Correlations for the specific heat capacity of (UPu)GdO derived from molecular dynamics

Galvin, C. O. T.*; Machida, Masahiko; Nakamura, Hiroki; Andersson, D. A.*; Cooper, M. W. D.*

Journal of Nuclear Materials, 572, p.154028_1 - 154028_8, 2022/12

https://doi.org/10.1016/j.jnucmat.2022.154028

UO is the primary conventional fuel used in most nuclear reactors with GdO commonly added as a burnable absorber to produce a more level power distribution in the reactor core at the beginning of operation. It can also be mixed with other actinide oxides to produce mixed oxide (MOx) fuel. In this study, molecular dynamics simulations were used to predict the specific heat capacity of Gd-doped PuO, UO and (U,Pu)O MOx accommodating Gd substituted at cation sites via two charge compensation mechanisms - oxygen vacancy formation and the oxidation of U to U. The specific heat capacity values for PuO and UO are in good agreement with other studies showing a distinct peak at high temperatures - above 1800 K. As Gd is added, the peak height reduces for each composition considered. An analytical fit was applied to the data where Gd was fully charge compensated by either oxygen vacancies or U. The expression was then validated by predicting the specific heat capacity for three compositions of (UPu)GdO containing both oxygen vacancies and U, and compared to molecular dynamics data.

Accumulation mechanisms of radiocaesium within lichen thallus tissues determined by means of microscale localisation observation

Dohi, Terumi; Iijima, Kazuki; Machida, Masahiko; Suno, Hiroya*; Omura, Yoshihito*; Fujiwara, Kenso; Kimura, Shigeru*; Kanno, Futoshi*

PLOS ONE (Internet), 17(7), p.e0271035_1 - e0271035_21, 2022/07

https://doi.org/10.1371/journal.pone.0271035

Defect equilibria and thermophysical properties of CeO based on experimental data and density functional theory calculation result

Watanabe, Masashi; Nakamura, Hiroki; Suzuki, Kiichi; Machida, Masahiko; Kato, Masato

Journal of the American Ceramic Society, 105(3), p.2248 - 2257, 2022/03

https://doi.org/10.1111/jace.18249

Properties of CeO were evaluated by DFT simulation to determine band gap, Frenkel defect formation energy and defect migration energy. Band gap and Frenkel defect formation energy were used to analyze defect equilibria. Oxygen partial pressure dependence of defect equilibria was evaluated based on oxygen potential experimental data and DFT calculation, and a Brouwer diagram was derived. The defect formation energies, including Frenkel defect, electron-hole pair and so on, were determined and used to evaluate the properties, including oxygen diffusion coefficients, electrical conduction, heat capacity and thermal conductivity. Mechanisms of various properties were discussed for a deeper understanding based on defect chemistry, and the relationship among properties were systematically described.

Development and evaluation of XRF imaging instrument for moving objects

Fuchita, Tomoki*; Urata, Taisei*; Matsuyama, Tsugufumi*; Murakami, Masashi; Yoshida, Yukihiko; Ueda, Akihiko; Machida, Masahiko; Sasaki, Toshiki; Tsuji, Koichi*

X-sen Bunseki No Shimpo, 53, p.77 - 87, 2022/03

X-ray fluorescence (XRF) analysis is an analytical method to obtain elemental information by detecting fluorescence X-rays emitted from a sample irradiated with X-rays. It is possible to obtain two-dimensional elemental distribution images by scanning a sample with micro X-ray beam. In this study, we developed an XRF analytical instrument to rapidly obtain the elemental distributions for moving samples on a belt conveyor by applying the micro XRF technique. X-rays were widely irradiated to the belt conveyor. The elemental distributions were measured by scanning an X-ray detector, crossing above the belt conveyor. A collimator was attached to the top of the detector to limit the analyzing area. Both detection limit and spatial resolutions for moving directions of the detector and the belt conveyor were evaluated. Finally, it was demonstrated that the multi-elemental imaging was possible with the developed XRF instrument.

Estimation of temporal variation of tritium inventory discharged from the port of Fukushima Dai-ichi Nuclear Power Plant; Analysis of the temporal variation and comparison with released tritium inventories from Japan and world major nuclear facilities

Machida, Masahiko; Iwata, Ayako; Yamada, Susumu; Otosaka, Shigeyoshi*; Kobayashi, Takuya; Funasaka, Hideyuki*; Morita, Takami*

