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Metal ions can be separated from one another by complexation with organic ligands–the chelating agent– to form uncharged chelates. Here, the chelating agent must contain hydrophobic groups and behave as a weak acid, losing a proton to bind with the metal. Since most organic ligands used in this process are insoluble or undergo oxidation in the aqueous phase, the chelating agent is initially added to the organic phase and extracted into the aqueous phase. The metal-ligand complex is...
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Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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Perturbing the Copper(III)-Hydroxide Unit through Ligand Structural Variation.

Debanjan Dhar1, Gereon M Yee1, Andrew D Spaeth1

  • 1Department of Chemistry, Center for Metals in Biocatalysis, Chemical Theory Center, and Minnesota Supercomputing Institute, University of Minnesota , 207 Pleasant Street Southeast, Minneapolis, Minnesota 55455, United States.

Journal of the American Chemical Society
|December 24, 2015
PubMed
Summary
This summary is machine-generated.

New copper complexes with modified ligands influence hydrogen-atom abstraction (HAT) reactions. Electronic tuning impacts thermodynamics and kinetics, revealing a linear trend between reaction enthalpy and rate, with subtle variations due to barriers and tunneling.

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Area of Science:

  • Organometallic Chemistry
  • Catalysis
  • Reaction Mechanisms

Background:

  • Copper complexes are crucial in catalysis.
  • Understanding ligand effects on metal-centered reactivity is key.
  • Hydrogen-atom abstraction (HAT) is a fundamental reaction pathway.

Purpose of the Study:

  • To synthesize and characterize new copper(III)-hydroxide complexes with tailored electronic properties.
  • To investigate the thermodynamic and kinetic effects of ligand modification on HAT reactions.
  • To elucidate the factors governing the reactivity of copper-hydroxide species.

Main Methods:

  • Synthesis of novel ligand sets: (pipMe)LH2 and (NO2)LH2.
  • Measurement of O-H bond dissociation energies (BDEs) for Cu(II)-OH2 complexes.
  • Kinetic studies of HAT reactions by Cu(III)-hydroxide complexes using substrates with varying C-H bond strengths.
  • Analysis of kinetic isotope effects (KIEs) and transition-state theory calculations.

Main Results:

  • Ligand modification resulted in modest differences in BDEs for the O-H bonds.
  • A linear correlation was observed between the logarithm of the second-order rate constant (log k) and the reaction enthalpy (ΔH).
  • Subtle variations in reaction rates were attributed to changes in HAT barrier heights and quantum tunneling efficiencies at low temperatures (-80 to -20 °C).

Conclusions:

  • Electronic tuning of copper complexes via ligand design significantly impacts HAT reaction thermodynamics and kinetics.
  • The observed linear trend highlights the dominant role of reaction enthalpy, but other factors like tunneling also play a role.
  • This study provides valuable insights into controlling the reactivity of copper-hydroxide complexes for catalytic applications.