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Journal Articles

Quantitation of trace lanthanide and actinide ions in radioactive samples by capillary electrophoresis-laser-induced fluorescence detection

Haraga, Tomoko; Saito, Shingo*

Bunseki Kagaku, 70(12), p.671 - 679, 2021/12

We developed highly sensitive capillary electrophoresis-laser-induced fluorescence detection methods for lanthanide (Ln) and actinide (An) ions with small sample volume and low emission of waste, by which the radiation risk can be minimized. Specifically, determination of Nd ion in spent nuclear fuel, effective separation between Am and Cm ion, and specific detection of UO$$_{2}$$$$^{2+}$$ in real radioactive samples were achieved by molecular design of fluorescence probes composed of an aminocarboxylate chelating moiety, a fluorophore and a spacer, and unique separation mode based on dynamic ternary complexation. We found that there are appropriate combination of probe and ternary complexation for detection and separation of each Ln and An ions. For example, acyclic and macrocyclic hexadentate is suitable for Ln$$^{3+}$$, Am$$^{3+}$$ and Cm$$^{3+}$$, and planer tetradentate with $$pi$$ electron system is specific for UO$$_{2}$$$$^{2+}$$, with ppt-sub ppt level detection.

Journal Articles

Stoichiometry between humate unit molecules and metal ions in supramolecular assembly induced by Cu$$^{2+}$$ and Tb$$^{3+}$$ measured by gel electrophoresis techniques

Nakano, Sumika*; Marumo, Kazuki*; Kazami, Rintaro*; Saito, Takumi*; Haraga, Tomoko; Tasaki-Handa, Yuiko*; Saito, Shingo*

Environmental Science & Technology, 55(22), p.15172 - 15180, 2021/11

Humic acid (HA) can strongly complex with metal ions to form a supramolecular assembly via coordination binding. However, determining the supramolecular size distribution and stoichiometry between small HA unit molecules constituting HA supramolecule and metal ions has proven to be challenging. Here, we investigated the changes in the size distributions of HAs induced by Cu$$^{2+}$$ and Tb$$^{3+}$$ ions using a unique polyacrylamide gel electrophoresis (PAGE) for the separation and quantification of HA complexes and metal ions bound, followed by UV-Vis spectroscopy and EEM-PARAFAC. It was found that the supramolecular behaviors of Cu$$^{2+}$$ and Tb$$^{3+}$$ complexes with HA collected from peat and deep groundwater (HHA) differed. Our results suggest that this supramolecular stoichiometry is related to the abundance of sulfur atoms in the elemental composition of HHA. Our results provide new insights into HA supramolecules formed via metal complexation.

Journal Articles

Purification of anionic fluorescent probes through precise fraction collection with a two-point detection system using multiple-stacking preparative capillary transient isotachophoresis

Haraga, Tomoko; Tsujimura, Hiroto*; Miyauchi, Saori*; Kamimura, Takuya*; Shibukawa, Masami*; Saito, Shingo*

Electrophoresis, 41(13-14), p.1152 - 1159, 2020/07

 Times Cited Count:3 Percentile:50.59(Biochemical Research Methods)

A novel combination of CE-based separation techniques was used for the precise fractionation of ionic compounds from impurities. The combination of on-capillary concentration and separation using transient isotachophoresis, with multiple injections and a two-point detection system provided higher efficiency, and accuracy at a microliter-scale injection volume, than when CE was individually used for purification. In this paper, we present successful applications of the CE fractionation techniques for the purification of fluorescein, fluorescein-4-isothiocyanate, two fluorescent metal ion probes, and a fluorescein-modified DNA aptamer. The purity of the isolated fluorescent probes ranged from 95 to 99%. The purified probe solutions were practical for use as purified stock solutions. The method developed was useful for the purification of anionic fluorescent reagents to be of ultratrace analytical grade for use with CE-LIF.

