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Journal Articles

Effect of O/M ratio on sintering behavior of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2-x}$$

Nakamichi, Shinya; Hirooka, Shun; Kato, Masato; Sunaoshi, Takeo*; Nelson, A. T.*; McClellan, K. J.*

Journal of Nuclear Materials, 535, p.152188_1 - 152188_8, 2020/07

 Times Cited Count:7 Percentile:72.51(Materials Science, Multidisciplinary)

Oxygen-to-metal ratio (O/M) of uranium and plutonium mixed oxide depends on its oxygen partial pressure. To attain the desirable microstructure and O/M ratio of sintered pellets, it is important to investigate the relation between the sintering behavior and the atmosphere of sintering process. In this study, sintering behavior of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2}$$ and (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{1.99}$$ in controlled po$$_{2}$$ atmosphere were investigated. It was found activation energy of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{1.99}$$ was higher than that of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2}$$. On the other hand, it was observed grain growth during sintering was suppressed in hypo-stoichiometric composition.

Journal Articles

Clades of huge phages from across Earth's ecosystems

Al-Shayeb, B.*; Sachdeva, R.*; Chen, L.-X.*; Ward, F.*; Munk, P.*; Devoto, A.*; Castelle, C. J.*; Olm, M. R.*; Bouma-Gregson, K.*; Amano, Yuki; et al.

Nature, 578(7795), p.425 - 431, 2020/02

 Times Cited Count:187 Percentile:99.48(Multidisciplinary Sciences)

Journal Articles

Thermal and mechanical properties of CeO$$_{2}$$

Suzuki, Kiichi; Kato, Masato; Sunaoshi, Takeo*; Uno, Hiroki*; Carvajal-Nunez, U.*; Nelson, A. T.*; McClellan, K. J.*

Journal of the American Ceramic Society, 102(4), p.1994 - 2008, 2019/04

 Times Cited Count:30 Percentile:90.26(Materials Science, Ceramics)

The fundamental properties of CeO$$_{2}$$ were assessed using a range of experimental techniques. The oxygen potential of CeO$$_{2}$$ was measured by the thermogravimetric technique, and a numerical fit for the oxygen potential of CeO$$_{2}$$ is derived based on defect chemistry. Mechanical properties of CeO$$_{2}$$ were obtained using sound velocity measurement, resonant ultrasound spectroscopy and nanoindentation. The obtained mechanical properties of CeO$$_{2}$$ are then used to evaluate the Debye temperature and Gruneisen constant. The heat capacity and thermal conductivity of CeO$$_{2}$$ were also calculated using the Debye temperature and the Gruneisen constant. Finally, the thermal conductivity was calculated based upon laser flash analysis measurements. This result demonstrates that the thermal conductivity has strong dependence upon material purity.

Journal Articles

Sintering behavior of (U,Ce)O$$_{2}$$ and (U,Pu)O$$_{2}$$

Nakamichi, Shinya; Hirooka, Shun; Sunaoshi, Takeo*; Kato, Masato; Nelson, A.*; McClellan, K.*

Transactions of the American Nuclear Society, 113(1), p.617 - 618, 2015/10

Cerium dioxide has been used as a surrogate material for plutonium dioxide. Dorr et al reported the use of hyper-stoichiometric conditions causes the start of shrinkage of (U,Ce)O$$_{2}$$ at low temperature compared with the sintering in reducing atmosphere. However, the precise stoichiometry of the samples investigated was not controlled or otherwise monitored, preventing any quantitative conclusions regarding the similarities or differences between (U,Ce)O$$_{2}$$ and (U,Pu)O$$_{2}$$. The motivation for the present work is therefore to compare the sintering behavior of MOX and the (U,Ce)O$$_{2}$$ MOX surrogates under controlled atmospheres to assess the role of oxygen defects on densification in both systems.

