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Journal Articles

Formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd$$_{3+x}$$ using cadmium chloride

Hayashi, Hirokazu; Shibata, Hiroki; Sato, Takumi; Otobe, Haruyoshi

Journal of Radioanalytical and Nuclear Chemistry, 8 Pages, 2023/00

 Times Cited Count:0

The formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu$$_3$$-type GdPd$$_{3.3}$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) and NpPd$$_3$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi$$_3$$-type NpPd$$_3$$. Chlorination of the MPd$$_{3+x}$$ (M = Gd, Np) samples was accomplished by the solid-state reaction using cadmium chloride at 673 K in a dynamic vacuum. Pd-rich solid solution phase saturated with Cd and an intermetallic compound PdCd were obtained as by-products of MCl$$_3$$ formation.

Journal Articles

The Formation mechanism of radiocesium-bearing microparticles derived from the Fukushima Daiichi Nuclear Power Plant using electron microscopy

Hagiwara, Hiroki; Kondo, Keietsu; Hidaka, Akihide

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5905 - 5914, 2022/12

 Times Cited Count:1 Percentile:71.47(Chemistry, Analytical)

Journal Articles

Design of MA(III)/Ln(III) separation process of extraction chromatography technology

Akuzawa, Tadashi*; Kim, S.-Y.*; Kubota, Masahiko*; Wu, H.*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5851 - 5858, 2022/12

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

Journal Articles

Potential bacterial alteration of nuclear fuel debris; A Preliminary study using simulants in powder and pellet forms

Liu, J.; Dotsuta, Yuma; Sumita, Takehiro; Kitagaki, Toru; Onuki, Toshihiko; Kozai, Naofumi

Journal of Radioanalytical and Nuclear Chemistry, 331(6), p.2785 - 2794, 2022/06

 Times Cited Count:2 Percentile:0.01(Chemistry, Analytical)

Remnant nuclear fuel debris in the damaged nuclear reactors at the Fukushima Daiichi Nuclear Power Plant (FDNPP) has contacted the groundwater containing microorganisms for over ten years. Herein, we report the possibility of bacterial alteration of fuel debris. We investigated the physical and chemical changes of fuel debris simulants (FDS) in the powder and pellet forms via exposure to two ubiquitous bacteria, Pseudomonas fluorescens and Bacillus subtilis. In the experiments using FDS composed of the powders of Fe(0), solid solution of CeO$$_{2}$$ and ZrO$$_{2}$$, and SiO$$_{2}$$, Ce, Zr, and Si were hardly dissolved, while Fe was dissolved, a fraction of the dissolved Fe was present in the liquid phase as Fe(II) and Fe(III), and the rest was precipitated as the nano-sized particles of iron (hydr)oxides. In the experiment using P. fluorescens and FDS pellet pieces prepared by melting the Fe(0) particles and solid solution of CeO$$_{2}$$ and ZrO$$_{2}$$, the bacteria selectively gathered on the Fe(0) particle surface and made corrosion pits. These results suggest that bacteria in groundwater corrode the iron in fuel debris at FDNPP, change fuel debris into porous one, releasing the nano-sized iron (hydr)oxide particles into the water.

Journal Articles

Sorption of Pu(IV) on biogenic Mn oxide and complexation of Pu(IV) with organic ligands secreted by fungal cells

Tanaka, Kazuya; Tani, Yukinori*; Kozai, Naofumi; Onuki, Toshihiko

Journal of Radioanalytical and Nuclear Chemistry, 331(2), p.1109 - 1114, 2022/02

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

We investigated the sorption of Pu(IV) on biogenic Mn oxide produced by Mn(II)-oxidizing fungus. The sorption of Pu(IV) on biogenic Mn oxide was similar to that of U(VI) and different from that of Th(IV), possibly due to oxidation of Pu(IV) to Pu(VI). When Pu(IV) was sorbed on hyphae only, it was desorbed into the solution phase over time. Pu(IV) could be solubilized by complexation with organic ligands secreted by fungal cells. In particular, Pu(IV) desorption was observed under circumneutral pH conditions.

