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Journal Articles

Oxygen self-diffusion in near stoichiometric (U,Pu)O$$_{2}$$ at high temperatures of 1673-1873 K

Watanabe, Masashi; Kato, Masato; Sunaoshi, Takeo*

Journal of Nuclear Materials, 542, p.152472_1 - 152472_7, 2020/12

 Times Cited Count:0 Percentile:0.01(Materials Science, Multidisciplinary)

The oxygen self-diffusion coefficients in near stoichiometric (U,Pu)O$$_{2}$$ at high temperatures were successfully measured by thermogravimetry combined with the oxygen isotope exchange method. The activation energy for oxygen diffusion in the stoichiometric composition of (U,Pu)O$$_{2}$$ was evaluated from experimental data, and the value was determined to be 248 kJ/mol. In addition, the defect migration energies of (U,Pu)O$$_{2 pm x}$$ were derived, and the oxygen self-diffusion coefficients were evaluated using these. As a result, good agreement was found between the experimental data and the oxygen self-diffusion coefficients calculated using the defect migration energies.

Journal Articles

Complexation and bonding studies on [Ru(NO)(H$$_{2}$$O)$$_{5}$$]$$^{3+}$$ with nitrate ions by using density functional theory calculation

Kato, Akane*; Kaneko, Masashi; Nakashima, Satoru*

RSC Advances (Internet), 10(41), p.24434 - 24443, 2020/06

 Times Cited Count:5 Percentile:62.74(Chemistry, Multidisciplinary)

Complexation reactions of ruthenium-nitrosyl complexes in HNO$$_{3}$$ solution were investigated by density functional theory (DFT) calculations in order to predict the stability of Ru species in high-level radioactive liquid waste (HLLW) solution. Equilibrium structure of [Ru(NO)(NO$$_{3}$$)$$_{3}$$(H$$_{2}$$O)$$_{2}$$] obtained by DFT calculations reproduced the experimental Ru-ligands bond lengths and IR frequencies reported previously. Comparison of the Gibbs energies among the geometrical isomers revealed that the complexation reactions of the ruthenium-nitrosyl complexes with NO$$_{3}$$$$^{-}$$ proceed via the NO$$_{3}$$$$^{-}$$ coordination to the equatorial plane toward the Ru-NO axis. We also estimated Gibbs energy differences on the stepwise complexation reactions to succeed in reproducing the fraction of Ru-NO species in 6 M HNO$$_{3}$$ solution, such as in HLLW, by considering the association energy between the Ru-NO species and the substituting ligands. Electron density analyses of the complexes indicated that the strength of the Ru-ligands coordination bonds depends on the stability of the Ru species and the Ru complex without NO$$_{3}$$$$^{-}$$ at the axial position is more stable than that wit NO$$_{3}$$$$^{-}$$, which might attribute to the difference in the trans influence between H$$_{2}$$O and NO$$_{3}$$$$^{-}$$. Finally, we demonstrated the complexation kinetics in the reactions $$x = 1 rightarrow x = 2$$. The present study is expected to enable us to model the precise complexation reactions of platinum-group metals in HNO$$_{3}$$ solution.

Journal Articles

Physical properties of non-stoichiometric (U,Pu)O$$_{2}$$

Watanabe, Masashi; Matsumoto, Taku; Hiroka, Shun; Morimoto, Kyoichi; Kato, Masato

2018 GIF Symposium Proceedings (Internet), p.315 - 320, 2020/05

Recently, a research group studying at Plutonium Fuel Development Facility (PFDF) in Japan Atomic Energy Agency has systematically measured vast amounts of physical properties in the non-stoichiometric (U, Pu)O$$_{2}$$. Lattice parameter, elastic modulus, thermal expansion, oxygen potential, oxygen chemical diffusion coefficient and thermal conductivity were successfully measured as function of Pu content, O/M ratio and temperature, and the effects of Pu content and O/M ratio on their physical properties were evaluated. In this work, those experimental data are reviewed, and latest experimental data set on the non-stoichiometric (U, Pu)O$$_{2}$$ are presented. The data set would be available in development of a fuel performance code.

Journal Articles

Upgrade of the 3-MeV linac for testing of accelerator components at J-PARC

Kondo, Yasuhiro; Hirano, Koichiro; Ito, Takashi; Kikuzawa, Nobuhiro; Kitamura, Ryo; Morishita, Takatoshi; Oguri, Hidetomo; Okoshi, Kiyonori; Shinozaki, Shinichi; Shinto, Katsuhiro; et al.

