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Journal Articles

Sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions onto sedimentary rock in the presence of gamma-irradiated humic acid

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$$^{3+}$$ 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$$^{3+}$$ 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$$^{3+}$$ in the liquid phase was high, indicating that the complexing ability of HA to Eu$$^{3+}$$ was higher than that of HA to Cs$$^{+}$$ ions. Therefore, the sorption of free Eu$$^{3+}$$ would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.

Journal Articles

Nanoscopic structure of borosilicate glass with additives for nuclear waste vitrification

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

Journal Articles

Vertical distribution of $$^{90}$$Sr and $$^{137}$$Cs in soils near the Fukushima Daiichi Nuclear Power Station

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

 Times Cited Count:1 Percentile:39.17(Chemistry, Analytical)

Journal Articles

Thermodynamic interpretation of uranium(IV/VI) solubility in the presence of $$alpha$$-isosaccharinic acid

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11

 Times Cited Count:0 Percentile:0.01(Thermodynamics)

The effect of $$alpha$$-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$$_{c}$$) range of 6$$sim$$13 and at total ISA concentration ([ISA]$$_{rm tot}$$) = 10$$^{-4}$$$$sim$$10$$^{-1.2}$$ mol/dm$$^{3}$$. The dependence of U(IV) solubility on pH$$_{c}$$ and [ISA]$$_{rm tot}$$ suggested the existence of U(OH)$$_{4}$$(ISA)$$_{2}$$$$^{2-}$$ as a dominant species within the investigated pH$$_{c}$$ range of 6$$sim$$12. For the U(VI)-ISA system, UO$$_{2}$$(OH)$$_{3}$$(ISA)$$_{2}$$$$^{2-}$$ was suggested as a dominant species at pH$$_{c}$$ 7$$sim$$13. 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.

Journal Articles

Structural approach to understanding the solubility of metal hydroxides

Kobayashi, Taishi*; Nakajima, Shogo*; Motokawa, Ryuhei; Matsumura, Daiju; Saito, Takumi*; Sasaki, Takayuki*

Langmuir, 35(24), p.7995 - 8006, 2019/06

 Times Cited Count:1 Percentile:9.61(Chemistry, Multidisciplinary)

Journal Articles

A Thermodynamic model for ZrO$$_{2}$$(am) solubility at 25$$^{circ}$$C in the Ca$$^{2+}$$-Na$$^{+}$$-H$$^{+}$$-Cl$$^{-}$$-OH$$^{-}$$-H$$_{2}$$O system; A Critical review

Rai, D.*; Kitamura, Akira; Altmaier, M.*; Rosso, K. M.*; Sasaki, Takayuki*; Kobayashi, Taishi*

Journal of Solution Chemistry, 47(5), p.855 - 891, 2018/05

 Times Cited Count:5 Percentile:8.63(Chemistry, Physical)

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$$_{2}$$(am). We have determined new/revised values for the formation constants of Zr(OH)$$_{2}$$$$^{2+}$$, Zr(OH)$$_{4}$$(aq), Zr(OH)$$_{5}$$$$^{-}$$, Zr(OH)$$_{6}$$$$^{2-}$$ and Ca$$_{3}$$Zr(OH)$$_{6}$$$$^{4+}$$, and the solubility product for ZrO$$_{2}$$(am) after the critical review.

Journal Articles

Determination of dissolved natural thorium and uranium in Horonobe and Mizunami Underground Research Laboratory groundwater and its thermodynamic analysis

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.

Journal Articles

Thermodynamic model for Zr solubility in the presence of gluconic acid and isosaccharinic acid

Kobayashi, Taishi*; Teshima, Takeshi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Nuclear Science and Technology, 54(2), p.233 - 241, 2017/02

 Times Cited Count:3 Percentile:40.62(Nuclear Science & Technology)

