Accurate determination of chlorine, bromine, and iodine in sedimentary rock reference samples by radiochemical neutron activation analysis and a detailed comparison with inductively coupled plasma mass spectrometry literature data.

Trace amounts of three halogens (chlorine, bromine, and iodine) were determined using radiochemical neutron activation analysis (RNAA) for nine sedimentary rocks and three rhyolite samples. To obtain high-quality analytical data, the radiochemical procedure of RNAA was improved by lowering the background in gamma-ray spectrometry and completing the chemical procedure more rapidly than in conventional procedures. A comparison of the RNAA data of Br and I with corresponding inductively coupled plasma mass spectrometry (ICPMS) literature data revealed that the values obtained by ICPMS coupled with pyrohydrolysis preconcentration were systematically lower than the RNAA data for some reference samples, suggesting that the quantitative collection of Br and I cannot always be achieved by the pyrohydrolysis for some solid samples. The RNAA data of three halogens can classify sedimentary rock reference samples into two groups (the samples from inland water and those from seawater), implying the geochemical significance of halogen data.

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.

Noble gases and nitrogen in samples of asteroid Ryugu record its volatile sources and recent surface evolution.

The near-Earth carbonaceous asteroid (162173) Ryugu is expected to contain volatile chemical species that could provide information on the origin of Earth's volatiles. Samples of Ryugu were retrieved by the Hayabusa2 spacecraft. We measured noble gas and nitrogen isotopes in Ryugu samples and found that they are dominated by presolar and primordial components, incorporated during Solar System formation. Noble gas concentrations are higher than those in Ivuna-type carbonaceous (CI) chondrite meteorites. Several host phases of isotopically distinct nitrogen have different abundances among the samples. Our measurements support a close relationship between Ryugu and CI chondrites. Noble gases produced by galactic cosmic rays, indicating a ~5 million year exposure, and from implanted solar wind record the recent irradiation history of Ryugu after it migrated to its current orbit.

First asteroid gas sample delivered by the Hayabusa2 mission: A treasure box from Ryugu.

The Hayabusa2 spacecraft returned to Earth from the asteroid 162173 Ryugu on 6 December 2020. One day after the recovery, the gas species retained in the sample container were extracted and measured on-site and stored in gas collection bottles. The container gas consists of helium and neon with an extraterrestrial 3He/4He and 20Ne/22Ne ratios, along with some contaminant terrestrial atmospheric gases. A mixture of solar and Earth's atmospheric gas is the best explanation for the container gas composition. Fragmentation of Ryugu grains within the sample container is discussed on the basis of the estimated amount of indigenous He and the size distribution of the recovered Ryugu grains. This is the first successful return of gas species from a near-Earth asteroid.

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.