Mechanism of phase transfer of uranyl ions: a vibrational sum frequency generation spectroscopy study on solvent extraction in nuclear reprocessing

Mechanism of phase transfer of uranyl ions: a vibrational sum frequency generation spectroscopy study on solvent extraction in nuclear reprocessing
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DOI:
10.1039/c8cp04558e
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发表时间:
2018-12-21
影响因子:
3.3
通讯作者:
Watanabe, Masayuki
Watanabe, Masayuki
中科院分区:
化学2区
文献类型:
--
作者:
Kusaka, Ryoji;Watanabe, Masayuki

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了解磷酸三丁酯(TBP)萃取铀酰离子(UO_(22+))的机理有助于改进乏核燃料的处理和处置技术。到目前为止,人们认为水相中的铀酰离子被吸附到富含TBP的有机/水界面,在界面处与TBP形成络合物,并被萃取到有机相中。在这里,我们使用振动和频发生(VSFG)光谱表明,铀酰-TBP络合物的形成不会发生在界面处,并提出了另一种萃取机制,即硝酸铀酰,UO 2(NO3)(2),穿过界面,并在有机相中形成铀酰-TBP络合物,UO 2(NO3)(2)(TBP)(2)。
Mechanistic understanding of solvent extraction of uranyl ions (UO22+) by tributyl phosphate (TBP) will help improve the technology for the treatment and disposal of spent nuclear fuels. So far, it has been believed that uranyl ions in the aqueous phase are adsorbed to a TBP-enriched organic/aqueous interface, form complexes with TBP at the interface, and are extracted into the organic phase. Here we show that uranyl-TBP complex formation does not take place at the interface using vibrational sum frequency generation (VSFG) spectroscopy and propose an alternative extraction mechanism that uranyl nitrate, UO2(NO3)(2), passes through the interface and forms the uranyl-TBP complex, UO2(NO3)(2)(TBP)(2), in the organic phase.