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Journal Articles

Thermodynamic study of the complexation of humic acid by calorimetry

Kimuro, Shingo; Kirishima, Akira*; Kitatsuji, Yoshihiro; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Chemical Thermodynamics, 132, p.352 - 362, 2019/05


A combination of potentiometry and calorimetry was used for the determination of the thermodynamic quantities of complexation of generic and groundwater humic acid (HA), which was isolated from deep groundwater at Horonobe, Hokkaido, Japan, with copper (II) ions and uranyl (VI) ions. The apparent complexation constant of Horonobe HA was independent of the pH, whereas that of generic HA was dependent on the pH. This observation indicates that the polyelectrolyte effect of Horonobe HA is negligible because of its small molecular size. In addition, the effect of the heterogeneity of Horonobe HA was not significant. Moreover, the complexation enthalpy of Horonobe HA was consistent with that of homogeneous poly(acrylic acid), which means the complexation of Horonobe HA was not affected by the functional group heterogeneity. Consequently, the characteristic complexation mechanism of Horonobe HA was revealed based on the determined thermodynamic quantities.

Journal Articles

Determination of $$^{107}$$Pd in Pd purified by selective precipitation from spent nuclear fuel by laser ablation ICP-MS

Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro

Analytical and Bioanalytical Chemistry, 411(5), p.973 - 983, 2019/02

 Percentile:100(Biochemical Research Methods)

Determination of radiopalladium $$^{107}$$Pd is required for ensuring the radiation safety of Pd extracted from spent nuclear fuel for recycling or disposal. We employed laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to simplify an analytical procedure of $$^{107}$$Pd. Pd was separated through selective Pd precipitation reaction from spent nuclear fuel. Laser ablation allows direct measurement of the Pd precipitates, skipping the dissolution and dilution procedure. In this study, $$^{102}$$Pd in natural Pd standard solution was used as an internal standard, taking advantage of its absence in spent nuclear fuel. The Pd precipitate was uniformly embedded on the surface of the centrifugal filter, forming a microscopically thin flat surface of Pd. The resulting homogeneous Pd layer is suitable for obtaining a stable signal ratio of $$^{107}$$Pd/$$^{102}$$Pd. The amount of $$^{107}$$Pd obtained by LA-ICP-MS corresponds to the values obtained by conventional solution nebulization measurement.

Journal Articles

Electrochemistry of actinide

Kitatsuji, Yoshihiro

Radioisotopes, 67(10), p.483 - 493, 2018/10

Electrochemical reactions and redox properties of actinides such as uranium and neptunium are outlined. The flow electrolysis enables rapid and high-efficient treatment. It was demonstrated to measure slow processes of actinide redox. Experimental results of electrolysis of actinide ions and the preparation method of oxidation state of the ions based on the fundamental data are described. Mediator reaction and catalysis observed in the process of electrolysis of actinide ions are also explained.

Journal Articles

Non-contact and selective Pd separation based on laser-induced photoreduction for determination of $$^{107}$$Pd by ICP-MS; The Relation between separation conditions and Pd recovery

Yomogida, Takumi; Asai, Shiho; Saeki, Morihisa*; Hanzawa, Yukiko; Horita, Takuma; Esaka, Fumitaka; Oba, Hironori*; Kitatsuji, Yoshihiro

Bunseki Kagaku, 66(9), p.647 - 652, 2017/09

 Times Cited Count:1 Percentile:85.18(Chemistry, Analytical)

Palladium-107 is a long-lived fission product, which can be found in high-level radioactive liquid wastes (HLLW). Determination of the $$^{107}$$Pd contents in HLLW is essential to evaluate the long-term safety of HLLW repositories. However, the $$^{107}$$Pd content in HLLW has not been reported because of difficulties in pretreatment for the measurement. In this study, we investigated applicability of laser-induced photoreduction to HLLW solution: it enables a simple and non-contact separation of Pd. The results showed the recovery of 60% was achieved at the conditions: 40% ethanol, 20 min irradiation, 100 mJ of pulse energy. Additionally, major radionuclides and potentially interfering components in ICP-MS were removed from the simulated HLLW over a wide concentration range of Pd from 0.24 to 24 mg L$$^{-1}$$, showing the applicability of the proposed separation technique to HLLW samples.

JAEA Reports

Preliminary missions for the decommissioning of the laboratory building No.1 for the plutonium research program

Segawa, Yukari; Horita, Takuma; Kitatsuji, Yoshihiro; Kumagai, Yuta; Aoyagi, Noboru; Nakada, Masami; Otobe, Haruyoshi; Tamura, Yukito*; Okamoto, Hisato; Otomo, Takashi; et al.

