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Journal Articles

Evaluation of oxidation efficiency of hydrophobic palladium catalyst for $$^{3}$$H monitoring in radioactive gaseous waste

Furutani, Misa; Kometani, Tatsunari; Nakagawa, Masahiro; Ueno, Yumi; Sato, Junya; Iwai, Yasunori*

Hoken Butsuri (Internet), 55(2), p.97 - 101, 2020/06

Herein, an oxidation catalyst was introduced after heating it to 600$$^{circ}$$C to oxidize tritium gas (HT) existing in exhaust into tritiated water vapor (HTO). This study aims to establish a safer $$^{3}$$H monitoring system by lowering the heating temperature required for the catalyst. In these experiments, which were conducted in the Nuclear Science Research Institute, Japan Atomic Energy Agency, cupric oxide, hydrophobic palladium/silicon dioxide (Pd/SiO$$_{2}$$), and platinum/aluminum oxide (Pt/Al$$_{2}$$O$$_{3}$$) catalysts were ventilated using standard hydrogen gas. After comparing the oxidation efficiency of each catalyst at different temperatures, we found that the hydrophobic Pd/SiO$$_{2}$$ and Pt/Al$$_{2}$$O$$_{3}$$ catalysts could oxidize HT into HTO at 25$$^{circ}$$C.

Journal Articles

Uncertainty analysis of toxic gas leakage accident in cogeneration high temperature gas-cooled reactor

Sato, Hiroyuki; Ohashi, Hirofumi

Mechanical Engineering Journal (Internet), 7(3), p.19-00332_1 - 19-00332_11, 2020/06

An uncertainty analysis method for control room habitability under toxic gas leakage accidents in cogeneration HTGR is proposed to support risk-informed design of the plant. The method is applied to representative toxic gas leakage accidents in a IS process hydrogen production plant coupled to the HTTR gas turbine test plant. Epistemic and aleatory uncertainties for each variable parameter are identified and are propagated using Latin hypercube sampling. The analyses show that the suggested method can successfully characterize and quantify uncertainties in the toxic gas concentration in control room. The results lead us to the conclusion that toxic gas dispersion behavior analysis should combine two evaluation methods: dense gas dispersion model and computational fluid dynamics simulation.

Journal Articles

Crystal and magnetic structures of double hexagonal close-packed iron deuteride

Saito, Hiroyuki*; Machida, Akihiko*; Iizuka, Riko*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; Sato, Toyoto*; Orimo, Shinichi*; Aoki, Katsutoshi*

Scientific Reports (Internet), 10, p.9934_1 - 9934_8, 2020/06

 Times Cited Count:0

Neutron powder diffraction profiles were collected for iron deuteride (FeDx) while the temperature decreased from 1023 to 300 K for a pressure range of 4-6 GPa. The $$varepsilon$$' deuteride with a double hexagonal close-packed (dhcp) structure, which coexisted with other stable or metastable deutrides at each temperature and pressure condition, formed solid solutions with a composition of FeD$$_{0.68(1)}$$ at 673 K and 6.1 GPa and FeD$$_{0.74(1)}$$ at 603 K and 4.8 GPa. Upon stepwise cooling to 300 K, the D-content x increased to a stoichiometric value of 1.0 to form monodeuteride FeD$$_{1.0}$$. In the dhcp FeD$$_{1.0}$$ at 300 K and 4.2 GPa, dissolved D atoms fully occupied the octahedral interstitial sites, slightly displaced from the octahedral centers in the dhcp metal lattice, and the dhcp sequence of close-packed Fe planes contained hcp-stacking faults at 12%. Magnetic moments with 2.11 $$pm$$ 0.06 B/Fe-atom aligned ferromagnetically in parallel on the Fe planes.

Journal Articles

Dynamics of atomic hydrogen in palladium probed by neutron spectroscopy

Kofu, Maiko; Yamamuro, Osamu*

Journal of the Physical Society of Japan, 89(5), p.051002_1 - 051002_12, 2020/05

 Times Cited Count:0 Percentile:100(Physics, Multidisciplinary)

The behavior of hydrogen in metals has attracted much attention in fundamental and applied research areas for many decades. Among metals, palladium is remarkable in that it can absorb large quantities of hydrogen, and hydrogen atoms are highly mobile in the fcc Pd lattice. The dynamics of hydrogen in Pd have been investigated by means of neutron spectroscopy which is the best tool to provide insights into microscopic dynamics of hydrogen atoms. In this article, we review recent and historical neutron scattering works to facilitate the latest understanding of the hydrogen dynamics in bulk and nanometer-sized Pd hydrides.

