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Journal Articles

Extraction of Se(iv) and Se(vi) from aqueous HCl solution by using a diamide-containing tertiary amine

Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Shiwaku, Hideaki; Yaita, Tsuyoshi

RSC Advances (Internet), 13(25), p.17001 - 17007, 2023/06

 Times Cited Count:1 Percentile:39.98(Chemistry, Multidisciplinary)

no abstracts in English

Journal Articles

Selective adsorption of Pd(II) over Ag(I) in nitric acid solutions using nitrogen-donor-type adsorbents

Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*

Separation and Purification Technology, 308, p.122943_1 - 122943_7, 2023/03

 Times Cited Count:2 Percentile:21.17(Engineering, Chemical)

HNO$$_{3}$$ leaching is used in recycling Pd metal from spent products that primarily contain Ag, and most Pd residues are separated from solutions containing Ag(I). However, a small amount of Pd(II) often remains in these Ag(I) solutions. Therefore, the separation of Pd(II) and Ag(I) in HNO$$_{3}$$ solutions is essential to promote efficient Pd recycling. In this study, the separation of Pd(II) and Ag(I) in HNO$$_{3}$$ solutions was investigated using four N-donor-type adsorbents functionalized with amine (R-Amine), iminodiacetic acid (R-IDA), pyridine (R-Py), or bis-picolylamine (R-BPA). R-Amine, R-IDA, and R-Py selectively adsorbed Pd(II) over Ag(I), Cu(II), Ni(II), and Fe(III) from HNO$$_{3}$$ solutions (0.3-7 M), but R-Amine exhibited a lower Pd adsorption efficiency. In contrast, $$>$$90% of Pd(II), Ag(I), and Cu(II) were adsorbed by R-BPA over the entire range of HNO$$_{3}$$ concentrations. Structural analyses of the adsorbed metal ions using Fourier transform infrared spectroscopy and extended X-ray absorption fine structure spectroscopy revealed the separation mechanisms of the N-donor-type adsorbents. Pd(II) adsorption on R-IDA, R-Py, and R-BPA occurred via Pd(II) coordination of the functional groups (iminodiacetic acid, pyridine, and bis-picolylamine, respectively), whereas that on R-Amine occurred via anion exchange of NO$$_{3}$$$$^{-}$$ with [Pd(NO$$_{3}$$)$$_{4}$$]$$^{2-}$$. The coordinative adsorption mechanisms resulted in the higher Pd(II) adsorption behaviors of R-IDA, R-Py, and R-BPA. HCl (5.0 M) and thiourea (0.1 M) eluents desorbed 83% of Pd(II) from R-IDA and 95% from R-Py, respectively. R-Py was the most effective Pd(II) adsorbent based on adsorption selectivity and desorption efficiency.

Journal Articles

Speciation and separation of platinum(IV) polynuclear complexes in concentrated nitric acid solutions

Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*

Dalton Transactions (Internet), 50(33), p.11390 - 11397, 2021/09

 Times Cited Count:2 Percentile:20.23(Chemistry, Inorganic & Nuclear)

no abstracts in English

JAEA Reports

Transfer and operation of WSPEEDI-II automatic calculation system for responses to nuclear tests by North Korea

Nemoto, Miho*; Ebine, Noriya; Okamoto, Akiko; Hosaka, Yasuhisa*; Tsuzuki, Katsunori; Terada, Hiroaki; Hayakawa, Tsuyoshi; Togawa, Orihiko

JAEA-Technology 2021-013, 41 Pages, 2021/08

JAEA-Technology-2021-013.pdf:2.52MB

When North Korea has carried out nuclear tests, Nuclear Emergency Assistance and Training Center (NEAT) predicts atmospheric dispersion of radionuclides by using the WSPEEDI-II upon requests from Nuclear Regulation Authority (NRA) and submits the predicted results to NRA in cooperation with Nuclear Science and Engineering Center (NSEC). This is a part of the activity of NEAT supporting the Japanese Government in emergency responses. The WSPEEDI-II automatic calculation system specialized for responses to nuclear tests by North Korea was developed by NSEC and was used for responses to three nuclear tests from February 2013 to September 2017. This report describes the transfer and installation of the calculation system to NEAT, and the subsequent maintenance and operation. Future issues for responses to nuclear tests are also described in this report.

