Matsueda, Makoto; Aoki, Jo; Koarai, Kazuma; Terashima, Motoki; Takagai, Yoshitaka*
Analytical Sciences, 38(11), p.1371 - 1376, 2022/11
The I analysis using ICP-MS is challenging caused by xenon-129 (Xe) and IH generated from excess stable isotope I. In this study, mass discrimination between iodine-129 (I) and interfering substances was achieved by inductively coupled plasma-tandem quadrupole mass spectrometry (ICP-MS/MS) with a dynamic reaction cell introduced a mixture gas of O and CO. As a result, the ratio of (background noise intensity at m/z 129)/I was 3.8 10 and 10 mBq/L of I was analyzed without chemical separation in the presence of 100 mg/L stable I. Spiked tests with actual rainwater were performed, and obtained values were agreed with the spiked amounts.
Shimojo, Kojiro; Fujiwara, Iori*; Oshima, Tatsuya*; Yokoyama, Keiichi; Yaita, Tsuyoshi
Analytical Sciences, 38(7), p.1003 - 1006, 2022/07
Liquid-liquid extraction of lanthanide (Ln) ions was investigated using -dioctylthiodiglycolamic acid (DOTDGAA), which is a sulfur donor ligand with an amide group and a carboxyl group connected by a thioether chain. The extraction performance and selectivity of DOTDGAA for Ln ions were compared with those of -dioctyldiglycolamic acid (DODGAA), which is also an oxygen donor ligand with a similar chemical structure, to assess the effect of the soft/hard donor atom on Ln separation. DOTDGAA quantitatively extracted all Ln ions while being selective toward light and middle Ln ions, in contrast to the selectivity of DODGAA for heavier Ln ions. Slope analysis demonstrated that the Ln transfer using DOTDGAA proceeded through a proton-exchange reaction, forming a 1:3 complex, Ln(DOTDGAA). The back-extraction of Ln ions from the extracting phase was successfully achieved under acidic conditions.
Ouchi, Kazuki; Tsukahara, Takehiko*; Brandt, A.*; Muto, Yuki*; Nabatame, Nozomi*; Kitatsuji, Yoshihiro
Analytical Sciences, 37(12), p.1789 - 1794, 2021/12
We attempted to scale down a separation process of uranium (U) using the microchip column loaded with anion exchange resin to develop safety and waste-reducing separation technique. The ideal separation performance of U was obtained by the properly design of a microchannel. The concentration of U in seawater as a real-world sample could be quantified with the prepared microchip column. It indicates that the microchip column is sufficiently practical. Compared to separation of U with a general column, the column size was successfully scaled down to 1/5000.
Yomogida, Takumi; Saeki, Morihisa*; Morii, Shiori; Oba, Hironori*; Kitatsuji, Yoshihiro
Analytical Sciences, 37(12), p.1843 - 1846, 2021/12
In this study, we developed a simple and one-step Pd separation technique based on photoreduction with Xe lamp irradiation for the determination of Pd in highly radioactive samples. A simulated high-level radioactive liquid wastes (HLLW) solution, which consists of 14 major elements (Rb, Sr, Zr, Mo, Ru, Rh, Pd, Cs, Ba, La, Ce, Pr, Nd, Sm) in a 3 mol L HNO solution, was used to evaluate the separation performance. The Pd precipitate were formed by Xe lamp irradiation and recovered by centrifugation. The results showed that the recovery of Pd from a simulated HLLW solution depend on the irradiation time and concentration of ethanol. By optimizing the conditions at photo irradiation, the Pd recovery from the simulated HLLW solution reached up to 50 %, while 99.5 % of the other 13 elements were separated. The Pd precipitate could be separated from the elements that are the main source of radioactivity (Sr, Cs, and Ba) and the source of spectral interference for the determination of Pd (Zr, and Ru). These results indicate that selective separation of Pd is achieved with the proposed method, showing the applicability of the proposed separation technique to HLLW samples.
Matsutani, Takafumi; Sasaki, Yuji; Katsuta, Shoichi*
Analytical Sciences, 37(11), p.1603 - 1609, 2021/11
We investigated the chemical behavior of lanthanides (Ln) using diglycolamide extractant with multistage extraction. We obtained the breakthrough curves for light and middle Ln. Our study reveals that the metal extraction limit depends on their values and metal concentrations used in the experiments. From the multistage extractions of 15 aqueous phases and 15 organic phases, three curves (extraction curves, back-extraction curves, and separation curves) were obtained by changing the nitric acid concentration. As an example, under a condition of the separation curve experiment (aqueous phase: 0.5 M HNO, organic phase: 0.1 M TDDGA (-tetradecyl-diglycolamide) in -dodecane), a recovery of more than 99% of Sm in the organic phase with less than 1% Nd can be obtained.