Journal Articles

An Evaluation of the thermophysical properties of stoichiometric CeO$$_{2}$$ in comparison to UO$$_{2}$$ and PuO$$_{2}$$

Nelson, A. T.*; Rittman, D. R.*; White, J. T.*; Dunwoody, J. T.*; Kato, Masato; McClellan, K. J.*

Journal of the American Ceramic Society, 97(11), p.3652 - 3659, 2014/11

 Times Cited Count:51 Percentile:93.07(Materials Science, Ceramics)

Journal Articles

Oxygen thermochemistry of urania-rare earth system; UO$$_2$$-CeO$$_2$$

Hirooka, Shun; Murakami, Tatsutoshi; Nelson, A. T.*; McClellan, K. J.*

INL/EXT-14-33515, p.34 - 36, 2014/10

Collaborative study has been done on the properties of nuclear materials between the DOE and Japan and the oxygen potential of (U,Ce)O$$_2$$ was measured in this year. Experimental measurements of the oxygen potential were conducted on Ce=20% and 30% composition rates simulating Pu content in advanced MOX fuel in JAEA by gas equilibrium method where oxygen partial pressure in the atmosphere was controlled with mixing dry/wet Ar/H$$_2$$ gas. More than 100 data points were obtained in the O/M range of 1.945 $$sim$$ 2.000 at 1200$$^{circ}$$C, 1400$$^{circ}$$C and 1600$$^{circ}$$C. The experimental results were analyzed by the defect analysis and analytical equations were obtained to calculate O/M as functions of temperature and oxygen potential. From the comparison with that of (U,Pu)O$$_2$$, applicability of the same defect chemistry and S-style curve are common. Also, it is revealed that (U,Ce)O$$_2$$ requires evidently higher oxygen potential for the O/M.

Journal Articles

Meeting nuclear data needs for advanced reactor systems

Harada, Hideo; Shibata, Keiichi; Nishio, Katsuhisa; Igashira, Masayuki*; Plompen, A.*; Hambsch, F.-J.*; Schillebeeckx, P.*; Gunsing, F.*; Ledoux, X.*; Palmiotti, G.*; et al.

NEA/NSC/WPEC/DOC(2014)446, 111 Pages, 2014/02

Journal Articles

Property measurements of (U$$_{0.7}$$,Pu$$_{0.3}$$)O$$_{2-x}$$ in $$P$$$$_{O2}$$-controlled atmosphere

Kato, Masato; Murakami, Tatsutoshi; Sunaoshi, Takeo*; Nelson, A. T.*; McClellan, K.*

Proceedings of International Nuclear Fuel Cycle Conference; Nuclear Energy at a Crossroads (GLOBAL 2013) (CD-ROM), p.852 - 856, 2013/09

Uranium and plutonium mixed oxide (U$$_{0.7}$$,Pu$$_{0.3}$$)O$$_{2-x}$$ which has been developed as a fast reactor fuel is nonstoichiometric compound. The stoichiometry significantly affects various properties. The relationship between oxygen potential and oxygen-to-metal (O/M) ratio has been investigated so far. The measurement results showed that it is essential to control oxygen partial pressure ($$P$$$$_{O2}$$) for holding constant O/M ratio in high temperature range. Therefore, properties of (U$$_{0.7}$$,Pu$$_{0.3}$$)O$$_{2-x}$$ were measured in $$P$$$$_{O2}$$-controlled atmosphere in this work. In this work, properties of O/M change, sintering and thermal expansion were investigated in $$P$$$$_{O2}$$-controlled atmosphere.

