulted in high ¹³³Xe activity concentrations as well as elevated levels of ⁸⁵Kr activity; there was a striking increase in the concentrations of both isotopes over the week running from 14 to 22 March as the radioactive plume released from the plant was captured. At Chiba, following the accident, the ⁸⁵Kr activity concentration increased from 1.38 to 17.7 Bq/m³, while the ¹³³Xe levels increased from below the minimum detectable concentration (MDC ≤ 1.9 × 10^?3 Bq/m³) to 1.3 × 10³ Bq/m³. Conversely, at Sapporo and Akita, high ⁸⁵Kr activity concentrations were not observed, due to differences in air transportation mechanisms based on wind directions. Duplicate samples were collected at Chiba to allow the simultaneous analyses of ⁸⁵Kr and ¹³³Xe at the Japan Chemical Analysis Center and the Bundesamt für Strahlenschutz in Germany and the results were in good agreement. The external effective radiation doses resulting from ⁸⁵Kr and ¹³³Xe releases following the accident were estimated to be approximately 7.0 × 10^?3 and 1.3 μSv, respectively, based on the activity concentrations of these nuclides from March to June in 2011 at Chiba.     

Effect of spring water on the radon concentration in the air at Masutomi spa in Yamanashi Prefecture,Japan

The concentrations of ²²²Rn existing in air have been studied by using a convenient and highly sensitive Pico-rad detector system at Masutomi spa in Yamanashi Prefecture, Japan. The measurements in air were carried out indoors and outdoors during the winter of 2000 and the summers of 1999 and 2005. The concentrations of ²²²Rn in spring water in this region were measured by the liquid scintillation method. The concentrations of natural radionuclides contained in soils surrounding spa areas were also examined by means of the γ-ray energy spectrometry technique using a Ge diode detector to investigate the correlation between the radionuclides contents and ²²²Rn concentrations in air at each point of interest. The atmospheric ²²²Rn concentrations in these areas were high, ranging from 5 Bq/m³ to 2676 Bq/m³. The radon concentration at each hotel was high in the order of the bath room, the dressing room, the lobby, and the outdoor area near the hotel, with averages and standard deviations of the concentration of 441 ± 79 Bq/m³, 351 ± 283 Bq/m³, 121 ± 5 Bq/m³, and 23 ± 1 Bq/m³, respectively. The source of ²²²Rn in the air in the bath room is more likely to be the spring water than the soil. The spring water plays carries the radon to the atmosphere. Our measurements indicated that the ²²²Rn concentration in the air was affected by the ²²²Rn concentration in spring water rather than that in soil.     

Environmental Tritium in the Vicinity of Tokai Reprocessing Plant

The distribution of ³H in the atmosphere, vegetations and soil water was observed in the vicinity of Tokai reprocessing plant (TRP) over the period 1990–2004. The annual means of the atmospheric HTO and HT concentrations were in the range of 12–40 mBqm^?3 with a significant seasonal variation and 14–51 mBqm^?3 with no seasonal variation, respectively. Long-term atmospheric dilution factors, defined as the annual mean of the atmospheric HTO concentration divided by the discharge rate of HTO from the TRP, were estimated to be 10^?8–10^?6 sm^?3. The atmospheric HTO concentrations decreased with distance from the TRP, falling to the current background level in Japan at 5 km off-site. The HTO concentrations observed were compared with those calculated by a simple mathematical model with input data of the monthly ³H discharge rates and actual meteorological conditions. The calculations were correlated well with the observations even for only a little HTO-elevated situation, considering the naturally occurring ³H level in atmospheric vapor around the TRP. Tritium concentrations in vegetation and soil water samples were roughly the same as the atmospheric HTO concentrations, suggesting the rapid equilibrium of ³H concentrations in the atmosphere-soil-vegetation system around the TRP.     

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.     

吸入性210Pb内照射剂量估算方法研究

本文通过建立包含沉积模型、生物动力学模型和剂量学模型的一整套内照射模型,计算得到吸入环境中的²¹⁰Pb对男女成年人各器官的当量剂量系数,从而得到有效剂量系数为1.1×10^-6 Sv/Bq。计算结果对²¹⁰Pb防护工作的开展提供了参考数据。     

Boiling and drying accident of high-level liquid waste in a reprocessing plant: Examination of the NO2 and NO generation using the simulated waste

ABSTRACT

NO₂ and NO generated during a boiling and drying accident, which affects the release of volatilized radioactive Ru into the atmosphere, were examined using various samples including simulated high-level liquid waste and a thermogravimetric analyzer. NO₂ and NO in the gas flowing out of the analyzer were measured separately using a NOx analyzer equipped with NO₂ and NO sensors. The samples were heated to 600°C at constant heating rates of mainly 0.2 and 1°C min^?1 that was adopted taking into account the decay heat of high-level liquid waste. It was found that under 180°C some nitrates in the liquid waste mainly separated their nitrate groups as HNO₃ without generating NOx (a mixture of NO and NO₂) and above 300°C the residual HNO₃ in the waste participated in thermal decomposition generating NOx. The generation rates of NO₂ and NO were obtained as a function of time using Arrhenius type equations, and the O₂ rate was derived from these equations using the stoichiometry of the reactions that generate NO₂, NO, and O₂.     

