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Journal Articles

Hydrogen isotope separation by quantum tunneling of hydrons through graphene

Yasuda, Satoshi; Di$~n$o, W. A.*; Fukutani, Katsuyuki

Vacuum and Surface Science, 66(9), p.514 - 519, 2023/09

Monolayer graphene, representative of atomically thin crystals, has recently shown unexpectedly high proton and deuteron permeability under ambient conditions. It also permeates (filters) hydrogen (deuterium) isotope ion with high selectivity. These results suggest possible ways of developing novel and efficient hydrogen isotope gas enrichment techniques for manufacturing silicon semiconductors, optical fibers, drug development, nuclear fusion, and other related applications. And yet, despite its importance, experimental studies remain scarce and the separation mechanism contentious. Here, we introduce our recent findings on how quantum tunneling of hydrons through graphene could account for the high hydron selectivity of graphene.

Journal Articles

Long and oriented graphene nanoribbon synthesis from well-ordered 10,10'-dibromo-9,9'-bianthracene monolayer on crystalline Au surfaces

Yano, Masahiro; Yasuda, Satoshi; Fukutani, Katsuyuki; Asaoka, Hidehito

RSC Advances (Internet), 13(21), p.14089 - 14096, 2023/05

 Times Cited Count:0 Percentile:0(Chemistry, Multidisciplinary)

Bottom-up synthesis on metal surfaces has attracted attention for the fabrication of graphene nanoribbons (GNRs) with atomically-precise chemical structures to realize novel electronic devices. However, control of length and orientation on surfaces during GNR synthesis is difficult, thus, achieving longer and aligned GNR growth is a significant challenge. Herein, we report GNR synthesis from a well-ordered dense monolayer on Au crystalline surfaces for long and oriented GNR growth. Scanning tunneling microscopy showed that 10,10'-dibromo-9,9'-bianthracene (DBBA) precursors deposited on Au(111) at room temperature self-assembled into a well-ordered dense monolayer, and the straight molecular wire structure was formed where Br atoms in each precursor were adjacent along the wire axis. The DBBAs in the monolayer were found to be hardly desorbed from the surface under subsequent heating and efficiently polymerize along with the molecular arrangement, resulting in more long and oriented GNR growth compared to the conventional growth method. The result is attributed to be suppression of random diffusion and desorption of the DBBAs on the Au surface during polymerization due to the densely-packed DBBA structure. Additionally, an investigation of the effect of the Au crystalline plane on the GNR growth revealed further anisotropic GNR growth on Au(100) compared to Au(111) due to the stronger interactions of DBBA with Au(100). These findings provide fundamental knowledge for controlling GNR growth from a well-ordered precursor monolayer to achieve more long and oriented GNRs.

Journal Articles

New material exploration to enhance neutron intensity below cold neutrons; Nanosized graphene flower aggregation

Teshigawara, Makoto; Ikeda, Yujiro*; Yan, M.*; Muramatsu, Kazuo*; Sutani, Koichi*; Fukuzumi, Masafumi*; Noda, Yohei*; Koizumi, Satoshi*; Saruta, Koichi; Otake, Yoshie*

Nanomaterials (Internet), 13(1), p.76_1 - 76_9, 2023/01

 Times Cited Count:2 Percentile:54.89(Chemistry, Multidisciplinary)

To enhance neutron intensity below cold neutrons, it is proposed that nanosized graphene aggregation could facilitate neutron coherent scattering under particle size conditions similar to nanodiamond. It might also be possible to use it in high neutron radiation conditions due to graphene's strong sp2 bonds. Using the RIKEN accelerator-driven compact neutron source and iMATERIA at J-PARC, we performed neutron measurement experiments, total neutron cross-section, and small-angle neutron scattering on nanosized graphene aggregation. The measured data revealed, for the first time, that nanosized graphene aggregation increased the total cross-sections and small-angle scattering in the cold neutron energy region, most likely due to coherent scattering, resulting in higher neutron intensities, similar to nanodiamond.