Journal Articles

Characterization of radiocesium-bearing microparticles with different morphologies in soil around the Fukushima Daiichi Nuclear Power Plant

Hagiwara, Hiroki; Funaki, Hironori; Shiribiki, Natsu*; Kanno, Marina*; Sanada, Yukihisa

Journal of Radioanalytical and Nuclear Chemistry, 331(1), p.415 - 426, 2022/01

 Times Cited Count:3 Percentile:68.44(Chemistry, Analytical)

Journal Articles

Large scale production of $$^{64}$$Cu and $$^{67}$$Cu via the $$^{64}$$Zn(n, p)$$^{64}$$Cu and $$^{68}$$Zn(n, np/d)$$^{67}$$Cu reactions using accelerator neutrons

Kawabata, Masako*; Motoishi, Shoji*; Ota, Akio*; Motomura, Arata*; Saeki, Hideya*; Tsukada, Kazuaki; Hashimoto, Shintaro; Iwamoto, Nobuyuki; Nagai, Yasuki*; Hashimoto, Kazuyuki*

Journal of Radioanalytical and Nuclear Chemistry, 330(3), p.913 - 922, 2021/12

 Times Cited Count:1 Percentile:30.57(Chemistry, Analytical)

Both $$^{64}$$Cu and $$^{67}$$Cu are promising radionuclides in nuclear medicine. Production yields of these radionuclides were quantified by irradiating 55.4 g of natural zinc with accelerator neutrons. Clinically suitable $$^{64}$$Cu and $$^{67}$$Cu yields were estimated by experimental based numerical simulations using 100 g of enriched $$^{64}$$Zn and $$^{68}$$Zn, respectively, and elevated neutron fluxes from 40 MeV, 2 mA deuterons. A combined thermal- and resin-separation method was developed to isolate $$^{64}$$Cu and $$^{67}$$Cu from zinc, resulting in 73% separation efficiency and 97% zinc recovery. Such methods can provide large scale production of $$^{64}$$Cu and $$^{67}$$Cu for clinical applications.

Journal Articles

Diffusion of acetic acid, butyric acid, and butanol in compacted montmorillonite

Ishidera, Takamitsu

Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.149 - 158, 2021/10

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

Journal Articles

Development of MA separation process with TEHDGA/SiO$$_{2}$$-P for an advanced reprocessing

Horiuchi, Yusuke; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Kida, Fukuka*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.237 - 244, 2021/10

 Times Cited Count:1 Percentile:30.57(Chemistry, Analytical)

Applicability of tetra2-ehylhexyl diglycolamide (TEHDGA) impregnated adsorbent for minor actinide (MA) recovery from high level liquid waste (HLLW) in extraction chromatography technology was investigated through batch-wise adsorption and column separation experiments. Distribution ratio of representative fission product elements were obtained by the batch-wise experiments, and TEHDGA adsorbent was shown to be preferable to TODGA adsorbent for decontamination of several species. All Ln(III) supplied into the TEHDGA adsorbent packed column was properly eluted from the column, and the applicability of the adsorbent was successfully showed by this study.

Journal Articles

Density functional study on Am(III)/Eu(III) selectivity using crown ether type ligands

Fukasawa, Yuto*; Kaneko, Masashi; Nakashima, Satoru*

Journal of Radioanalytical and Nuclear Chemistry, 329(1), p.77 - 84, 2021/07

 Times Cited Count:1 Percentile:30.57(Chemistry, Analytical)

Density functional theory calculations were applied to understand the selectivity between Am$$^{3+}$$ and Eu$$^{3+}$$ ions with the crown ethers type ligands. 18C6 is predicted to form the most stable complex with Eu$$^{3+}$$ and show the higher stability for Am$$^{3+}$$ over Eu$$^{3+}$$, being consistent with previously reported Am$$^{3+}$$/Eu$$^{3+}$$ selectivity. We modeled N- and S-donor complexes by using framework of 18C6 complex and analyzed the complexation Gibbs energies, indicating that 18C6 with N-donor atoms is suitable for both complexation and higher Am$$^{3+}$$ stability over Eu$$^{3+}$$ due to the stronger covalent interaction.

Journal Articles

Factors affecting $$^{137}$$Cs concentrations in river water under base-flow conditions near the Fukushima Dai-ichi Nuclear Power Plant

Nakanishi, Takahiro; Funaki, Hironori; Sakuma, Kazuyuki

Journal of Radioanalytical and Nuclear Chemistry, 328(3), p.1243 - 1251, 2021/06

 Times Cited Count:3 Percentile:53.86(Chemistry, Analytical)

To confirm factors affecting $$^{137}$$Cs concentration in river water after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, this study conducted monthly observations of nine rivers near the FDNPP from April 2017 to March 2018 under base-flow conditions. The annual mean dissolved and particulate $$^{137}$$Cs concentrations correlated well with the mean $$^{137}$$Cs deposition in the catchment. The normalized $$^{137}$$Cs concentrations in both phases by dividing by the mean $$^{137}$$Cs deposition in the catchment showed significant negative correlations with the $$^{137}$$Cs deposition ratio for forests. The inflow from the downstream plain areas increased the $$^{137}$$Cs concentrations near the FDNPP.