14C analysis via intracavity optogalvanic spectroscopy

A new ultra sensitive laser-based analytical technique, intracavity optogalvanic spectroscopy (ICOGS), allowing extremely high sensitivity for detection of ¹⁴C-labeled carbon dioxide has recently been demonstrated. Capable of replacing accelerator mass spectrometers (AMS) for many applications, the technique quantifies zeptomoles of ¹⁴C in sub micromole CO₂ samples. Based on the specificity of narrow laser resonances coupled with the sensitivity provided by standing waves in an optical cavity, and detection via impedance variations, limits of detection near 10^{?15 14}C/¹²C ratios have been obtained with theoretical limits much lower. Using a 15 W ¹⁴CO₂ laser, a linear calibration with samples from 5 × 10^?15 to >1.5 × 10^?12 in ¹⁴C/¹²C ratios, as determined by AMS, was demonstrated. Calibration becomes non-linear over larger concentration ranges due to interactions between CO₂ and buffer gas, laser saturation effects and changes in equilibration time constants. The instrument is small (table top), low maintenance and can be coupled to GC or LC input. The method can also be applied to detection of other trace entities. Possible applications include microdosing studies in drug development, individualized sub-therapeutic tests of drug metabolism, carbon dating and real time monitoring of atmospheric radiocarbon.     

Source term estimation of atmospheric release due to the Fukushima Dai-ichi Nuclear Power Plant accident by atmospheric and oceanic dispersion simulations

The source term of the atmospheric release of ¹³¹I and ¹³⁷Cs due to the Fukushima Dai-ichi Nuclear Power Plant accident estimated by previous studies was validated and refined by coupling atmospheric and oceanic dispersion simulations with observed ¹³⁴Cs in seawater collected from the Pacific Ocean. By assuming the same release rate for ¹³⁴Cs and ¹³⁷Cs, the sea surface concentration of ¹³⁴Cs was calculated using the previously estimated source term and was compared with measurement data. The release rate of ¹³⁷Cs was refined to reduce underestimation of measurements, which resulted in a larger value than that previously estimated. In addition, the release rate of ¹³¹I was refined to follow the radioactivity ratio of ¹³⁷Cs. As a result, the total amounts of ¹³¹I and ¹³⁷Cs discharged into the atmosphere from 5 JST on March 12 to 0 JST on March 20 were estimated to be approximately 2.0 × 10¹⁷ and 1.3 × 10¹⁶ Bq, respectively.     

Temperature effect study of silicon-on-insulator structures prepared by high dose implantation of nitrogen

The temperature effect on the microstructure of the N⁺-ion implantation-induced Si₃N₄ buried layer was investigated. The underlying silicon nitride layers were formed in a Si (1 1 1) wafer after implantation of 50 keV nitrogen ions (fluence: 1 × 10¹⁷, 2 × 10¹⁷ and 5 × 10¹⁷ ions/cm²). It was observed that a continuous amorphous layer of about 200 nm thickness was formed in all implanted samples due to the irradiation damage. After 30 min annealing at 900 °C, poly-crystalline Si₃N₄ products were found by TEM examination in the specimen implanted with 5 × 10¹⁷ ions/cm² dose. In the case of annealing at 1200 °C a continuous single-crystalline α-Si₃N₄ buried layer was formed indicating that the amorphous layer in the implanted samples could be transformed into three successive layers, which are amorphous SiO₂, single-crystal α-Si₃N₄ and retained defects from surface to inner substrate, respectively.     

