Density functional study of uranyl (VI) amidoxime complexes

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

中国物理B ›› 2012, Vol. 21 ›› Issue (9): 93102-093102.doi: 10.1088/1674-1056/21/9/093102

• ATOMIC AND MOLECULAR PHYSICS • 上一篇下一篇

Density functional study of uranyl (VI) amidoxime complexes

匙芳廷^{a b}, 李鹏^c, 熊洁^a, 胡胜^a, 高涛^c, 夏修龙^a, 汪小琳^{a b}

a Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang 621900, China;
b College of Chemistry, Sichuan University, Chengdu 610064, China;
c Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, China

收稿日期:2011-12-12 修回日期:2012-04-26 出版日期:2012-08-01 发布日期:2012-08-01
基金资助:
Project supported by the Science and Technology Development Foundation of China Academy of Engineering Physics (Grant No. 2011A0301003).

Density functional study of uranyl (VI) amidoxime complexes

Chi Fang-Ting (匙芳廷)^{a b}, Li Peng (李鹏)^c, Xiong Jie (熊洁)^a, Hu Sheng (胡胜)^a, Gao Tao (高涛)^c, Xia Xiu-Long (夏修龙)^a, Wang Xiao-Lin (汪小琳)^{a b}

a Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang 621900, China;
b College of Chemistry, Sichuan University, Chengdu 610064, China;
c Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, China

Received:2011-12-12 Revised:2012-04-26 Online:2012-08-01 Published:2012-08-01
Contact: Wang Xiao-Lin E-mail:xlwang@caep.ac.cn
Supported by:
Project supported by the Science and Technology Development Foundation of China Academy of Engineering Physics (Grant No. 2011A0301003).

摘要/Abstract

摘要： 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.

关键词: uranyl amidoxime complexes, intra-molecular hydrogen bonds, bond order, Mulliken populations

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.

Key words: uranyl amidoxime complexes, intra-molecular hydrogen bonds, bond order, Mulliken populations

中图分类号: (Applications of density-functional theory (e.g., to electronic structure and stability; defect formation; dielectric properties, susceptibilities; viscoelastic coefficients; Rydberg transition frequencies))

31.15.es

21.60.Jz (Nuclear Density Functional Theory and extensions (includes Hartree-Fock and random-phase approximations))

匙芳廷, 李鹏, 熊洁, 胡胜, 高涛, 夏修龙, 汪小琳. Density functional study of uranyl (VI) amidoxime complexes[J]. 中国物理B, 2012, 21(9): 93102-093102.

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[J]. Chin. Phys. B, 2012, 21(9): 93102-093102.

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Density functional study of uranyl (VI) amidoxime complexes

Density functional study of uranyl (VI) amidoxime complexes

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