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Bonding Trends in Tetravalent Th-Pu Monosalen Complexes. | LitMetric

Bonding Trends in Tetravalent Th-Pu Monosalen Complexes.

Chemistry

Institute of Resource Ecology, Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Bautzner Landstrasse 400, 01328, Dresden, Germany.

Published: December 2020

AI Article Synopsis

  • The study reports the synthesis of complex compounds involving tetravalent actinides (Thorium, Uranium, Neptunium, Plutonium) paired with particular N-donor ligands, aiming to understand how these heavy elements interact with small neutral molecules.
  • Structural analysis using techniques like single-crystal X-ray diffraction and infrared spectroscopy shows consistent structures within each series, with all complexes exhibiting the same overall conformation.
  • The data, backed by quantum chemical calculations, reveals that the interactions between actinides and ligands exhibit mostly ionic character, particularly in An-N and An-Cl bonds, whereas An-O bonds are more covalent for actinides heavier than thorium, with minimal influence from the extra substitutes.

Article Abstract

The synthesis of three complex series of the form [AnCl (salen)(Pyx) ] (H salen=N,N'-bis(salicylidene)ethylenediamine; Pyx=pyridine, 4-methylpyridine, 3,5-dimethylpyridine) with tetravalent early actinides (An=Th, U, Np, Pu) is reported with the goal to elucidate the affinity of these heavy elements for small neutral N-donor molecules. Structure determination by single-crystal XRD and characterization of bulk powders with infrared spectroscopy reveals isostructurality within each respective series and the same complex conformation in all reported structures. Although the trend of interatomic distances for An-Cl and An-N (imine nitrogen of salen or pyridyl nitrogen of Pyx) was found to reflect an ionic behavior, the trend of the An-O distances can only be described with additional covalent interactions for all elements heavier than thorium. All experimental results are supported by quantum chemical calculations, which confirm the mostly ionic character in the An-N and An-Cl bonds, as well as the highest degree of covalency of the An-O bonds. Structurally, the calculations indicate just minor electronic or steric effects of the additional Pyx substituents on the complex properties.

Download full-text PDF

Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7984231PMC
http://dx.doi.org/10.1002/chem.202003241DOI Listing

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