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We synthesized a novel mixed-valent dicerium complex with an azide bridge, revealing significant electron delocalization through 4f/5d orbital mixing. This finding advances understanding of bonding in lanthanide chemistry.

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Area of Science:

  • Inorganic Chemistry
  • Lanthanide Chemistry
  • Materials Science

Background:

  • Dilanthanide complexes with one-electron delocalization are key to understanding 4f/5d-bonding in lanthanide chemistry.
  • Investigating mixed-valent lanthanide complexes provides insights into electronic structures and bonding.

Purpose of the Study:

  • To synthesize and characterize a novel isolable azide-bridged dicerium complex.
  • To elucidate the electronic structure and bonding nature of the mixed-valent dicerium complex.
  • To explore the phenomenon of one-electron delocalization in lanthanide chemistry.

Main Methods:

  • Synthesis of the dicerium complex using a tripodal ligand-supported cerium precursor and sodium azide.
  • Structural and bonding characterization via X-ray crystal diffraction, EPR, magnetic measurements, cyclic voltammetry, and X-ray absorption spectroscopy.
  • Quantum-theoretical studies to analyze electronic structure and orbital mixing.

Main Results:

  • An isolable azide-bridged dicerium complex, [{(TrapenTMS)Ce}2(μ-N3)]•, was successfully synthesized.
  • The complex exhibits a trans-bent Ce-N3-Ce unit with a single delocalized electron across two mixed-valent cerium atoms.
  • Low-temperature anisotropic EPR signals and quantum chemical analyses confirm strong 4f/5d orbital mixing and multicentered one-electron interaction.

Conclusions:

  • The study reports a new class of mixed-valent dilanthanide complexes.
  • The findings provide a model system for understanding multicentered one-electron delocalization in ligand-bridged dilanthanide systems.
  • This research deepens the understanding of specific 4f/5d-bonding features in lanthanide chemistry.