Journal of Physics; Conference Series, 1350, p.012077_1 - 012077_7, 2019/12

 Times Cited Count:0 Percentile:0.07

We have upgraded a 3-MeV linac at J-PARC. The ion source is same as the J-PARC linac's, and the old 30-mA RFQ is replaced by a spare 50-mA RFQ, therefore, the beam energy is 3 MeV and the nominal beam current is 50 mA. The main purpose of this system is to test the spare RFQ, but also used for testing of various components required in order to keep the stable operation of the J-PARC accelerator. The accelerator has been already commissioned, and measurement programs have been started. In this paper, present status of this 3-MeV linac is presented.

Journal Articles

Density Functional Theory (DFT)-based bonding analysis correlates ligand field strength with $$^{99}$$Ru M$"o$ssbauer parameters of ruthenium-nitrosyl complexes

Kaneko, Masashi; Kato, Akane*; Nakashima, Satoru*; Kitatsuji, Yoshihiro

Inorganic Chemistry, 58(20), p.14024 - 14033, 2019/10

 Times Cited Count:7 Percentile:62.61(Chemistry, Inorganic & Nuclear)

We applied density functional theory calculations to ruthenium-nitrosyl complexes, which are known to exist in high-level radioactive waste, to give a theoretical correlation between $$^{99}$$Ru M$"o$ssbauer spectroscopic parameters ($$delta$$ and $$Delta$$$$E_{rm Q}$$) and ligand field strength ($$Delta$$$$_{rm o}$$) for the first time. The structures of the series of complexes, [Ru(NO)L$$_{5}$$] (L = Br$$^{-}$$, Cl$$^{-}$$, NH$$_{3}$$, CN$$^{-}$$), were modeled based on the corresponding single-crystal X-ray coordinates. The comparisons of the geometries and total energies between the different spin states suggested that the singlet spin state of [Ru(II)(NO$$^{+}$$)L$$_{5}$$] complexes were the most stable. The calculated results of both the $$delta$$ and $$Delta$$$$E_{rm Q}$$ values reproduced the experimental results by reported previously and increased in the order of L = Br$$^{-}$$, Cl$$^{-}$$, NH$$_{3}$$, CN$$^{-}$$. Finally, we estimated the ligand field strength ($$Delta$$$$_{rm o}$$) based on molecular orbitals, assuming C$$_{rm 4v}$$ symmetry and showed the increase of $$Delta$$$$_{rm o}$$ values in that order, being consistent with well-known spectrochemical series of ligands. The increase attributes to the strengthening of the abilities of $$sigma$$-donor and $$pi$$-acceptor of the L-ligands to the Ru atom, resulting in the increase of the $$delta$$ values.

Journal Articles

Modeling and simulation of redistribution of oxygen-to-metal ratio in MOX

Hiroka, Shun; Kato, Masato; Watanabe, Masashi

Transactions of the American Nuclear Society, 118, p.1624 - 1626, 2018/06

This study suggested the time development of oxygen-to-metal ratio (O/M) redistribution model with oxygen-related properties in MOX. Irradiation simulation including the suggested O/M redistribution and pore migration with vaporization-condensation model which bares density redistribution was demonstrated. The simulation results showed that O/M redistribution proceeded at lower temperature than density redistribution, which indicated that oxygen diffusion got influential at lower temperature than vaporization-condensation of MOX. Another find was that O/M redistribution was very slow at the surface because temperature kept low. However, near the surface (inside from the surface) where the temperature exceeded 1000 K, O/M redistribution was rather recognizable with oxygen flown from inner region to the near-surface. The results will be evaluated by comparison with post-irradiation examination data.

Journal Articles

Oxygen chemical diffusion coefficients of (U, Pu)O$$_{2-x}$$

Watanabe, Masashi; Sunaoshi, Takeo*; Kato, Masato

Defect and Diffusion Forum, 375, p.84 - 90, 2017/05

The oxygen chemical diffusion coefficient in (U, Pu)O$$_{2-x}$$ was determined by thermo-gravimetry as functions of the Pu content, oxygen-to-metal ratio and temperature. The surface reaction was considered in the diffusion coefficient determination. The activation energy for the chemical diffusion coefficient was 60 kJ/mol and 65 kJ/mol, respectively, in (U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2-x}$$ and (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2-x}$$.