Journal Articles

Oxidation and reduction behaviors of plutonium and uranium mixed oxide powders

Hirooka, Shun; Kato, Masato; Tamura, Tetsuya*; Nelson, A. T.*; McClellan, K. J.*; Suzuki, Kiichi

Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Safe Technologies and Sustainable Scenarios (FR-13) (USB Flash Drive), 8 Pages, 2013/03

As research and development activities for MOX fuel pellet production, oxidation and reduction behaviors of MOX powders were investigated by thermogravimetry and X-ray diffraction measurements. It was observed that the oxidation limit decreased with oxidizing temperature and Pu content. The MOX powders showed a two-step oxidation and kinetic stability under non-stoichiometry. The oxidation rates were evaluated from the isothermal oxidation tests. It was found that the reduction temperature of M$$_{4}$$O$$_{9}$$ + M$$_{3}$$O$$_{8}$$ was higher than that of M$$_{4}$$O$$_{9}$$. This indicated that the reduction of M$$_{4}$$O$$_{9}$$ was prevented by the existence of M$$_{3}$$O$$_{8}$$. Activation energy of the reduction was derived from the non-isothermal reduction tests. The data are expected to contribute to establishing a control technique for O/M ratio during MOX powder storage and pellet production.

Journal Articles

The Reaction $$^{48}$$Ca + $$^{248}$$Cm $$rightarrow$$ $$^{296}$$116$$^{*}$$ studied at the GSI-SHIP

Hofmann, S.*; Heinz, S.*; Mann, R.*; Maurer, J.*; Khuyagbaatar, J.*; Ackermann, D.*; Antalic, S.*; Barth, B.*; Block, M.*; Burkhard, H. G.*; et al.

European Physical Journal A, 48(5), p.62_1 - 62_23, 2012/05

 Times Cited Count:157 Percentile:98.92(Physics, Nuclear)

Journal Articles

Manufacturing and maintenance technologies developed for a thick-wall structure of the ITER vacuum vessel

Onozuka, Masanori*; Alfile, J. P.*; Aubert, P.*; Dagenais, J.-F.*; Grebennikov, D.*; Ioki, Kimihiro*; Jones, L.*; Koizumi, Koichi; Krylov, V.*; Maslakowski, J.*; et al.

Fusion Engineering and Design, 55(4), p.397 - 410, 2001/09

 Times Cited Count:25 Percentile:84.39(Nuclear Science & Technology)

Development of welding, cutting and non-destructive testing (NDT) techniques, and development of remotized systems, have been conducted for on-site manufacturing and maintenance of the thick wall structure of the ITER vacuum vessel (VV). Conventional techniques, including TIG (tungsten inert gas) welding, plasma cutting and ultrasonic inspection, have been improved and optimized for the application to thick austenitic stainless steel plates. In addition, advanced methods have been investigated including reduced-pressure electron-beam and multi-pass NdYAG (neodymium-doped yttrium aluminum garnet) laser welding, NdYAG laser cutting, and EMAT (electro-magnetic acoustic transducer) inspection to improve cost and technical performance. Two types of remotized systems with different payloads have been investigated and one of them has been fabricated and demonstrated in field joint welding, cutting, and NDT tests on test mockups and full-scale ITER VV sector models. The progress and results of this development to date provide a high level of confidence that the manufacturing and maintenance of the ITER VV is feasible.

Oral presentation

Oxygen potential measurement of (U,Ce)O$$_{2}$$

Murakami, Tatsutoshi; Kato, Masato; Nelson, A.*; McClellan, K.*

no journal, , 

no abstracts in English

Oral presentation

Thermal properties of (U,Ce)O$$_{2pm x}$$

Hirooka, Shun; Murakami, Tatsutoshi; Kato, Masato; Suzuki, Kiichi; Nelson, A.*; White, J.*; McClellan, K.*

no journal, , 

no abstracts in English

Oral presentation

Evaluation of (U,Ce)O$$_{2}$$ thermal conductivity

Hirooka, Shun; Kato, Masato; Nelson, A.*; McClellan, K.*; White, J.*

no journal, , 

Thermal diffusivity of (U,Ce)O$$_{2}$$ was measured as a function of O/M, and the thermal conductivity was calculated. Thermal conductivity of (U,Ce)O$$_{2}$$ decreased more sharply with increasing temperature compared with that of (U,Pu)O$$_{2}$$. Also, thermal conductivity of (U,Ce)O$$_{2}$$ showed the highest peak at O/M of 2 and decreased as the O/M is apart from 2 on both hypo-stoichiometric and hyper-stoichimetric regions.