Journal Articles

Investigation of the phonon dispersion associated with superlattice reflections in the BiS$$_{2}$$-based superconductor LaBiS$$_{2}$$O$$_{0.5}$$F$$_{0.5}$$

Tamatsukuri, Hiromu; Hasegawa, Takumi*; Sagayama, Hajime*; Mizumaki, Masaichiro*; Murakami, Yoichi*; Kajitani, Joe*; Higashinaka, Ryuji*; Matsuda, Tatsuma*; Aoki, Yuji*; Tsutsui, Satoshi*

Physical Review B, 107(2), p.024303_1 - 024303_8, 2023/01

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

Journal Articles

Efficient hydrogen isotope separation by tunneling effect using graphene-based heterogeneous electrocatalysts in electrochemical hydrogen isotope pumping

Yasuda, Satoshi; Matsushima, Hisayoshi*; Harada, Kenji*; Tanii, Risako*; Terasawa, Tomoo; Yano, Masahiro; Asaoka, Hidehito; Gueriba, J. S.*; Di$~n$o, W. A.*; Fukutani, Katsuyuki

ACS Nano, 16(9), p.14362 - 14369, 2022/09

 Times Cited Count:12 Percentile:85.62(Chemistry, Multidisciplinary)

The fabrication of hydrogen isotope enrichment system is essential for the development of industrial, medical, life science, and nuclear fusion fields, therefore alternative enrichment techniques with high separation factor and economic feasibility have been still explored. Herein, we report the fabrication of heterogeneous electrode with layered structures consisting of palladium and graphene layers for polymer electrolyte membrane electrochemical hydrogen pumping for the hydrogen isotope enrichment. We demonstrated significant bias voltage dependence of hydrogen/deuterium (H/D) separation ability and its high H/D at lower bias voltage. Theoretical analysis also demonstrated that the observed high H/D at low bias voltage stems from hydrogen isotopes tunneling through atomically-thick graphene during the electrochemical reaction, and the bias dependent H/D results in a transition from the quantum tunneling regime to classical over- barrier regime for hydrogen isotopes transfer via the graphene. These findings provide new insight for a novel economical methodology of efficient hydrogen isotope enrichment.

Journal Articles

Development of ultraslow, monochromatic, and mass-selected ion source toward measurement of hydrogen ion permeability of graphene

Terasawa, Tomoo; Fukutani, Katsuyuki; Yasuda, Satoshi; Asaoka, Hidehito

e-Journal of Surface Science and Nanotechnology (Internet), 20(4), p.196 - 201, 2022/07

Graphene is a perfect impermeable membrane for gases but permeable to hydrogen ions. Hydrogen ion permeation shows the isotope effect, i.e., deuteron is slower than proton when permeating graphene. However, the permeation mechanism and the origin of the isotope effect are still unclear. Here, we propose a strategy to discuss the hydrogen ion permeation mechanism of graphene by developing an ion source with ultraslow, monochromatic, and mass-selected hydrogen ion beam. We employed a hemispherical monochromator and a Wien filter for the ion source to achieve the energy and mass resolutions of 0.39 eV and 1 atomic mass unit, respectively. The energetically sharp ion beam is expected to allow us to directly measure the permeability of graphene with high accuracy.

Journal Articles

Mesospheric ionization during substorm growth phase

Murase, Kiyoka*; Kataoka, Ryuho*; Nishiyama, Takanori*; Nishimura, Koji*; Hashimoto, Taishi*; Tanaka, Yoshimasa*; Kadokura, Akira*; Tomikawa, Yoshihiro*; Tsutsumi, Masaki*; Ogawa, Yasunobu*; et al.

