Zhao, Q.*; Saito, Takeshi*; Miyakawa, Kazuya; Sasamoto, Hiroshi; Kobayashi, Taishi*; Sasaki, Takayuki*
Journal of Hazardous Materials, 428, p.128211_1 - 128211_10, 2022/04
The influence of humic acid and its radiological degradation on the sorption of Cs and Eu by sedimentary rock was investigated to understand the sorption process of metal ions and humic substances. Aldrich humic acid (HA) solution was irradiated with different doses of gamma irradiation using a Co-60 gamma-ray source prior to the contact between the metal ions and the solid sorbent. The HA molecule decomposed to smaller molecules with a lower complexation affinity. Batch sorption experiments were performed to evaluate the effect of gamma-irradiated HA on the sorption of Cs and Eu ions. The addition of non-irradiated HA weakened the sorption of Eu because of the lower sorption of the neutral or negatively charged Eu-HA complexes compared with free Eu ions. The sorption of monovalent Cs ions was barely affected by the presence of HA and its gamma irradiation. The concentration ratio of HA complexed species and non-complexed species in the solid and liquid phases was evaluated by sequential filtration and chemical equilibrium calculations. The ratios supported the minimal contribution of HA to Cs sorption. However, the concentration ratio for Eu in the liquid phase was high, indicating that the complexing ability of HA to Eu was higher than that of HA to Cs ions. Therefore, the sorption of free Eu would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.
Koiwai, Takuma*; Wimmer, K.*; Doornenbal, P.*; Obertelli, A.*; Barbieri, C.*; Duguet, T.*; Holt, J. D.*; Miyagi, Takayuki*; Navrtil, P.*; Ogata, Kazuyuki*; et al.
Physics Letters B, 827, p.136953_1 - 136953_7, 2022/04
no abstracts in English
Motoshima, Takayuki*; Matsui, Hiroya; Kawakubo, Masahiro*; Kobayashi, Masato*; Ichimura, Tetsuhiro*; Sugita, Yutaka
Nihon Genshiryoku Gakkai-Shi ATOMO, 64(3), p.163 - 167, 2022/03
no abstracts in English
Motokawa, Ryuhei; Kaneko, Koji; Oba, Yojiro; Nagai, Takayuki; Okamoto, Yoshihiro; Kobayashi, Taishi*; Kumada, Takayuki; Heller, W. T.*
Journal of Non-Crystalline Solids, 578, p.121352_1 - 121352_7, 2022/02
Hasegawa, Yuta; Aoki, Takayuki*; Kobayashi, Hiromichi*; Idomura, Yasuhiro; Onodera, Naoyuki
Parallel Computing, 108, p.102851_1 - 102851_12, 2021/12
The aerodynamics simulation code based on the lattice Boltzmann method (LBM) using forest-of-octrees-based block-structured local mesh refinement (LMR) was implemented, and its performance was evaluated on GPU-based supercomputers. We found that the conventional Space-Filling-Curve-based (SFC) domain partitioning algorithm results in costly halo communication in our aerodynamics simulations. Our new tree cutting approach improved the locality and the topology of the partitioned sub-domains and reduced the communication cost to one-third or one-fourth of the original SFC approach. In the strong scaling test, the code achieved maximum speedup at the performance of 2207 MLUPS (mega- lattice update per second) on 128 GPUs. In the weak scaling test, the code achieved 9620 MLUPS at 128 GPUs with 4.473 billion grid points, while the parallel efficiency was 93.4% from 8 to 128 GPUs.
Hasegawa, Yuta; Aoki, Takayuki*; Kobayashi, Hiromichi*; Idomura, Yasuhiro; Onodera, Naoyuki
Keisan Kogaku Koenkai Rombunshu (CD-ROM), 26, 6 Pages, 2021/05
We introduce an improved domain partitioning method called "tree cutting approach" for the aerodynamics simulation code based on the lattice Boltzmann method (LBM) with the forest-of-octrees-based local mesh refinement (LMR). The conventional domain partitioning algorithm based on the space-filling curve (SFC), which is widely used in LMR, caused a costly halo data communication which became a bottleneck of our aerodynamics simulation on the GPU-based supercomputers. Our tree cutting approach adopts a hybrid domain partitioning with the coarse structured block decomposition and the SFC partitioning in each block. This hybrid approach improved the locality and the topology of the partitioned sub-domains and reduced the amount of the halo communication to one-third of the original SFC approach. The code achieved speedup on 8 GPUs, and achieved speedup at the performance of 2207 MLUPS (mega-lattice update per second) on 128 GPUs with strong scaling test.