Recovery of neutron-irradiation-induced defects of Al2O3, Y2O3, and yttrium-aluminum garnet

SiC fiber-reinforced SiC matrix composites (SiC_f/SiC) are considered as one of the candidates for blanket materials in future fusion reactors and as an advanced fuel cladding material for next-generation fission reactors. Generally, the densification of SiC needs sintering additives and oxides such as Al₂O₃, Y₂O₃, and yttrium-aluminum garnet (YAG, Y₃Al₅O₁₂), which are frequently added to SiC. However, the effects of neutron irradiation on sintering additives are still unclear. In this study, we performed the neutron irradiation of Al₂O₃, Y₂O₃, and YAG at fluences up to 2.0–2.5 × 10²⁴ n/m² (E > 0.1 MeV) at 60–90 °C. The isochronal recovery of the macroscopic volume of Al₂O₃ against annealing temperature showed smooth and continuous shrinkage at a temperature of up to 1200 °C, and the volume slightly increased above that temperature. In contrast, the volume of Y₂O₃ showed quick shrinkage at the low temperature range, and slower and smooth recovery was observed up to ～1100 °C. In the case of YAG, the recovery of volume occurred in a step-wise manner at 600–750 °C, and continuous shrinkage occurred at temperatures lower and higher than that temperature range. The activation energies for the macroscopic volume recoveries of three oxides were obtained from the Arrhenius plots of the rate coefficients. Two-stage recovery was observed for Al₂O₃, whereas more complicated recovery processes were suggested for Y₂O₃ and YAG.     

Production of high-purity medical radio isotope 64Cu with accelerator-based neutrons generated with 9 and 12 MeV deuterons

We conducted a feasibility study for producing a high-purity medical radioisotope ⁶⁴Cu from natural zinc with accelerator-based neutrons. ⁶⁴Cu isotopes were produced via the ⁶⁴Zn(n,p) reaction. The accelerator-based neutrons were generated via the C(d,n) reaction using low-energy deuterons of 9 and 12 MeV on a 1-mm-thick carbon target. First, the production purity was estimated using the evaluated nuclear data library JENDL-4.0 and our previously measured thick target neutron yield. We found that even when natural zinc was used as the starting material, significantly high-purity ⁶⁴Cu could be obtained. Next, irradiation experiments for producing ⁶⁴Cu using natural zinc were conducted at Kyushu University Tandem Laboratory, with the amounts of ⁶⁴Cu isotopes and other gamma-emission nuclides measured by a high-purity germanium detector. As a result, high-purity ⁶⁴Cu isotopes of 1.11(49) × 10⁰ and 3.70 (17) × 10⁰ Bq/g/μC were produced with incident deuteron energies of 9 and 12 MeV, respectively.     

Oxidation of Uranium Dioxide

The oxidation of UO₂ was studied by thermogravimetry and X-ray diffraction. It was clarified that the thermal history covering the first stage of the oxidation from UO₂ to U₃O UO₇ significantly influenced the rate of the oxidation of the second stage from U₃O₇ to U₃ O₈.

The entire oxidation reaction proceeded in what to all appearances, was a single stage when the specimen temperature was raised rapidly, whereas at slower rates of heating up, two distinct stages of oxidation were observed, separated by an intermediate induction period. These findings suggest the existence of a close connection between the rate of formation of the U₃O₇ phase and the rate of the subsequent oxidation of this phase: A slow formation of U₃O₇ would tend to prolong the induction period preceding the second stage of the oxidation. A similar effect was observed also with annealing of the intermediate U₃O₇ at 200°C: The increase of annealing time prolonged the induction stage.

The rate of the second stage oxidation was fairly well expressed by Johnson & Mehl's equation, log (1/(1-y/)=(1/2.303)kⁿtⁿ . The time exponent n in this equation varied in the range of 1.0~2.5, and the rate constant k of 1.15×10^?4~2.04 ×10^?1 min^?1, depending on the experimental conditions.     

H310BO3/ZnS(Ag)热中子闪烁体转换屏的涂布法制备及性能研究

本文采用涂布法制备了一系列H₃¹⁰BO₃/ZnS(Ag)闪烁体转换屏样品,对其成分配比进行了优化。结果表明,最佳的H₃¹⁰BO₃/ZnS(Ag)质量比在1∶6~1∶7之间,最佳的黏合剂用量为总质量的25%。利用中子照相设备对转换屏的发光均匀性进行了成像分析,结果显示光输出非常均匀;对楔形镉条进行中子成像,并采用调制传递函数(modulation transfer function,MTF)方法计算了系统分辨率,结果显示,在MTF值为0.1时,对于厚度分别为270(11)、350(14)、404(9)及505(15)μm的转换屏,其相应的系统空间分辨率分别为255.6、315.9、371.0和471.3 μm。     

Synthesis and thermal conductivity of Y6UO12

Y₆UO₁₂ was synthesized by solid-state reactions of Y₂O₃ and U₃O₈. The high-density pellet of Y₆UO₁₂ was prepared by the spark plasma sintering followed by heat treatment in air for oxygen supplementation. The thermal conductivity (κ) was evaluated using the laser flash method from room temperature to 1173 K. The κ of Y₆UO₁₂ decreased with increasing temperature in the whole temperature range, indicating that the phonon contribution was predominant. The room temperature κ value of Y₆UO₁₂ was 4.90 Wm^?1K^?1. The magnitude relationship of κ among Y₆UO₁₂, Y₆WO₁₂, and Yb₆WO₁₂, i.e. κ of Yb₆WO₁₂ < κ of Y₆UO₁₂ < κ of Y₆WO₁₂, was discussed based on the general lattice thermal conductivity theory.     

