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Transition metal-carbon complexes. A theoretical study.

Andreas Krapp1, Krishna K Pandey, Gernot Frenking

  • 1School of Chemical Sciences, Devi Ahilya University Indore, Indore-452017, India.

Journal of the American Chemical Society
|May 29, 2007
PubMed
Summary
This summary is machine-generated.

Ruthenium and iron complexes with carbon ligands exhibit strong metal-carbon bonds, particularly in 16-electron-valent (16VE) species. Metal-carbon bonds are stronger than metal-carbonyl bonds, with 16VE complexes showing greater stabilization than 18-electron-valent (18VE) complexes.

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Area of Science:

  • Organometallic Chemistry
  • Computational Chemistry
  • Inorganic Chemistry

Background:

  • Investigating metal-ligand bonding is crucial for understanding chemical reactivity.
  • Ruthenium and iron complexes with carbon ligands are of interest due to their potential applications.

Purpose of the Study:

  • To determine the equilibrium geometries and bond dissociation energies of 16- and 18-electron-valent (16VE and 18VE) ruthenium and iron complexes with a naked carbon ligand.
  • To compare the strength of metal-carbon bonds with metal-carbonyl bonds.
  • To analyze the bonding interactions using charge and energy decomposition analyses (EDA).

Main Methods:

  • Density Functional Theory (DFT) at the BP86/TZ2P level.
  • Coupled cluster calculations with singles and doubles (CCSD(T)) using TZ2P basis sets.
  • Energy Decomposition Analysis (EDA).

Main Results:

  • 16VE ruthenium-carbon (Ru-C) bonds are stronger than iron-carbon (Fe-C) bonds.
  • Metal-carbon bonds in 18VE complexes are weaker than in 16VE species.
  • Metal-carbon bonds are significantly stronger than metal-carbonyl bonds.
  • 18VE iron complexes show higher bond dissociation energies (BDEs) than 18VE ruthenium complexes, with the opposite trend for 16VE compounds.

Conclusions:

  • The strong Ru-C and Fe-C bonds in 16VE complexes are stabilized by metal-C sigma interactions.
  • The bonding in 18VE complexes is better described by closed-shell donor-acceptor interactions.
  • The nature of metal-carbon and metal-carbonyl binding interactions are similar, but absolute energy terms are larger for carbon complexes.
  • 18VE compounds exhibit longer and weaker metal-carbon and metal-carbonyl bonds compared to 16VE compounds.