Behavior of light elements in iron-silicate-water-sulfur system during early Earth's evolution

Iizuka, Riko*; Goto, Hirotada*; Shito, Chikara*; Fukuyama, Ko*; Mori, Yuichiro*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; Kagi, Hiroyuki*

Scientific Reports (Internet), 11(1), p.12632_1 - 12632_10, 2021/06

https://doi.org/10.1038/s41598-021-91801-3

The Earth's core consist of Fe-Ni alloy with some light elements (H, C, O, Si, S etc.). Hydrogen (H) is the most abundant element in the universe and one of the promising candidates. In this study, we have investigated the effects of sulfur(S) on hydrogenation of iron-hydrous silicate system containing saturated water in the ideal composition of the primitive Earth. We observed a series of phase transitions of Fe, dehydration of the hydrous mineral, and formation of olivine and enstatite with increasing temperature. The FeS formed as the coexisting phase of Fe under high-pressure and temperature condition, but its unit cell volume did not increase, suggesting that FeS is hardly hydrogenated. Recovered samples exhibited that H and S can be incorporated into solid Fe, which lowers the melting temperature as Fe(H)-FeS system. No detection of other light elements (C, O, Si) in solid Fe suggests that they dissolve into molten iron hydride and/or FeS in the later process of Earth's core-mantle differentiation.

Neutron diffraction study of hydrogen site occupancy in FeSi at 14.7 GPa and 800 K

Mori, Yuichiro*; Kagi, Hiroyuki*; Kakizawa, Sho*; Komatsu, Kazuki*; Shito, Chikara*; Iizuka, Riko*; Aoki, Katsutoshi*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; et al.

Journal of Mineralogical and Petrological Sciences, 116(6), p.309 - 313, 2021/00

https://doi.org/10.2465/jmps.210825

The Earth's core is believed to contain some light elements because it is 10% less dense than pure Fe under the corresponding pressure and temperature conditions. Hydrogen, a promising candidate among light elements, has phase relations and physical properties that have been investigated mainly for the Fe-H system. This study specifically examined an Fe-Si-H system using in-situ neutron diffraction experiments to investigate the site occupancy of deuterium of hcp-FezSi hydride at 14.7 GPa and 800 K. Results of Rietveld refinement indicate hcp-FeSi hydride as having deuterium (D) occupancy of 0.24(2) exclusively at the interstitial octahedral site in the hcp lattice. The effect on the site occupancy of D by addition of 2.6 wt% Si into Fe (FeSi) was negligible compared to results obtained from an earlier study of an Fe-D system (Machida et al., 2019).

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; Dllmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.

EPJ Web of Conferences, 131, p.07005_1 - 07005_7, 2016/12

https://doi.org/10.1051/epjconf/201613107005

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO). Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO), W(CO), and Sg(CO).

Fluorido complex formation of element 104, rutherfordium (Rf)

Ishii, Yasuo; Toyoshima, Atsushi; Tsukada, Kazuaki; Asai, Masato; Li, Z.*; Nagame, Yuichiro; Miyashita, Sunao*; Mori, Tomotaka*; Suganuma, Hideo*; Haba, Hiromitsu*; et al.

Bulletin of the Chemical Society of Japan, 84(9), p.903 - 911, 2011/09

https://doi.org/10.1246/bcsj.20110126

The cation-exchange behavior of element 104, rutherfordium (Rf), was investigated together with its lighter group-4 homologues Zr and Hf, and the tetravalent pseudo-homologue Th in HF/HNO mixed solution. The results demonstrate that distribution coefficients () of Rf in HF/0.10 M HNO decrease with increasing concentration of the fluoride ion [F], indicating the consecutive formation of fluorido complexes of Rf. We also measured the values of Rf and the homologues as a function of the hydrogen ion concentration [H]. The log values decrease linearly with an increase of log [H] with slopes between -2.1 and -2.5. This indicates that these elements are likely to form the same chemical compounds: mixture of [MF] and [MF] (M = Rf, Zr, Hf and Th) in the studied solution. It is also ascertained that sequence in the fluoride complex formation is Zr Hf Rf Th.

Fluoride complexation of element 104, rutherfordium (Rf), investigated by cation-exchange chromatography

Ishii, Yasuo; Toyoshima, Atsushi; Tsukada, Kazuaki; Asai, Masato; Tome, Hayato; Nishinaka, Ichiro; Nagame, Yuichiro; Miyashita, Sunao*; Mori, Tomotaka*; Suganuma, Hideo*; et al.

