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New tris(pyrazolyl)borate ligands with functionalized arms enable tunable intramolecular H-bonding. Copper complexes demonstrate this H-bonding, influencing hydroxide ligand properties and acidity.

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Area of Science:

  • Coordination Chemistry
  • Supramolecular Chemistry
  • Ligand Design

Background:

  • Tris(pyrazolyl)borate ligands are versatile scaffolds in coordination chemistry.
  • Intramolecular hydrogen bonding can significantly influence metal complex properties.
  • Designing ligands with tunable H-bonding capabilities is crucial for developing new catalysts and materials.

Purpose of the Study:

  • To synthesize novel tris(pyrazolyl)borate ligands (XpyMeTpK) with functionalized pendant arms.
  • To investigate the ability of these ligands to form intramolecular hydrogen bonds with metal-bound functionalities.
  • To explore the impact of these H-bonding interactions on the structure and reactivity of copper complexes.

Main Methods:

  • Modular synthesis of tris(pyrazolyl)borate ligands.
  • Synthesis and characterization of copper complexes ([XpyMeTpCu]2(μ-OH)2 and XpyMeTpCu-OAc).
  • Single crystal X-ray diffraction for structural analysis.
  • Infrared (IR) spectroscopy to study vibrational frequencies of hydroxide ligands.
  • Protonation studies to assess ligand acidity.

Main Results:

  • Successful synthesis of a series of XpyMeTpK ligands.
  • X-ray structures revealed intramolecular H-bonding between pendant heterocycles and bridging hydroxide ligands in dinuclear copper complexes.
  • IR studies showed reduced νOH frequencies correlated with the H-bond accepting ability of the pendant arm.
  • Protonation studies indicated that the acidity of aquo ligands decreases with increasing H-bond accepting ability of the pendant arm.

Conclusions:

  • The developed XpyMeTpK ligands effectively facilitate tunable intramolecular H-bonding in copper complexes.
  • This H-bonding influences the structural and electronic properties of the metal center and its bound ligands.
  • The findings provide a foundation for designing ligands with controlled reactivity through directed hydrogen bonding interactions.