Journal Articles

Solvent extraction of technetium(VII) and rhenium(VII) using a hexaoctylnitrilotriacetamide extractant

Shimojo, Kojiro; Suzuki, Hideya; Yokoyama, Keiichi; Yaita, Tsuyoshi; Ikeda, Atsushi

Analytical Sciences, 36(12), p.1435 - 1437, 2020/12

 Times Cited Count:14 Percentile:65.87(Chemistry, Analytical)

Liquid-liquid extraction for the removal of pertechnetate ($$^{99}$$TcO$$_{4}$$$$^{-}$$) and perrhenate (ReO$$_{4}$$$$^{-}$$) is reported using tripodal extractant $$N,N,N',N',N'',N''$$-hexa-$$n$$-octylnitrilotriacetamide (HONTA) composed of three amide groups and a tertiary amine. The extraction behavior was compared with those using alkyldiamideamines (ADAAM(Oct) and ADAAM(EH)), and the commercial amine-type extractant, trioctylamine (TOA). HONTA quantitatively extracted $$^{99}$$TcO$$_{4}$$$$^{-}$$ and ReO$$_{4}$$$$^{-}$$ in the pH range from 1.0 to 2.5 by co-extraction of protons. Extraction performance of extractants was improved in the order of HONTA $$>$$ ADAAM(Oct) $$>$$ ADAAM(EH) $$>$$ TOA. $$^{99}$$TcO$$_{4}$$$$^{-}$$ and ReO$$_{4}$$$$^{-}$$ in the extracting phase were successfully stripped using neutral aqueous solutions as the receiving phase, and the extraction ability of HONTA was maintained after five repeated uses.

Journal Articles

Lanthanide intra-series separation by a 1,10-phenanthroline derivative; Counterion effect

Simonnet, M.; Suzuki, Shinichi; Miyazaki, Yuji*; Kobayashi, Toru; Yokoyama, Keiichi; Yaita, Tsuyoshi

Solvent Extraction and Ion Exchange, 38(4), p.430 - 440, 2020/00

 Times Cited Count:18 Percentile:68.40(Chemistry, Multidisciplinary)

Journal Articles

Unique anion-exchange properties of 3,3'-diaminobenzidine resulting in high selectivity for rhodium(III) over palladium(II) and platinum(IV) in a concentrated hydrochloric acid solution

Suzuki, Tomoya*; Ogata, Takeshi*; Tanaka, Mikiya*; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi; Narita, Hirokazu*

Analytical Sciences, 35(12), p.1353 - 1360, 2019/12

 Times Cited Count:4 Percentile:16.62(Chemistry, Analytical)

no abstracts in English

Journal Articles

Intercomparison of numerical atmospheric dispersion prediction models for emergency response to emissions of radionuclides with limited source information in the Fukushima Dai-ichi Nuclear Power Plant accident

Iwasaki, Toshiki*; Sekiyama, Tsuyoshi*; Nakajima, Teruyuki*; Watanabe, Akira*; Suzuki, Yasushi*; Kondo, Hiroaki*; Morino, Yu*; Terada, Hiroaki; Nagai, Haruyasu; Takigawa, Masayuki*; et al.

Atmospheric Environment, 214, p.116830_1 - 116830_11, 2019/10

 Times Cited Count:6 Percentile:25.16(Environmental Sciences)

The utilization of numerical atmospheric dispersion prediction (NDP) models for accidental discharge of radioactive substances was recommended by a working group of the Meteorological Society of Japan. This paper is to validate the recommendation through NDP model intercomparison in the accidental release from the Fukushima Dai-ichi Nuclear Power Plant in 2011. Emission intensity is assumed to be constant during the whole forecast period for the worst-case scenario unless time sequence of emission is available. We expect to utilize forecasts of surface air contaminations for preventions of inhalations of radioactive substances, and column-integrated amounts for mitigation of radiation exposure associated with wet deposition. Although NDP forecasts have ensemble spread, they commonly figure out relative risk in space and time. They are of great benefit to disseminating effective warnings to public without failure. The multi-model ensemble technique may be effective to improve the reliability.