Oral presentation

Thermophyisical properties of (U,Ce)O$$_{2pm x}$$

White, J.*; Hirooka, Shun; Murakami, Tatsutoshi; Nelson, A.*; McClellan, K.*; Kato, Masato

no journal, , 

Use of CeO$$_{2}$$ as a surrogate to better understand the behavior of MOX fuels requires a fundamental investigation of the thermophysical properties to assess the appropriate use. The challenge in performing thermophysical property measurements on oxygen non-toichiometric MOX is in handling the kinetics at elevated temperatures and also in determining a reference state from which to measure the oxygen:metal ratio (O:M). This study integrated the use of identical gas handling systems installed on a thermogravimetric analyzer and the property measurement system (differential scanning calorimeter and laser flash analyzer) to control the partial pressure of oxygen, PO$$_{2}$$, between the system and maintain stoichiometry from ambient temperature to 1200$$^{circ}$$C.

Oral presentation

Oxygen potential representation of (U,Ce)O$$_{2 pm x}$$

Suzuki, Kiichi; Murakami, Tatsutoshi; Hirooka, Shun; Nelson, A.*; McClellan, K.*; Kato, Masato

no journal, , 

The relationship between equilibrium oxygen partial pressure, $$P_{rm O2}$$, and deviation from stoichiometric composition, x, was evaluated using a Kroger-Vink diagram. It was found that x was proportional to $$P_{rm O2}$$$$^{+1/2}$$ and $$P_{rm O2}$$$$^{-1/2}$$ near stoichiometry for all compositions. This suggests that intrinsic ionization is dominant near stoichiometry. Also, in the reducing region, x was proportional to $$P_{rm O2}$$$$^{-1/4}$$ for 20 and 30% of Ce, and was proportional to $$P_{rm O2}$$$$^{-1/6}$$ for 5% of Ce. Defect reactions and defect concentrations were evaluated by the relationship between x and $$P_{rm O2}$$$$^{1/n}$$. Then, the oxygen potential expression was derived using the defect concentrations as functions of O/M ratio, temperature and Ce content. The calculated values reproduced experimental values well.

Oral presentation

Thermal conductivity of uranium-cerium mixed oxide

Hirooka, Shun; Nelson, A.*; White, J.*; Kato, Masato; McClellan, K.*

no journal, , 

Thermal diffusivity of (U$$_{0.7}$$Ce$$_{0.3}$$)O$$_{2}$$ and (U$$_{0.8}$$Ce$$_{0.2}$$)O$$_{2}$$ was measured by laser flash method as a function of oxygen-to-metal ratio over the temperature range of 373 K to 1473 K and the thermal conductivity was evaluated. Only stoichiometric data of thermal conductivity of (U,Ce)O$$_{2}$$ was reported and that was comparable with thermal conductivity obtained in this work. Thermal conductivity was highest at stoichiometry, and was not perfectly symmetric with respect to the stoichiometry but slightly lower for hyper-stoichiometric compositions. The thermal conductivity of (U,Ce)O$$_{2}$$ showed the trend with temperature to be comparable to that of (U,Pu)O$$_{2}$$. However, the thermal resistivity did not follow the linear function of temperature, A+BT, which is an unique characteristics in (U,Ce)O$$_{2}$$.

Oral presentation

Effect of atmosphere on sintering behavior of (U,Ce)O$$_{2}$$

Nakamichi, Shinya; Hirooka, Shun; Kato, Masato; Sunaoshi, Takeo*; Nelson, A.*; McClellan, K.*

no journal, , 

Sintering behavior of (U$$_{0.70}$$Ce$$_{0.30}$$)O$$_{2}$$ was estimated and compared with that of MOX. Sintering of (U$$_{0.70}$$Ce$$_{0.30}$$)O$$_{2}$$ in CO$$_{2}$$ was not accelerated in contrast with that of MOX.

18 (Records 1-18 displayed on this page)
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