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Solvent-dependent dihydrogen/dihydride stability for [Mo(CO)(Cp*)H(2)(PMe(3))(2)](+)[BF(4)](-) determined by multiple

Pavel A Dub1, Natalia V Belkova, Oleg A Filippov

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Solvent choice dictates molybdenum complex protonation outcomes. Dihydrogen and dihydride isomers form, with non-covalent interactions influencing stability. Both isomers decompose similarly, yielding novel HF-ligated species.

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Area of Science:

  • Organometallic Chemistry
  • Computational Chemistry

Background:

  • Protonation of transition metal complexes can yield diverse products.
  • Understanding factors controlling isomer formation is crucial for reactivity studies.

Purpose of the Study:

  • To investigate the solvent-dependent protonation of a molybdenum complex.
  • To characterize the resulting dihydrogen and dihydride isomers.
  • To elucidate the role of non-covalent interactions in isomer stability.

Main Methods:

  • Low-temperature protonation reactions.
  • Infrared (IR) and Nuclear Magnetic Resonance (NMR) spectroscopy for characterization.
  • X-ray crystallography for structural determination.
  • Density Functional Theory (DFT) calculations.

Main Results:

  • Protonation of [Mo(CO)(Cp*)H(PMe(3))(2)] (1) yields either a dihydrogen complex (2) in THF or a dihydride complex (3) in dichloromethane.
  • Both isomers (2 and 3) decompose to [Mo(CO)(Cp*)(FBF(3))(PMe(3))(2)] (4) at similar rates.
  • A novel complex [Mo(CO)(Cp*)(FHFBF(3))(PMe(3))(2)] (5) featuring an HF ligand was characterized.
  • DFT calculations highlighted the importance of anion-solvent interactions in determining isomer stability.

Conclusions:

  • Solvent effects significantly influence the outcome of low-temperature protonation reactions of molybdenum complexes.
  • Non-covalent interactions between anions and solvent molecules play a critical role in stabilizing different isomeric forms.
  • The study reveals novel reactivity and structural motifs in organometallic chemistry.