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N2 Functionalization via Molybdenum-Nitride Complex: Stepwise BH Bond Additions.

Idir Benaissa1,2, Barbara Rialland1,2, Soukaina Bennaamane1,2

  • 1Laboratoire Hétérochimie, Fondamentale et Appliquée, Université Paul Sabatier, CNRS, 118 Route de Narbonne, 31062, Toulouse, France.

Angewandte Chemie (International Ed. in English)
|April 29, 2024
PubMed
Summary
This summary is machine-generated.

The reactivity of a molybdenum-nitrido complex, generated from nitrogen splitting, with boranes is detailed. This study reveals new reaction pathways and unprecedented complexes, advancing nitrogen functionalization chemistry.

Keywords:
DFT calculationsMolybdenumN2 reductionboranesnitride functionalization

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Area of Science:

  • Organometallic Chemistry
  • Inorganic Chemistry
  • Nitrogen Fixation

Background:

  • Nitrogen splitting by transition metal complexes is a key step towards nitrogen functionalization.
  • Understanding the reactivity of metal-nitrido species is crucial for developing new catalytic processes.

Purpose of the Study:

  • To investigate the reactivity of a (triphosphine)molybdenum(IV)-nitrido complex towards boranes.
  • To elucidate the reaction mechanisms and characterize the resulting adducts and complexes.

Main Methods:

  • Synthesis and characterization of the (triphosphine)Mo(IV)-nitrido complex.
  • Reactions with various borane reagents (BH3.SMe2, 9-BBN).
  • Spectroscopic analysis (NMR, X-ray crystallography) to determine structures.

Main Results:

  • Formation of a simple adduct Mo≡N→BH3 with BH3.SMe2.
  • Evidence of 1,2-addition with 9-BBN, yielding H-Mo=NBR2.
  • Observation of an unprecedented complex with two bridging hydrogens after a second BH3.SMe2 addition.
  • Reductive elimination and N-H bond formation promoted by PMe3 or BH3.SMe2.

Conclusions:

  • The study demonstrates a full sequence of functionalization at the Mo≡N moiety after N2 splitting.
  • New reaction pathways and unprecedented complexes involving molybdenum-nitrido and borane interactions were discovered.
  • This work provides insights into the controlled functionalization of nitrogen coordinated to transition metals.