Unusual redox stability of pentavalent uranium with hetero-bifunctional phosphonocarboxylate: insight into aqueous speciation

Srivastava, Ashutosh; Ali, Sk. Musharaf; Dumpala, Rama Mohan Rao; Kumar, Sumit; Kumar, Pranaw; Rawat, Neetika; Mohapatra, P. K.

doi:10.1039/d4dt00173g

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2024

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Cited by 2 publications

References 92 publications

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Molecular and environmental facets of pentavalent uranium chemistry

Hopkins,

Simmonds,

Cryer

et al. 2024

Handbook on the Physics and Chemistry of Rare Earths

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Molecular and environmental facets of pentavalent uranium chemistry

Hopkins,

Simmonds,

Cryer

et al. 2024

Handbook on the Physics and Chemistry of Rare Earths

View full text Add to dashboard Cite

Complexation of Trivalent Lanthanides with Hexaalkyl Nitrilotriacetamides into Methylimidazolium-Based Ionic Liquids: Spectroscopic, Electrochemical, Calorimetric, and Theoretical Insights

Goyal,

Srivastava,

Sengupta

et al. 2024

Inorg. Chem.

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Exothermic, spontaneous inner-sphere complexation of trivalent lanthanides with N,N,N′,N′,N″,N″-hexaalkyl-substituted nitrilotriacetamides (HRNTAs) into 1-hexyl-3-methylimidazolium-bis(trifluoromethylsulfonyl)imide (C 6 mim NTf 2 ) is reported with a predominant presence of ML and ML 2 complexes having complexation constants, β 1 Eu 3.10 ± 0.02 ,β 1 Nd 2.67 ± 0.03 and β 2 Eu 5.22 ± 0.04, β 2 Nd 4.95 ± 0.02, respectively, for the n-butyl-substituted HRNTA (HBNTA); while those for the n-hexyl derivative (HHNTA) are β 1 Eu 4.27 ± 0.03, β 1 Nd 3.71 ± 0.03 and β 2 Eu 7.70 ± 0.03, β 2 Nd 7.18 ± 0.04, respectively. HHNTA shows better complexing ability; whereas the stronger complexation of the Nd 3+ over Eu 3+ is attributed to the lanthanide contraction. Furthermore, the nature of the ionic liquid also influences the extent of complexation with the trend: C 4 mim NTf 2 > C 6 mim NTf 2 > C 8 mim NTf 2 , which follows the order of their dielectric constants. Judd− Ofelt parameters were calculated from photoluminescence data to get an idea about the symmetry of the Eu 3+ complexes. Electrochemical investigations give diffusion coefficient values of 1.17 × 10 −7 and 8.26 × 10 −8 cm 2 /s for the Eu 3+ complexes of HBNTA and HHNTA, respectively. Changes in the spectral characteristics and peak positions are evidenced in the FTIR spectra on the complexation of Eu 3+ with the HRNTA ligands in C 6 mim NTf 2 . Structure optimization for the complexes was performed by DFT computations.

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Unusual redox stability of pentavalent uranium with hetero-bifunctional phosphonocarboxylate: insight into aqueous speciation

Abstract: The +5 state is an unusual oxidization state of uranium due to its instability in the aqueous phase. As a result, gaining information about its aqueous speciation is extremely difficult....

Cited by 2 publications

References 92 publications

Molecular and environmental facets of pentavalent uranium chemistry

Molecular and environmental facets of pentavalent uranium chemistry

Complexation of Trivalent Lanthanides with Hexaalkyl Nitrilotriacetamides into Methylimidazolium-Based Ionic Liquids: Spectroscopic, Electrochemical, Calorimetric, and Theoretical Insights

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