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Synthesis, structural investigation and kinetic studies of uranyl(VI) unsymmetrical Schiff base complexes

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Abstract

Uranyl(VI) complexes with unsymmetrical N2O2 Schiff base ligands were synthesized and characterized. Their characterization was performed using UV-Vis, 1H NMR, cyclic voltammetry, single-crystal X-ray crystallography, IR, TG and C.H.N. techniques. X-ray crystallography of the complexes show that beside coordination of the tetradentate Schiff base, one DMF molecule is also coordinated. In order to investigate the effect of the substitutional groups of the Schiff base on the oxidation and reduction potentials, we used the cyclic voltammetry method. Electrochemistry of these complexes showed that the presence of electron releasing groups accelerates oxidation of the complexes. The kinetics of thermal decomposition was studied using thermal gravimetric method (TG) and Coats-Redfern equation. According to Coats-Redfern plots, the kinetics of thermal decomposition of the studied complexes is first-order in all stages. Also the kinetics and mechanism of the exchange reaction of the coordinated solvent with tributylphosphine was carried out in solution, using spectrophotometric method. As a result, the second order rate constants at four temperatures and the activation parameters were calculated showing an associative mechanism for all corresponding complexes. It was concluded that the steric and the electronic properties of the complexes influence the reaction rate significantly.

X-ray crystallography of the Uranyl (VI) complexes shows that besides coordination of the tetradentate Schiff base, one DMFmolecule is also coordinated.

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Acknowledgements

We are grateful to Shiraz University Research Council for its financial support. The project P204/11/0809 of the Grant agency of the Czech Republic supported the crystallographic part of the work.

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Authors and Affiliations

  1. Chemistry Department, College of Sciences, Shiraz University, Shiraz, 71454, I. R. Iran

    ZAHRA ASADI, MOZAFFAR ASADI, AZADE ZEINALI & MOHAMMAD RANJKESHSHORKAEI

  2. Institute of Physics ASCR, v.v.i, Na Slovance 2, 182 21, Praha, Czech Republic

    KARLA FEJFAROVA, VACLAV EIGNER & MICHAL DUSEK

  3. Department of Chemistry, Faculty of Science, Golestan University, Gorgan, Iran

    ALIAKBAR DEHNOKHALAJI

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  1. ZAHRA ASADI
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  2. MOZAFFAR ASADI
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Correspondence to ZAHRA ASADI.

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Supplementary Information

CCDC 914883 (3-OMe) and 949507 (4-OMe) contains the supplementary crystallographic data for this paper. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif.

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ASADI, Z., ASADI, M., ZEINALI, A. et al. Synthesis, structural investigation and kinetic studies of uranyl(VI) unsymmetrical Schiff base complexes. J Chem Sci 126, 1673–1683 (2014). https://doi.org/10.1007/s12039-014-0720-y

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