JAEA-Technology 2016-039, 64 Pages, 2017/03


The laboratory building No.1 for the plutonium research program (Bldg. Pu1) was chosen as one of the facilities to decommission by Japan Atomic Energy Agency Reform in September, 2013. The research groups, users of Bldg. Pu1, were driven by necessity to remove used equipment and transport nuclear fuel to other facilities from Bldg. Pu1. Research Group for Radiochemistry proactively established the Used Equipment Removal Team for the smooth operation of the removal in April, 2015. The team classified six types of work into the nature of the operation, removal of used equipment, disposal of chemicals, stabilization of mercury, stabilization of nuclear fuel, transportation of nuclear fuel and radioisotope, and survey of contamination status inside the glove boxes. These works were completed in December, 2015. This report circumstantially shows six works process, with the exception of the approval of the changes on the usage of nuclear fuel in Bldg. Pu1 to help prospective decommission.

Journal Articles

Preparation of Sr adsorptive fiber by impregnating with crown ether derivative for $$^{90}$$Sr measurement

Horita, Takuma; Asai, Shiho; Konda, Miki; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Sugo, Takanobu*; Kitatsuji, Yoshihiro

Bunseki Kagaku, 66(3), p.189 - 193, 2017/03

A Sr-selective adsorption fiber was prepared for rapid analysis of $$^{90}$$Sr content by using radiation-induced emulsion graft polymerization and subsequent chemical modification. A polyethylene fiber with a diameter of 13 $$mu$$m was first immersed in a methanol solution of an epoxy-group-containing vinyl monomer, glycidyl methacrylate (GMA), and polyoxyethylene sorbitol ester (Tween20) as a surfactant for graft-polymerization of GMA. Octadecylamine was then bound to a polymer chain extending from the fiber surface providing hydrophobicity to the polymer chain. Dicyclohexano-18-crown-6 (DCH18C6) was finally impregnated onto the polymer chain via a hydrophobic interaction between the octadecyl moiety of the polymer chain and the cyclohexyl moiety of DCH18C6. The fiber surface structure, characterized by DCH18C6 molecules loosely entangled with polymer chains, afforded realizes the rapid and selective adsorption of Sr ions with an adsorption rate approximately 100 times higher than that of a commercially available Sr-selective resin (Sr Resin).

Journal Articles

Deposition of uranium oxide following the reduction in weak acid solution using Electrochemical Quartz Crystal Microbalance (EQCM)

Ouchi, Kazuki; Otobe, Haruyoshi; Kitatsuji, Yoshihiro; Yamamoto, Masahiro

ECS Transactions, 75(27), p.51 - 57, 2017/01


We investigated the deposition of U(IV) following a valence change of U as electrodeposition using an electrochemical quartz crystal microbalance (EQCM). When measurements of the reduction of U(VI) in a weak acid solution were performed, deposits of U(IV) were observed on the electrode surface. From deposition rates, pH dependence of them, and oxidation potentials of deposits, we proposed the following deposition mechanism. The deposition is divided into the three phases; First, in the induction phase, U(IV) produced by the disproportionation forms U(IV) hydroxide nucleus. Next, in the growth phase, U(IV) deposits begin to grow. In this phase, the deposits catalyze the reduction of U(V) to U(IV), resulting an increase of the reduction current. Finally, in the transformation phase, U(IV) hydroxide species transform into U dioxide having more stable state.

Journal Articles

Determination of $$^{107}$$Pd in Pd recovered by laser-induced photoreduction with inductively coupled plasma mass spectrometry

Asai, Shiho; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro

Analytical Chemistry, 88(24), p.12227 - 12233, 2016/12

 Times Cited Count:4 Percentile:63.41(Chemistry, Analytical)

Safety evaluation of a radioactive waste repository requires credible activity estimates confirmed by actual measurements. A long-lived radionuclide, $$^{107}$$Pd, which can be found in radioactive wastes, is one of the difficult-to-measure nuclides and results in a deficit in experimentally determined contents. In this study, a precipitation-based separation method has been developed for the determination of $$^{107}$$Pd with ICP-MS. The photoreduction induced by laser irradiation at 355 nm provides short-time and one-step recovery of Pd. The proposed method was verified by applying it to a spent nuclear fuel sample. In order to efficiently recover Pd, a natural Pd standard was employed as the Pd carrier. The chemical yield of Pd was about 90% with virtually no impurities, allowing accurate quantification of $$^{107}$$Pd.