Okamura, Hiroyuki; Hirayama, Naoki*
Analytical Sciences, 37(1), p.119 - 130, 2021/01
This review summarizes recent progress in solvent extraction of rare earth elements (REEs) using an ionic liquid (IL) as the extraction solvent. These IL extraction systems are advantageous owing to the affinity of ILs for both charged and neutral hydrophobic species, in contrast to conventional organic solvent extraction systems. Herein, REE extraction studies using ILs are detailed and classified based on the type of extraction system. In IL extraction systems, the extracted complexes are often different from those in organic solvent systems, and the REE extraction and separation efficiencies are often significantly enhanced. Synergistic IL extraction is an effective approach to improving the extractability and separability of REEs. The development of novel task-specific ionic liquids (TSILs) suitable for IL extraction systems is also effective for REE separation.
Shimojo, Kojiro; Suzuki, Hideya; Yokoyama, Keiichi; Yaita, Tsuyoshi; Ikeda, Atsushi
Analytical Sciences, 36(12), p.1435 - 1437, 2020/12
Liquid-liquid extraction for the removal of pertechnetate (TcO) and perrhenate (ReO) is reported using tripodal extractant -hexa--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 TcO and ReO 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. TcO and ReO 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.
Sasaki, Yuji; Matsumiya, Masahiko*; Tsuchida, Yusuke*
Analytical Sciences, 36(11), p.1303 - 1309, 2020/11
The mutual separation of lanthanides is studied by multi-stage extraction using extractant, DGA (diglycolamide) compounds. Tetraoctyl-DGA (TODGA) has a high extractability to lanthanides and relatively high separation factor (SF) between Dy and Nd (SF: over 20). The complete separation with such SF value can be achieved by multi-stage extraction. Less information on multi-stage extraction compared to batch extraction is presented up to now, thus we conduct the basic study about that. Confirming the experimental data to be identical to the calculation, the sample solution including both metals is employed for the batchwise multi-stage extraction. Ninety-seven % of Dy with under detection limit of Nd can be recovered into the organic phase from Nd with ten times higher concentration than Dy using the condition, 0.1 M TODGA/n-dodecane and 0.3 M HNO by multi-stage extraction of 99 for organic and aqueous phases.
Saeki, Morihisa*; Yomogida, Takumi; Matsumura, Daiju; Saito, Takumi*; Nakanishi, Ryuzo*; Tsuji, Takuya; Oba, Hironori*
Analytical Sciences, 36(11), p.1371 - 1378, 2020/11
We measured X-ray absorption fine structure (XAFS) and Raman spectra of isopolymolybdates(VI) in HNO solution (0.15- 4.0 M), which change their geometries depending on acid concentration, and performed simultaneous resolution of the XAFS and Raman data using a multivariate curve resolution by alternating least-squares (MCR-ALS) analysis. In iterative ALS optimization, initial data matrices were prepared by two different methods. The MCR-ALS result of single XAFS data matrix shows large dependence on the preparation method of the initial data matrices. The MCR-ALS result of an augmented matrix of Raman and XAFS data has little dependence on the initial data matrices. It indicates that the augmentation method effectively improves the rotation ambiguities in the MCR-ALS analysis of the XAFS data. Based on the model fitting of the pure EXAFS oscillations, we revealed the change of [MoO(HO)] [MoO(HO)] [HMoO(HO)] in the highly concentrated HNO solution.
Yanagisawa, Kayo*; Matsueda, Makoto; Furukawa, Makoto*; Takagai, Yoshitaka*
Analytical Sciences, 36(9), p.1131 - 1135, 2020/09
In this paper, we propose an online water infusion system for rapid quantification of radioactive strontium-90 (Sr) with inductively coupled plasma mass spectrometry coupled solid-phase extraction and O dynamic reaction (cascade ICP-MS). The proposed system automatically provides a higher dilution ratio, which is at most 3.3 times the ratio obtained by the previous method, without increasing the analysis time (within 15 min). A detection limit of 2.7 Bq/kg wet (0.54 pg/kg wet) was achieved. The recovery test results were consistent with two different spiked values.
Tsutsui, Nao; Ban, Yasutoshi; Suzuki, Hideya*; Nakase, Masahiko*; Ito, Sayumi*; Inaba, Yusuke*; Matsumura, Tatsuro; Takeshita, Kenji*
Analytical Sciences, 36(2), p.241 - 246, 2020/02
To investigate the effective separation of actinides (Ans) from lanthanides (Lns), single-stage batch extraction experiments were performed with a novel extractant, tetradodecyl-1,10-phenanthroline-2,9-diamide (TDdPTDA) with various diluents such as 3-nitrobenzotrifluoride (F-3), nitrobenzene, and -dodecane for Am, Cm, and Lns. The extraction kinetics with TDdPTDA was rapid enough to perform the actual extraction flow sheet. The slopes of the distribution ratio versus TDdPTDA concentration and the distribution ratio versus nitric acid concentration were similar for F-3 and nitrobenzene systems but different from -dodecane system. These differences were attributed to the characteristics of the diluents. This study reveals high distribution ratios of Am ( ) and Cm ( ) for TDdPTDA, with the high separation factors (s) of Am from Lns enough for their separation.
