Coordination behavior of uranyl with PDAM derivatives in solution: Combined study with ESI-MS and DFT

doi:10.1016/j.molliq.2019.112287

CORC > 宁波材料技术与工程研究所 > 中国科学院宁波材料技术与工程研究所 > 2020专题

	Coordination behavior of uranyl with PDAM derivatives in solution: Combined study with ESI-MS and DFT
	Kong, Xiang-He ; Wu, Qun-Yan ; Zhang, Xin-Rui ; Wang, Cui ; Hu, Kong-Qiu ; Chai, Zhi-Fang ; Nie, Chang-Ming ; Shi, Wei-Qun
刊名	JOURNAL OF MOLECULAR LIQUIDS
	2020
卷号	300
关键词	SEGMENTED CONTRACTION SCHEME DENSITY-FUNCTIONAL THEORY SELECTIVE EXTRACTION MASS-SPECTROMETRY LIGAND COMPLEXES ACTINIDES SEPARATION ELEMENTS EU(III)
DOI	10.1016/j.molliq.2019.112287
英文摘要	Although the extraction behaviors of the tetradentate 1,10-phenanthroline-2,9-dicarboxamide (PDAM, L) derivative ligands toward actinide and lanthanide ions have been reported, the coordination structures and species determination of the complexes are still involved and are also of great significance. To reveal the coordination structure of U(VI) ion and three PDAM derivative ligands with different alkyl chain, electrospray ionization mass spectrometry (ESI-MS) combined with density functional theory (OFT) calculations were carried out. The [UO2L(NO3)](+) complexes are the dominant species for the three PDAM derivative ligands based on the ESI-MS spectra. Collision-induced dissociation (CID) results further show that the U(VI) ions strongly bind with the phenanthroline fragment, while the amine groups and the alkyl moieties are apt to lost. Furthermore, DFT calculations further confirm that three PDAM derivative ligands can be well combined with uranyl, and [UO2L(NO3)](+) species are more stable than [UO2L(OH)center dot H2O](+) one. The length of the alkyl chain has little effect on the coordination structure of uranyl complexes, but affects their thermodynamic behaviors due to the steric hindrance effect. Therefore, the studies on the coordination chemistry of uranyl with three PDAM derivative ligands at the molecular level provide basic information for efficient actinides separation in spent fuel reprocessing. (C) 2019 Elsevier B.V. All rights reserved.
学科主题	Chemistry ; Physics
内容类型	期刊论文
源URL	[http://ir.nimte.ac.cn/handle/174433/19967]
专题	2020专题
作者单位	1.Shi, WQ (corresponding author), Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China. 2.Nie, CM (corresponding author), Univ South China, Sch Resource & Environm & Safety Engn, Hengyang 421001, Peoples R China.
推荐引用方式 GB/T 7714	Kong, Xiang-He,Wu, Qun-Yan,Zhang, Xin-Rui,et al. Coordination behavior of uranyl with PDAM derivatives in solution: Combined study with ESI-MS and DFT[J]. JOURNAL OF MOLECULAR LIQUIDS,2020,300.
APA	Kong, Xiang-He.,Wu, Qun-Yan.,Zhang, Xin-Rui.,Wang, Cui.,Hu, Kong-Qiu.,...&Shi, Wei-Qun.(2020).Coordination behavior of uranyl with PDAM derivatives in solution: Combined study with ESI-MS and DFT.JOURNAL OF MOLECULAR LIQUIDS,300.
MLA	Kong, Xiang-He,et al."Coordination behavior of uranyl with PDAM derivatives in solution: Combined study with ESI-MS and DFT".JOURNAL OF MOLECULAR LIQUIDS 300(2020).