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A Terminally Bound Niobium Methylidyne.

Takashi Kurogi1, Patrick J Carroll1, Daniel J Mindiola1

  • 1Department of Chemistry, University of Pennsylvania , 231 South 34th Street, Philadelphia, Pennsylvania 19104, United States.

Journal of the American Chemical Society
|March 16, 2016
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Summary
This summary is machine-generated.

This study reports the synthesis of rare niobium methylidene and methylidyne complexes. These complexes undergo reactions to form a unique niobium nitride, advancing organometallic chemistry.

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Area of Science:

  • Organometallic Chemistry
  • Niobium Complexes
  • Carbene and Carbide Chemistry

Background:

  • Niobium complexes with alkyl and aryl ligands are crucial in catalysis and materials science.
  • Synthesis and characterization of low-coordinate niobium species, such as methylidenes and methylidynes, remain challenging.
  • Understanding the reactivity of these species is key to developing new synthetic methodologies.

Purpose of the Study:

  • To synthesize and characterize novel niobium methylidene and methylidyne complexes.
  • To investigate the reactivity of these complexes, including their conversion to niobium nitrides.
  • To elucidate the structural features of these unique organometallic compounds.

Main Methods:

  • Synthesis of a niobium dimethyl precursor, (PNP)Nb(CH3)2(OAr).
  • Oxidation to form a niobium methyl triflate complex, (PNP)Nb(CH3)2(OAr)(OTf).
  • Photolysis and ylide reactions to generate methylidene and methylidyne complexes.
  • Cross-metathesis reactions for niobium nitride synthesis.
  • Solid-state structural analysis (X-ray diffraction).

Main Results:

  • Successful synthesis of a rare niobium methylidene complex, (PNP)Nb═CH2(OAr)(OTf), via photolysis.
  • Formation of a mononuclear niobium methylidyne complex, (PNP)Nb≡CH(OAr), through ylide addition or base treatment.
  • Structural confirmation of terminal methylidene and methylidyne moieties with short Nb-C bond lengths.
  • Synthesis of a neutral, mononuclear niobium nitride, (PNP)Nb≡N(OAr), via methylidyne-nitride cross-metathesis.

Conclusions:

  • This work expands the known chemistry of low-coordinate niobium carbene and carbide complexes.
  • The facile conversion of methylidyne to nitride complexes opens new avenues for synthesizing transition metal nitrides.
  • The characterized complexes provide valuable insights into the bonding and reactivity of niobium-carbon and niobium-nitrogen multiple bonds.