Tris-amidoximate uranyl complexes via η2 binding mode coordinated in aqueous solution shown by X-ray absorption spectroscopy and density functional theory methods

Journal of Synchrotron Radiation
Linjuan ZhangJian Qiang Wang

Abstract

The present study sheds some light on the long-standing debate concerning the coordination properties between uranyl ions and the amidoxime ligand, which is a key ingredient for achieving efficient extraction of uranium. Using X-ray absorption fine structure combined with theoretical simulation methods, the binding mode and bonding nature of a uranyl-amidoxime complex in aqueous solution were determined for the first time. The results show that in a highly concentrated amidoxime solution the preferred binding mode between UO22+ and the amidoxime ligand is η2 coordination with tris-amidoximate species. In such a uranyl-amidoximate complex with η2 binding motif, strong covalent interaction and orbital hybridization between U 5f/6d and (N, O) 2p should be responsible for the excellent binding ability of the amidoximate ligand to uranyl. The study was performed directly in aqueous solution to avoid the possible binding mode differences caused by crystallization of a single-crystal sample. This work also is an example of the simultaneous study of local structure and electronic structure in solution systems using combined diagnostic tools.

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Citations

May 16, 2019·Organic Chemistry Frontiers : an International Journal of Organic Chemistry·Daniel A Decato, Orion B Berryman
Jul 2, 2021·Inorganic Chemistry·Ashok Kumar YadavKinkar P Bhattacharyya
Jan 6, 2022·Journal of Synchrotron Radiation·Jian SunJian Qiang Wang

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