Journal Articles

Mechanism of palladium(II) adsorption from nitric acid solutions by a styrene-divinylbenzene copolymer functionalized with $$N,N,N$$-trimethylglycine

Suzuki, Tomoya*; Narita, Hirokazu*; Ogata, Takeshi*; Suzuki, Hideya; Matsumura, Tatsuro; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi

Solvent Extraction Research and Development, Japan, 26(1), p.11 - 19, 2019/06

 Times Cited Count:3 Percentile:13.55(Chemistry, Multidisciplinary)

The ability of AMP03, a styrene-divinylbenzene copolymer functionalized with $$N,N,N$$-trimethylglycine moieties, to adsorb Pd(II) from HNO$$_{3}$$ solutions was investigated to elucidate the affinity of $$N,N,N$$-trimethylglycine for Pd(II). In the present study, we investigated the mechanism of Pd(II) adsorption by AMP03 by means of adsorption experiments, Fourier Transform Infrared (FT-IR) spectroscopy, and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy.

Journal Articles

Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations

Suzuki, Chikashi; Yaita, Tsuyoshi; Suzuki, Shinichi; Pacold, J.*; Altman, A. B.*; Minasian, S. G.*; Tyliszczak, T.*; Shuk, D. K.*; Yoshida, Hiroyuki; Osaka, Masahiko

Journal of Physics and Chemistry of Solids, 127, p.169 - 177, 2019/04

 Times Cited Count:3 Percentile:15.75(Chemistry, Multidisciplinary)

A combined method of NEXAFS measurement and DFT-calculation was employed for Cs evaluation in clay minerals. The Cs M$$_{4,5}$$ NEXAFS spectra of Cs halides were analyzed using the DFT-calculations, and were well reproduced by incorporating the core-hole strength. The Cs M$$_{4,5}$$ NEXAFS spectrum of clay minerals was well-reproduced by the DFT-calculations including the major transitions and tail structures with the established method. The further evaluation of this spectrum by charge density suggests that these major transitions and the tail structures likely reflect bonding states and local environments around the Cs atoms. Comparison of electronic states of Cs in the clay mineral with those in the Cs halides by DFT-calculations has shown that the interaction between Cs and the nearest-neighbor atom is largest in the clay mineral, because the energy level of Cs-5s and 5p is closer to that of O-2s and 2p than the s and p orbitals of other alkali metal and alkali earth metal elements.

Journal Articles

Electrochemical Cs removal and crystal formation from Fukushima weathered biotite in molten NaCl-CaCl$$_{2}$$

Honda, Mitsunori; Goto, Takuya*; Sakanaka, Yoshihide*; Yaita, Tsuyoshi; Suzuki, Shinichi*

AIMS Electronics and Electrical Engineering (Internet), 3(2), p.102 - 110, 2019/03

The possibility of removal and controlling crystal formation from weathered biotite (WB) in clay minerals were investigated using molten salt electrochemistry (EC) in molten NaCl-CaCl$$_{2}$$ under an electrochemical reductive reaction. Cyclic Voltammogram (CV) measurements were performed in the range of +0.5 V to -2.2 V. Several peaks were confirmed in the CV spectra. The peak at -1.4 V represents a reduction reaction of Fe in WB, so we conducted an experiment at -1.4 V for 2 h to reduce Iron (Fe). The Cs removal rate after EC treatment was determined by X-ray fluorescence analysis, and almost 100% Cs removal was confirmed. To understand the effect of the reductive reaction, we performed X-ray Adsorption Fine Structure (XAFS) analysis. Before EC treatment, the Fe in WB was present as a mixture of Fe$$^{3+}$$ and Fe$$^{2+}$$. After EC treatment, the presence of Fe$$^{2+}$$ was confirmed by XAFS analysis. Based on this finding, EC treatment is effective for reducing Fe in WB. This result indicated that Fe$$_{2}$$O$$_{3}$$ formation was suppressed, and the reduction reaction was effective for controlling crystal formation.