Journal of Space Weather and Space Climate (Internet), 12, p.18_1 - 18_16, 2022/06

 Times Cited Count:1 Percentile:22.72(Astronomy & Astrophysics)

We identified two energetic electron precipitation (EEP) events during the growth phase of moderate substorms and estimated the mesospheric ionization rate for an EEP event for which the most comprehensive dataset from ground-based and space-born instruments was available. The mesospheric ionization signature reached below 70 km altitude and continued for ~15 min until the substorm onset, as observed by the PANSY radar and imaging riometer at Syowa Station in the Antarctic region. We also used energetic electron flux observed by the Arase and POES 15 satellites as the input for the air-shower simulation code PHITS to quantitatively estimate the mesospheric ionization rate. Combining the cutting-edge observations and simulations, we shed new light on the space weather impact of the EEP events during geomagnetically quiet times, which is important to understand the possible link between the space environment and climate.

Journal Articles

Effects of a corrosion inhibitor on the corrosion of steels under thin solution layers

Momma, Yuichiro*; Sakairi, Masatoshi*; Ueno, Fumiyoshi; Otani, Kyohei

Zairyo To Kankyo, 71(5), p.133 - 137, 2022/05

The effect of the corrosion inhibitor on the corrosion of steel under a thin solution layer was investigated. As a result of forming a thin solution layer with a thickness of 1.0-0.2 mm on the specimen, adding a mixed solution of sodium molybdate and aluminum lactate as a corrosion inhibitor, and performing electrochemical measurement, the corrosion inhibitor suppresses the anodic reaction. And in the thin solution layer, it was suggested that the morphology of the protective layer structure by the corrosion inhibitor changed according to the amount of liquid as compared with the bulk immersion.

Journal Articles

Approach to elucidate corrosion mechanism on metal surface using first-principles calculations

Igarashi, Takahiro; Otani, Kyohei; Komatsu, Atsushi; Kato, Chiaki; Sakairi, Masatoshi*

Bosei Kanri, 66(4), p.141 - 145, 2022/04

Metal corrosion is a material deterioration phenomenon based on electrochemical reactions on an atomic scale. In this paper, various methods for acquiring physical properties on metal surfaces using first-principles calculations were described. As examples of applying first-principles calculation to metal corrosion, the effect of hydrogen adsorption on the metal surface on the potential change and the effect of cation atoms in the aqueous solution on the corrosion resistance of the metal were reported.

Journal Articles

Electrochemical behavior of carbon steels under thickness-controlled solution layer

Momma, Yuichiro*; Sakairi, Masatoshi*; Ueno, Fumiyoshi; Otani, Kyohei

Zairyo To Kankyo, 71(4), p.121 - 125, 2022/04

The effect of solution layer thickness on the atmospheric corrosion of carbon steel was investigated using novel devices fabricated by a 3D printer. These novel devices allowed us to control the solution layer thickness precisely. Potentiodynamic polarization measurements were performed under thickness-controlled solution layer, and oxygen diffusion limiting current density ($$j_{rm lim}$$) and anodic current density ($$j_{rm anode}$$) were measured. As the solution layer become thinner, $$j_{rm lim}$$ increased and $$j_{rm anode}$$ decreased. This result indicates that corrosion accelerates when the solution layer becomes thinner. The diffusion coefficient of oxygen was calculated as 3.20$$times$$10$$^{-5}$$ cm$$^{2}$$ s$$^{-1}$$ from the relationship between $$j_{rm lim}$$ and solution layer thickness, and the critical diffusion thickness was estimated to be 0.87 mm.