Zr solubility in the presence of gluconic acid (GLU) and isosaccharinic acid (ISA) was investigated as a function of hydrogen ion concentration (pH$$_{rm c}$$) and the total concentration of GLU or ISA. The dependence of the increase in Zr solubility on the pH$$_{rm c}$$ and GLU concentration suggested the existence of Zr(OH)$$_{4}$$(GLU)$$_{2}$$$$^{2-}$$ in the neutral pH region and Zr(OH)$$_{4}$$(GLU)(GLU$$_{rm -H}$$)$$^{3-}$$ in the alkaline pH region above pH$$_{rm c}$$ 10 as the dominant species in the presence of 10$$^{-3}$$ - 10$$^{-1}$$ mol/dm$$^{3}$$ (M) GLU. In the presence of ISA, the dominant species Zr(OH)$$_{4}$$(ISA)$$_{2}$$$$^{2-}$$ and Zr(OH)$$_{4}$$(ISA)(ISA$$_{rm -H}$$)$$^{3-}$$ 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)$$_{4}$$(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.

Journal Articles

Issues concerning the determination of solubility products of sparingly soluble crystalline solids; Solubility of HfO$$_{2}$$(cr)

Rai, D.*; Kitamura, Akira; Rosso, K. M.*; Sasaki, Takayuki*; Kobayashi, Taishi*

Radiochimica Acta, 104(8), p.583 - 592, 2016/08

 Times Cited Count:4 Percentile:45.9(Chemistry, Inorganic & Nuclear)

Solubility studies were conducted with HfO$$_{2}$$(cr) solid as a function of acid concentrations. These studies involved (1) using two different amounts of the solid phase, (2) acid washing the bulk solid phase, (3) preheating the solid phase to 1400 $$^{circ}$$C, and (4) heating amorphous HfO$$_{2}$$(am) suspensions to 90 $$^{circ}$$C to ascertain whether the HfO$$_{2}$$(am) converts to HfO$$_{2}$$(cr) and to determine the solubility from the oversaturation direction. Based on the results of these treatments it is concluded that the HfO$$_{2}$$(cr) contains a small fraction of less crystalline, but not amorphous, material [HfO$$_{2}$$(lcr)] and this, rather than the HfO$$_{2}$$(cr), is the solubility-controlling phase in the range of experimental variables investigated in this study. The solubility data are interpreted using both the Pitzer and SIT models. The log$$_{10}$$ of the solubility product of HfO$$_{2}$$(cr) is estimated. The observation of a small fraction of less crystalline higher solubility material is consistent with the general picture that mineral surfaces are often structurally and/or imperfect leading to a higher solubility than the bulk crystalline solid. This study stresses the urgent need, during interpretation of solubility data, of taking precautions to make certain that the observed solubility behavior for sparingly-soluble solids is assigned to the proper solid phase.

Journal Articles

Sorption of Eu$$^{3+}$$ on Na-montmorillonite studied by time-resolved laser fluorescence spectroscopy and surface complexation modeling

Sasaki, Takayuki*; Ueda, Kenyo*; Saito, Takumi; Aoyagi, Noboru; Kobayashi, Taishi*; Takagi, Ikuji*; Kimura, Takaumi; Tachi, Yukio

Journal of Nuclear Science and Technology, 53(4), p.592 - 601, 2016/04

 Times Cited Count:9 Percentile:75.69(Nuclear Science & Technology)

The influences of pH and the concentrations of Eu$$^{3+}$$ and NaNO$$_{3}$$ on the sorption of Eu$$^{3+}$$ to Na-montmorillonite were investigated through batch sorption measurements and time-resolved laser fluorescence spectroscopy (TRLFS). The pH had a little effect on the distribution coefficients (Kd) in 0.01 M NaNO$$_{3}$$, whereas the Kd strongly depended on pH at 1 M NaNO$$_{3}$$. A cation exchange model combined with a one-site non-electrostatic surface complexation model was successfully applied to the measured Kd. The TRLFS spectra of Eu$$^{3+}$$ sorbed were processed by parallel factor analysis (PARAFAC), which corresponded to one outer-sphere (factor A) and two inner-sphere (factor B and C) complexes. It turned out that factors A and B correspond to Eu$$^{3+}$$ sorbed by ion exchange sites and inner-sphere complexation with hydroxyl groups of the edge faces, respectively. Factor C became dominant at relatively high pH and ionic strength and likely correspond to the precipitation of Eu(OH)$$_{3}$$ on the surface.