Journal Articles

Crack expansion and fracturing mode of hydraulic refracturing from Acoustic Emission monitoring in a small-scale field experiment

Ishida, Tsuyoshi*; Fujito, Wataru*; Yamashita, Hiroto*; Naoi, Makoto*; Fujii, Hirokazu*; Suzuki, Kenichiro*; Matsui, Hiroya

Rock Mechanics and Rock Engineering, 52(2), p.543 - 553, 2019/02

AA2017-0694.pdf:2.54MB

 Times Cited Count:16 Percentile:66.04(Engineering, Geological)

We pressurized and injected water in a hole drilled downward from a floor of the 500 m level gallery in MIU, central Japan. Acoustic emissions (AEs) monitored with 16 sensors in four boreholes located 1 m away from the HF hole exhibited two-dimensional distributions, which likely delineate a crack induced by the fracturing. Expansions of the regions in which AEs occurred were observed only immediately after the first and second BDs. Many AE events in other periods were distributed within the regions where AE events had already occurred. The initial motion polarities of P-waves indicate that tensile-dominant AE events occurred when the regions expanded and they were distributed primarily on the frontiers of the regions where AE events had already occurred. The experimental results suggest that increasing the injection flow rate is effective for generating new cracks in the refracturing, with the new crack expansions being induced by tensile fracturing.

Journal Articles

Complexation properties and structural character of lanthanides complexes of $$O,N$$-hetero donor ligand BIZA

Kobayashi, Toru; Akutsu, Kazuhiro*; Nakase, Masahiko*; Suzuki, Shinichi; Shiwaku, Hideaki; Yaita, Tsuyoshi

Separation Science and Technology, 54(13), p.2077 - 2083, 2019/02

 Times Cited Count:5 Percentile:21.84(Chemistry, Multidisciplinary)

Development of separation reagent, which can efficiently separate lanthanides, is of increasing importance because it concerns establishment of purification and recycle techniques rare-earth elements. In our research group, several hetero donor type ligands, which have both oxygen and heterocyclic nitrogen atoms as donor atoms, were developed and revealed that this type of ligands show the selective complexation with specific lanthanide. In this paper, we will discuss the lanthaides complexation properties of the hetero donor type ligand containing benzimidazole group as nitrogen donor ($$N$$-methyl-$$N$$-phenyl-2-(1$$H$$-benzimidazol-2-yl)-pyridine-6-carboxamide) based on structural investigation by crystallography.

Journal Articles

Quantitative analysis of Cs extraction by some dialkoxycalix[4]arene-crown-6 extractants

Simonnet, M.; Miyazaki, Yuji*; Suzuki, Shinichi; Yaita, Tsuyoshi

Solvent Extraction and Ion Exchange, 37(1), p.81 - 95, 2019/00

 Times Cited Count:5 Percentile:21.38(Chemistry, Multidisciplinary)

Journal Articles

Cesium liquid-liquid extraction by calix-crown ethers; Solvent effect

Simonnet, M.; Miyazaki, Yuji; Suzuki, Shinichi; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.66 - 69, 2018/11

Journal Articles

Absorbent property of fullerene for cesium isotope separation investigated using X-ray photoelectron spectroscopy

Sekiguchi, Tetsuhiro; Yokoyama, Keiichi; Uozumi, Yuki*; Yano, Masahiro; Asaoka, Hidehito; Suzuki, Shinichi; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.161 - 164, 2018/11

For nuclear transmutation of cesium-135 ($$^{135}$$Cs), which is long-lived fission product, we are developing selective absorbent which takes only Cs atom in, but does not CsI. In this study, absorbing property of Cs atom onto the surface of fullerene (C$$_{60}$$) film has been investigated using synchrotron-based angle-dependent X-ray photoelectron spectroscopy (XPS). The results were compared with those of CsI. It was found that Cs penetrates into C$$_{60}$$ deep bulk. In contrast, CsI deposits on shallow surface. Furthermore, XPS spectra were measured as a function of Ar$$^{+}$$-sputtering time in order to know Cs concentration profiles in deep region. Results showed that Cs penetrates into deep region of several hundreds ${AA}$.