Okamoto, Yoshihiro; Kobayashi, Hidekazu; Shiwaku, Hideaki; Sasage, Kenichi; Hatakeyama, Kiyoshi*; Nagai, Takayuki
Journal of Non-Crystalline Solids, 551, p.120393_1 - 120393_8, 2021/01
The chemical state of ruthenium in simulated iron phosphate radioactive waste glass was investigated by conventional X-ray absorption fine structure (XAFS) and imaging XAFS analyses. The EXAFS analysis suggested that ruthenium was contained as glass phase when content of the waste components was less than 10wt.% in 30 mol%FeO-PO base glass. In other samples, crystalline RuO was predominant. According to the imaging XAFS analysis, RuO particles in all samples had length smaller than 50m. Aggregations of RuO, which are found in nuclear waste borosilicate glass, were not seen in any of the iron phosphate glass samples.
Sasaki, Takayuki*; Matoba, Daisuke*; Dohi, Terumi; Fujiwara, Kenso; Kobayashi, Taishi*; Iijima, Kazuki
Journal of Radioanalytical and Nuclear Chemistry, 326(1), p.303 - 314, 2020/10
Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira
Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11
The effect of -isosaccharinic acid (ISA) on the solubility and redox of tetravalent and hexavalent uranium (U(IV), U(VI)) was investigated in the hydrogen ion concentration (pH) range of 613 and at total ISA concentration ([ISA]) = 1010 mol/dm. The dependence of U(IV) solubility on pH and [ISA] suggested the existence of U(OH)(ISA) as a dominant species within the investigated pH range of 612. For the U(VI)-ISA system, UO(OH)(ISA) was suggested as a dominant species at pH 713. The formation constants of the U(IV)-ISA and U(VI)-ISA complexes were determined by least-squares fitting of the solubility data. The solubility of U(IV) and U(VI) in the presence of ISA and its effect on the redox behavior were thermodynamically interpreted based on the obtained constants.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*; Uehara, Akihiro*; Fujii, Toshiyuki*; Sekimoto, Shun*
KURNS Progress Report 2018, P. 105, 2019/08
To understand this structural change of a borosilicate glass by a neutron irradiation in detail, the irradiation test was carried out in KUR in 2017FY. The glass structure was estimated by using Raman spectrometry in 2018FY. Comparing with the Raman spectra of glass samples before and after irradiation, it could be observed the change of peak height of Si-O bridging structure by the irradiation.
Kobayashi, Taishi*; Nakajima, Shogo*; Motokawa, Ryuhei; Matsumura, Daiju; Saito, Takumi*; Sasaki, Takayuki*
Langmuir, 35(24), p.7995 - 8006, 2019/06
Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Kano, Shigeru; Himeno, Haruyuki*; Kobayashi, Hiroshi*; Nakatani, Mikio*
JAEA-Research 2018-013, 18 Pages, 2019/03
The chemical state and local structure of some elements in the simulated nuclear waste glass samples (20 batches) prepared by bottom drain test in the full scale mock-up tests using KMOC melter were investigated by synchrotron radiation based X-ray absorption fine structure (XAFS) analysis. As a result of the analysis of cerium element, it was confirmed that the oxidation proceeds gently as the batch advanced. For manganese, iron, and zinc, there was almost no difference between batches, which seemed to be stabilized by getting into the frame structure of the borosilicate glass. There were no elements that seemed to be clearly crystalline except for platinum group elements. Remarkable precipitation was hardly observed in zirconium and molybdenum with the imaging analysis.
Nagai, Takayuki; Okamoto, Yoshihiro; Shiwaku, Hideaki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Hirono, Kazuya*; Homma, Masanobu*; Kobayashi, Hiromi*; Takahashi, Tomoe*; et al.
JAEA-Research 2018-007, 87 Pages, 2018/11
To select the chemical composition of a glass frit which can increase the waste content, the simulated waste glass samples prepared from a borosilicate glass frit including vanadium (V) were investigated by using Laser Ablation (LA) ICP-AES analysis, Raman spectrometry, and synchrotron XAFS measurement in this study on foundation business of the Agency for Natural Resources and Energy.
Nagai, Takayuki; Kobayashi, Hidekazu; Shimamura, Keisuke; Oyama, Koichi; Sasage, Kenichi; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*
JAEA-Research 2018-005, 72 Pages, 2018/09
Addition of radioactive waste to a borosilicate glass frit affects the local structures of glass-forming elements and waste elements in a waste glass produced in a vitrification process. In this study, simulated waste glass samples were prepared from borosilicate glass frit including phosphorus pentaoxide, and we investigated local structures of sodium (Na), boron (B), and waste elements in these glass samples by using synchrotron XAFS measurements in soft and hard X ray region.
