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Trivalent Actinide and Lanthanide Complexation of 5,6-Dialkyl-2,6-bis(1,2,4-triazin-3-yl)pyridine (RBTP; R = H, Me, Et) Derivatives: A Combined Experimental and First-Principles Study

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Inorg. Chem. 2013, 52, 2, 761-776
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    Trivalent Actinide and Lanthanide Complexation of 5,6-Dialkyl-2,6-bis(1,2,4-triazin-3-yl)pyridine (RBTP; R = H, Me, Et) Derivatives: A Combined Experimental and First-Principles Study
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    † Department of Chemistry, University of Nevada—Las Vegas, Las Vegas, Nevada 89154, United States
    ‡ Radiochemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai 400-085, India
    § Department of Physics and Astronomy, University of Nevada—Las Vegas, Las Vegas, Nevada 89154, United States
    ⊥ Sandia National Laboratories, Albuquerque, New Mexico 87185-0747, United States
    *E-mail: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2013, 52, 2, 761–776
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    https://doi.org/10.1021/ic301881w
    Published December 27, 2012
    Copyright © 2012 American Chemical Society
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    Abstract

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    Complexations of lanthanide ions with 5,6-dialkyl-2,6-bis(1,2,4-triazin-3-yl)pyridine [RBTP; R = H (HBTP), methyl (MeBTP), ethyl (EtBTP)] derivatives have been studied in the acetonitrile medium by electrospray ionization mass spectrometry, time-resolved laser-induced fluorescence spectroscopy, and UV–vis spectrophotometric titration. These studies were carried out in the absence and presence of a nitrate ion in order to understand the effect of the nitrate ion on their complexation behavior, particularly in the poor solvating acetonitrile medium where strong nitrate complexation of hard lanthanide ions is expected. Consistent results from all three techniques undoubtedly show the formation of lower stoichiometric complexes in the presence of excess nitrate ion. This kind of nitrate ion effect on the speciation of Ln3+ complexes of RBTP ligands has not so far been reported in the literature. Different Am3+ and Ln3+ complexes were observed with RBTP ligands in the presence of 0.01 M tetramethylammonium nitrate, and their stability constant values are determined using UV–vis spectrophotometric titrations. The formation of higher stoichiometric complexes and higher stability constants for Am3+ compared to Ln3+ ions indicates the selectivity of these classes of ligands. A single-crystal X-ray diffraction (XRD) study of europium(III) complexes shows the formation of a dimeric complex with HBTP and a monomeric complex with EtBTP, whereas MeBTP forms both the dimeric and monomeric complexes. Density functional theory calculations confirm the findings from single-crystal XRD and also predict the structures of Eu3+ and Am3+ complexes observed experimentally.

    Copyright © 2012 American Chemical Society

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    Supporting Information

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    X-ray crystallographic data in CIF format, crystal data and structure refinement, atomic coordinates, bond lengths and angles, anisotropic displacement parameters, and hydrogen coordinates and isotropic displacement parameters for 1, 2a, 2b, and 3. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cited By

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    This article is cited by 18 publications.

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2013, 52, 2, 761–776
    Click to copy citationCitation copied!
    https://doi.org/10.1021/ic301881w
    Published December 27, 2012
    Copyright © 2012 American Chemical Society
    Request reuse permissions

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