Journal Articles

Defect chemistry and basic properties of non-stoichiometric PuO$$_{2}$$

Kato, Masato; Nakamura, Hiroki; Watanabe, Masashi; Matsumoto, Taku; Machida, Masahiko

Defect and Diffusion Forum, 375, p.57 - 70, 2017/05

The basic properties of PuO$$_{2-x}$$ were reviewed, and the equilibrium defects in PuO$$_{2-x}$$ were evaluated from the experimental data of the oxygen potential and electrical conductivity as well as the Ab-initio calculation results. Consistency among various properties was confirmed, and the mechanistic models for thermal property representations were derived.

Journal Articles

Oxygen potentials, oxygen diffusion coefficients and defect equilibria of nonstoichiometric (U,Pu)O$$_{2pm x}$$

Kato, Masato; Watanabe, Masashi; Matsumoto, Taku; Hiroka, Shun; Akashi, Masatoshi

Journal of Nuclear Materials, 487, p.424 - 432, 2017/04

 Times Cited Count:5 Percentile:58.67(Materials Science, Multidisciplinary)

Oxygen potential of (U,Pu)O$$_{2pm x}$$ was evaluated based on defect chemistry using an updated experimental data set. The relationship between oxygen partial pressure and deviation $$x$$ in (U,Pu)O$$_{2pm x}$$ was analyzed, and equilibrium constants of defect formation were determined as functions of Pu content and temperature. Brouwer's diagrams were constructed using the determined equilibrium constants, and a relational equation to determine O/M ratio was derived as functions of O/M ratio, Pu content and temperature. In addition, relationship between oxygen potential and oxygen diffusion coefficients were described.

Journal Articles

Oxygen potential measurement and point defect chemistry of UO$$_{2}$$

Watanabe, Masashi; Kato, Masato; Sunaoshi, Takeo*

Transactions of the American Nuclear Society, 114, p.1081 - 1082, 2016/06

Many studies on the oxygen potential of UO$$_{2}$$ have been carried out so far. However, the oxygen potential data for UO$$_{2}$$ near the stoichiometric composition in the high temperature region (1673-1873 K) are limited. In this work, the oxygen potential data of UO$$_{2+x}$$ were extended to high temperature range of 1673-1873 K by gas equilibrium method. The measured data were analyzed based on a defect chemistry model.

Journal Articles

Changes in risk perceptions before and after nuclear accidents; Evidence from Japan

Nishikawa, Masashi*; Kato, Takaaki*; Homma, Toshimitsu; Takahara, Shogo

Environmental Science & Policy, 55(1), p.11 - 19, 2016/01

Journal Articles

Oxygen chemical diffusion coefficients of (Pu,Am)O$$_{2}$$ fuels

Watanabe, Masashi; Matsumoto, Taku*; Kato, Masato

NEA/NSC/R(2015)2 (Internet), p.376 - 380, 2015/06

no abstracts in English

Journal Articles

Development of embedded Mach-Zehnder optical waveguide structures in polydimethylsiloxane thin films by proton beam writing

Kada, Wataru*; Miura, Kenta*; Kato, Hijiri*; Saruya, Ryota*; Kubota, Atsushi*; Sato, Takahiro; Koka, Masashi; Ishii, Yasuyuki; Kamiya, Tomihiro; Nishikawa, Hiroyuki*; et al.

Nuclear Instruments and Methods in Physics Research B, 348, p.218 - 222, 2015/04

 Times Cited Count:6 Percentile:54.79(Instruments & Instrumentation)

Journal Articles

Development of science-based fuel technologies for Japan's Sodium-Cooled Fast Reactors

Kato, Masato; Hiroka, Shun; Ikusawa, Yoshihisa; Takeuchi, Kentaro; Akashi, Masatoshi; Maeda, Koji; Watanabe, Masashi; Komeno, Akira; Morimoto, Kyoichi

Proceedings of 19th Pacific Basin Nuclear Conference (PBNC 2014) (USB Flash Drive), 12 Pages, 2014/08

Uranium and plutonium mixed oxide (MOX) fuel has been developed for Japan sodium-cooled fast reactors. Science based fuel technologies have been developed to analyse behaviours of MOX pellets in the sintering process and irradiation conditions. The technologies can provide appropriate sintering conditions, irradiation behaviour analysis results and so on using mechanistic models which are derived based on theoretical equations to represent various properties.

