A quantitative description of the compatibility of technetium-selective chromatographic technetium-99m separation with low specific activity molybdenum-99.

Technetium-99m generators employing a technetium-selective stationary phase are a chromatographic instrument developed for use with 99Mo having low specific activity (LSA); particularly, 99Mo produced by electron accelerators. This paper presents a mathematical description of technetium-selective chromatographic (TSC) 99mTc separation and analyzes its compatibility with LSA 99Mo. We developed a theoretical formula for TSC 99mTc separation by discretizing its pertechnetate selectivity, and validated it using an electron linear accelerator and activated carbon-based TSC (AC-TSC) 99mTc generators. We confirmed that the activity concentration of 99mTc obtained from a TSC 99mTc generator can be calculated directly from its input 99Mo activity regardless of the 99Mo specific activity. The formula corroborates that TSC 99mTc separation is compatible with LSA 99Mo, and has a practical application in estimating the number of TSC 99mTc generators required for 99mTc demand of interest.

Coprecipitation with samarium hydroxide using multitracer produced through neutron-induced fission of 235U toward chemical study of heavy elements.

For new chemical studies on heavy elements, we previously investigated the coprecipitation behaviors with samarium hydroxide for various elements. Herein, we report the coprecipitation experiment using multitracer produced by neutron-induced fission of 235U. The coprecipitation behaviors of 10 elements were investigated: new data were obtained for Sr, Ru, I, Pm, and Np. The present results support the previously obtained conclusion that the hydroxide precipitation properties of various elements can be qualitatively investigated through their coprecipitation behaviors.

Co-precipitation behaviour of single atoms of rutherfordium in basic solutions.

All superheavy elements (SHEs), with atomic numbers (Z) ≥104, have been artificially synthesized one atom at a time and their chemical properties are largely unknown. Because these heavy nuclei have short lifetimes as well as extremely low production rates, chemical experiments need to be carried out on single atoms and have mostly been limited to adsorption and extraction. We have now investigated the precipitation properties of the SHE Rf (Z = 104). A co-precipitation method with samarium hydroxide had previously established that the co-precipitation behaviour of a range of elements reflected these elements' tendency to form hydroxide precipitates and/or ammine complex ions. Here we investigated co-precipitation of Rf in basic solutions containing NH3 or NaOH. Comparisons between the behaviour of Rf with that of Zr and Hf (lighter homologues of Rf) and actinide Th (a pseudo-homologue of Rf) showed that Rf does not coordinate strongly with NH3, but forms a hydroxide (co)precipitate that is expected to be Rf(OH)4.

Creation of Mo/Tc@C60 and Au@C60 and molecular-dynamics simulations.

The formation of middle- and/or high-weight atom (Mo, Au)-incorporated fullerenes was investigated using radionuclides produced by nuclear reactions. From the trace radioactivities of 99Mo/99mTc or 194Au after high-performance liquid chromatography, it was found that the formation of endohedral and/or heterofullerene fullerenes in 99Mo/99mTc and 194Au atoms could occur by a recoil process following the nuclear reactions. Furthermore, the 99mTc (and 194Au) atoms recoiled against ß-decay remained present inside these cages. To confirm the produced materials experimentally, ab initio molecular dynamics (MD) simulations based on an all-electron mixed-basis approach were performed. The possibility of the formation of endohedral fullerenes containing Mo/Tc and Au atoms is verified; here, the formation of heterofullerenes is excluded by MD simulations. These findings suggest that radionuclides stably encapsulated by fullerenes could potentially play a valuable role in diagnostic nuclear medicine.

Isolation, characterization and source analysis of radiocaesium micro-particles in soil sample collected from vicinity of Fukushima Dai-ichi nuclear power plant.

