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	Understanding am3+/cm3+ separation with h(4)tpaen and its hydrophilic derivatives: a quantum chemical study
	Huang, Pin-Wen1,2,3; Wang, Cong-Zhi1,2; Wu, Qun-Yan1,2; Lan, Jian-Hui1,2; Song, Gang4; Chai, Zhi-Fang1,2,5,6; Shi, Wei-Qun1,2
刊名	Physical chemistry chemical physics
	2018-05-28
卷号	20期号:20页码:14031-14039
ISSN号	1463-9076
DOI	10.1039/c7cp08441b
通讯作者	Shi, wei-qun(shiwq@ihep.ac.cn)
英文摘要	Am3+/cm3+ separation is an extremely hard but important task in nuclear waste treatment. in this study, am and cm complexes formed with a back-extraction agent n,n,n,n-tetrakis[(6-carboxypyridin-2-yl)methyl]ethylene-diamine (h(4)tpaen) and its two derivatives with hydrophilic substituents (methoxy and morpholine groups) were investigated using the density functional theory (dft). the optimized geometrical structures indicated that the am3+ cation matched better with the cavities of the three studied ligands than cm3+, and the am3+ cations were located deeper in the cavities of the ligands. the bond order and quantum theory of atoms in molecules (qtaim) analyses suggested that ionic interactions dominated an-n and an-o (an = cm and am) bonds. however, weak and different extents of partial covalency could also be found in the am-n and cm-n bonds. the o donor atoms in the carboxylate groups preferably coordinated with cm3+ rather than am3+, whereas the n atoms preferred am3+. therefore, the am3+/cm3+ selectivity of h(4)tpaen and its two hydrophilic derivatives may be ascribed to the competition between the an-n and an-o interactions and the few dissimilarities in their geometrical structures. based on our calculations, the methoxy and morpholine groups in the two derivatives can serve as electron-donating groups and enhance the strength of the an-n-py bonds (n-py denotes the nitrogen atom of pyridine ring). when compared with the am-complex, the cm-complex exhibited significant strength effect, resulting in the relatively lower am3+/cm3+ separation ability of the h(4)tpaen's hydrophilic derivatives.
WOS关键词	SOLVENT-EXTRACTION ; DIGLYCOLAMIDE TODGA ; LANTHANIDE CATIONS ; MINOR ACTINIDES ; HARTREE-FOCK ; BASIS-SETS ; DENSITY ; COMPLEXATION ; ENERGY ; LIGANDS
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000433262300036
内容类型	期刊论文
URI标识	http://www.corc.org.cn/handle/1471x/2177547
专题	高能物理研究所
通讯作者	Shi, Wei-Qun
作者单位	1.Chinese Acad Sci, Lab Nucl Energy Chem, Inst High Energy Phys, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Key Lab Biomed Effects Nanomat & Nanosafety, Inst High Energy Phys, Beijing 100049, Peoples R China 3.Zhejiang Univ Water Resources & Elect Power, Hangzhou 310018, Zhejiang, Peoples R China 4.Guangdong Prov Key Lab Radionuclides Pollut Contr, Guangzhou 510006, Guangdong, Peoples R China 5.Soochow Univ, Sch Radiol & Interdisciplinary Sci RAD X, Suzhou 215123, Peoples R China 6.Soochow Univ, Collaborat Innovat Ctr Radiat Med, Jiangsu Higher Educ Inst, Suzhou 215123, Peoples R China
推荐引用方式 GB/T 7714	Huang, Pin-Wen,Wang, Cong-Zhi,Wu, Qun-Yan,et al. Understanding am3+/cm3+ separation with h(4)tpaen and its hydrophilic derivatives: a quantum chemical study[J]. Physical chemistry chemical physics,2018,20(20):14031-14039.
APA	Huang, Pin-Wen.,Wang, Cong-Zhi.,Wu, Qun-Yan.,Lan, Jian-Hui.,Song, Gang.,...&Shi, Wei-Qun.(2018).Understanding am3+/cm3+ separation with h(4)tpaen and its hydrophilic derivatives: a quantum chemical study.Physical chemistry chemical physics,20(20),14031-14039.
MLA	Huang, Pin-Wen,et al."Understanding am3+/cm3+ separation with h(4)tpaen and its hydrophilic derivatives: a quantum chemical study".Physical chemistry chemical physics 20.20(2018):14031-14039.

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