Journal Articles

Age determination analysis of a single uranium particle for safeguards

Suzuki, Daisuke; Tomita, Ryohei; Tomita, Jumpei; Esaka, Fumitaka; Yasuda, Kenichiro; Miyamoto, Yutaka

Journal of Radioanalytical and Nuclear Chemistry, 328(1), p.103 - 111, 2021/04

 Times Cited Count:2 Percentile:30.57(Chemistry, Analytical)

An analytical technique was developed to determine the age of uranium particles for safeguards. After the chemical separation of uranium and thorium, the $$^{230}$$Th/$$^{234}$$U ratio was measured using single-collector inductively coupled plasma mass spectrometry and a $$^{233}$$U-based reference material comprising a certain amount of $$^{229}$$Th as a progeny nuclide of $$^{233}$$U. The results allowed us to determine the purification age of two certified materials, i.e., U-850 and U-100, which was in good agreement with the reference purification age (61 y). Moreover, the age of a single U-850 particle was determined with a difference of -28 to 2 years from the reference date.

Journal Articles

Effect on $$^{99}$$Mo-adsorption/$$^{99m}$$Tc-elution properties of alumina with different surface structures

Fujita, Yoshitaka; Seki, Misaki; Sano, Tadafumi*; Fujihara, Yasuyuki*; Kitagawa, Tomoya*; Matsukura, Minoru*; Hori, Junichi*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko

Journal of Radioanalytical and Nuclear Chemistry, 327(3), p.1355 - 1363, 2021/03


 Times Cited Count:1 Percentile:30.57(Chemistry, Analytical)

We prepared three types of Al$$_{2}$$O$$_{3}$$ with different surface structures and investigated $$^{99}$$Mo-adsorption/$$^{99m}$$Tc-elution properties using [$$^{99}$$Mo]MoO$$_{3}$$ that was irradiated in the Kyoto University Research Reactor. Al$$_{2}$$O$$_{3}$$ adsorbed [$$^{99}$$Mo]molybdate ions in solutions at different pH; the lower was the pH, the higher was the Mo-adsorption capacity of Al$$_{2}$$O$$_{3}$$. The $$^{99m}$$Tc-elution properties of molybdate ion adsorbed Al$$_{2}$$O$$_{3}$$ were elucidated by flowing saline. Consequently, it was suggested that $$^{99}$$Mo-adsorption/desorption properties are affected by the specific surface of Al$$_{2}$$O$$_{3}$$ and $$^{99m}$$Tc-elution properties are affected by the crystal structure of Al$$_{2}$$O$$_{3}$$.

Journal Articles

Prediction of thermodynamic data for radium suitable for thermodynamic database for radioactive waste management using an electrostatic model and correlation with ionic radii among alkaline earth metals

Kitamura, Akira; Yoshida, Yasushi*

Journal of Radioanalytical and Nuclear Chemistry, 327(2), p.839 - 845, 2021/02

 Times Cited Count:2 Percentile:53.86(Chemistry, Analytical)

Thermodynamic data for radium for radioactive waste management have been predicted using an electrostatic model and correlation with the ionic radii of the alkaline earth metals. Estimation of the standard Gibbs free energy of formation and standard molar entropy of aqueous radium species and compounds has been based on such approaches as extrapolation of the thermodynamic properties of strontium and barium, and use of a model of ion pair formation. The predicted thermodynamic data for radium have been compared with previously reported values.

Journal Articles

Determination of alkali and alkaline earth elements in radioactive waste generated from reprocessing plant by liquid electrode plasma optical emission spectrometry

Yamamoto, Masahiko; Do, V. K.; Taguchi, Shigeo; Kuno, Takehiko; Takamura, Yuzuru*

Journal of Radioanalytical and Nuclear Chemistry, 327(1), p.433 - 444, 2021/01

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

A simple, practical, and reliable analytical method for determination of Na, K, Ca, Sr, and Ba by liquid electrode plasma optical emission spectrometry is developed. Appropriate emission lines for quantification, interferences from co-existing elements, and effect of measurement conditions with cell damage have been investigated. The spike and recovery tests using actual sample have been performed for method validation, and negligible sample matrix effect has been observed. Consequently, the method is successfully applied to several radioactive wastes. The obtained data have been agreed well with data from computer calculation and inductively coupled plasma optical emission spectrometry within 10% difference.

