Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers

doi:10.11862/CJIC.2019.066

科研成果详情

题名	Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers
其他题名	Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers
作者	Mou Yong-Xiao 1; Cao Jian-Ping 1; Weng Yue-Yue 1,2; Sun Xiang 1,3; Wei Tao1; Wang Chao-Jie1
发表日期	2019-05-10
发表期刊	CHINESE JOURNAL OF INORGANIC CHEMISTRY 影响因子和分区
语种	中文
原始文献类型	Article
关键词	uranyl ion uracil tautomers binding energies electronic structures solvent effect
其他关键词	DENSITY-FUNCTIONAL METHODS ; EFFECTIVE CORE POTENTIALS ; X-RAY-DIFFRACTION ; VIBRATIONAL FREQUENCIES ; AB-INITIO ; GAS-PHASE ; IN-VITRO ; COMPLEXES ; DFT ; BINDING
摘要	The geometric structure, vibrational spectra and binding energies of [UO2(Uracil)(j)(H2O)(k)](2+) (Uijk, i represents six kinds of uracil tautomers and j+k=5) have been studied by B3LYP method with 6-311++G(d, p) and RLC ECP basis sets. The solvent effect of water was simulated by polarized continuum model. The results show that as the number of the uracil increases, the U-O-uracil bond and the U=O bond in coordination ions are elongated and the stretching vibrational frequencies of the U=O bond gradually decrease in the aqueous solution. Meanwhile, the total binding energies of the coordination ions obviously increase, and the calculation also shows a linear relationship between the binding energies and the number of uracil ligand. Besides, the affinity of uracil ligand for the uranyl ion far exceeds that of H2O ligand. The U-O-uracil bond lengths calculated in the gaseous phase are slightly shorter than those obtained in the aqueous phase, however, the lengths of the U-OH2 bond show opposite behavior. In the Ui14 system, the bond length of U-O-uracil is negatively correlated with the bond length of U-OH2, while is positively correlated with the vibrational frequency of U=O bond. The maximum binding energy of the coordination ion is evidently not formed by the lowest energy conformer of uracil. The topological analysis of electron density indicates that the coordination bond shows ionic character. Atomic charge analysis reveals that the charge transfer is from uracil to uranyl during the coordination process, and the amount of the uracil charge is inversely related with coordination number. The Ur6 tautomer possesses the most charge among six kinds of uracil tautomers because of forming bidentate complexation with uranyl.
其他摘要	The geometric structure, vibrational spectra and binding energies of [UO_2 (Uracil)j (H_2O)k]2 + (Uijk, i represents six kinds of uracil tautomers and j+k=5) have been studied by B3LYP method with 6-311++G(d, p) and RLC ECP basis sets. The solvent effect of water was simulated by polarized continuum model. The results show that as the number of the uracil increases, the U-O_(uracil) bond and the U=O bond in coordination ions are elongated and the stretching vibrational frequencies of the U =O bond gradually decrease in the aqueous solution. Meanwhile, the total binding energies of the coordination ions obviously increase, and the calculation also shows a linear relationship between the binding energies and the number of uracil ligand. Besides, the affinity of uracil ligand for the uranyl ion far exceeds that of H_2O ligand. The U-O_(uracil) bond lengths calculated in the gaseous phase are slightly shorter than those obtained in the aqueous phase, however, the lengths of the U-OH_2 bond show opposite behavior. In the Ui14 system, the bond length of U-O_(uracil) is negatively correlated with the bond length of U-OH_2, while is positively correlated with the vibrational frequency of U=O bond. The maximum binding energy of the coordination ion is evidently not formed by the lowest energy conformer of uracil. The topological analysis of electron density indicates that the coordination bond shows ionic character. Atomic charge analysis reveals that the charge transfer is from uracil to uranyl during the coordination process, and the amount of the uracil charge is inversely related with coordination number. The Ur6 tautomer possesses the most charge among six kinds of uracil tautomers because of forming bidentate complexation with uranyl.
资助项目	国家自然科学基金 ; 浙江省自然科学基金
出版者	CHINESE CHEMICAL SOC
出版地	BEIJING
ISSN	1001-4861
卷号	35 期号:3 页码:403-412
DOI	10.11862/CJIC.2019.066
页数	10
WOS类目	Chemistry, Inorganic & Nuclear
WOS研究方向	Chemistry
WOS记录号	WOS:000469161800005
收录类别	SCIE ; CSCD ; 万方 ; PKU ; 北大核心 ; ISTIC ; SCI
学科领域	化学
URL	查看原文
CSCD记录号	CSCD:6449884
通讯作者地址	[Wang Chao-Jie]Wenzhou Med Univ, Sch Pharmaceut Sci, Wenzhou 325035, Zhejiang, Peoples R China.
万方分类号	O614.62(无机化学)
引用统计	被引频次：1[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	https://kms.wmu.edu.cn/handle/3ETUA0LF/15689
专题	药学院（分析测试中心）第一临床医学院（信息与工程学院）、附属第一医院_药学部
通讯作者	Wang Chao-Jie
作者单位	1.Wenzhou Med Univ, Sch Pharmaceut Sci, Wenzhou 325035, Zhejiang, Peoples R China; 2.Wenzhou Cent Hosp, Dept Pharm, Wenzhou 325000, Zhejiang, Peoples R China; 3.Wenzhou Med Univ, Dept Pharm, Affiliated Hosp 1, Wenzhou 325000, Zhejiang, Peoples R China
第一作者单位	药学院（分析测试中心）
通讯作者单位	药学院（分析测试中心）
第一作者的第一单位	药学院（分析测试中心）
推荐引用方式 GB/T 7714	Mou Yong-Xiao,Cao Jian-Ping,Weng Yue-Yue,et al. Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers[J]. CHINESE JOURNAL OF INORGANIC CHEMISTRY,2019,35(3):403-412.
APA	Mou Yong-Xiao, Cao Jian-Ping, Weng Yue-Yue, Sun Xiang, Wei Tao, & Wang Chao-Jie. (2019). Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers. CHINESE JOURNAL OF INORGANIC CHEMISTRY, 35(3), 403-412.
MLA	Mou Yong-Xiao,et al."Computational Study on the Coordination Systems of Hydrated Uranyl with Uracil Tautomers".CHINESE JOURNAL OF INORGANIC CHEMISTRY 35.3(2019):403-412.