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Trimetallic gold and copper complexes with acetylide ligands show different dynamic behaviors. The gold complex exhibits dynamic sigma, pi-exchange, while the copper complex remains static, offering insights into metal-ligand interactions.

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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Supramolecular Chemistry

Background:

  • Gold and copper complexes with acetylide ligands are of interest due to their unique electronic and structural properties.
  • Understanding the dynamic behavior of these complexes is crucial for designing new materials and catalysts.

Purpose of the Study:

  • To synthesize and characterize novel trimetallic cationic gold and copper acetylide complexes.
  • To investigate the dynamic behavior of these complexes in solution using variable-temperature NMR spectroscopy.
  • To explore the influence of metal identity (gold vs. copper) on complex fluxionality.

Main Methods:

  • Synthesis of trimetallic cationic gold and copper acetylide complexes.
  • Variable-temperature 1H NMR spectroscopy (VT-NMR) to study dynamic processes.
  • Computational studies (DFT) to elucidate reaction mechanisms and electronic structures.

Main Results:

  • Selective formation of trimetallic cationic species [IPrAuC≡C(π-MIPr)AuIPr][OTf] (M = Au or Cu).
  • Homotrimetallic gold complex exhibits dynamic σ,π-exchange even at -130 °C.
  • Heterometallic gold-copper analogue shows a static scenario.
  • Extension of the acetylide bridge introduces π,π-exchange, which is rapid in the copper complex and thermally arrested in the gold complex.
  • Computational studies suggest differences in transition state geometries explain the divergent behavior.

Conclusions:

  • The study reveals distinct dynamic behaviors between homotrimetallic gold and heterometallic gold-copper acetylide complexes.
  • Metal identity significantly influences the fluxional processes (σ,π-exchange and π,π-exchange) in these trimetallic systems.
  • Computational insights highlight the role of transition state geometry in governing the observed differences in dynamic behavior.