Journal Articles

Novel ${it Methanobacterium}$ strain induces severe corrosion by retrieving electrons from Fe$$^{0}$$ under a freshwater environment

Hirano, Shinichi*; Ihara, Sota*; Wakai, Satoshi*; Dotsuta, Yuma; Otani, Kyohei; Kitagaki, Toru; Ueno, Fumiyoshi; Okamoto, Akihiro*

Microorganisms (Internet), 10(2), p.270_1 - 270_12, 2022/02

 Times Cited Count:7 Percentile:84.82(Microbiology)

To understand the role of methanogens in corrosion under anoxic conditions in freshwater, we investigated the corrosion activities of methanogens in samples collected from groundwater and rivers. We enriched microorganisms that can grow with CO$$_{2}$$/NaHCO$$_{3}$$ and Fe$$^{0}$$ as the sole carbon source and electron donor, respectively, in ground fresh water. Electrochemical analysis revealed that ${it Methanobacterium}$ strain can uptake electrons from the cathode at lower than -0.61 V vs SHE and has a redox-active component with electrochemical potential different from those of other previously reported methanogens with extracellular electron transfer ability. This study indicated the corrosion risk by methanogens capable of taking up electrons from Fe$$^{0}$$ in anoxic freshwater environments and the necessity of understanding the corrosion mechanism to contribute to risk diagnosis.

Journal Articles

PSTEP: Project for solar-terrestrial environment prediction

Kusano, Kanya*; Ichimoto, Kiyoshi*; Ishii, Mamoru*; Miyoshi, Yoshizumi*; Yoden, Shigeo*; Akiyoshi, Hideharu*; Asai, Ayumi*; Ebihara, Yusuke*; Fujiwara, Hitoshi*; Goto, Tadanori*; et al.

Earth, Planets and Space (Internet), 73(1), p.159_1 - 159_29, 2021/12

 Times Cited Count:6 Percentile:51.19(Geosciences, Multidisciplinary)

The PSTEP is a nationwide research collaboration in Japan and was conducted from April 2015 to March 2020, supported by a Grant-in-Aid for Scientific Research on Innovative Areas from the Ministry of Education, Culture, Sports, Science and Technology of Japan. It has made a significant progress in space weather research and operational forecasts, publishing over 500 refereed journal papers and organizing four international symposiums, various workshops and seminars, and summer school for graduate students at Rikubetsu in 2017. This paper is a summary report of the PSTEP and describes the major research achievements it produced.

Journal Articles

Effect of bacterial siderophore on cesium dissolution from biotite

Kimura, Tatsuki*; Fukutani, Satoshi*; Ikegami, Maiko*; Sakamoto, Fuminori; Kozai, Naofumi; Grambow, B.*; Yoneda, Minoru*

Chemosphere, 276, p.130121_1 - 130121_7, 2021/08

 Times Cited Count:1 Percentile:6.09(Environmental Sciences)

The adsorption of cesium (Cs) on biotite and dissolution of Cs from Cs-bearing biotite using a siderophore were investigated aiming to contribute to the elucidation of radiocesium migration mechanisms in the soil environment. Cs was adsorbed on a hardly weathered biotite powder sample. A siderophore was extracted and purified from the bacterial culture medium, and the purified siderophore was used in five consecutive dissolution experiments of the biotite samples. The major components of the biotite (Al, Fe, and Mg) were dissolved almost stoichiometrically, strongly suggesting that the siderophore selectively dissolves the broken edges of the biotite. The Cs adsorbed on the broken edges was dissolved rapidly as the siderophore dissolved the broken edges, and then, the Cs adsorbed on the outer planar surface of the biotite particles was slowly dissolved.

Journal Articles

Development of an integrated computer code system for analyzing irradiation behaviors of a fast reactor fuel

Uwaba, Tomoyuki; Nemoto, Junichi*; Ito, Masahiro*; Ishitani, Ikuo*; Doda, Norihiro; Tanaka, Masaaki; Otsuka, Satoshi

Nuclear Technology, 207(8), p.1280 - 1289, 2021/08

 Times Cited Count:3 Percentile:35.51(Nuclear Science & Technology)

Computer codes for irradiation behavior analysis of a fuel pin and a fuel pin bundle and for coolant thermal hydraulics analysis were coupled into an integrated code system. In the system, each code provides data required by other codes and the analyzed results are shared among them. The system allows for the synthesizing of analyses of thermal, chemical and mechanical behaviors in a fuel subassembly under irradiation. A test analysis was made for a fuel subassembly containing a mixed oxide fuel pin bundle irradiated in a fast reactor. The results of the analysis were presented with transverse cross-sectional images of the fuel subassembly and three-dimensional images of a fuel pin and fuel pin bundle models. For detailed evaluation, various irradiation behaviors of all fuel pins in the subassembly were analyzed and correlated with irradiation conditions.