Rai, D.*; Kitamura, Akira; Altmaier, M.*; Rosso, K. M.*; Sasaki, Takayuki*; Kobayashi, Taishi*
Journal of Solution Chemistry, 47(5), p.855 - 891, 2018/05
We have critically reviewed experimental data for Zr hydrolysis constant values for formation of several mononuclear and polynuclear species and a solubility product value for ZrO(am). We have determined new/revised values for the formation constants of Zr(OH), Zr(OH)(aq), Zr(OH), Zr(OH) and CaZr(OH), and the solubility product for ZrO(am) after the critical review.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*
Photon Factory Activity Report 2017, 2 Pages, 2018/00
no abstracts in English
Nagai, Takayuki; Kobayashi, Hidekazu; Sasage, Kenichi; Ayame, Yasuo; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*
JAEA-Research 2017-005, 54 Pages, 2017/06
Addition of radioactive waste to a borosilicate frit affects the local structures of boron (B) and waste elements in a waste glass. Synchrotron XAFS measurement was applied to investigate the local structural changes by using simulated waste borosilicate glass samples. Following results were obtained by the B K-edge XAFS analysis. It was confirmed that B K-edge XAFS analysis enables us to discriminate sp type boron (BO) from sp type boron (BO). Addition of waste elements to a glass frit increases the percentage of BO and decreases that of BO. By decreasing the SiO/AlO ratio or increasing the (SiO+BO)/AlO ratio in the glass composition, the BO percentage increases and the BO percentage decreases. Addition of PO decreases the BO percentage and increases the BO percentage. Following results were obtained from XAFS measurement of the waste elements. Cerium (Ce) valence is more reduced with the increase of the BO content. Addition of PO has a tendency to reduce the Ce valence and to enhance deposition of Zr oxide. Deposition of ruthenium compounds separated from glass phase can not be improved by changing the BO content. This study was performed as a part of the project, "Improvement of vitrification process of high-level radioactive liquid wastes" on the foundation business of the Agency for Natural Resources and Energy.
Sasaki, Takayuki*; Kokami, Takayuki*; Kobayashi, Taishi*; Kirishima, Akira*; Murakami, Hiroaki; Amano, Yuki; Mizuno, Takashi; Iwatsuki, Teruki; Sasamoto, Hiroshi; Miyakawa, Kazuya
Journal of Nuclear Science and Technology, 54(3), p.373 - 381, 2017/03
Trace amounts of natural thorium and uranium in deep groundwater were investigated at two underground research laboratories situated at Horonobe and Mizunami, Japan. The groundwater was sampled from underground boreholes, and the colloid contribution was checked by in situ two size-fractionated ultrafiltration systems. A decrease in the concentration after in situ filtration suggested the presence of natural colloids and suspended matter that were carriers of a portion of the elements. The result of the Th and U concentrations in groundwater after 10 kDa filtration was analyzed thermodynamically using existing hydrogeological and geochemical data such as the mineral components in the groundwater at a given pH, ionic strength, concentration of co-existing ions, redox potential, and solid phase assumed. A crystalline solid phase made the solubility very low compared with that of the amorphous phase, and the solubility agreed well with the concentrations measured.
Kobayashi, Taishi*; Teshima, Takeshi*; Sasaki, Takayuki*; Kitamura, Akira
Journal of Nuclear Science and Technology, 54(2), p.233 - 241, 2017/02
Zr solubility in the presence of gluconic acid (GLU) and isosaccharinic acid (ISA) was investigated as a function of hydrogen ion concentration (pH) and the total concentration of GLU or ISA. The dependence of the increase in Zr solubility on the pH and GLU concentration suggested the existence of Zr(OH)(GLU) in the neutral pH region and Zr(OH)(GLU)(GLU) in the alkaline pH region above pH 10 as the dominant species in the presence of 10 - 10 mol/dm (M) GLU. In the presence of ISA, the dominant species Zr(OH)(ISA) and Zr(OH)(ISA)(ISA) were proposed to occur in the neutral and alkaline pH regions, similar to those found in the presence of GLU. From X-ray diffraction analysis, the solubility-limiting solid phase in the presence of GLU and ISA was considered to be Zr(OH)(am). The formation constants of the Zr gluconate and isosaccharinate complexes were determined by least squares fitting analysis of the solubility data, and the obtained values were discussed in comparison with those of tetravalent actinides.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro
Photon Factory Activity Report 2016, 2 Pages, 2017/00
To estimate the valence state of iron in the preparation process of iron phosphate glass frit, mixtures of ferric oxide and phosphoric acid was heated and XANES spectra of Fe-K edge was measured in this study. This report described the situation of high temperature XAFS measurement and results of this study.