Radioactive caesium was released during the accident of Fukushima Dai-ichi nuclear power plant (FDNPP) into the surrounding environment. In the current work, radiocaesium micro-particles (CsMPs) and radiocaesium-rich soil particles were selectively separated from soil particles as well as from each other using autoradiography-based procedure. The applied separation scheme is based on water dilution followed by drying of the soil sample prior to imaging plate autoradiography. The SEM/EDS investigation of the individual CsMPs showed that these particles have a silicate glass structure and vary in shape with a diameter less than 10 µm. For the first time, a two-stage formation mechanism was suggested for a CsMP based on shape and structure heterogeneity of its two parts. Perfect spherical core might be formed in the first stage with a remarkable lower content of Al, and relatively higher concentrations of Si and K than an outer angulated structure, which might be attached to the core sphere during a late stage. The radiocaesium-rich soil particles have bigger size than CsMPs and have a plate-like structure with cleavages inside the grains, which suggest that these particles might be a weathered biotite. The average radioactivity ratio of 134Cs/137Cs (dated March 11, 2011) in the investigated particles was found to be 1.05 ± 0.01, which confirmed that the radiocaesium in CsMPs and in the contaminated soil particles has the same source of origin, which could be unite 3 of FDNPP.

Use of different surface covering materials to enhance removal of radiocaesium in plants and upper soil from orchards in Fukushima prefecture.

The effectiveness of a decontamination methodology whereby herbaceous plants were grown through different materials covering the soil surface followed by subsequent removal of the material, associated plant tissues and attached soil on 137Cs removal from soil was evaluated. Revegetation netting sown with Kentucky bluegrass and white clover had a high effectiveness in 137Cs removal when rolling up the plants, roots, and rhizosphere soil approximately 6 months after sowing. The removal rate was lower when there was higher 137Cs vertical migration down the soil profile. The maximum removal effectiveness of 93.1% was observed by rolling up fertilized Kentucky bluegrass with a well-developed root mat without netting, indicating that applying nutrients to encourage the development of roots or root mats in the 3 cm topsoil rhizosphere is an efficient technology to increase the decontamination effect of plant removal in orchards. Netting and weeding were able to remove up to 80% of 137Cs in the soil without the use of heavy machinery. There was a significant relationship between the removal ratio and the removed soil weight per area. Using the relationship on the site below the canopy, removal of 14.3 kg m-2 DW soil would achieve a removal ratio of 80%. The effectiveness of the technique will decrease with time as radiocaesium migrates down the soil profile but this would be expected to occur slowly in many soils.

Desorption of radioactive cesium by seawater from the suspended particles in river water.

In 2011, the accident at the Fukushima-Daiichi nuclear power plant dispersed radioactive cesium throughout the environment, contaminating the land, rivers, and sea. Suspended particles containing clay minerals are the transportation medium for radioactive cesium from rivers to the ocean because cesium is strongly adsorbed between the layers of clay minerals, forming inner sphere complexes. In this study, the adsorption and desorption behaviors of radioactive cesium from suspended clay particles in river water have been investigated. The radioactive cesium adsorption and desorption experiments were performed with two kinds of suspended particulate using a batch method with 137Cs tracers. In the cesium adsorption treatment performed before the desorption experiments, simulated river water having a total cesium concentration ([133+137Cs+]total) of 1.3 nM (10-9 mol/L) was used. The desorption experiments were mainly conducted at a solid-to-liquid ratio of 0.17 g/L. The desorption agents were natural seawater collected at 10 km north of the Fukushima-Daiichi nuclear power plant, artificial seawater, solutions of NaCl, KCl, NH4Cl, and 133CsCl, and ultrapure water. The desorption behavior, which depends on the preloaded cesium concentration in the suspended particles, was also investigated. Based on the cesium desorption experiments using suspended particles, which contained about 1000 ng/g loaded cesium, the order of cesium desorption ratios for each desorption agent was determined as 1 M NaCl (80%) > 470 mM NaCl (65%) > 1 M KCl (30%) ≈ seawater (natural seawater and Daigo artificial seawater) > 1 M NH4Cl (20%) > 1 M 133CsCl (15%) ≫ ultrapure water (2%). Moreover, an interesting result was obtained: The desorption ratio in the 470 mM NaCl solution was much higher than that in seawater, even though the Na+ concentrations were identical. These results indicate that the cesium desorption mechanism is not a simple ion exchange reaction but is strongly related to structural changes in the clay minerals in the suspended particles. Hydrated Na+ ions expand the interlayer distance of the clay minerals, resulting in the facile desorption of cesium; in contrast, dehydrated K+ ions reduce the interlayer distance and inhibit the desorption of cesium. In conclusion, the desorption of cesium from the suspended particles is controlled by the presence of sodium and potassium ions and the preloaded cesium concentration in the suspended particles.