Journal Articles

Negatively charged muonium and related centers in solids

Ito, Takashi; Higemoto, Wataru; Shimomura, Koichiro*

Journal of the Physical Society of Japan, 89(5), p.051007_1 - 051007_8, 2020/05

 Times Cited Count:0 Percentile:100(Physics, Multidisciplinary)

Journal Articles

Polaronic nature of a muonium-related paramagnetic center in SrTiO$$_3$$

Ito, Takashi; Higemoto, Wataru; Koda, Akihiro*; Shimomura, Koichiro*

Applied Physics Letters, 115(19), p.192103_1 - 192103_4, 2019/11

 Times Cited Count:2 Percentile:42.97(Physics, Applied)

Journal Articles

Hexagonal close-packed iron hydride behind the conventional phase diagram

Machida, Akihiko*; Saito, Hiroyuki*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; Sato, Toyoto*; Orimo, Shinichi*; Aoki, Katsutoshi*

Scientific Reports (Internet), 9(1), p.12290_1 - 12290_9, 2019/08

 Times Cited Count:3 Percentile:36.63(Multidisciplinary Sciences)

Hexagonal close-packed iron hydride, hcp FeHx, is absent from the conventional phase diagram of the Fe-H system, although hcp metallic Fe exists stably over extensive temperature ($$T$$) and pressure ($$P$$) conditions, including those corresponding to the Earth's inner core. ${{it In situ}}$ X-ray and neutron diffraction measurements at temperatures ranging from 298 to 1073 K and H pressures ranging from 4 to 7 GPa revealed that the hcp hydride was formed for FeH$$_{x}$$ compositions when $$x < 0.6$$. Hydrogen atoms occupied the octahedral interstitial sites of the host metal lattice both partially and randomly. The hcp hydride exhibited a H-induced volume expansion of 2.48(5) $AA $^{3}$$/H-atom, which was larger than that of the face-centered cubic (fcc) hydride. The hcp hydride showed an increase in $$x$$ with $$T$$, whereas the fcc hydride showed a corresponding decrease. The present study provides guidance for further investigations of the Fe-H system over an extensive $$x$$-$$T$$-$$P$$ region.

Journal Articles

Study on B$$_{4}$$C decoupler with burn-up reduction aiming at 1-MW pulsed neutron source

Oi, Motoki; Teshigawara, Makoto; Harada, Masahide; Ikeda, Yujiro

Journal of Nuclear Science and Technology, 56(7), p.573 - 579, 2019/07

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

In pulsed neutron sources, a neutron absorber called decoupler is attached to the moderator to sharpen the neutron pulses for achieving good neutron energy resolutions. Cadmium and boron carbide (B$$_{4}$$C) are widely used as the decoupler materials. However, it is difficult to use B$$_{4}$$C in MW-class spallation neutron sources owing to high burn-up, which decreases cut-off energy and increase of helium gas swelling. To solve these issues, we introduce the concept of pre-decoupler to reduce neutron absorption in the B$$_{4}$$C decoupler, which is sandwiched by appropriate neutron absorption materials. Then, we study impacts of the pre-decouplers on B$$_{4}$$C decoupler in terms of burn-up by performing simplified model calculations. It is shown that neutron absorption in B$$_{4}$$C is reduced by 60% by using a Cd pre-decoupler without neutron intensity penalty. Moreover, helium gas swelling in B$$_{4}$$C is restrained to be one-third of the value when not using the pre-decoupler.

Journal Articles

High-pressure structure and electronic properties of YbD$$_{2}$$ to 34 GPa

Klotz, S.*; Casula, M.*; Komatsu, Kazuki*; Machida, Shinichi*; Hattori, Takanori

Physical Review B, 100(2), p.020101_1 - 020101_5, 2019/07

 Times Cited Count:3 Percentile:64.71(Materials Science, Multidisciplinary)

Ytterbium dihydride (YbH$$_{2}$$) shows a well-known transition at $$approx$$16 GPa from a CaH$$_{2}$$-type structure to a high-pressure (high-$$P$$) phase with Yb at hcp sites and unknown H-positions. Here, we report its complete structure determination by neutron diffraction at 34 GPa. Hydrogen(deuterium) is located at 2$$a$$ and 2$$d$$ positions of space group $$P6_{3}/mmc$$, thus forming a high-symmetry "collapsed" close-packed lattice. The transition is sluggish and can be seen as a transfer of 1/2 of the hydrogen atoms from strongly corrugated H-layers to interstitial sites of the Yb-lattice. We demonstrate by first-principles calculations that the transition is related to a change from a completely filled $$f$$-electron configuration to a fractional $$f$$-hole ($$approx$$0.25 h) occupation in the high-$$P$$ phase. The $$f$$ $$to$$ $$d$$ charge transfer closes the gap at the transition and leads to a metallic ground state with sizeable electron-phonon interaction involving out-of-plane vibrational modes of interstitial hydrogen.

