Efficient Trivalent Actinide-Lanthanide Separations Using Hydrophilic CHON-Compliant Phenanthroline-Dicarboxamide Ligands

被引：0

作者：

Wan, Yong Qiang ^{[1
]}

Hao, Huai Xin ^{[2
]}

Zhang, Yang Yang ^{[3
]}

Guo, Yu Xiao ^{[2
]}

Ma, Zhi Jun ^{[1
]}

Wang, Zhi Peng ^{[2
]}

Li, Jun ^{[3
,4
,5
]}

Mocilac, Pavle ^{[1
]}

机构：

[1] Lanzhou Univ, Sch Nucl Sci & Technol, Lanzhou 730000, Peoples R China

[2] Tsinghua Univ, Inst Nucl & New Energy Technol, Beijing 100084, Peoples R China

[3] Chinese Acad Sci, Ganjiang Innovat Acad, Fundamental Sci Ctr Rare Earths, Ganzhou 341000, Peoples R China

[4] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

[5] Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Minist Educ, Beijing 100084, Peoples R China

来源：

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH | 2025年 / 64卷 / 24期

基金：

中国国家自然科学基金;

关键词：

SELECTIVE EXTRACTION; SOLVENT-EXTRACTION; COMPLEXATION; APPROXIMATION; SUBSTITUENTS; AMERICIUM; EUROPIUM; ELEMENTS; SANEX;

D O I：

10.1021/acs.iecr.5c00795

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

Experimental studies are reported herein on novel hydrophilic CHON-compliant ligands based on 1,10-phenanthroline-dicarboxamide derivatives bearing ethylene glycol (AE-DAPhen) and diethylene glycol (AEE-DAPhen) hydrophilizing terminal groups. These ligands exhibit high solubility in nitric acid solutions and demonstrate strong selectivity for Am(III) over Eu(III) in mildly acidic conditions against the TODGA (N,N,N ',N '-tetraoctyl diglycolamide) ligand in organic phase using two different extraction methods. The maximum separation factors (SFEu/Am) achieved were 325 for AE-DAPhen and 291 for AEE-DAPhen. In addition, solvent extraction tests with Cm(III) were also conducted, and SFEu/Cm turned out to be surprisingly lower: 50 for AE-DAPhen and 55 for AEE-DAPhen. Overall, these observations amount to a relative SFCm/Am of 7.4-7.8, which is one of the best reported values for any CHON-compliant ligands. The theoretical results from quantum-chemical studies suggest a coordinative role of hydroxyl and etheric oxygen atoms, providing an understanding of the bonding interaction between the metal ions and ligands.

引用

页码：12185 / 12199

页数：15

共 58 条

[1]

ADF, 2021, US

[2] 1,10-Phenanthroline-2,9-dicarboxamides as ligands for separation and sensing of hazardous metals [J].

Alyapyshev, M. ;

Ashina, J. ;

Dar'in, D. ;

Kenf, E. ;

Kirsanov, D. ;

Tkachenko, L. ;

Legin, A. ;

Starova, G. ;

Babain, V. .

RSC ADVANCES, 2016, 6 (73) :68642-68652

[3] Isolation and Purification of Actinides Using N,O-Hybrid Donor Ligands for Closing the Nuclear Fuel Cycle [J].

Alyapyshev, Mikhail ;

Babain, Vasiliy ;

Kirsanov, Dmitry .

ENERGIES, 2022, 15 (19)

[4]

[Anonymous], 2016, Gaussian16

[5] N,N,N′,N′-Tetraoctyl diglycolamide (TODGA):: a promising extractant for actinide-partitioning from high-level waste (HLW) [J].

Ansari, SA ;

Pathak, PN ;

Manchanda, VK ;

Husain, M ;

Prasad, AK ;

Parmar, VS .

SOLVENT EXTRACTION AND ION EXCHANGE, 2005, 23 (04) :463-479

[6] Aqueous Partitioning of Minor Actinides by Different Processes [J].

Ansari, Seraj A. ;

Pathak, Priyanath ;

Mohapatra, Prashanta K. ;

Manchanda, Vijay K. .

SEPARATION AND PURIFICATION REVIEWS, 2011, 40 (01) :43-76

[7] First Example of Fluorinated Phenanthroline Diamides: Synthesis, Structural Study, and Complexation with Lanthanoids [J].

Avagyan, Nane A. ;

Lemport, Pavel S. ;

Lysenko, Konstantin A. ;

Gudovannyy, Alexey O. ;

Roznyatovsky, Vitaly A. ;

Petrov, Valentine S. ;

Vokuev, Mikhail F. ;

Ustynyuk, Yuri A. ;

Nenajdenko, Valentine G. .

MOLECULES, 2022, 27 (15)

[8] Hydrophilic polymers: Current trends and visions for the future [J].

Bayliss, Niamh ;

Schmidt, Bernhard V. K. J. .

PROGRESS IN POLYMER SCIENCE, 2023, 147

[9] DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].

BECKE, AD .

PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100

[10] The structurally rigid tetradentate N,N',O,O'-ligands based on phenanthroline for binding of f-elements: The substituents vs. structures of the complexes [J].

Borisova, Nataliya E. ;

Kostin, Andrey A. ;

Reshetova, Marina D. ;

Lyssenko, Konstantin A. ;

Belova, Elena V. ;

Myasoedov, Boris F. .

INORGANICA CHIMICA ACTA, 2018, 478 :148-154

← 1 2 3 4 5 6 →