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Valence Bond Theory02:42

Valence Bond Theory

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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Magnetometric Characterization of Intermediates in the Solid-State Electrochemistry of Redox-Active Metal-Organic Frameworks
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Characterization of noninnocent metal complexes using solid-state NMR spectroscopy: o-dioxolene vanadium complexes.

Pabitra B Chatterjee1, Olga Goncharov-Zapata, Laurence L Quinn

  • 1Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523-1872, USA.

Inorganic Chemistry
|August 17, 2011
PubMed
Summary

Solid-state NMR studies reveal that vanadium NMR chemical shifts, not quadrupolar couplings, effectively characterize noninnocent vanadium(V) catechol complexes. This method aids in understanding electronic properties of diverse vanadium systems.

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Area of Science:

  • Inorganic Chemistry
  • Solid-State NMR Spectroscopy
  • Computational Chemistry

Background:

  • Vanadium(V) catechol complexes are crucial in various chemical applications.
  • Solid-state Nuclear Magnetic Resonance (SSNMR) offers insights into material properties.
  • Characterizing noninnocent ligands in metal complexes is essential for understanding their reactivity.

Purpose of the Study:

  • To investigate the utility of (51)V SSNMR observables in characterizing vanadium(V) catechol complexes.
  • To correlate (51)V NMR parameters with the electronic structures of these compounds.
  • To explore the influence of ligand substitution on electronic properties and NMR signals.

Main Methods:

  • Solid-state (51)V NMR spectroscopy was performed on a series of vanadium(V) catechol complexes.
  • Quantum chemical calculations (Density Functional Theory) were used to model NMR parameters.
  • Systematic variation of catechol ligands with electron-donating and electron-withdrawing groups was employed.

Main Results:

  • A linear correlation was observed between solution and solid-state (51)V NMR chemical shifts.
  • (51)V NMR chemical shift anisotropy was found to be a sensitive probe of electronic distribution.
  • Small quadrupolar coupling constants suggested symmetric charge distribution, but were insufficient for detailed characterization.
  • Ligand substitution influenced the HOMO-LUMO gap, correlating with upfield (electron-donating) or downfield (electron-withdrawing) shifts.

Conclusions:

  • (51)V SSNMR chemical shifts and anisotropy are valuable for characterizing vanadium complexes, especially those with noninnocent ligands.
  • Quadrupolar coupling constants alone do not fully capture the electronic complexity of these systems.
  • The study provides a framework for applying (51)V SSNMR to a broader range of redox-active complexes.