Journal Articles

Sorption behavior of nickel and palladium in the presence of NH$$_{3}$$(aq)/NH$$_{4}$$$$^{+}$$

Kobayashi, Taishi*; Sasaki, Takayuki*; Ueda, Kenyo*; Kitamura, Akira

Materials Research Society Symposium Proceedings, Vol.1518, p.231 - 236, 2013/10

For the nuclear waste management of TRU waste, it is necessary to assess the impact of nitrate salts contained in the waste. In the present study, the sorption behavior of Ni and Pd on the pumice tuff was investigated in the presence of NH$$_{3}$$(aq)/NH$$_{4}$$$$^{+}$$. Under different NH$$_{3}$$(aq)/NH$$_{4}$$$$^{+}$$ concentration, pH and ionic strength conditions, distribution coefficient ($$K_{rm d}$$) of Ni and Pd on the pumice tuff was determined by batch experiment. For Ni system, the $$K_{rm d}$$ values showed no significant dependence on the initial NH$$_{4}$$$$^{+}$$ concentration in neutral pH region, agrees with the prediction from thermodynamic data. For Pd system, the $$K_{rm d}$$ values decreased with an increase of [NH$$_{4}$$$$^{+}$$]ini, suggesting the formation of stable ammine complex (Pd(NH$$_{3}$$)$$_{m}$$$$^{2+}$$ ($$m$$: 1 - 4)). The obtained $$K_{rm d}$$ values for Ni and Pd were analyzed using the surface complexation model. By taking complexes predicted by thermodynamic data into account, the sorption behavior of Ni and Pd in the presence of NH$$_{3}$$(aq)/NH$$_{4}$$$$^{+}$$ were well explained.

Journal Articles

Report on MIGRATION 2011

Tachi, Yukio; Kobayashi, Taishi*

Genshiryoku Bakkuendo Kenkyu (CD-ROM), 18(2), p.113 - 115, 2011/12

The 13th International Conference on the Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere (MIGRATION 2011) was held at Peking University, China on 18th-23rd, September, 2011. This report summaries overview of the conference and topics in each technical session, which indicate the state-of-the-art of international research activities on radionuclide migration for geological disposal.

Journal Articles

Study on stabilization effect of neutral soft donor on trivalent lanthanide and actinide dicarboxylate complexes by time-resolved laser-induced fluorescence spectroscopy

Sasaki, Takayuki*; Kubo, Shintaro*; Kobayashi, Taishi*; Kirishima, Akira*; Kimura, Takaumi; Kubota, Takumi*; Takagi, Ikuji*; Moriyama, Hirotake*

Journal of Nuclear and Radiochemical Sciences, 6(1), p.51 - 54, 2005/07

no abstracts in English

Oral presentation

Spontaneous excitation of waves due to anisotropic velocity distribution in GAMMA 10 and JT-60U

Ichimura, Makoto*; Yamaguchi, Yusuke*; Sato, Shoichi*; Katano, Makoto*; Ouchi, Toshiaki*; Muro, Taishi*; Sekihara, Yusuke*; Murakami, Tatsuya*; Moriyama, Shinichi; Kobayashi, Takayuki; et al.

no journal, , 

Fluctuations in the ion cyclotron range of frequency are investigated both on GAMMA 10 and JT-60U. Ion cyclotron emissions (ICEs) due to deuterium-deuterium fusion-product (FP) ions on JT-60U are described. ICE due to H-ions is newly identified. ICE(T) with lower frequency has larger wave numbers than ICE ($$^{3}$$He) in the same discharge. The excitation of slow Alfv$'e$n waves is elucidated for the first time as the mechanism for ICE due to T-ions. The anisotropy of T-ions at the outer plasma edge is evaluated by using Escape Particle Orbit analysis Code (EPOC).

Oral presentation

Solubility of technetium(IV) in NaNO$$_{3}$$ solutions

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

no journal, , 

We focused on the solubility of TcO$$_{2}$$.${it x}$H$$_{2}$$O(s) in the existence of the dilute to concentrated NaNO$$_{3}$$ in order to investigate the potential effect of nitrate on the Tc species. It was found that the solublity of TcO$$_{2}$$.${it x}$H$$_{2}$$O(s) was promoted under high NaNO$$_{3}$$ and/or electrolyte conditions.