Journal Articles

Research and examination of seismic safety evaluation and function maintenance for important equipment in nuclear facilities

Furuya, Osamu*; Fujita, Satoshi*; Muta, Hitoshi*; Otori, Yasuki*; Itoi, Tatsuya*; Okamura, Shigeki*; Minagawa, Keisuke*; Nakamura, Izumi*; Fujimoto, Shigeru*; Otani, Akihito*; et al.

Proceedings of ASME 2021 Pressure Vessels and Piping Conference (PVP 2021) (Internet), 6 Pages, 2021/07

Since the Fukushima accident, with the higher safety requirements of nuclear facilities in Japan, suppliers, manufacturers and academic societies have been actively considering the reconstruction of the safety of nuclear facilities from various perspectives. The Nuclear Regulation Authority has formulated new regulatory standards and is in operation. The new regulatory standards are based on defense in depth, and have significantly raised the levels of natural hazards and have requested to strengthen the countermeasures from the perspective of preventing the simultaneous loss of safety functions due to common factors. Facilities for dealing with specific serious accidents are required to have robustness to ensure functions against earthquakes that exceed the design standards to a certain extent. In addition, since the probabilistic risk assessment (PRA) and the safety margin evaluation are performed to include the range beyond the design assumption in the safety improvement evaluation, it is very important to extent the special knowledge in the strength of important equipment for seismic safety. This paper summarizes the research and examination results of specialized knowledge on the concept of maintaining the functions of important seismic facilities and the damage index to be considered by severe earthquakes. In the other paper, the study on reliability of seismic capacity analysis for important equipment in nuclear facilities will be reported.

Journal Articles

Synergistic effects of metal cations and sodium gluconate on the inhibition of freshwater corrosion of mild steel

Otani, Kyohei; Sakairi, Masatoshi*

Materials Transactions, 62(6), p.815 - 820, 2021/06

 Times Cited Count:3 Percentile:25.78(Materials Science, Multidisciplinary)

The synergistic effects of metal cations in a solution on the ability of sodium gluconate to inhibit the corrosion of mild steel were investigated quantitatively focus on the parameter Y, which represents the "corrosion inhibitory effect of cations" by immersion and electrochemical tests. The results of the investigations showed that the inhibition ability of gluconates improved with increasing Y value of the metal cations in model freshwater. The electrochemical and surface analyses indicated that gluconate ligands and large-Y metal cations formed a protective film with few defects on the mild steel.

Journal Articles

Study on the free corrosion potential at an interface between an Al electrode and an acidic aqueous NaCl solution through density functional theory combined with the reference interaction site model

Kano, Koichi*; Hagiwara, Satoshi*; Igarashi, Takahiro; Otani, Minoru*

Electrochimica Acta, 377, p.138121_1 - 138121_10, 2021/05

AA2020-0599.pdf:0.95MB

 Times Cited Count:17 Percentile:71.29(Electrochemistry)

We investigated the free corrosion potential at an interface between an Al electrode and an aqueous NaCl solution under acidic conditions via density functional theory combined with the effective screening medium and reference interaction site model (ESM-RISM). The electrode potentials for the anodic and cathodic corrosion reactions were obtained from the grand potential profile as a function of the electron chemical potential at the interface. Thereafter, we determined the free corrosion potential using the Tafel extrapolation method. The results of the free corrosion potential were consistent with previous experimental data. By controlling the pH, we determined the pH dependence of the free corrosion potential, and the results agreed well with the experimental results. Our results indicated that the ESM-RISM method duly described the environmental effect of an acidic solution and precisely determined the free corrosion potential.

