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This study reports the synthesis of a stable paramagnetic polyhydrido cluster containing diiron and tetrairidium centers. This novel cluster exhibits unique reactivity and stability, expanding the known chemistry of polyhydrido transition metal complexes.

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Area of Science:

  • Organometallic Chemistry
  • Inorganic Chemistry
  • Materials Science

Background:

  • Polyhydrido transition metal complexes are valuable for their diverse bonding and reactivity.
  • Well-defined paramagnetic polyhydrido systems are scarce due to inherent instability.

Purpose of the Study:

  • To explore the protonolysis reactivity of Cp*IrH4 with transition metal silylamides.
  • To synthesize and characterize novel paramagnetic polyhydrido clusters.

Main Methods:

  • Reaction of Fe-(HMDS)2(THF) with Cp*IrH4 to form the target cluster.
  • Characterization using spectroscopic and analytical techniques.
  • Investigating reactivity through reduction and oxidation studies.

Main Results:

  • Synthesis and characterization of the paramagnetic polyhydrido diiron tetrairidium cluster [Fe-(Cp*IrH3)2]2 (1).
  • Formation of an anionic species K-[Fe-(Cp*IrH3)3] (2) via a proposed disproportionation mechanism upon reduction of 1.
  • Oxidation studies revealed preferential oxidation at iridium centers, not iron.

Conclusions:

  • The synthesized tetrairidium diiron cluster is exceptionally stable.
  • The study highlights an unexpected driving force towards this specific cluster formation.
  • This work expands the scope of known paramagnetic polyhydrido complexes.