Journal Articles

Electrochemistry at liquid/liquid interface

Kitatsuji, Yoshihiro

Bunseki, 2015(6), p.239 - 244, 2015/06


Electrochemical studies of ion transfer and charge transfer at liquid/liquid interface reported between 2012 and 2014 were surveyed. They were categorized by method of measurement. The merit of the method, improvement, species of application were described. Applied research such as analyses of redox inactive species, sensitive analyses based on adsorption at the interface and developments of new functional materials had been widely carried out.

Journal Articles

Theoretical and experimental study of the vibrational frequencies of UO$$_{2}$$$$^{2+}$$ and NpO$$_{2}$$$$^{2+}$$ in highly concentrated chloride solutions

Fujii, Toshiyuki*; Uehara, Akihiro*; Kitatsuji, Yoshihiro; Yamana, Hajimu*

Journal of Radioanalytical and Nuclear Chemistry, 303(1), p.1015 - 1020, 2015/01

 Times Cited Count:3 Percentile:53.75(Chemistry, Analytical)

The $$nu$$$$_{1}$$ symmetric vibrational frequency of UO$$_{2}$$$$^{2+}$$ in chloride solutions was studied by Raman spectrometry and ab initio calculations. The $$nu$$$$_{1}$$ frequency experimentally obtained decreased with the increase of concentration of Cl in solvent chlorides. This is attributable to that hydration water molecules in the equatorial plane of UO$$_{2}$$$$^{2+}$$ are substituted by Cl$$^{-}$$ ions, which was consistent with the calculation results. The theoretical part was expanded to aqua- and chloro- Np(VI) complexes. The $$nu$$$$_{1}$$ frequencies of neptunyl species computed were acceptable compared with the reported Raman shifts.

Journal Articles

Corrosion of uranium and plutonium dioxides in aqueous solutions

Otobe, Haruyoshi; Kitatsuji, Yoshihiro; Kurata, Masaki; Takano, Masahide

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 11 Pages, 2014/10

The chemical and transport behaviors of Pu and U in the corroded debris must be understood for the criticality safety control of Pu and U in the debris, especially for the removal operations and storage. Therefore, the chemical changes of UO$$_{2}$$ and PuO$$_{2}$$ powders, disks and U and Pu metal disks in H$$_{2}$$O$$_{2}$$ aqueous solution have been checked, where H$$_{2}$$O$$_{2}$$ is formed by the radiolysis of H$$_{2}$$O. As a result, UO$$_{2}$$ changed to hydrated uranium peroxide, whereas the PuO$$_{2}$$ remained unchanged. U metal was more reactive with H$$_{2}$$O$$_{2}$$ aqueous solution than Pu metal. The chemical changes of the mixed UO$$_{2}$$/PuO$$_{2}$$ powders in H$$_{2}$$O$$_{2}$$ aqueous solution have been investigated. The dried slurry of the middle zone of H$$_{2}$$O$$_{2}$$ aqueous solution was mainly composed of hydrated uranium peroxide, whereas the dried powder of the bottom zone was mainly composed of PuO$$_{2}$$.

Journal Articles

Propagation of U(V)-reduction in the presence of U(IV) aggregate in a weakly acidic solution

Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kimura, Takaumi; Kihara, Sorin*

Electrochimica Acta, 141, p.6 - 12, 2014/09

 Times Cited Count:2 Percentile:93.74(Electrochemistry)

Reduction processes of U(VI) in weakly acidic solutions were investigated based on electrochemical and spectrophotometric measurements. A reversible one-electron reduction of U(VI) to U(V) and a further irreversible reduction of U(V) were observed voltammetrically at a gold microdisk electrode in solutions of pH from 2.0 to 3.5. Aggregates of U(IV) were formed as a deposit on the electrode and a colloid in the bulk solution, when the electrolysis was carried out at a gold gauze electrode, even though the potential applied was that available for the first one-electron reduction wave of U(VI) observed. It was elucidated that the aggregate was produced by the combination of the one-electron reduction to U(V) and the disproportionation of U(V) producing U(IV) and U(VI). The aggregate enhanced the rate of the disproportionation of U(V), and hence the reduction current of U(VI) increased abruptly when a definite amount of aggregate was formed on the electrode, in the solution, or both.

