Density functional study of uranyl (VI) amidoxime complexes

doi:10.1088/1674-1056/21/9/093102

Abstract Uranyl (VI) amidoxime complexes are investigated using relativistic density functional theory. The equilibrium structures, bond orders, and Mulliken populations of the complexes have been systematically investigated under a generalized gradient approximation (GGA). Comparison of (acet) uranyl amidoxime complexes ([UO₂(AO)_n]^2-n, 1 ≤ n ≤ 4) with available experimental data shows an excellent agreement. In addition, the U-O(1), U-O(3), C(1)-N(2), and C(3)-N(4) bond lengths of [UO₂(CH₃AO)₄]^2- are longer than experimental data by about 0.088, 0.05, 0.1, and 0.056 Å. The angles of N(3)-O(3)-U, O(2)-N(1)-C(1), N(3)-C(3)-N(4), N(4)-C(3)-C(4), and C(4)-C(3)-N(3) are different from each other, which are due to existing interaction between oxygen in uranyl and hydrogen in amino group. This interaction is found to be intra-molecular hydrogen bond. Studies on the bond orders, Mulliken charges, and Mulliken populations demonstrate that uranyl oxo group functions as hydrogen-bond acceptors and H atoms in ligands act as hydrogen-bond donors forming hydrogen bands within the complex.

Keywords: uranyl amidoxime complexes intra-molecular hydrogen bonds bond order Mulliken populations

Received: 12 December 2011
Revised: 26 April 2012
Accepted manuscript online:

PACS:	31.15.es	(Applications of density-functional theory (e.g., to electronic structure and stability; defect formation; dielectric properties, susceptibilities; viscoelastic coefficients; Rydberg transition frequencies))
	21.60.Jz	(Nuclear Density Functional Theory and extensions (includes Hartree-Fock and random-phase approximations))

Fund: Project supported by the Science and Technology Development Foundation of China Academy of Engineering Physics (Grant No. 2011A0301003).

Corresponding Authors: Wang Xiao-Lin
E-mail: xlwang@caep.ac.cn

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Chi Fang-Ting (匙芳廷), Li Peng (李鹏), Xiong Jie (熊洁), Hu Sheng (胡胜), Gao Tao (高涛), Xia Xiu-Long (夏修龙), Wang Xiao-Lin (汪小琳) Density functional study of uranyl (VI) amidoxime complexes 2012 Chin. Phys. B 21 093102

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Density functional study of uranyl (VI) amidoxime complexes

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