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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

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:0

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:0 Percentile:0.02(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:0 Percentile:0.02(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:0 Percentile:0.02(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:0 Percentile:0.02(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

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:0 Percentile:0.02(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:42.23(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:0.01(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:0 Percentile:0.01(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.

Journal Articles

Sorption behavior of selenide on montmorillonite

Sugiura, Yuki; Tomura, Tsutomu*; Ishidera, Takamitsu; Doi, Reisuke; Francisco, P. C. M.; Shiwaku, Hideaki; Kobayashi, Toru; Matsumura, Daiju; Takahashi, Yoshio*; Tachi, Yukio

Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05

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

Journal Articles

Cesium concentrations in various environmental media at Namie, Fukushima

Heged$"u$s, M.*; Shiroma, Yoshitaka*; Iwaoka, Kazuki*; Hosoda, Masahiro*; Suzuki, Takahito*; Tamakuma, Yuki*; Yamada, Ryohei; Tsujiguchi, Takakiyo*; Yamaguchi, Masaru*; Ogura, Koya*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 323(1), p.197 - 204, 2020/01

 Times Cited Count:3 Percentile:58.77(Chemistry, Analytical)

The radioactivity of cesium in the water and sediments of two major rivers was measured along with airborne radioactivity in Namie Town, after the recent partial lift on the evacuation order in 2017. The observed concentrations were up to 384 $$pm$$ 11 mBq/L for $$^{137}$$Cs in unfiltered water and 1.28 $$pm$$ 0.09 mBq/m$$^{3}$$ for $$^{137}$$Cs in air, while the sediment had a maximum of 44900 $$pm$$ 23.4 Bq/kg for $$^{137}$$Cs. The $$^{134}$$Cs/$$^{137}$$Cs ratios indicate the main origin of the cesium in the sediment to be Unit 1 in good agreement with previous reports on the accident.

Journal Articles

Improvement in flow-sheet of extraction chromatography for trivalent minor actinides recovery

Watanabe, So; Senzaki, Tatsuya; Shibata, Atsuhiro; Nomura, Kazunori; Takeuchi, Masayuki; Nakatani, Kiyoharu*; Matsuura, Haruaki*; Horiuchi, Yusuke*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 322(3), p.1273 - 1277, 2019/12

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

Journal Articles

Repeatability and reproducibility of measurements of low dissolved radiocesium concentrations in freshwater using different pre-concentration methods

Kurihara, Momo*; Yasutaka, Tetsuo*; Aono, Tatsuo*; Ashikawa, Nobuo*; Ebina, Hiroyuki*; Iijima, Takeshi*; Ishimaru, Kei*; Kanai, Ramon*; Karube, Jinichi*; Konnai, Yae*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 322(2), p.477 - 485, 2019/11

 Times Cited Count:2 Percentile:24.18(Chemistry, Analytical)

We assessed the repeatability and reproducibility of methods for determining low dissolved radiocesium concentrations in freshwater in Fukushima. Twenty-one laboratories pre-concentrated three of 10 L samples by five different pre-concentration methods (prussian-blue-impregnated filter cartridges, coprecipitation with ammonium phosphomolybdate, evaporation, solid-phase extraction disks, and ion-exchange resin columns), and activity of radiocesium was measured. The z-scores for all of the $$^{137}$$Cs results were within $$pm$$2, indicating that the methods were accurate. The relative standard deviations (RSDs) indicating the variability in the results from different laboratories were larger than the RSDs indicating the variability in the results from each separate laboratory.

Journal Articles

Studies on processes for recovering uranium from sediment wastes

Ohashi, Yusuke; Ikeda, Yasuhisa*

Journal of Radioanalytical and Nuclear Chemistry, 321(2), p.683 - 691, 2019/08

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

Sediment waste generated from the waste solution of uranium handling facilities contains uranium and iron. In this study, we examined methods to selectively separate uranium from the waste without using nitric acid. Uranium dissolved in 0.5 $$ sim$$ 2.5M sulfuric acid, 1M hydrochloric acid, and 5M perchloric acid was selectively precipitated by adding oxalic acid. In addition, when oxalic acid and NCP are added together in 2.5M sulfuric acid, it seems that new insoluble uranium compounds are formed. Consequently, precipitation ratios of uranium was improved. Uranium was selectively precipitated from the sulfuric acid solution containing Fe and Al, and the precipitation ratio of uranium became 99%.