Oral presentation

Solubility of technetium(IV) in NaNO$$_{3}$$ solutions

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

no journal, , 

Solubility of amorphous technetium(IV) hydroxide was investigated using redox buffers to control various redox potentials in NaNO$$_{3}$$ media. Aqueous technetium concentration increased with increasing NaNO$$_{3}$$ concentration. It was found that the obtained aqueous technetium concentration was well interpreted by thermodynamic calculations using the obtained redox potentials.

Oral presentation

Sorption of Eu$$^{3+}$$ on montmorillonite studied by time-resolved laser fluorescence spectroscopy and surface complexation modeling

Sasaki, Takayuki*; Ueda, Kenyo*; Saito, Takumi*; Aoyagi, Noboru; Kobayashi, Taishi*; Takagi, Ikuji*; Kimura, Takaumi; Tachi, Yukio

no journal, , 

The influence of pH, ionic strength, and the concentrations of Eu$$^{3+}$$ and nitrate salts on the sorption of Eu$$^{3+}$$ on Na-montmorillonite was investigated by batch sorption measurements. The distribution coefficient (Kd) indicated that the cation exchange reaction is significant in pH 4-7 at low ionic strength, and the formation of surface complexation is related to the pH dependence of Kd at high ionic strength. The Eu$$^{3+}$$ surface species were investigated using time-resolved laser fluorescence spectroscopy (TRLFS) with parallel factor analysis (PARAFAC). The PARAFAC modeling indicated two surface species, the outer-sphere (factor A) and inner-sphere (factor B) Eu$$^{3+}$$ complexes. Factor B was dominant at high pH and ionic strength, which was determined to be a Eu colloidal species formed at high Eu$$^{3+}$$ concentrations. A cation exchange model combined with a one-site non-electrostatic surface complexation model was applied to the measured Kd data, using the results of the TRLFS-PARAFAC analyses.

Oral presentation

Solubility of zirconium in highly-basic solutions containing calcium

Kitamura, Akira; Kobayashi, Taishi*; Sasaki, Takayuki*

no journal, , 

Solubility of zirconium was investigated in highly basic solutions containing calcium to evaluate effect of cementitious materials for setting parameters on radionuclide migration for TRU waste disposal. The obtained aqueous concentration of zirconium as functions of hydrogen and calcium concentrations was compared with thermodynamic calculations using published thermodynamic data.

Oral presentation

Estimation and thermodynamic analysis of natural thorium, uranium, and REE concentrations in groundwater at Horonobe URL

Sasaki, Takayuki*; Kokami, Takayuki*; Amamiya, Hiroki; Murakami, Hiroaki; Amano, Yuki; Iwatsuki, Teruki; Mizuno, Takashi; Kobayashi, Taishi*; Kirishima, Akira*

no journal, , 

For thermodynamic analysis of the trace metals in groundwater, concentrations of Th, U, and rare earth elements (REEs) were investigated at Horonobe Underground Research Laboratory. Groundwater was sampled in anaerobic condition directly from a packed section in the boreholes drilled to 140 m and 250 m depth in drift. The colloidal distribution was checked by an on-site batch ultrafiltration unit using 0.2 $$mu$$m or 10 kDa membranes. As the result, both Th and U concentrations could be estimated by thermodynamic calculations, assuming that the soluble solid phases are restricted to ThO$$_{2}$$(cr) and UO$$_{2}$$(cr), respectively. Meanwhile, the concentrations of REEs were also very low, and significant colloidal distribution for lighter REEs was observed. In the thermodynamic analysis where the lanthanide phosphate was assumed to be a solid phase, the experimental plots matched better with the calculated one, even though the changing trend differs from each other.

Oral presentation

Influence of organic acids on solubility of tetravalent metal hydroxide

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

no journal, , 

Solubility of zirconium was measured under gluconate conditions. Gluconate is known as an analogous materials to isosaccharinate which is an organic substance degraded from cellulose. An attempt was applied to obtain an equilibrium constant for zirconium-gloconate systems using the zirconium solubility values as a function of hydrogen and gluconate concentrations.

30 (Records 1-20 displayed on this page)