Use of thermal treatment with CaCl2 and CaO to remove 137Cs in the soil collected from the area near the Fukushima Daiichi Nuclear Power Plant.

A massive amount of soils and inflammable materials of plants etc. contaminated by radiocesium are generated from decontamination work in the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident affected area. In present study, the removal experiments of 137Cs in a soil collected from the FDNPP accident affected area were carried out in a lab-scale electrical heating horizontal furnace through thermal treatment with CaCl2 addition over a temperature of 900 - 1300 °C. The results indicated that the average radioactive concentration of 137Cs in the soil was 52.8 Bq/g. The removal ratio of 137Cs in the soil treated at 1300 °C was 96.3 % when 20 % CaCl2 was added. The addition of CaCl2 and CaO mixture exhibited a synergistic effect on the removal of 137Cs, relative to the addition of CaCl2 alone. Accordingly, the addition of CaCl2 or its mixture with CaO during thermal treatment is suggested to remove 137Cs in the soil collected from the FDNPP accident affected area. Additionally, segregation of the soil sample to fine and coarse fraction and then treated individually are also recommended.

Distribution and settling behavior of americium-241 in the tropical East Pacific.

The distribution of the anthropogenic radionuclide 241Am, a decay product of 241Pu discharged from atmospheric tests of nuclear weapons, was investigated to resolve its horizontal and vertical migration in the Tropical East Pacific. We analyzed 241Am concentrations in seawater samples collected in 2003. On comparing the 241Am concentrations with the previously determined concentrations of 239+240Pu in the same samples, the vertical profiles of 241Am were found to be similar to those of 239+240Pu. At some stations, the maximum concentration of 241Am occurred 100-200 m deeper than that of 239+240Pu. The 241Am/239+240Pu ratios in the North Pacific and South Pacific were comparable to one another, and were the typical ratio for the Pacific. The 241Am distribution was influenced by the water mass at depths below 400 m. The 241Am data support the view there is a current flowing at depths of 400-3000 m from the North Pacific through the Equator to the South Pacific. In addition, the 241Am vertical profile was explained by using a 1-D scavenging model that considers the decay of 241Pu and adsorption and scavenging by suspended particles. The different depths for the maximum concentrations of 241Am and 239+240Pu observed at some stations were well explained by the model and by the distribution of CaCO3 particles. The residence time of 241Am in the Pacific was also estimated by using the model.

Vaporization Mechanisms of Water-Insoluble Cs in Ash During Thermal Treatment with Calcium Chloride Addition.

The vaporization mechanisms of water-insoluble Cs in raw ash and Cs-doped ash during thermal treatment with CaCl2 addition was systematically examined in a lab-scale electrical heating furnace over a temperature range of 500-1500 °C. The results indicate that the water-insoluble Cs in the ash was associated with aluminosilicate as pollucite. Addition of 10% CaCl2 caused the maximum vaporization ratio of Cs in the raw ash to reach approximately 80% at temperatures higher than 1200 °C, whereas approximately 95% of Cs was vaporized at temperatures higher than 1300 °C when 30% CaCl2 was added. The formation of an intermediate compound, CsCaCl3, through the chemical reaction of Cs with CaCl2 was responsible for Cs vaporization by means of the subsequent decomposition of this intermediate upon the increase in temperature. The indirect chlorination of Cs by the gaseous chlorine released from the decomposition of CaCl2 was insignificant. A high CaCl2 content in the resulting annealed products with 30% CaCl2 addition delayed the decomposition of CsCaCl3 and thus lowered the Cs vaporization ratio compared to that with 10% CaCl2 addition at 900-1250 °C. Thermal treatment with CaCl2 addition is a proposed method to remove Cs from Cs-contaminated incineration ash.

Pre- and post-accident (129)I and (137)Cs levels, and (129)I/(137)Cs ratios in soil near the Fukushima Dai-ichi Nuclear Power Plant, Japan.