Journal Articles

Trichotomic separation of light and heavy lanthanides and Am by batchwise multi-stage extractions using TODGA

Matsumiya, Masahiko*; Tsuchida, Yusuke*; Sasaki, Yuji; Ono, Ryoma*; Nakase, Masahiko*; Takeshita, Kenji*

Journal of Radioanalytical and Nuclear Chemistry, 327(1), p.597 - 607, 2021/01

 Times Cited Count:1 Percentile:17.77(Chemistry, Analytical)

To achieve trichotomic separation of light lanthanides (Ln), heavy Ln, and Am, batchwise multi-stage extractions using tetraoctyl-diglycolamide (TODGA) extractant from organic acids are studied. Malonic acid (MA) has high solubility in water and is used as the main component of the aqueous phase. It is clear that the separation factor (SF) for Nd/Am from MA and that for La/Am from MA + HNO$$_{3}$$ are both around 30. The light Ln (e.g., La and Ce) flowed-out in 1 M MA+0.05 M HNO$$_{3}$$ (1st soln.), Am is recovered into 3 M MA (2nd soln.), and middle and heavy Ln (Nd and other heavy Ln) are back-extracted into 0.1 M TEDGA/water (3rd soln.). This extraction method can give 95% recovery of Am with total Ln of less than 16% present in high-level radioactive waste.

Journal Articles

Development of HCl-free solid phase extraction combined with ICP-MS/MS for rapid assessment of difficult-to-measure radionuclides, 1; Selective measurement of $$^{93}$$Zr and $$^{93}$$Mo in concrete rubble

Do, V. K.; Furuse, Takahiro; Murakami, Erina; Aita, Rena; Ota, Yuki; Sato, Soichi

Journal of Radioanalytical and Nuclear Chemistry, 327(1), p.543 - 553, 2021/01

 Times Cited Count:4 Percentile:78.24(Chemistry, Analytical)

A new HCl-free chromatographic separation procedure has been developed for sequential separation of Zr and Mo from concrete matrices. Accordingly, $$^{93}$$Zr and $$^{93}$$Mo could be sensitively and selectively measured by ICP-MS/MS using ammonia reaction gas. The recoveries of greater than 90% for Zr and Mo from concretes could be achieved. The measurement condition was optimized for complete suppression of interferences from $$^{93}$$Nb and peak tailing from abundant isotopes of Zr and Mo in concrete matrices. The removal of interferences was verified by measurement of radio-contamination-free concretes used as a sample matrix blank. Method detection limits of 1.7 mBq g$$^{-1}$$ and 0.2 Bq g$$^{-1}$$ were achieved for $$^{93}$$Zr and $$^{93}$$Mo, respectively, in the concrete matrices. The interference removal factor for Nb (equivalent to the decontamination factor in radiochemical separation) was of the order of 10$$^{5}$$, and the abundance sensitivity was of the order of 10$$^{-8}$$, indicating that the developed method is reliable for verifying the presence of ultralow concentrations of $$^{93}$$Zr and $$^{93}$$Mo. The present method is suitable for the rapid assessment of $$^{93}$$Zr and $$^{93}$$Mo for radioactivity inventory of concrete rubble.

Journal Articles

Analytical method for the determination of $$^{211}$$At using an $$alpha$$-scintillation-camera system and thin-layer chromatography

Segawa, Mariko; Nishinaka, Ichiro*; Toh, Yosuke; Maeda, Makoto

Journal of Radioanalytical and Nuclear Chemistry, 326(1), p.773 - 778, 2020/10

 Times Cited Count:1 Percentile:17.77(Chemistry, Analytical)

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:17.77(Chemistry, Analytical)

Journal Articles

Measurement of cesium isotopic ratio by thermal ionization mass spectrometry for neutron capture reaction studies on $$^{135}$$Cs

Shibahara, Yuji*; Nakamura, Shoji; Uehara, Akihiro*; Fujii, Toshiyuki*; Fukutani, Satoshi*; Kimura, Atsushi; Iwamoto, Osamu

Journal of Radioanalytical and Nuclear Chemistry, 325(1), p.155 - 165, 2020/07

 Times Cited Count:6 Percentile:67.23(Chemistry, Analytical)

The measurements of isotopic ratios of Cs samples by thermal ionization mass spectrometry were performed for the analysis of their samples used to evaluate nuclear data obtained for $$^{135}$$Cs. To obtain a high intensity and stable ion beam, the effects of additive agents on the ionization of Cs were examined. The effect of silicotungstic acid on the ionization of Cs was the largest among the additive agents studied in the present study, while the silicotungstic acid also showed the largest isobaric interference of polyatomic ions. It was demonstrated that as small as 2$$times$$10$$^{-13}$$ g of a Cs sample was sufficient to achieve the analytical precision required to measure the $$^{135}$$Cs/$$^{137}$$Cs ratio in the case where an additive agent of TaO/glucose was employed. After examining of the analytical conditions, such as the interference effect due to Ba, the measurements of the isotopic ratios of two Cs samples used in our study using TIMS were conducted, and it was discussed how much the ratios contributed to evaluation of the neutron capture cross-section of $$^{135}$$Cs.

254 (Records 1-20 displayed on this page)