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 η2coordination with tris-amidoximate species. In such a uranyl–amidoximate complex with η2binding motif, strong covalent interaction and orbital hybridization between U 5f/6dand (N, O) 2pshould 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.
Funder
National Natural Science Foundation of China
Joint Funds of the National Natural Science Foundation of China
Youth Innovation Promotion Association of the Chinese Academy of Sciences
Key Project of Science and Technology of Shanghai
Publisher
International Union of Crystallography (IUCr)
Subject
Instrumentation,Nuclear and High Energy Physics,Radiation
Cited by
11 articles.
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