Journal of Nuclear Science and Technology, 19 Pages, 2022/00

https://doi.org/10.1080/00223131.2022.2093800

We estimate monthly discharge inventory of tritium from the port of Fukushima Dai-ichi Nuclear Power Plant (1F) from Jun. 2013 to Mar. 2020 using the Voronoi tessellation scheme, following the tritium monitoring results inside the port started in Jun. 2013. As for the missing period from the first month of 1F accident, Apr. 2011 to May 2013, we calculate the tritium discharge inventory by utilizing the concentration ratio of tritium to Cs in stagnant contaminant water during the initial direct run-off period until Jun. 2011 and the discharge inventory correlation between tritium and Cs for the next-unknown continuous-discharge period from Jul. 2011 to May 2013. From all the estimated results over 9 years, we find that the monthly discharge inventory sharply dropped immediately after closing the seaside impermeable wall in Oct. 2015 and consequently coincided well with the sum of input inventories of drainage water and subdrain etc. purified water into the port. By comparing the above estimated results with those in the normal operation period before the accident, we point out that the discharge inventory from 1F port after the accident is not so large. Even the estimation value for the accident year 2011 is found to be comparable to the maximum of operating pressurized water reactors releasing relatively large inventories in the order. At the national level, the total domestic release inventory in Japan significantly decreased after the accident owing to the operational shutdown of most plants. Furthermore, the total Japanese discharge inventory including 1F are found to be minor compared with those of nuclear reprocessing plants and heavy-water reactors on a worldwide level. From the above results, we suggest that various scenarios can be openly discussed regarding the management of tritium stored inside 1F with the help of the present estimated data and its comparison with the past discharge inventory as well as those of other nuclear facilities.

Hydration structures of barium ions; molecular dynamics simulations using the SCAN meta-GGA density functional and EXAFS spectroscopy studies

Yamaguchi, Akiko; Kobayashi, Keita; Takahashi, Yoshio*; Machida, Masahiko; Okumura, Masahiko

Chemical Physics Letters, 780, p.138945_1 - 138945_5, 2021/10

https://doi.org/10.1016/j.cplett.2021.138945

no abstracts in English

Present status and future perspective of R&D for 3D-ADRES (3-Dimensional Air Dose Rate Evaluation System); Evaluation scheme for air dose rate distributions in city and forest areas towards Fukushima's revitalization

Kim, M.; Malins, A.; Machida, Masahiko; Yoshimura, Kazuya; Saito, Kimiaki; Yoshida, Hiroko*; Yanagi, Hideaki*; Yoshida, Toru*; Hasegawa, Yukihiro*

RIST News, (67), p.3 - 15, 2021/09

https://www.rist.or.jp/rnews/67/ristnews_67.html

no abstracts in English

Quantum chemical calculation studies toward microscopic understanding of retention mechanism of Cs radioisotopes and other alkali metals in lichens

Suno, Hiroya; Machida, Masahiko; Dohi, Terumi; Omura, Yoshihito*

Scientific Reports (Internet), 11(1), p.8228_1 - 8228_13, 2021/04

https://doi.org/10.1038/s41598-021-87617-w

We evaluate stability of caesium (Cs) and other alkali-metal cation complexes of lichen metabolites in both gas and aqueous phases to discuss why lichens can retain radioactive Cs in the thalli over several years. We focus on oxalic acid, (+)-usnic acid, atranorin, lecanoric acid, and protocetraric acid, which are common metabolite substances in various lichens including, e.g., and retaining Cs in Fukushima, Japan. By performing quantum chemical calculations, their gas-phase complexation energies and aqueous-solution complexation free energies with alkali-metal cations are computed for their neutral and deprotonated cases. Consequently, all the molecules are found to energetically favor cation complexations and the preference order is LiNaKRbCs for all conditions, indicating no specific Cs selectivity but strong binding with all alkali cations. Comparing complexation stabilities among these metabolites, lecanoric and protocetraric acids seen in medullary layer are found to keep higher affinity in their neutral case, while (+)-usnic acid and atranorin in upper cortex exhibit rather strong affinity only in deprotonated cases through forming stable six atoms' ring containing alkali cation chelated by two oxygens. These results suggest that the medullary layer can catch all alkali cations in a wide pH range around the physiological one, while the upper cortex can effectively block penetration of metal ions when the metal stress grows. Such insights highlight a physiological role of metabolites like blocking of metal-cation migrations into intracellular tissues, and explain long-term retention of alkali cations including Cs in lichens containing enough such metabolites to bind them.

Machine learning potentials for tobermorite minerals

Kobayashi, Keita; Nakamura, Hiroki; Yamaguchi, Akiko; Itakura, Mitsuhiro; Machida, Masahiko; Okumura, Masahiko

Computational Materials Science, 188, p.110173_1 - 110173_14, 2021/02

https://doi.org/10.1016/j.commatsci.2020.110173

no abstracts in English

Homogeneity of neutron transmission imaging over a large sensitive area with a four-channel superconducting detector

Vu, TheDang; Shishido, Hiroaki*; Kojima, Kenji M*; Koyama, Tomio*; Oikawa, Kenichi; Harada, Masahide; Miyajima, Shigeyuki*; Oku, Takayuki; Soyama, Kazuhiko; Aizawa, Kazuya; et al.

Superconductor Science and Technology, 34(1), p.015010_1 - 015010_10, 2021/01

https://doi.org/10.1088/1361-6668/abc2af