Journal Articles

Observation of deep levels and their hole capture behavior in p-type 4H-SiC epilayers with and without electron irradiation

Kato, Masashi*; Yoshihara, Kazuki*; Ichimura, Masaya*; Hatayama, Tomoaki*; Oshima, Takeshi

Japanese Journal of Applied Physics, 53(4S), p.04EP09_1 - 04EP09_5, 2014/04

 Times Cited Count:3 Percentile:16.04(Physics, Applied)

Journal Articles

Impact of carrier lifetime on efficiency of photolytic hydrogen generation by p-type SiC

Miyake, Keiko*; Yasuda, Tomonari*; Kato, Masashi*; Ichimura, Masaya*; Hatayama, Tomoaki*; Oshima, Takeshi

Materials Science Forum, 778-780, p.503 - 506, 2014/02

Journal Articles

Identification of structures of the deep levels in 4H-SiC

Nakane, Hiroki*; Kato, Masashi*; Ichimura, Masaya*; Oshima, Takeshi

Materials Science Forum, 778-780, p.277 - 280, 2014/02

Journal Articles

A Case study of economic incentives and local citizens' attitudes towards hosting a nuclear power plant in Japan; Impacts of the Fukushima accident

Kato, Takaaki*; Takahara, Shogo; Nishikawa, Masashi*; Homma, Toshimitsu

Energy Policy, 59, p.808 - 818, 2013/08

AA2012-0147.pdf:0.43MB

 Times Cited Count:24 Percentile:80.72(Economics)

This case study of the areas that host Kashiwazaki Kariwa NPP compares local citizens' attitude towards the benefits and the drawbacks of hosting the NPP. In December 2011, our survey respondents became more negative about hosting the NPP after the Fukushima accident in March 2011 compared to the survey in January 2010. Another comparison between the November 2005 and the December 2011 surveys provided a different look. The magnitude of the negative shift in Kariwa Village, which saw a large expansion of social welfare programs, was modest in the sense that its 2011 results were similar to its 2005 results. Local tax revenues, subsidies from the national government and the donation from a utility contributed to this budget expansion in Kariwa. The negative shifts from 2005 to 2011 were clear in the other two municipalities which did not see such a large expansion of economic benefits during this period.

Journal Articles

The Result of beam commissioning in J-PARC 3-GeV RCS

Harada, Hiroyuki; Hotchi, Hideaki; Saha, P. K.; Shobuda, Yoshihiro; Hayashi, Naoki; Yamamoto, Kazami; Yoshimoto, Masahiro; Tamura, Fumihiko; Yamamoto, Masanobu; Kinsho, Michikazu; et al.

Proceedings of 52nd ICFA Advanced Beam Dynamics Workshop on High-Intensity and High-Brightness Hadron Beams (HB 2012) (Internet), p.339 - 343, 2012/09

J-PARC 3-GeV RCS has started the beam commissioning since Oct. 2007. In the beam commissioning, the beam tuning for basic parameters and high-intensity operation has been continuously performed. This presentation will describe the results of the beam-loss reduction and minimization for high-intensity operation.

JAEA Reports

Annual report on the environmental radiation monitoring around the Tokai Reprocessing Plant FY2010

Sumiya, Shuichi; Watanabe, Hitoshi; Nakano, Masanao; Takeyasu, Masanori; Nakada, Akira; Fujita, Hiroki; Isozaki, Tokuju; Morisawa, Masato; Mizutani, Tomoko; Kokubun, Yuji; et al.

JAEA-Review 2012-015, 166 Pages, 2012/05

JAEA-Review-2012-015.pdf:3.53MB

Environmental radiation monitoring around the Tokai Reprocessing Plant has been performed by the Nuclear Fuel Cycle Engineering Laboratories, based on "Safety Regulations for the Reprocessing Plant of Japan Atomic Energy Agency, Chapter IV - Environmental Monitoring". This annual report presents the results of the environmental monitoring and the dose estimation to the hypothetical inhabitant due to the radioactivity discharged from the plant to the atmosphere and the sea during April 2010 to March 2011. In this report, some data include the influence of the accidental release from the Fukushima Daiichi Nuclear Power Plant on Tokyo Electric Power Co. in 2011 March. Appendices present comprehensive information, such as monitoring program, monitoring methods, monitoring results and their trends, meteorological data and discharged radioactive wastes. In addition, the data exceeded the normal range of fluctuation by the accidental release was evaluated in the appendices.

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