Otaka, Toshiki*; Sato, Tatsumi*; Ono, Shimpei; Nagoshi, Kohei; Abe, Ryoji*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Nakatani, Kiyoharu*
Analytical Sciences, 35(10), p.1129 - 1133, 2019/10
Mori, Masanobu*; Sugita, Tsuyoshi; Fujii, Kengo*; Yamazaki, Taiki*; Isaka, Mayu*; Kobayashi, Kentaro*; Iwamoto, Shinji*; Itabashi, Hideyuki*
Analytical Sciences, 34(12), p.1449 - 1453, 2018/12
The photocatalyst coating stainless-steel wire mesh (TiO-WM) was prepared by double-layer coating method. The TiO-WM was evaluated using flow analytical system, which included the reactor and conductimetric detector (FAS-CD). The DMSO decomposition test through the FAS-CD reveal that photocatalytst was stable coating on the stainless-steel wire mesh.
Analytical Sciences, 34(12), p.1345 - 1346, 2018/12
Solvent extraction is one of the most effective analytical methods for separation, purification, and removal of target metal ions (e.g. valuable metal ions, toxic metal ions and radioactive fission products) from aqueous solutions containing various metal ions. In this paper, we introduce the papers related to (1) novel extractant, (2) ionic liquids and deep eutectic solvents, (3) new extractors, among papers on solvent extraction published between 2016 and 2018.
Sakamoto, Tetsuo*; Morita, Masato*; Kanenari, Keita*; Tomita, Hideki*; Sonnenschein, V.*; Saito, Kosuke*; Ohashi, Masaya*; Kato, Kotaro*; Iguchi, Tetsuo*; Kawai, Toshihide*; et al.
Analytical Sciences, 34(11), p.1265 - 1270, 2018/11
Nagano, Tetsushi; Naganawa, Hirochika; Suzuki, Hideya; Toshimitsu, Masaaki*; Mitamura, Hisayoshi*; Yanase, Nobuyuki*; Grambow, B.
Analytical Sciences, 34(9), p.1099 - 1102, 2018/09
A previously reported emulsion flow (EF) extraction system does not include a device for refining used solvent. Therefore, the processing of large quantities of wastewater by using the EF extractor alone could lead to the accumulation of wastewater components into the solvent and diminished extraction performance. In the present study, we have developed a solvent-washing-type EF system, which is equipped with a unit for washing used solvent to prevent accumulation, and successfully applied it for treating uranium-containing wastewater.
Atanassova, M.*; Okamura, Hiroyuki; Eguchi, Ayano; Ueda, Yuki; Sugita, Tsuyoshi; Shimojo, Kojiro
Analytical Sciences, 34(8), p.973 - 978, 2018/08
The distribution constants of 4-benzoyl-3-phenyl-5-isoxazolone (HPBI) and deprotonated one (PBI) between hydrophobic ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([CCim][TfN]) and aqueous phases were determined, together with the acid-dissociation constant of HPBI. The solvent extraction of three selected lanthanoid ions (La, Eu, and Lu) with HPBI from aqueous nitrate phase into [CCim][TfN] has been investigated. Application of the ionic liquid as the extracting phase greatly enhanced the extraction performance of HPBI for lanthanoid ions compared with that in the chloroform system. The composition of the extracted species was established to be anionic tetrakis entities, Ln(PBI), for light, middle, and heavy lanthanoid ions in an ionic environment.
Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Motokawa, Ryuhei; Shiwaku, Hideaki; Yaita, Tsuyoshi
Analytical Sciences, 33(11), p.1305 - 1309, 2017/11
Analytical Sciences, 33(10), p.1097 - 1098, 2017/10
Inductively coupled plasma-mass spectrometry (ICP-MS) is widely used in various fields such as environmental, geological, and clinical sciences. In this report, recent advances of the ICP-MS analysis and expected applications are described.
Suzuki, Hideya; Tsubata, Yasuhiro; Matsumura, Tatsuro
Analytical Sciences, 33(2), p.239 - 242, 2017/02
Alkyl diamide amine (ADAAM), a new high-performance reagent with a simple structure, was examined for the mutual separation of Am(III) and Cu(III). The combination of ADAAM and Tetraethyldiglycolamide (TEDGA) as a masking agent shows selectivity for Am(III) over Cm(III) in highly acidic media with separation factors up to 41.