Journal Articles

Advanced gel electrophoresis techniques reveal heterogeneity of humic acids based on molecular weight distributions of kinetically inert Cu$$^{2+}$$-humate complexes

Marumo, Kazuki*; Matsumoto, Atsumasa*; Nakano, Sumika*; Shibukawa, Masami*; Saito, Takumi*; Haraga, Tomoko; Saito, Shingo*

Environmental Science & Technology, 53(24), p.14507 - 14515, 2019/12

 Times Cited Count:0 Percentile:0(Engineering, Environmental)

Humic acids (HA) are responsible for the fate of metal ions in the environment. We developed a polyacrylamide gel electrophoresis (PAGE) technique to investigate the MW distributions of metal ion (copper ion). Combining contaminant-metal-free and high-resolution PAGE systems for HA provided accurate MW distributions for the metal ions. Coupling this system with UV-Vis spectrometry and the excitation-emission matrix (EEM) spectrometry-parallel factor analysis (PARAFAC) method revealed new insights into metal-HA complex. Interestingly, the MW distributions of the three metal ions were entirely different, indicating that the presence of specific binding environments in HA for the metal ions depending its MW. The MW distributions of five fluorescent components were associated with the metal ion distributions. Our PAGE-based methodology suggests that metal binding sites and fluorescent components in HA exhibit heterogeneity in terms of metal binding affinity and MW.

Journal Articles

Safe and rapid development of capillary electrophoresis for ultratrace uranyl ions in radioactive samples by way of fluorescent probe selection for actinide ions from a chemical library

Haraga, Tomoko; Ouchi, Kazuki; Sato, Yoshiyuki; Hoshino, Hitoshi*; Tanana, Rei*; Fujihara, Takashi*; Kurokawa, Hideki*; Shibukawa, Masami*; Ishimori, Kenichiro; Kameo, Yutaka; et al.

Analytica Chimica Acta, 1032, p.188 - 196, 2018/11

 Times Cited Count:6 Percentile:33.4(Chemistry, Analytical)

The development of safe, rapid and highly sensitive analytical methods for radioactive samples, especially actinide (An) ions, represents an important challenge. Here we propose a methodology for selecting appropriate emissive probes for An ions with very low consumption and emission of radioactivity by capillary electrophoresis-laser-induced fluorescence detection (CE-LIF), using a small chemical library of probes with eight different chelating moieties. It was found that the emissive probe, which possesses the tetradentate chelating moiety, was suitable for detecting uranyl ions. The detection limit for the uranyl-probe complex using CE-LIF combined with dynamic ternary complexation and on-capillary concentration techniques was determined to be 0.7 ppt. This method was successfully applied to real radioactive liquid samples collected from nuclear facilities.

Journal Articles

Characterization and thermodynamic study of humic acid in deep groundwater at Horonobe, Hokkaido, Japan

Kimuro, Shingo*; Kirishima, Akira*; Nagao, Seiya*; Saito, Takumi*; Amano, Yuki; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Nuclear Science and Technology, 55(5), p.503 - 515, 2018/05

 Times Cited Count:3 Percentile:45.99(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Generation of megahertz-band spin currents using nonlinear spin pumping

Watanabe, Shingo*; Hirobe, Daichi*; Shiomi, Yuki*; Iguchi, Ryo*; Daimon, Shunsuke*; Kameda, Mai*; Takahashi, Saburo*; Saito, Eiji

Scientific Reports (Internet), 7, p.4576_1 - 4576_6, 2017/07

 Times Cited Count:4 Percentile:28.18(Multidisciplinary Sciences)

Journal Articles

Development of simple and rapid analytical method for radioactive samples by capillary electrophoresis

Haraga, Tomoko; Sato, Yoshiyuki; Kameo, Yutaka; Saito, Shingo*

Dekomisshoningu Giho, (55), p.22 - 27, 2017/03

no abstracts in English

Journal Articles

Application of capillary electrophoresis with laser-induced fluorescence detection for the determination of trace neodymium in spent nuclear fuel using complexation with an emissive macrocyclic polyaminocarboxylate probe

Haraga, Tomoko; Saito, Shingo*; Sato, Yoshiyuki; Asai, Shiho; Hanzawa, Yukiko; Hoshino, Hitoshi*; Shibukawa, Masami*; Ishimori, Kenichiro; Takahashi, Kuniaki