Journal Articles

Effect of the central frames and substituents attached to N atoms on extraction ability of podand-type extractants

Sasaki, Yuji; Kitatsuji, Yoshihiro; Sugo, Yumi; Tsubata, Yasuhiro; Suzuki, Tomoya; Kimura, Takaumi; Morita, Yasuji

Proceedings of 20th International Solvent Extraction Conference (ISEC 2014), p.431 - 435, 2014/09

The eight amide extractants including podand-types, which introduce oxygen, nitrogen and sulfur donor atoms in their central frame, are synthesized and their D values for actinide extraction are compared. The central frame affect greatly on their extractability and it is clear that diglycolamide (DGA) has the highest extractability among extractants used here. In addition, DGA having the different length of alkyl chain or phenyl groups attached to amidic N atoms are obtained and the effect of these substituents is studied. Due to the steric hindrance or hydrogen bond, DGA with long and branched alkyl chains, phenyl group, and proton give relatively low D values.

Journal Articles

Raman spectroscopic study on NpO$$_{2}$$$$^{+}$$-Ca$$^{2+}$$ interaction in highly concentrated calcium chloride

Fujii, Toshiyuki*; Uehara, Akihiro*; Kitatsuji, Yoshihiro; Yamana, Hajimu*

Journal of Radioanalytical and Nuclear Chemistry, 301(1), p.293 - 296, 2014/07

 Times Cited Count:3 Percentile:61.51(Chemistry, Analytical)

Coordination circumstance of neptunyl ion in concentrated CaCl$$_{2}$$ solutions was analyzed by Raman spectrometry. Besides the symmetric stretch ($$nu$$$$_{1}$$) mode of NpO$$_{2}$$$$^{+}$$ and NpO$$_{2}$$$$^{2+}$$, the asymmetric stretch ($$nu$$$$_{3}$$) mode of NpO$$_{2}$$$$^{+}$$ was found. The Raman intensity of the $$nu$$$$_{3}$$ mode increased with the concentration of CaCl$$_{2}$$ in the system. This would be attributable to the cation-cation interaction between Np(V) and Ca(II).

JAEA Reports

"Development of mutual separation technology of minor actinides by the novel hydrophilic and lipophilic diamide compounds" summary of the researches for three years (Contract research)

Sasaki, Yuji; Tsubata, Yasuhiro; Kitatsuji, Yoshihiro; Sugo, Yumi; Shirasu, Noriko; Ikeda, Yasuhisa*; Kawasaki, Takeshi*; Suzuki, Tomoya*; Mimura, Hitoshi*; Usuda, Shigekazu*; et al.

JAEA-Research 2014-008, 220 Pages, 2014/06


The researches on Development of mutual separation technology of minor actinides by the novel hydrophilic and lipophilic diamide compounds, entrusted to Japan Atomic Energy Agency by the Ministry of Education, Culture, Sports, Science and Technology of Japan, from 2010 to 2012 are summarized. This project was composed of three themes, those are (1) Development of total recovery of MA+Ln: basic researches for new extractant, DOODA, (2) Development of mutual separation of Am/Cm/Ln: basic researches of Ln-complex, solvent extraction, and extraction chromatography, and (3) Evaluation of separation technique: process simulation. For topic (1), we summarized the information on characteristic of DOODA extractant. For topic (2), we summarized the information on structures of Ln-complexes, solvent extraction and chromatography. For topic (3), we summarized the information on conditions of mixer-settler and evaluation of each fraction separated.

Journal Articles

Electroanalytical study of actinide ions

Kitatsuji, Yoshihiro

Review of Polarography, 60(1), p.25 - 34, 2014/05

no abstracts in English

Journal Articles

Measurement of the Md$$^{3+}$$/Md$$^{2+}$$ reduction potential studied with flow electrolytic chromatography

Toyoshima, Atsushi; Li, Z.*; Asai, Masato; Sato, Nozomi; Sato, Tetsuya; Kikuchi, Takahiro; Kaneya, Yusuke; Kitatsuji, Yoshihiro; Tsukada, Kazuaki; Nagame, Yuichiro; et al.

Inorganic Chemistry, 52(21), p.12311 - 12313, 2013/11

 Times Cited Count:3 Percentile:78.65(Chemistry, Inorganic & Nuclear)

The reduction behavior of mendelevium (Md) was studied using a flow electrolytic chromatography apparatus. By applying appropriate potentials on the chromatography column, the more stable Md$$^{3+}$$ is reduced to Md$$^{2+}$$. The reduction potential of the Md$$^{3+}$$ + e$$^{-}$$ $$rightarrow$$ Md$$^{2+}$$ couple was determined to be -0.16$$pm$$0.05 V vs. a normal hydrogen electrode.

