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論文

Complexation properties and structural character of lanthanides complexes of $$O,N$$-hetero donor ligand BIZA

小林 徹; 阿久津 和宏*; 中瀬 正彦*; 鈴木 伸一; 塩飽 秀啓; 矢板 毅

Separation Science and Technology, 54(13), p.2077 - 2083, 2019/02

 被引用回数:0 パーセンタイル:100(Chemistry, Multidisciplinary)

ランタノイドを効率よく分離できる分離剤の開発は、レアアースの精錬やリサイクル技術の確立に関連する重要なテーマである。アクチノイド化学研究グループでは、酸素と複素環窒素をドナー元素とするヘテロドナー型配位子をいくつか開発し、これらの配位子が特定のランタノイドと選択的に錯形成することを見出している。本論文では、窒素ドナーとしてベンズイミダゾール基を有する配位子($$N$$-methyl-$$N$$-phenyl-2-(1$$H$$-benzimidazol-2-yl)-pyridine-6-carboxamide)のランタノイドとの錯形成特性について、結晶構造解析による構造化学的な検討に基づいて議論する。

口頭

Construction of ultra low concentration sample preparation and measurement system for Es-XAFS measurement in SPring-8

鈴木 伸一; 塩飽 秀啓; 小林 徹; 矢板 毅; 塚田 和明; 浅井 雅人; 豊嶋 厚史

no journal, , 

An element having an atomic number equal to or greater than neptunium is one of synthetic elements, and its abundance is governed by the half-life. In a general laboratory scale structural analyzer, it is difficult to clarify the hydration structure of these artificial elements, due to the problem of abundance and the radioactivity. At this time, we secured microgram amount of Einsteinium (Es). Es is the heaviest element in the periodic table that can acquire the microgram amount. Then, hydration structure study of Es was carried out at SPring-8 BL22XU. Approximately 0.2 microgram of 254 Es (half life 275 days) used for the experiment was irradiated and generated in 2017 in the HFIR reactor of Oak Ridge National Laboratory (ORNL). After that, it took about a half year to isolate 254Es in ORNL and it was delivered to JAEA 4 months later. Since other nuclides such as 253Es, 249Cf, 250Cf and 249Bk were also mixed in addition to 254Es at the time of acquisition, it is necessary to separate and purify and sample preparation for optimum condition for SPring-8 synchrotron radiation experiment. Therefore, 254Es was separated using a cation exchange separation method using alpha-HIB(alpha hydroxyl isobutyric acid). Furthermore, in order to remove alpha-HIB, an unnecessary complexing agent for SPring-8 experiments, hydrochloric acid-based cation exchange separation was carried out. The purified sample was dissolved in 50 macro liter of 0.1 N perchloric acid, sealed in a plastic container, and used as a synchrotron radiation experiment sample. The hydration structure elucidation experiment was measured by fluorescence method using 19 element semiconductor detector. In ultra-low concentration XAFS measurement, it is important to remove scattered rays from various materials around the measurement system. For this reason, BCLA: Bent Crystal Laue Analyzer which uses a curved Si crystal for spectroscopy in a Laue type arrangement was used as a spectroscopic crystal.

口頭

Mechanism elucidation of biphasic extraction system by utilizing direct observation based on the synchrotron radiation (I)

矢板 毅; 鈴木 伸一; 小林 徹; 塩飽 秀啓

no journal, , 

Important factors of selectivity for a special ion in the biphasic extraction system utilized by complexation with organic ligands: (1) Complexation between ion and organic ligand, (2) Complex formation dynamics, (3) Hydration and dehydration, (5) Complexation at liquid-liquid interface and so on, are estimated by various approaches such as thermodynamics, spectroscopy, theoretical calculations and so on, and then, many researchers have been tried to empirical or semi-empirical design of separation system based on these information. On these backgrounds, this study aims to development for direct observation systems for biphasic extraction phenomena under dynamics and static condition by utilizing synchrotron radiation and neutron proves in order to understand detailed mechanism. In this presentation, we will present the relationship between separation results and analyses such as X-ray crystallography, XAFS, Time-resolved XAFS applying to (1)- (5) mentioned above and discuss effectiveness of these analytical methods.

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