Journal Articles

Progress of long-time operation and industrial use of negative ion source for particle accelerator

Oguri, Hidetomo

Purazuma, Kaku Yugo Gakkai-Shi, 95(7), p.340 - 344, 2019/07

no abstracts in English

Journal Articles

Mass transport in the PdCu phase structures during hydrogen adsorption and absorption studied by XPS under hydrogen atmosphere

Tang, J.*; Yamamoto, Susumu*; Koitaya, Takanori*; Yoshigoe, Akitaka; Tokunaga, Takuma*; Mukai, Kozo*; Matsuda, Iwao*; Yoshinobu, Jun*

Applied Surface Science, 480, p.419 - 426, 2019/06

 Times Cited Count:1 Percentile:64.71(Chemistry, Physical)

Mass transports during hydrogen adsorption and absorption processes of PdCu alloys that has advantages of higher hydrogen diffusivity and economically lower-cost than the other Pd-alloys were studied. The research was made with a comparison of the well-known ordered phase of the bcc structure (the B2 phase) and a mixed phase of the fcc and B2 structures. ${it In-situ}$ ultrahigh vacuum X-ray photoelectron spectroscopy and ambient pressure X-ray photoelectron spectroscopy using synchrotron radiation were carried out to trace the chemical states of the Pd and Cu atoms as a function of temperatures. It is elucidated that the initial adsorption and absorption processes were similar in the two phases, but a hydrogen diffusion rate to the bulk was higher in the ordered phase than in the mixed one. We found the dynamics of the Pd and Cu atoms during the hydrogen adsorption/absorption processes largely depend on temperature. In the hydrogen atmosphere, the Pd atoms segregate at the surface below 373 K and Cu atoms segregate at the surface above 373 K. The present results agree well with the previous theoretical calculations and, thus, provide appropriate inputs toward developments of the hydrogen permeation materials.

Journal Articles

Research on hydrogen safety technology utilizing the automotive catalyst

Ono, Hitomi*; Takenaka, Keisuke*; Kita, Tomoaki*; Taniguchi, Masashi*; Matsumura, Daiju; Nishihata, Yasuo; Hino, Ryutaro; Reinecke, E.-A.*; Takase, Kazuyuki*; Tanaka, Hirohisa*

E-Journal of Advanced Maintenance (Internet), 11(1), p.40 - 45, 2019/05

Journal Articles

Uncertainty analysis of toxic gas leakage accident in cogeneration high temperature gas-cooled reactor

Sato, Hiroyuki; Ohashi, Hirofumi

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05

To establish a probabilistic approach for assessment of toxic gas leakage accidents in a H$$_{2}$$ plant, the present study focusses on development of an uncertainty analysis method for toxic gas concentration in a control room. The method consists of 6 steps; (1) Identification of uncertainty factors, (2) derivation of variable parameters, (3) identification of uncertainties in variable parameters, (4) identification of important factors considering the sensitivity analysis results and expert opinions, (5) uncertainty propagation analysis, (6) assessment of uncertainty analysis results. The method is then applied to representative toxic gas leakage accidents in a H$$_{2}$$ plant by IS process coupled to the HTTR. The results obtained in the study leads us to the conclusion that the suggested method can successfully characterize and quantify uncertainties in the toxic gas concentration in control room.

Journal Articles

Enhancement of hydrogen generation, radionuclides release at time of resumption of water injection after cooling interruption for several hours during Fukushima Daiichi NPP accident

Hidaka, Akihide; Himi, Masashi*; Addad, Y.*

Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05

no abstracts in English

Journal Articles

Effect of H$$_{2}$$O$$_{2}$$ concentration on oxidative dissolution of U$$_{2}$$O

Kumagai, Yuta

Hoshasen Kagaku (Internet), (107), p.77 - 78, 2019/04

Reaction of hydrogen peroxide (H$$_{2}$$O$$_{2}$$) with uranium dioxide (UO$$_{2}$$) oxidizes U(IV) to water-soluble U(VI). In the concept of direct geological disposal of spent nuclear fuel, this reaction is expected to induce dissolution of UO$$_{2}$$ matrix of the spent fuel. This study investigate effect of H$$_{2}$$O$$_{2}$$ concentration on the kinetics and the yield of U(VI) dissolution of this reaction. A series of experiments of the reaction of H$$_{2}$$O$$_{2}$$ with UO$$_{2}$$ powder dispersed in water has been carried out. The experimental results reveal that increase in the H$$_{2}$$O$$_{2}$$ concentration slows down the reaction and decreases the yield of U(VI) dissolution. This observation suggests that a reaction intermediate is generated in the course of the H$$_{2}$$O$$_{2}$$ reaction on the surface of UO$$_{2}$$.