Journal Articles

Mutual separation of Am/Cm/Ln by the use of novel-triamide, NTAamide and water-soluble diglycolamide

Sasaki, Yuji; Tsubata, Yasuhiro; Kitatsuji, Yoshihiro; Sugo, Yumi; Shirasu, Noriko; Morita, Yasuji

Proceedings of International Nuclear Fuel Cycle Conference; Nuclear Energy at a Crossroads (GLOBAL 2013) (CD-ROM), p.1079 - 1082, 2013/09

Mutual separation of Am, Cm and lanthanides (Ln) is important to develop the partitioning process of high-level radioactive liquid waste, because the application to their different disposal methods are advantageous. Namely, Am is studied for transmutation due to the reduction of long half-life radionuclides, Cm should be kept in interim storage in order to reduce the calorific value, and Ln should be present in the vitrified radioactive waste toward the geological disposal. However, this mutual separation method is difficult to establish because they have very similar chemical behavior, same oxidation state (III) and similar ionic radii. The development of their mutual separation is termed as the challenging study. In order to obtain the satisfactory results, the property of extractant requires the differentiation of actinide (An) from Ln, high preferability to different ionic radii between Am and Cm, and high extractability to hard acids. Therefore, the extractant have to include both N atom, whose soft donor has high selectivity between An and Ln, and O atoms for the strong extractability to An. The new extractant, NTAamide (N,N,N',N',N'',N''-hexaoctyl-nitrirotriacetamide) is a triamide having N donor at the center of backbone, then NTAamide has hybrid performance of complexation to metals by soft N and three hard amidic O atoms. It is clear that NTAamide can extract trivalent An at diluted HNO$$_{3}$$ with small D(Ln), the separation of An from Ln can be carried out at that condition. The SF of Am/Cm by NTAamide is approximate 1.8, which is not so high to separate each other. The combination of NTAamide of extractant and TEDGA (N,N,N',N'-tetraethyl-diglycolamide) as a masking agent in the aqueous phase shows very high SF(Am/Cm) of maximal 6.5. It is obvious that NTAamide is a promising extractant to achieve the mutual separation among Am/Cm/Ln.

Journal Articles

Novel soft-hard donor ligand, NTAamide, for mutual separation of trivalent actinides and lanthanides

Sasaki, Yuji; Tsubata, Yasuhiro; Kitatsuji, Yoshihiro; Morita, Yasuji

Chemistry Letters, 42(1), p.91 - 92, 2013/01

 Times Cited Count:16 Percentile:39.04(Chemistry, Multidisciplinary)

The new N-donor extractant, NTAamide, is synthesized and tested for extraction and separation of Am-Cm-Ln. It was found that the high separation factors for An-Ln can be seen at 0.1-0.2M HNO$$_{3}$$, which suggest the de-protonation to N donor is important to show the high SF between An and Ln. From the present work, the stable N-donor extractant having high SF of An-Ln from nitric acid to n-dodecane can be obtained. The highest separation factor, 6.5, of Am-Cm for the condition of 0.5M NTAamide (C8) in n-dodecane and 10 mM TEDGA in 0.2M HNO$$_{3}$$ as one of the highest SF values is found. NTAamide is the promising extractants for partitioning process of Am-Cm-Ln.

Journal Articles

Flow electrolysis of U, Np and Pu ions utilizing electrocatalysis at a column electrode with platinized glassy carbon fiber working electrode

Kitatsuji, Yoshihiro; Kimura, Takaumi; Kihara, Sorin*

Electrochimica Acta, 74, p.215 - 221, 2012/07

 Times Cited Count:2 Percentile:92.14(Electrochemistry)

Redox reactions of U, Np and Pu ions of various oxidation states were investigated by flow electrolysis at a column electrode (CE) equipped with a platinized glassy carbon (GC) fiber working electrode (Pt/GC-WE), and compared with those observed at the CE with an ordinary activated GC fiber working electrode (GC$$_{rm act}$$-WE). Since the overpotential for the reduction of NpO$$_{2}$$$$^{+}$$ and PuO$$_{2}$$$$^{+}$$ were decreased when Pt/GC-WE was employed, the one-electron reduction of NpO$$_{2}$$$$^{+}$$ to Np$$^{4+}$$ followed by that of Np$$^{4+}$$ to Np$$^{3+}$$ and the one-step three-electron reduction of PuO$$_{2}$$$$^{2+}$$ to Pu$$^{3+}$$ proceeded at the CE with Pt/GC-WE, different from the reduction processes of NpO$$_{2}$$$$^{+}$$ and PuO$$_{2}$$$$^{2+}$$ at the CE with GC$$_{rm act}$$-WE. A rapid and precise method for the preparation of U, Np and Pu ion of a desired oxidation state was proposed by taking advantage of the unique characteristics of the CE with Pt/GC-WE.

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