Strong influence of weak hydrogen bonding on actinide-phosphonate complexation: accurate predictions from DFT followed by experimental validation

Physical Chemistry Chemical Physics : PCCP
Aditi ChandrasekarN Sivaraman

Abstract

Among the varied classes of weak hydrogen bond, the CHO type is one of immense interest as it governs the finer structures of biological and chemical molecules, hence determining their functionalities. In the present work, this weak hydrogen bond has been shown to strongly influence the complexation behaviour of uranyl nitrate [UO2(NO3)2] with diamyl-H-phosphonate (DAHP) and its branched isomer disecamyl-H-phosphonate (DsAHP). The structures of the bare ligands and complexes have been optimized by density functional theory (DFT) calculations. Surprisingly, despite having the same chemical composition the branched UO2(NO3)2·2DsAHP complex shows a remarkably higher stability (by ∼14 kcal mol-1) compared to the UO2(NO3)2·2DAHP complex. Careful inspection of the optimized structures reveals the existence of multiple CHO hydrogen-bonding interactions between the nitrate oxygens or U[double bond, length as m-dash]O oxygens and the α-hydrogens in the alkyl chains of the ligands. Comparatively stronger such bonds are found in the UO2(NO3)2·2DsAHP complex. The binding free energies associated with the complexes are computed and favoured superior binding energetics for the more stable UO2(NO3)2·2DsAHP complex. Calculations involving diis...Continue Reading

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Citations

Jul 26, 2021·European Journal of Medicinal Chemistry·Victor T SabeHendrik G Kruger

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Methods Mentioned

BETA
column chromatography
NMR

Software Mentioned

NUMFREQ
COSMO
ZORA
Multiwfn
2aim
orca

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