Analytical Sciences, 30(7), p.773 - 776, 2014/07

 Times Cited Count:5 Percentile:21.87(Chemistry, Analytical)

A simple and rapid method with low radiation exposure risk was developed for the determination of neodymium in spent nuclear fuel by CE with LIF detection using a fluorescent ligand having a macrocyclic hexadentate polyaminocarboxylate structure. The concentration of Nd(III) in a spent nuclear fuel sample was determined with no interference from various matrix elements, including lanthanides and uranium (at a 200-fold excess), with 92 $$pm$$ 3% recovery. This is due to method's high resolution based on establishing a ternary complex equilibrium during migration in which the hydroxyl ion plays an auxiliary role.

Journal Articles

Highly sensitive detection of neodymium ion in small amount of spent nuclear fuel samples using novel fluorescent macrocyclic hexadentate polyaminocarboxylate probe in capillary electrophoresis-laser-induced fluorescence detection

Saito, Shingo*; Sato, Yoshiyuki*; Haraga, Tomoko; Nakano, Yuta*; Asai, Shiho; Kameo, Yutaka; Takahashi, Kuniaki; Shibukawa, Masami*

Journal of Chromatography A, 1232, p.152 - 157, 2012/04

 Times Cited Count:11 Percentile:41.46(Biochemical Research Methods)

A rapid and high-sensitive detection method of total concentration of Nd ion in a spent nuclear fuel sample is desirable since precise quantification of total Nd is useful as indicator of burnup. In this work, a capillary electrophoresis-laser-induced fluorescent detection method (CE-LIF) was proposed for analysis of total Nd in the spent fuel sample solution, employing a newly synthesized metal fluorescent probe with a fluorescein and a macrocylic hexadentate chelating group, FTC-ABNOTA, for lanthanide (Ln) ions. The mutual separation among the Ln-FTC-ABNOTA complexes was achieved by pH control providing dynamic ternary complexation with hydroxide ions. In this method, high resolution of Nd from other Ln ions with high resolution of 1.3-1.9 and a very low detection limit of 3.2 ppt were successfully obtained. A simulated spent fuel sample containing various metal ions was examined, so that a good quantification result with 99.3% recovery was obtained even with large excess of U.

Journal Articles

Capillary electrophoresis with laser-induced fluorescent detection method using highly emissive probes for analysis of actinides in radioactive wastes

Haraga, Tomoko; Nakano, Yuta*; Shibukawa, Masami*; Kameo, Yutaka; Takahashi, Kuniaki; Saito, Shingo*

Proceedings of 14th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2011) (CD-ROM), p.1461 - 1465, 2011/09

Actinides are important nuclides for the analysis of radioactive wastes from nuclear fuel cycle facilities. In order to achieve simple and rapid analysis of actinides, capillary electrophoresis-laser-induced fluorescent detection method (CE-LIF) is one of the potential candidates. In this study, new emissive probes of actinide ions suitable for CE-LIF were developed for the first time. The detection and separation of americium and neptunium ions as model nuclides were examined using several new emissive complexing probes, each of which possessed a fluorophore and a different chelating moiety. Using acyclic and macrocyclic multidentate probes, the highly sensitive fluorescent detection of Am and Np was successfully achieved. The results suggests that the probe with an acyclic hexadentate chelating moiety is suitable for detection and separation of Am and Np. The detection limit of mid-ppt levels was determined.

Journal Articles

Identified charged hadron production in $$p + p$$ collisions at $$sqrt{s}$$ = 200 and 62.4 GeV

Adare, A.*; Afanasiev, S.*; Aidala, C.*; Ajitanand, N. N.*; Akiba, Yasuyuki*; Al-Bataineh, H.*; Alexander, J.*; Aoki, Kazuya*; Aphecetche, L.*; Armendariz, R.*; et al.