Journal Articles

Optimization of an isothermal gas-chromatographic setup for the chemical exploration of dubnium (Db, Z = 105) oxychlorides

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Ito, Yuta; Shirai, Kaori*; Suzuki, Hayato; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; et al.

Journal of Radioanalytical and Nuclear Chemistry, 320(3), p.633 - 642, 2019/06

 Times Cited Count:1 Percentile:24.18(Chemistry, Analytical)

An isothermal gas-chromatographic (IGC) device has been developed and tested for on-line gas phase studies of volatile oxychlorides of short-lived group-5 transition metals. Radioisotopes of niobium and tantalum, produced in nuclear fusion evaporation reactions, are directly flushed into the IGC setup by an inert gas-jet. Oxychloride compounds are formed by the addition of SOCl$$_2$$ and O$$_2$$. Parameters influencing the formation and transport of NbOCl$$_3$$ and TaOCl$$_3$$ are investigated. For nuclides with half-lives ($$t_{1/2}$$) of about 30 s, an overall efficiency of 7% is obtained, rendering the IGC setup suitable for the chemical exploration of $$^{262}$$Db($$t_{1/2}$$ = 34s).

Journal Articles

Low $$^{137}$$Cs retention capability of organic layers in Japanese forest ecosystems affected by the Fukushima nuclear accident

Koarashi, Jun; Atarashi-Andoh, Mariko

Journal of Radioanalytical and Nuclear Chemistry, 320(1), p.179 - 191, 2019/04

 Times Cited Count:11 Percentile:91.93(Chemistry, Analytical)

To quantify the $$^{137}$$Cs retention behavior in forest-floor organic layers in relation to the litter dynamics, litter samples were collected at five forest sites in Fukushima in 2011 and 2015, and separated into eight fractions with different precursor species and degrees of degradation; afterward, $$^{137}$$Cs inventory was determined in each litter fraction. The ecological half-lives of $$^{137}$$Cs in the litter fractions were estimated to be from 0.7 to 4.4 years and found to depend not on the sampling site but rather on the precursor species of the litter materials. Broadleaf- and pine-needle-originated litter fractions exhibited shorter ecological half-lives of $$^{137}$$Cs, while those of cedar-originated and finely fragmented litter fractions were longer. The results suggested that the organic layers in Japanese forest ecosystems have a low $$^{137}$$Cs retention capability, although it differs depending on the forest type.

Journal Articles

Secondary radiocesium contamination of agricultural products by resuspended matter

Nihei, Naoto*; Yoshimura, Kazuya; Okumura, Taiga*; Tanoi, Keitaro*; Iijima, Kazuki; Kogure, Toshihiro*; Nakanishi, Tomoko*

Journal of Radioanalytical and Nuclear Chemistry, 318(1), p.341 - 346, 2018/10

 Times Cited Count:1 Percentile:18.37(Chemistry, Analytical)

Journal Articles

Correlation between Am(III)/Eu(III) selectivity and covalency in metal-chalcogen bonds using density functional calculations

Kaneko, Masashi; Watanabe, Masayuki

Journal of Radioanalytical and Nuclear Chemistry, 316(3), p.1129 - 1137, 2018/06

BB2017-0005.pdf:0.86MB

 Times Cited Count:12 Percentile:90(Chemistry, Analytical)

We applied density functional theory calculations to Am(III) and Eu(III) complexes with chalcogen-donor ligands of the formula N(EPMe$$_{2}$$)$$_{2}$$$$^{-}$$ (E = O, S, Se, Te). We calculated the equilibrium structures and relative stabilities of the complexes in the complexation reaction. The results indicated that the tendency of the relative stability is O $$ll$$ S $$sim$$ Se $$sim$$ Te, which is consistent with the trend of soft acid classification. Molecular orbital overlap population analysis suggested that this tendency can be correlated with the bonding type in the covalent interaction between the f-orbitals of the metal atom and the chalcogen-donor atoms.

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