Journal Articles

Impact of stoichiometry on the mechanism and kinetics of oxidative dissolution of UO$$_{2}$$ induced by H$$_{2}$$O$$_{2}$$ and $$gamma$$-irradiation

Kumagai, Yuta; Fidalgo, A. B.*; Jonsson, M.*

Journal of Physical Chemistry C, 123(15), p.9919 - 9925, 2019/04

 Times Cited Count:3 Percentile:33.88(Chemistry, Physical)

Radiation-induced oxidative dissolution of uranium dioxide (UO$$_{2}$$) is one of the most important chemical processes of U driven by redox reactions. We have examined the effect of UO$$_{2}$$ stoichiometry on the oxidative dissolution of UO$$_{2}$$ induced by hydrogen peroxide (H$$_{2}$$O$$_{2}$$) and $$gamma$$-ray irradiation. By comparing the reaction kinetics of H$$_{2}$$O$$_{2}$$ between stoichiometric UO$$_{2.0}$$ and hyper-stoichiometric UO$$_{2.3}$$, we observed a significant difference in reaction speed and U dissolution kinetics. The stoichiometric UO$$_{2.0}$$ reacted with H$$_{2}$$O$$_{2}$$ much faster than the hyper-stoichiometric UO$$_{2.3}$$. The U dissolution from UO$$_{2.0}$$ was initially much lower than that from UO$$_{2.3}$$, but gradually increased as the oxidation by H$$_{2}$$O$$_{2}$$ proceeded. The $$gamma$$-ray irradiation induced the U dissolution that is analogous to the kinetics by the exposure to a low concentration (0.2 mM) of H$$_{2}$$O$$_{2}$$. The exposure to higher H$$_{2}$$O$$_{2}$$ concentrations caused lower U dissolution and resulted in deviation from the U dissolution behavior by $$gamma$$-ray irradiation.

Journal Articles

Development of hydrogen production technology by thermal water splitting with solar heat

Inagaki, Yoshiyuki; Sakaba, Nariaki

Shokubai, 61(2), p.92 - 96, 2019/04

The outline of the membrane IS process to produce hydrogen by thermochemical water splitting using solar heat at around 650$$^{circ}$$C is described. The membrane technology has been applied to the three main reaction of the IS process to lower the reaction temperature and reduce the amount of circulation materials in the process. The key component technologies such as catalysts, membranes and corrosion resistant materials have been developed. The study was supported in part by the Council for Science, Technology and Innovation, Cross-ministerial Strategic Innovation Promotion Program, "Energy Carrier".

Journal Articles

Hydrogen gas measurements of phosphate cement irradiated during heat treatment

Irisawa, Keita; Kudo, Isamu*; Taniguchi, Takumi; Namiki, Masahiro*; Osugi, Takeshi; Nakazawa, Osamu

QST-M-16; QST Takasaki Annual Report 2017, P. 63, 2019/03

no abstracts in English

Journal Articles

Hydrogen-based metabolism as an ancestral trait in lineages sibling to the Cyanobacteria

Matheus Carnevali, P. B.*; Schulz, F.*; Castelle, C. J.*; Kantor, R. S.*; Shih, P. M.*; Sharon, I.*; Santini, J.*; Olm, M. R.*; Amano, Yuki; Thomas, B. C.*; et al.

Nature Communications (Internet), 10, p.463_1 - 463_15, 2019/01

 Times Cited Count:6 Percentile:15.49(Multidisciplinary Sciences)

Journal Articles

Numerical and experimental study of H$$^{-}$$ beam dynamics in J-PARC LEBT

Shibata, Takanori*; Ikegami, Kiyoshi*; Liu, Y.*; Miura, Akihiko; Naito, Fujio*; Nammo, Kesao*; Oguri, Hidetomo; Okoshi, Kiyonori; Otani, Masashi*; Shinto, Katsuhiro; et al.

Proceedings of 29th International Linear Accelerator Conference (LINAC 2018) (Internet), p.519 - 521, 2019/01

Transport process of negative hydrogen ion (H$$^{-}$$) in LEBT (Low Energy Beam Transport) is investigated by comparison of experimental and numerical results. A three dimensional Particle-In-Cell (PIC) particle transport model has been developed in order to take into account (i) axial magnetic field by two solenoids in J-PARC LEBT and (ii) radial electric field by space charge (SC) effect. Ratio of H$$^-$$ beam particles inside the RFQ (Radio Frequency Quadrupole) acceptance to the total particles at the RFQ entrance is calculated for different current conditions in LEBT solenoid 1 and 2. The results are compared with RFQ transmission rate measured in the J-PARC linac commissioning. The double peak of RFQ transmission rate to the solenoid applied current seen in the measurement is explained by the calculation results. The results indicate that presence of the LEBT orifice for differential pumping plays a role as a collimator to reduce emittance at RFQ entrance.

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