Physical Review C, 83(6), p.064903_1 - 064903_29, 2011/06

 Times Cited Count:156 Percentile:99.42(Physics, Nuclear)

Transverse momentum distributions and yields for $$pi^{pm}, K^{pm}, p$$, and $$bar{p}$$ in $$p + p$$ collisions at $$sqrt{s}$$ = 200 and 62.4 GeV at midrapidity are measured by the PHENIX experiment at the RHIC. We present the inverse slope parameter, mean transverse momentum, and yield per unit rapidity at each energy, and compare them to other measurements at different $$sqrt{s}$$ collisions. We also present the scaling properties such as $$m_T$$ and $$x_T$$ scaling and discuss the mechanism of the particle production in $$p + p$$ collisions. The measured spectra are compared to next-to-leading order perturbative QCD calculations.

Journal Articles

Azimuthal correlations of electrons from heavy-flavor decay with hadrons in $$p+p$$ and Au+Au collisions at $$sqrt{s_{NN}}$$ = 200 GeV

Adare, A.*; Afanasiev, S.*; Aidala, C.*; Ajitanand, N. N.*; Akiba, Yasuyuki*; Al-Bataineh, H.*; Alexander, J.*; Aoki, Kazuya*; Aphecetche, L.*; Aramaki, Y.*; et al.

Physical Review C, 83(4), p.044912_1 - 044912_16, 2011/04

 Times Cited Count:8 Percentile:52.71(Physics, Nuclear)

Measurements of electrons from the decay of open-heavy-flavor mesons have shown that the yields are suppressed in Au+Au collisions compared to expectations from binary-scaled $$p+p$$ collisions. Here we extend these studies to two particle correlations where one particle is an electron from the decay of a heavy flavor meson and the other is a charged hadron from either the decay of the heavy meson or from jet fragmentation. These measurements provide more detailed information about the interaction between heavy quarks and the quark-gluon matter. We find the away-side-jet shape and yield to be modified in Au+Au collisions compared to $$p+p$$ collisions.

Journal Articles

Electronic properties of femtosecond laser induced modified spots on single crystal silicon carbide

Tomita, Takuro*; Iwami, Masahiro*; Yamamoto, Minoru*; Deki, Manato*; Matsuo, Shigeki*; Hashimoto, Shuichi*; Nakagawa, Yoshinori*; Kitada, Takahiro*; Isu, Toshiro*; Saito, Shingo*; et al.

Materials Science Forum, 645-648, p.239 - 242, 2010/04

no abstracts in English

Journal Articles

The H-Invitational Database (H-InvDB); A Comprehensive annotation resource for human genes and transcripts

Yamasaki, Chisato*; Murakami, Katsuhiko*; Fujii, Yasuyuki*; Sato, Yoshiharu*; Harada, Erimi*; Takeda, Junichi*; Taniya, Takayuki*; Sakate, Ryuichi*; Kikugawa, Shingo*; Shimada, Makoto*; et al.

Nucleic Acids Research, 36(Database), p.D793 - D799, 2008/01

 Times Cited Count:51 Percentile:74.53(Biochemistry & Molecular Biology)

Here we report the new features and improvements in our latest release of the H-Invitational Database, a comprehensive annotation resource for human genes and transcripts. H-InvDB, originally developed as an integrated database of the human transcriptome based on extensive annotation of large sets of fulllength cDNA (FLcDNA) clones, now provides annotation for 120 558 human mRNAs extracted from the International Nucleotide Sequence Databases (INSD), in addition to 54 978 human FLcDNAs, in the latest release H-InvDB. We mapped those human transcripts onto the human genome sequences (NCBI build 36.1) and determined 34 699 human gene clusters, which could define 34 057 protein-coding and 642 non-protein-coding loci; 858 transcribed loci overlapped with predicted pseudogenes.

JAEA Reports

Study on the Development of Geological Environmental Model(II) -Outline-

Tsujimoto, Keiichi*; Shinohara, Yoshinori*; Saito, Shigeyuki*; Ueda, Shinzo*; Ohashi, Toyo*; Sasaki, Ryoichi*; Shingo, Tomiyama*

JNC TJ8400 2003-040, 78 Pages, 2003/02

JNC-TJ8400-2003-040.pdf:1.45MB

The safety performance assessment was carried out in imaginary geological environment in the conventional research and development of geological disposal, but the importance of safety assessment based on the repository design and considering the concrete geological environment will increase in the future. The research considering the link of the major three fields of geological disposal, investigation of geological environment, repository design and safety performance assessment, is the contemporary worldwide research theme. Hence it is important to organize information flow that contains the series if information process from the data production to analysis in the three fields, and to systemize the knowledge base that unifies the information flow hierarchically.The information flow for geological environment model generation process is examined and modified base on the product of the research of "Study on the development of geological environment model" that of the research in 2002. The work flow diagram for geological structure and hydrology are modified, and those for geochemical and rock property are examined from the search. Furthermore, database design was examined to build geochemical environment database (knowledgebase) based on the result of the systemization of the environment model generation technology. The geochemical environment database was designed and the prototype system is build to contribute database design.

