Inorganic Chemistry, volume 60, issue 19, pages 14563-14581
Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters
Matveev Petr I
1
,
Huang Pin Wen
2, 3
,
Kirsanova Anna A
1
,
Ananyev Ivan V
4
,
Sumyanova Tsagana B
1
,
Kharcheva Anastasia V
1, 5
,
Khvorostinin Evgenii Yu
1
,
Shi Wei-Qun
3
,
Borisova Nataliya E.
1, 4
2
Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
|
Publication type: Journal Article
Publication date: 2021-09-21
Journal:
Inorganic Chemistry
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 4.6
ISSN: 00201669, 1520510X
Inorganic Chemistry
Physical and Theoretical Chemistry
Abstract
Hybrid donor extractants are a promising class of compounds for the separation of trivalent actinides and lanthanides. Here, we investigated a series of sterically loaded diphosphonate ligands based on bipyridine (BiPy-PO-iPr and BiPy-PO-cHex) and phenanthroline (Phen-PO-iPr and Phen-PO-cHex). We studied their complex formation with nitrates of trivalent f-elements in solvent extraction systems (Am and Eu) and homogeneous acetonitrile solutions (Nd, Eu, and Lu). Phenanthroline extractants demonstrated the highest efficiency and selectivity [SF(Am/Eu) up to 14] toward Am(III) extraction from nitric acid solutions among all of the studied diphosphonates of N-heterocycles. The binding constants established by UV-vis titration also indicated stronger binding of sterically impaired diphosphonates compared to the primary substituted diphosphonates. NMR titration and slope analysis during solvent extraction showed the formation of 2:1 complexes at high concentrations (>10-3 mol/L) for phenanthroline-based ligands. According to UV-vis titrations at low concentrations (10-5-10-6 mol/L), the phenanthroline-based ligands formed 1:1 complexes. Bipyridine-based ligands formed 1:1 complexes regardless of the ligand concentration. Luminescence titrations revealed that the quantum yields of the complexes with Eu(III) were 81 ± 8% (BiPy-PO-iPr) and 93 ± 9% (Phen-PO-iPr). Single crystals of the structures [Lu(μ2,κ4-(iPrO)2P(O)Phen(O)2(OiPr))(NO3)2]2 and Eu(Phen-PO-iPr)(NO3)3 were obtained by chemical synthesis with the Phen-PO-iPr ligand. X-ray diffraction studies revealed a closer contact of the f-element with the aromatic N atoms in the case of sterically loaded P═O ligands compared with sterically deficient ligands. Density functional theory calculations allowed us to rationalize the observed selectivity trends in terms of the bond length, Mayer bond order, and preorganization energy.
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Matveev P. I. et al. Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters // Inorganic Chemistry. 2021. Vol. 60. No. 19. pp. 14563-14581.
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Matveev P. I., Huang P. W., Kirsanova A. A., Ananyev I. V., Sumyanova T. B., Kharcheva A. V., Khvorostinin E. Yu., Petrov V. G., Shi W., Kalmykov S. N., Borisova N. E. Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters // Inorganic Chemistry. 2021. Vol. 60. No. 19. pp. 14563-14581.
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TY - JOUR
DO - 10.1021/acs.inorgchem.1c01432
UR - https://doi.org/10.1021%2Facs.inorgchem.1c01432
TI - Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters
T2 - Inorganic Chemistry
AU - Huang, Pin Wen
AU - Kirsanova, Anna A
AU - Khvorostinin, Evgenii Yu
AU - Matveev, Petr I
AU - Ananyev, Ivan V
AU - Petrov, Vladimir G
AU - Shi, Wei-Qun
AU - Borisova, Nataliya E.
AU - Sumyanova, Tsagana B
AU - Kharcheva, Anastasia V
AU - Kalmykov, Stepan N.
PY - 2021
DA - 2021/09/21 00:00:00
PB - American Chemical Society (ACS)
SP - 14563-14581
IS - 19
VL - 60
SN - 0020-1669
SN - 1520-510X
ER -
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@article{2021_Matveev,
author = {Pin Wen Huang and Anna A Kirsanova and Evgenii Yu Khvorostinin and Petr I Matveev and Ivan V Ananyev and Vladimir G Petrov and Wei-Qun Shi and Nataliya E. Borisova and Tsagana B Sumyanova and Anastasia V Kharcheva and Stepan N. Kalmykov},
title = {Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters},
journal = {Inorganic Chemistry},
year = {2021},
volume = {60},
publisher = {American Chemical Society (ACS)},
month = {sep},
url = {https://doi.org/10.1021%2Facs.inorgchem.1c01432},
number = {19},
pages = {14563--14581},
doi = {10.1021/acs.inorgchem.1c01432}
}
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Matveev, Petr I., et al. “Way to Enforce Selectivity via Steric Hindrance: Improvement of Am(III)/Eu(III) Solvent Extraction by Loaded Diphosphonic Acid Esters.” Inorganic Chemistry, vol. 60, no. 19, Sep. 2021, pp. 14563-14581. https://doi.org/10.1021%2Facs.inorgchem.1c01432.