Journal Articles

Characteristics of TPDN/SiO$$_{2}$$-P adsorbent for MA(III) recovery

Kofuji, Hirohide; Watanabe, So; Takeuchi, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.61 - 65, 2018/11

Journal Articles

Lanthanides complexation properties of O, N-hetero donor ligand PTA

Kobayashi, Toru; Suzuki, Shinichi; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.74 - 77, 2018/11

Development of extractant, which can efficiently separate actinides, is of increasing importance because it concerns establishment and simplification of separation techniques in nuclear fuel cycle and decontamination of radioactive wastes. In this study, the complexation properties of N-alkyl-N-phenyl-1,10-phenanthroline-2-carboxamide (PTA) with trivalent lanthanides (Ln$$^{3+}$$) were investigated based on structural analysis by using X-ray crystallography and extended X-ray absorption fine structure (EXAFS) methods. As a result, it is revealed that two PTA molecules coordinate with Ln$$^{3+}$$ as tridentate ligand via two nitrogen in phenanthroline moiety and one oxygen in amide moiety in both crystal and solution states. The slight difference in coordination bond distances are observed between Eu$$^{3+}$$ and Nd$$^{3+}$$ complexes, this difference corresponds to the difference in ionic radius between Nd$$^{3+}$$ and Eu$$^{3+}$$. This result indicates slight difference in ionic radii of Ln$$^{3+}$$ hardly affects coordination properties of PTA.

JAEA Reports

Activities on predictions of atmospheric dispersion of radionuclides for nuclear tests by North Korea

Ishizaki, Shuhei; Hayakawa, Tsuyoshi; Tsuzuki, Katsunori; Terada, Hiroaki; Togawa, Orihiko

JAEA-Technology 2018-007, 43 Pages, 2018/10

JAEA-Technology-2018-007.pdf:5.67MB

When North Korea has carried out a nuclear test, by a request from Nuclear Regulation Authority (NRA), Nuclear Emergency Assistance and Training Center (NEAT) predicts atmospheric dispersion of radionuclides by WSPEEDI-II system in cooperation with Nuclear Science and Engineering Center (NSEC), and submits the predicted results to NRA as the activity to assist responses by the Japanese Government. This report explains frameworks of the Japanese Government and Japan Atomic Energy Agency (JAEA) to cope with nuclear tests by North Korea, and describes a series of activities by NEAT regarding predictions of atmospheric dispersion of radionuclides in response to the 5th and 6th nuclear tests carried out by North Korea in September 2016 and September 2017. Future plans and issues to be solved for responses to nuclear tests are also described in this report, together with an outline of a computer program system used in the predictions.

Journal Articles

Speciation of ruthenium(III) chloro complexes in hydrochloric acid solutions and their extraction characteristics with an amide-containing amine compound

Suzuki, Tomoya*; Ogata, Takeshi*; Tanaka, Mikiya*; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi; Narita, Hirokazu*

Metals, 8(7), p.558_1 - 558_10, 2018/07

AA2018-0670.pdf:2.11MB

 Times Cited Count:13 Percentile:55.72(Materials Science, Multidisciplinary)

The refining of platinum group metals is based mainly on solvent extraction methods, whereas Ru is selectively recovered by distillation as RuO$$_4$$. Replacement of distillation byextraction is expected to simplify the purification process. To develop an effective extraction system for Ru, we analyzed the Ru species in HCl with UV-Vis and EXAFS spectroscopies, and we examined the properties of Ru extracted with N-2-ethylhexyl-bis(N-di-2-ethylhexyl-ethylamide) amine (EHBAA). EXAFS and UV-Vis spectra of Ru in HCl solutions revealed that the predominant Ru species in 0.5-10 M HCl solutions changed from [RuCl$$_4$$(H$$_2$$O)$$_2$$]$$^-$$ to [RuCl$$_6$$]$$^3$$$$^-$$ with the HCl concentration. The extraction percentages of Ru in the EHBAA system increased with increasing HCl concentration, reached 80% at [HCl] = 5 M, and decreased athigher HCl concentrations. EXAFS analysis of the extracted complex indicated that the Ru$$^3$$$$^+$$ had 5 Cl$$^-$$ and 1 H$$_2$$O in its inner coordination sphere. The similarity of the dependence on HCl concentrations of the extraction in the EHBAA system and the distribution profile of [RuCl$$_5$$(H$$_2$$O)]$$^2$$$$^-$$ on [RuCl$$_n$$(H$$_2$$O)$$_6$$$$_-$$$$_n$$]$$^3$$$$^-$$$$^n$$ suggested that the EHBAA extracted the pentachlorido species.

348 (Records 1-20 displayed on this page)