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Development of heavy element chemistry at interfaces; Observing actinide complexes at the oil/water interface in solvent extraction by nonlinear vibrational spectroscopy

重元素化学の界面研究への展開; 非線形振動分光法を用いた溶媒抽出系の油/水界面におけるアクチノイド錯体の観測

日下 良二  ; 渡邉 雅之   

Kusaka, Ryoji; Watanabe, Masayuki

Understanding the chemistry of elements at the bottom of the periodic table is a challenging goal in chemistry. Observing actinide species at interfaces using interface-selective second-order nonlinear optical spectroscopy, such as vibrational sum frequency generation (VSFG) spectroscopy, is a promising route for developing heavy element chemistry; however, such attempts are scarce. Here, we investigated the phase transfer mechanism of uranyl ions (UO$$_{2}$$$$^{2+}$$) in solvent extraction using the di-(2-ethylhexyl)phosphoric acid (HDEHP) extractant dissolved in dodecane organic phase by probing the oil/water liquid-liquid interface using VSFG spectroscopy. The POO$$^{-}$$ symmetric stretch vibrational signals of the HDEHP ligands clearly demonstrated that uranyl ions form interfacial complexes with HDEHP at the oil/water interface. The interfacial uranyl-HDEHP complexes were formed with uranyl ions coming from both the aqueous and oil phases, strongly suggesting that the interfacial complex is an intermediate to cross the oil/water interface. Density functional theory (DFT) calculations proposed the molecular structure of the interfacial uranyl-HDEHP complex.

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パーセンタイル:67.66

分野:Chemistry, Physical

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