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The lanthanide contraction revisited.

Michael Seitz1, Allen G Oliver, Kenneth N Raymond

  • 1Department of Chemistry, University of California, Berkeley, California 94720-1460, USA.

Journal of the American Chemical Society
|August 21, 2007
PubMed
Summary
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Researchers synthesized a complete series of lanthanide complexes using a multidentate ligand, revealing a consistent quadratic contraction across the coordination sphere. This finding advances understanding of rare-earth metal coordination chemistry.

Area of Science:

  • Inorganic Chemistry
  • Coordination Chemistry
  • Materials Science

Background:

  • Lanthanide complexes are crucial in various applications, but their coordination chemistry, especially with multidentate ligands, requires further elucidation.
  • Understanding lanthanide contraction is key to predicting and controlling the properties of rare-earth compounds.

Purpose of the Study:

  • To synthesize and structurally characterize a complete, isostructural series of lanthanide complexes with the multidentate ligand TREN-1,2-HOIQO.
  • To investigate the geometric arrangement and lanthanide contraction within this series.
  • To establish the universality of observed coordination sphere contraction patterns.

Main Methods:

  • Synthesis of lanthanide complexes with TREN-1,2-HOIQO for lanthanum (La) through lutetium (Lu), excluding promethium (Pm).

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  • Single-crystal X-ray diffraction analysis to determine the solid-state structures.
  • Geometric analysis using shape parameter metrics and bond length measurements.

    • Main Results:

    • A complete, isostructural series of 1D-polymeric lanthanide complexes was obtained, featuring eight-coordinate, distorted trigonal-dodecahedral environments.
    • Individual Ln-O bond lengths showed a deviation from the expected quadratic decrease, but the sum of all bond lengths exhibited ideal quadratic behavior.
    • The coordination sphere contraction demonstrated a universal quadratic dependence, confirmed across multiple lanthanide complex series.

    Conclusions:

    • The study presents the first complete isostructural series of lanthanide complexes with a ligand of denticity greater than two.
    • The findings provide a significant advance in predicting and rationalizing the geometric features of lanthanide complexes.
    • This work has broad implications for lanthanide coordination chemistry and the design of rare-earth metal-based materials.