Journal Articles

Hydrogen absorption mechanism into iron in aqueous solution including metal cations by laser ablation tests and first-principles calculations

Igarashi, Takahiro; Otani, Kyohei; Kato, Chiaki; Sakairi, Masatoshi*; Togashi, Yusuke*; Baba, Kazuhiko*; Takagi, Shusaku*

ISIJ International, 61(4), p.1085 - 1090, 2021/04

 Times Cited Count:1 Percentile:8.06(Metallurgy & Metallurgical Engineering)

In order to clarify the effect of metal cations (Zn$$^{2+}$$, Mg$$^{2+}$$, Na$$^{+}$$) in aqueous solution on hydrogen permeation into iron, the amount of hydrogen permeation from iron surface was measured by electrochemical tests with a laser ablation. Moreover, in order to obtain the basic mechanism of hydrogen permeation with metal cation, first-principles calculations were used to acquire the adsorption potential of the metal cation and the electronic state around iron surface. By Zn$$^{2+}$$ in solution, anodic reaction on ablated surface by laser irradiation was suppressed. Also, by quantum analysis Zn atoms were chemically bonded stronger than Na and Mg atoms to iron surface. It was suggested that the dissolution reaction of iron was suppressed by the formation of the Zn layer, and that lead suppression of hydrogen permeation into iron.

Journal Articles

Thermally altered subsurface material of asteroid (162173) Ryugu

Kitazato, Kohei*; Milliken, R. E.*; Iwata, Takahiro*; Abe, Masanao*; Otake, Makiko*; Matsuura, Shuji*; Takagi, Yasuhiko*; Nakamura, Tomoki*; Hiroi, Takahiro*; Matsuoka, Moe*; et al.

Nature Astronomy (Internet), 5(3), p.246 - 250, 2021/03

 Times Cited Count:43 Percentile:96.93(Astronomy & Astrophysics)

Here we report observations of Ryugu's subsurface material by the Near-Infrared Spectrometer (NIRS3) on the Hayabusa2 spacecraft. Reflectance spectra of excavated material exhibit a hydroxyl (OH) absorption feature that is slightly stronger and peak-shifted compared with that observed for the surface, indicating that space weathering and/or radiative heating have caused subtle spectral changes in the uppermost surface. However, the strength and shape of the OH feature still suggests that the subsurface material experienced heating above 300 $$^{circ}$$C, similar to the surface. In contrast, thermophysical modeling indicates that radiative heating does not increase the temperature above 200 $$^{circ}$$C at the estimated excavation depth of 1 m, even if the semimajor axis is reduced to 0.344 au. This supports the hypothesis that primary thermal alteration occurred due to radiogenic and/or impact heating on Ryugu's parent body.

Journal Articles

Simple pretreatment method for tritium measurement in environmental water samples using a liquid scintillation counter

Nakasone, Shunya*; Yokoyama, Sumi*; Takahashi, Tomoyuki*; Ota, Masakazu; Kakiuchi, Hideki*; Sugihara, Shinji*; Hirao, Shigekazu*; Momoshima, Noriyuki*; Tamari, Toshiya*; Shima, Nagayoshi*; et al.

Plasma and Fusion Research (Internet), 16, p.2405035_1 - 2405035_5, 2021/02

Removal of impurities such as organic and other types of dissolved matters from environmental water samples is required for precise analysis of tritium with a liquid scintillation counting method. In general, a distillation method is a conventional one for tritium analysis in environmental water samples, but is a time-consuming process that takes 24 hours for removal of impurities. We have proposed a rapid pretreatment method for tritium analysis, that uses ion exchange resins. In this study, we performed batch experiments, to evaluate the effectiveness of the ion exchange resins on the tritium measurement. The results obtained demonstrated that removal of impurities in the sample water by ion exchange resins can be achieved during a short period of time (i.e., in 5 min).

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