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Labile capping bonds in lanthanide(III) complexes: shorter and weaker.

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The Journal of Physical Chemistry. A
|December 31, 2014
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Lanthanide coordination complexes exhibit unusual bonding where shorter bonds are weaker due to ligand screening. This "labile capping bonds phenomenon" explains lanthanide hydration complexities and offers new chemical insights.

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Area of Science:

  • Inorganic Chemistry
  • Coordination Chemistry
  • Lanthanide Chemistry

Background:

  • Trivalent lanthanide ions form coordination complexes with diverse geometries.
  • Badger's rule typically predicts bond strength increases with shorter bond lengths.
  • Observed anomalies in lanthanide complex bonding necessitate further investigation.

Purpose of the Study:

  • To investigate the violation of Badger's rule in lanthanide coordination complexes.
  • To elucidate the underlying mechanisms responsible for anomalous bonding.
  • To introduce and validate the concept of "labile capping bonds phenomenon".

Main Methods:

  • Analysis of coordination complexes with tricapped trigonal prism and monocapped square antiprism configurations.
  • Theoretical examination of screening and repulsion effects from prism ligands.
  • Correlation of theoretical findings with experimental observations in lanthanide(III) hydration.

Main Results:

  • Lanthanide-capping ligand bonds were found to weaken as they shorten, violating Badger's rule.
  • Ligand screening and repulsion effects were identified as the primary cause of this anomaly.
  • Heavier lanthanides exhibit more labile capping bonds due to these effects.

Conclusions:

  • The "labile capping bonds phenomenon" provides a new framework for understanding lanthanide complex behavior.
  • This phenomenon explains variations in water exchange rates in different coordination geometries.
  • The study offers novel insights into the chemical properties and reactivity of lanthanide complexes.