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.     

Fragmentation by Beta-Decay in Tritium-Labelled Compounds, (III)

The potential energy curves of LiHe⁺, BeHHe⁺ and FHe⁺ in the ground state are calculated with a scale factor optimized STO-6G basis set, and these potential curves are compared with those of HHe⁺, CH₃He⁺, NH₂He⁺ and OHHe⁺ already reported. In the T→He⁺ β-decay, ground state daughter ions HHe⁺, LiHe⁺ and BeHHe⁺ are found to be bound, whereas CH₃He⁺, NH₂He⁺, OHHe⁺ and FHe⁺ ions dissociate into a He atom and residual fragments.     

LiMgPO4:Tb,B - A new sensitive OSL phosphor for dosimetry

Optically Stimulated Luminescence (OSL) technique has emerged as a serious competitor to Thermally Stimulated Luminescence (TSL) technique in various dosimetric applications, especially after the development of crystalline alumina (Al₂O₃:C) doped with carbon. Since then, several attempts are being made to develop other possible materials for OSL based dosimetric applications. Efforts conducted in our laboratory in this direction have led to the development of a new phosphor, Lithium Magnesium Phosphate doped with terbium and boron (LiMgPO₄:Tb,B). This phosphor is prepared by solid-state diffusion method involving conventional air furnaces with operating temperature 1000 °C and easily amenable to large scale production without compromising primary dosimetric advantages. In this work we present some of the dosimetric OSL characteristics of this phosphor. The phosphor exhibits a main TSL peak at 250 °C. The phosphor also emits OSL, when the irradiated phosphor is stimulated with 470 nm light with the OSL sensitivity 1.3 times that of commercially available Al₂O₃:C. Photoluminescence (PL) emission spectrum consists of sharp lines characteristics of Tb³⁺ emission. The OSL discs made out of this phosphor are reusable up to at least 50 cycles, the phosphor exhibits dose linearity up to 1 kGy. Minimum detectable dose is found to be 20 μGy and fading of the OSL signal is found to be about 16% in four days, after which the OSL signal stabilizes.     

Clarification of high density electronic excitation effects on the microstructural evolution in UO2

In order to understand the properties of ion tracks and the microstructural evolution under accumulation of ion tracks in UO₂, 100 MeV Zr¹⁰⁺ and 210 MeV Xe¹⁴⁺ ions irradiation examinations have been done at a tandem accelerator facility of JAEA-Tokai, and it has been observed the microstructure by means of a transmission electron microscope (TEM) and a scanning electron microscope (SEM) in CRIEPI.Comparison of the diameter of ion tracks between UO₂ and CeO₂ under irradiation with 100 MeV Zr¹⁰⁺ and 210 MeV Xe¹⁴⁺ ions at room temperature clarify that the sensitivity on high density electronic excitation of UO₂ is much less than that of CeO₂. By the cross-sectional observation of UO₂ under irradiation with 210 MeV Xe¹⁴⁺ ions at 300 °C, elliptical changes of fabricated pores that exist till ∼6 μm depth and the formation of dislocations have been observed in the ion fluence over 5 × 10¹⁴ ions/cm². The drastic changes of surface morphology and inner structure in UO₂ indicate that the overlapping of ion tracks will cause the point defects, enhance the diffusion of point defects and dislocations, and form the sub-grains at relatively low temperature.     

Development of Flexible Neutron-Shielding Resin as an Additional Shielding Material

A soft-type neutron-shielding resin has been developed by improving an existing hard-type neutronshielding material using the epoxy-based resin as an additional shielding material. A flexible heat-resistant neutron-shielding material has been developed, which consists of a new polymer-based resin with boron. The neutron shielding performance of the developed flexible heat-resistant resin with the ²⁵²Cf neutron source is almost the same as that of polyethylene. The outgases of H, H₂, NH₄, H₂O, CO, O₂, C₄H₁₀, and CO₂ from the developed resin have been measured at high temperature (up to 250°C) by thermal desorption spectroscopy methods. The soft-type resin and the newly developed heat-resistant resin will be applied to prevent the effects of neutron streaming and to control the movement of a vibrated pipe as the seal material around the plumbing in the future fast reactor and innovative fission reactor.