JAEA Reports

Study on the Development of Geological Environmental Model(II)

Tsujimoto, Keiichi*; Shinohara, Yoshinori*; Saito, Shigeyuki*; Ueda, Shinzo*; Ohashi, Toyo*; Sasaki, Ryoichi*; Shingo, Tomiyama*

JNC TJ8400 2003-039, 395 Pages, 2003/02

JNC-TJ8400-2003-039.pdf:7.74MB

The safety performance assessment was carried out in imaginary geological environment in the conventional research and development of geological disposal, but the importance of safety assessment based on the repository design and considering the concrete geological environment will increase in the future. The research considering the link of the major three fields of geological disposal, investigation of geological environment, repository design and safety performance assessment, is the contemporary worldwide research theme. Hence it is important to organize information flow that contains the series if information process from the data production to analysis in the three fields, and to systemize the knowledge base that unifies the information flow hierarchically.The information flow for geological environment model generation process is examined and modified base on the product of the research of "Study on the development of geological environment model" that of the research in 2002. The work flow diagram for geological structure and hydrology are modified, and those for geochemical and rock property are examined from the search. Furthermore, database design was examined to build geochemical environment database (knowledgebase) based on the result of the systemization of the environment model generation technology. The geochemical environment database was designed and the prototype system is build to contribute database design.

Oral presentation

Separation and enrichment of rare-earth elements by high-speed countercurrent chromatography with an aqueous biphasic system

Shimizu, Kohei; Saito, Shingo*; Naganawa, Hirochika; Shibukawa, Masami*

no journal, , 

no abstracts in English

Oral presentation

Study on highly emissive probes with various chelating moieties for analysis of actinides by capillary electrophoresis with laser-induced fluorescent detection

Haraga, Tomoko; Nakano, Yuta*; Shibukawa, Masami*; Saito, Shingo*; Kameo, Yutaka; Takahashi, Kuniaki

no journal, , 

For the safe disposal of radioactive wastes, a simple and highly sensitive analytical method for actinides in waste samples is required. In this study, a capillary electrophoresis with laser induced fluorescent detection was examined for analysis of neptunium ($$^{237}$$Np) and americium ($$^{243}$$Am). Applying a pre-capillary complexation technique using several new emissive complexing probes with various chelating moieties, the highly sensitive fluorescent detection of Np and Am was succeeded. In addition, the separation of Np and Am was achieved for a multidentate probe. The detection limit was obtained at mid-ppt levels.

Oral presentation

Capillary electrophoresis with laser-induced fluorescent detection method using highly emissive probes for analysis of uranium in radioactive wastes

Haraga, Tomoko; Sato, Yoshiyuki*; Shibukawa, Masami*; Kameo, Yutaka; Takahashi, Kuniaki; Saito, Shingo*

no journal, , 

JP, 2012-034711   Patent publication (In Japanese)

Actinides (Th, U, Np, Pu, Am, Cm) are important nuclides for the analysis of radioactive wastes from nuclear facilities. In order to achieve simple and rapid analysis of actinides, capillary electrophoresis-laser-induced fluorescent detection method (CE-LIF) is one of the potential candidates. In this study, new emissive probes of uranium suitable for CE-LIF were developed. The detection and separation of uranyl ions were examined using several new emissive complexing probes, each of which possessed a fluorophore and a different chelating moiety. Using acyclic tetradentate probes, the highly sensitive fluorescent detection of uranyl ions was successfully achieved. The detection limit of mid-ppt levels was determined.

36 (Records 1-20 displayed on this page)