Chemistry Letters, 37(3), p.288 - 289, 2008/03

https://doi.org/10.1246/cl.2008.288

We have investigated cation-exchange behavior of Rf together with the lighter homologues of the group-4 elements Zr and Hf, and the tetravalent pseudo-homologue Th, in HF/HNO solution using Automated Ion exchange separation apparatus coupled with the Detection system for Alpha spectroscopy (AIDA). The values of Zr, Hf, Th and Rf in HF/0.1 M HNO were decreased with increasing the concentration of the fluoride ion [F], indicating the formation of the fluoride complexes. The sequence of the fluoride complexation strength is Zr Hf Rf Th.

Development of water radiolysis code for the JMTR IASCC test loop

Hanawa, Satoshi; Sato, Tomonori; Mori, Yuichiro; Ogiyanagi, Jin; Kaji, Yoshiyuki; Uchida, Shunsuke*

Proceedings of 14th International Conference on Nuclear Engineering (ICONE-14) (CD-ROM), 9 Pages, 2006/07

no abstracts in English

Design study of water chemistry control system for IASCC irradiation test

Mori, Yuichiro*; Ide, Hiroshi; Nabeya, Hideaki; Tsukada, Takashi

JAERI-Tech 2002-003, 32 Pages, 2002/02

JAERI-Tech-2002-003.pdf:2.24MB

In relation to the aging of Light Water Reactor (LWR), the Irradiation Assisted Stress Corrosion Cracking (IASCC) has been regarded as a significant and urgent issue for the reliability of in-core components of LWR, and the irradiation research on the IASCC is now under schedule. With the progress of the irradiation research on reactor materials, well-controlled environment conditions during irradiation testing are required. Especially for irradiation testing of IASCC studies, water chemistry control is essential in addition to the control of neutron fluence and irradiation temperature.According to these requirements, at the Japan Atomic Energy Research Institute (JAERI), an irradiation testing facility that simulates in-core environment of Boiling Water Reactor (BWR) has been designed to be installed in the Japan Materials Testing Reactor (JMTR). This facility is composed of the Saturated Temperature Capsules (SATCAP) that are installed into the JMTR's core to irradiate material specimens, the Water Control Unit that is able to supply high-temperature and high-pressure chemical controlled water to SATCAP, and other components.This report describes the design study of water chemistry control system of the Water Control Unit. The design work has been performed in the fiscal year 1999.

Water chemistry in JMTR in-pile loop, 2; Calculation result of water chemistry in the loop

Mori, Yuichiro*; Hanawa, Satoshi; Sato, Tomonori; Ogiyanagi, Jin; Nabeya, Hideaki; Uchida, Shunsuke*

no journal, , 

no abstracts in English

Cation-exchange behavior of Rf in HNO/HF mixed solution, 2

Ishii, Yasuo; Tome, Hayato; Toyoshima, Atsushi; Asai, Masato; Nishinaka, Ichiro; Tsukada, Kazuaki; Nagame, Yuichiro; Miyashita, Sunao*; Mori, Tomotaka*; Suganuma, Hideo*; et al.

no journal, , 

Chemical properties of rutherfordium (Rf, the element 104) in HNO/HF mixed solutions have been investigated using cation-exchange chromatography. Distribution coefficients of Rf on the cation-exchange resin as a function of hydrofluoric-acid and nitric-acid concentrations have been measured precisely, and it was found that the strength of the fluoride complex formation of Rf is much weaker than those of lighter group 4 homologs Zr and Hf. The same result was obtained through the anion-exchange chromatography. These results enabled us to quantitatively account for the fluoride complexation of Rf.

Electronic structure of CeIrSi studied by angle-resolved resonant photoemission spectroscopy

Toshimitsu, Takafumi; Okochi, Takuo; Yasui, Akira; Kobayashi, Masaki*; Takeda, Yukiharu; Okane, Tetsuo; Saito, Yuji; Fujimori, Atsushi*; Yamagami, Hiroshi*; Miyauchi, Yuichiro*; et al.

no journal, , 

We performed angle-resolved resonant photoemission spectroscopy on CeIrSi. CeIrSi is said to be the superconductor which lacks inversion symmetry and therefore the measurements of electronic conductivity, magnetoresistance, dHvA, and so on, have been made on so far. In this study, we observed extremely clear 4 derived band dispersions and Fermi surfaces. By these obtained profiles and comparison with those predicted by LDA calculation, Ce 4 electrons in CeIrSi have relatively itinerant electronic states.