To evaluate the deposition density and extent of subsurface infiltration of (129)I and (137)Cs in the restricted area that was highly contaminated by the accident of Fukushima Dai-ichi Nuclear Power Plant, cumulative inventories of (129)I and (137)Cs, concentrations of (129)I and (137)Cs, and (129)I/(137)Cs ratio in 30-cm-long soil columns were compared with pre-accident levels from the same area. The cores were collected before and after the accident from locations of S-1 (4 km west of FDNPP) and S-2 (8 km west of FDNPP). Deposition densities of (129)I and (137)Cs in the soil following the accident were 0.90-2.33 Bq m(-2) and 0.80-4.04 MBq m(-2), respectively, which were 14-39 and 320-510 times larger than the pre-accident levels of (129)I (59.3-63.3 mBq m(-2)) and (137)Cs (2.51-7.88 kBq m(-2)), respectively. Approximately 90% of accident-derived (129)I and (137)Cs deposited in the 30-cm soil cores was concentrated in the surface layer from 0 to 44-95 kg m(-2) of mass depth (0-4.3-6.2 cm depth) and from 0 to 16-25 kg m(-2) of mass depth (0-1.0-3.1 cm depth), respectively. The relaxation mass depths (h0) of 10.8-11.2 kg m(-2) for (129)I estimated in the previous study were larger than those of 8.1-10.6 kg m(-2) for (137)Cs at both sites, owing to the larger infiltration depth of radioiodine mainly by the gravitational water penetration in the surface soil in our study sites. Approximately 7-9% of the accident-derived (129)I was present in the lower layer from 44 to 100 kg m(-2) (4.3-8.6 cm depth) at S-1, and from 95 to 160 kg m(-2) (6.2-10.2 cm depth) at S-2. Approximately 1% of (137)Cs seems to infiltrate deeper than (129)I in the lower layer at each site in contrast to the surface layer.

Assessment of individual radionuclide distributions from the Fukushima nuclear accident covering central-east Japan.

A tremendous amount of radioactivity was discharged because of the damage to cooling systems of nuclear reactors in the Fukushima No. 1 nuclear power plant in March 2011. Fukushima and its adjacent prefectures were contaminated with fission products from the accident. Here, we show a geographical distribution of radioactive iodine, tellurium, and cesium in the surface soils of central-east Japan as determined by gamma-ray spectrometry. Especially in Fukushima prefecture, contaminated area spreads around Iitate and Naka-Dori for all the radionuclides we measured. Distributions of the radionuclides were affected by the physical state of each nuclide as well as geographical features. Considering meteorological conditions, it is concluded that the radioactive material transported on March 15 was the major contributor to contamination in Fukushima prefecture, whereas the radioactive material transported on March 21 was the major source in Ibaraki, Tochigi, Saitama, and Chiba prefectures and in Tokyo.

Anthropogenic Pu distribution in Tropical East Pacific.

The geographical distribution of the anthropogenic radionuclides (238)Pu and (239+240)Pu in the Tropical East Pacific in 2003 was studied from the viewpoint of material migration. We measured the contents of Pu isotopes in seawater and in sediment from the sea bottom. The distributions of Pu isotopes, together with those of coexisting nitrate and phosphate species and dissolved oxygen, are discussed in relation to the potential temperature and potential density (sigma-θ). The Pu contents in sediment samples were compared with those in the seawater. Horizontal migration across the Equator from north to south was investigated at depths down to ~800m in the eastern Pacific. The Pu distribution at 0-400m correlated well with the distribution of potential temperature. Maximum Pu levels were observed in the subsurface layer at 600-800m, corresponding to the depth where sigma-θ≈27.0. It is suggested that the Pu distribution depends on the structure of the water mass and the particular temperature and salinity. The water column/sediment column inventory ratio and the vertical distribution of Pu may reflect the efficiency of scavenging in the relevant water areas.

Development of an online preparation system for multitracer solutions.

We have developed a new target-irradiation system for the online preparation of multitracer solutions, where the nuclear-reaction products recoiling out of the target are directly implanted in a solvent as a liquid catcher. A rapid online transportation of the solution has enabled highly efficient recovery of the multitracer solutions having even short-lived radioactive isotopes without any chemical treatments. It has been suggested that the collection efficiency depends on the chemical properties of the recoil elements.

Fluoride complexation of element 104, rutherfordium.

Fluoride complexation of element 104, rutherfordium (Rf), produced in the 248Cm(18O,5n)261Rf reaction has been studied by anion-exchange chromatography on an atom-at-a-time scale. The anion-exchange chromatographic behavior of Rf was investigated in 1.9-13.9 M hydrofluoric acid together with those of the group-4 elements Zr and Hf produced in the 18O-induced reactions on Ge and Gd targets, respectively. It was found that the adsorption behavior of Rf on anion-exchange resin is quite different from those of Zr and Hf, suggesting the influence of relativistic effects on the fluoride complexation of Rf.