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Series of Tetravalent Actinide Amidinates: Structure Determination and Bonding Analysis. | LitMetric

AI Article Synopsis

  • Two series of isostructural tetravalent actinide amidinates were synthesized using the chiral ligand (()-PEBA, expanding the range of studied actinides to include thorium and uranium alongside neptunium.
  • The newly synthesized Ce(IV) amidinate was analyzed to compare its properties with those of the tetravalent actinide complexes.
  • Characterization methods included single-crystal X-ray diffraction and NMR spectroscopy, revealing that thorium has the least covalent character in bonds, while uranium, neptunium, and plutonium show similar but varying covalent bonding contributions.

Article Abstract

Two series of isostructural tetravalent actinide amidinates [AnX(()-PEBA)] (An = Th, U, Np; X = Cl, N) bearing the chiral (,)-,'-bis(1-phenylethyl)benzamidinate (()-PEBA) ligand have been synthesized and thoroughly characterized in solid and in solution. This study expands the already reported tetravalent neptunium complexes to the lighter actinides thorium and uranium. Furthermore, a rare Ce(IV) amidinate [CeCl(()-PEBA)] was synthesized to compare its properties to those of the analogous tetravalent actinide complexes. All compounds were characterized in the solid state using single-crystal XRD and infrared spectroscopy and in solution using NMR spectroscopy. Quantum chemical bonding analysis including also the isostructural Pa and Pu complexes was used to characterize the covalent contributions to any bond involving the metal cation. Th shows the least covalent character throughout the series, even substantially smaller than for the Ce complex. For U, Np, and Pu, similar covalent bonding contributions are found, but a natural population analysis reveals different origins. The 6 participation is the highest for U and decreases afterward, whereas the 5 participation increases continuously from Pa to Pu.

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Source
http://dx.doi.org/10.1021/acs.inorgchem.0c01969DOI Listing

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