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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes
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Macrocyclic Triruthenium Complexes Having Electronically Coupled Mixed-Valent States.

Daniel Fink1, Michael Bodensteiner2, Michael Linseis1

  • 1Fachbereich Chemie, Universität Konstanz, Universitätsstrasse 10, 78457, Konstanz, Germany.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|November 3, 2017
PubMed
Summary

Researchers created novel C3-symmetric triangular triruthenium alkenyl complexes. These macrocycles exhibit unique electrochemical properties, showing valence delocalization in mixed-valent states for conductive molecular loops.

Keywords:
density functional calculationselectrochemistrymacrocyclesmixed-valent compoundsruthenium

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Area of Science:

  • Organometallic Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • Self-assembly of ligands with metal precursors is a key strategy in coordination chemistry.
  • Macrocyclic complexes offer unique structural and electronic properties.
  • Ruthenium complexes are widely studied for their catalytic and electronic applications.

Purpose of the Study:

  • To synthesize and characterize novel C3-symmetric triangular triruthenium alkenyl macrocyclic complexes.
  • To investigate the electrochemical behavior and charge delocalization in these multinuclear ruthenium systems.
  • To explore their potential as molecule-based conductive materials.

Main Methods:

  • Self-assembly of 5-ethynyl-2-furancarboxylic acid or 3-ethynylbenzoic acid with [HRu(CO)Cl(PiPr3)2].
  • Characterization using multinuclear NMR spectroscopy, high-resolution ESI mass spectrometry, and X-ray crystallography.
  • Electrochemical studies (cyclic voltammetry) to determine oxidation potentials and assess charge delocalization.

Main Results:

  • Successful synthesis of C3-symmetric triangular triruthenium alkenyl complexes [{Ru(CO)(PiPr3)2(CH=CHArCOO)}3].
  • Complexes were fully characterized, with structure confirmed by X-ray crystallography for 1-B.
  • Electrochemical studies revealed three consecutive one-electron oxidation steps.
  • Mixed-valent states exhibited signs of valence delocalization, indicating through-bond charge transport.

Conclusions:

  • The synthesized macrocycles represent rare examples of molecule-based conductive loops.
  • Evidence of through-bond charge delocalization in mixed-valent states highlights their potential for electronic applications.
  • This work expands the scope of multinuclear ruthenium macrocycles with tunable electronic properties.