0000000000072249

AUTHOR

Yuichiro Nagame

Chemical studies of Fl (element 114): Heaviest chemically studied element

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Chemical studies of elements with Z≥ 104 in liquid phase

Abstract Recent studies of the chemical separation and characterization experiments of the first three transactinide elements, rutherfordium (Rf), dubnium (Db), and seaborgium (Sg), conducted atom-at-a-time in liquid phases, are reviewed. A short description on experimental techniques based on partition methods, specifically automated rapid chemical separation systems, is also given. A newly developed experimental approach to investigate single atoms of the heaviest elements with an electrochemical method is introduced. Perspectives for liquid-phase chemistry experiments on heavier elements are briefly discussed.

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Fluoride Complexation of Element 104, Rutherfordium (Rf), Investigated by Cation-exchange Chromatography

We report on new and much more precise cation-exchange data of element 104, rutherfordium (Rf), in the fluoride ion concentration [F−] range of 5.29×10−5−1.04×10−3 M. The result based on one-atom-a...

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First ionization potential of the heaviest actinide lawrencium, element 103

The first ionization potential (IP1 ) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP 1 value is 4.9630.08 0.07 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s 2 5f 14 7p 1 1/2 , which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens t…

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Complex chemistry with complex compounds

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the investigation of fragile single molecular species by gas-phase chromatography. The latest success with the heaviest group 6 transactinide seaborgium is highlighted. The formation of a very volatile hexacarbonyl compound Sg(CO)6 was observed similarly to its lighter homologues molybdenum and tungsten. The interactions of these gaseous carbonyl complex compounds with quartz surfaces were investigated by thermochromatography. Second-generation experiments are under way to investigate the intramolecular bond between the central metal atom of the complexes and the ligands addressing the influence of re…

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Production Cross Sections of 261Rf and 262Db in Bombardments of 248Cm with 18O and 19F Ions

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First Ionization Potentials of Fm, Md, No, and Lr

We report the first ionization potentials (IP1) of the heavy actinides, fermium (Fm, atomic number Z = 100), mendelevium (Md, Z = 101), nobelium (No, Z = 102), and lawrencium (Lr, Z = 103), determined using a method based on a surface ionization process coupled to an online mass separation technique in an atom-at-a-time regime. The measured IP1 values agree well with those predicted by state-of-the-art relativistic calculations performed alongside the present measurements. Similar to the well-established behavior for the lanthanides, the IP1 values of the heavy actinides up to No increase with filling up the 5f orbital, while that of Lr is the lowest among the actinides. These results clear…

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Anionic Fluoro Complex of Element 105, Db

We report on the characteristic anion-exchange behavior of the superheavy element dubnium (Db) with atomic number Z=105 in HF/HNO3 solution at the fluoride ion concentration [F−]=0.003 M. The resul...

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Chemical properties of rutherfordium (Rf) and dubnium (Db) in the aqueous phase

Recent experimental studies of the chemical characterization of the first two transactinide elements, rutherfordium (Rf) and dubnium (Db), conducted atom-at-a-time in aqueous phases are reviewed. A short description on experimental techniques based on partition methods, specifically automated rapid chemical separation systems, is also given. Perspectives for aqueous-phase chemistry experiments on heavier elements are briefly discussed.

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Actinides and Transactinides

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First successful ionization of Lr (Z = 103) by a surface-ionization technique.

We have developed a surface ionization ion-source as part of the JAEA-ISOL (Isotope Separator On-Line) setup, which is coupled to a He/CdI2 gas-jet transport system to determine the first ionization potential of the heaviest actinide lawrencium (Lr, Z = 103). The new ion-source is an improved version of the previous source that provided good ionization efficiencies for lanthanides. An additional filament was newly installed to give better control over its operation. We report, here, on the development of the new gas-jet coupled surface ion-source and on the first successful ionization and mass separation of 27-s (256)Lr produced in the (249)Cf + (11)B reaction.

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Anion-exchange Behavior of Rf in HCl and HNO3 Solutions

H. Haba,∗,a K. Tsukada,a M. Asai,a S. Goto,a,b A. Toyoshima,a,c I. Nishinaka,a K. Akiyama,a M. Hirata,a S. Ichikawa,a Y. Nagame,a Y. Shoji,c M. Shigekawa,c T. Koike,c M. Iwasaki,c A. Shinohara,c T. Kaneko,b T. Maruyama,b S. Ono,b H. Kudo,b Y. Oura,d K. Sueki,d H. Nakahara,a,d M. Sakama,e A. Yokoyama,f J. V. Kratz,g M. Schadel,h and W. Bruchleh Advanced Science Research Center, Japan Atomic Energy Research Institute, Tokai-mura, Ibaraki 3191195, Japan Department of Chemistry, Faculty of Science, Niigata University, Niigata-shi, Niigata 950-2181, Japan Department of Chemistry, Graduate School of Science, Osaka University, Toyonaka-shi, Osaka 5600043, Japan Department of Chemistry, Graduate Sc…

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Measurement of the Md3+/Md2+ Reduction Potential Studied with Flow Electrolytic Chromatography

The reduction behavior of mendelevium (Md) was studied using a flow electrolytic chromatography apparatus. By application of the appropriate potentials on the chromatography column, the more stable Md(3+) is reduced to Md(2+). The reduction potential of the Md(3+) + e(-) → Md(2+) couple was determined to be -0.16 ± 0.05 V versus a normal hydrogen electrode.

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Liquid-Phase Chemistry of Superheavy Elements

An overview over the chemical separation and characterization experiments of the four transactinide elements so far studied in liquid phases, rutherfordium (Rf), dubnium (Db), seaborgium (Sg), and hassium (Hs), is presented. Results are discussed in view of the position of these elements in the Periodic Table and of their relation to theoretical predictions. Short introductions on experimental techniques in liquid-phase chemistry, specifically automated rapid chemical separation systems, are also given. Studies of nuclear properties of transactinide nuclei by chemical isolation will be mentioned. Some perspectives for further liquid-phase chemistry on heavier elements are briefly discussed.

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Fluoride Complexation of Element 104, Rutherfordium

Fluoride complexation of element 104, rutherfordium (Rf), produced in the 248Cm(18O,5n)261Rf reaction has been studied by anion-exchange chromatography on an atom-at-a-time scale. The anion-exchange chromatographic behavior of Rf was investigated in 1.9-13.9 M hydrofluoric acid together with those of the group-4 elements Zr and Hf produced in the 18O-induced reactions on Ge and Gd targets, respectively. It was found that the adsorption behavior of Rf on anion-exchange resin is quite different from those of Zr and Hf, suggesting the influence of relativistic effects on the fluoride complexation of Rf.

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Fluorido Complex Formation of Element 104, Rutherfordium (Rf)

We have investigated the cation-exchange behavior of element 104, rutherfordium (Rf), together with its lighter group-4 homologs Zr and Hf, and the tetravalent pseudo-homolog Th in HF/HNO3 mixed so...

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TASCAを用いたCn, Nh, Fl化学実験のためのHg, Tl, PbのSiO2及びAu表面に対するオンライン化学吸着研究

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$_{2}$ and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO$_{2}$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$_{2}$ surface at room temperature. On the other hand, the Hg did no…

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