A ligand substitution reaction of oxo-centred triruthenium complexes assembled as monolayers on gold electrodes

A. Sato, M. Abe, T. Inomata, T. Kondo, S. Ye, K. Uosaki, Y. Sasaki

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27 Citations (Scopus)

Abstract

A terminal ligand-substitution reaction at triruthenium redox centres within monolayer films is investigated. For this purpose, a new redox-active trinuclear ruthenium complex containing one carbonyl ligand at a terminal site, [Ru3(O)(CH3COO)6(CO)(mpy)(C10PY)](mpy = 4-methylpyridine, C10PY = {(NC5H4)CH2NHC(O)(CH2) 10S-}2)1, has been chemically adsorbed onto a gold electrode surface with a disulfide-alkyl spacer C10PY. Densely packed monolayers of complex 1 on Au electrodes (surface coverage, Γ(Ru3) = 1.8 × 10-10 mol cm-2) display the {RuII-CO}RuIIIRuIII/{RuIII-CO}Ru IIIRuIII couple at E1/2 = +0.61 V vs. Ag-AgCl in a 0.1 mol dm-3 HClO4 aqueous solution. Upon electrochemical oxidation of the adsorbed complex at +0.80 V, where the triruthenium carbonyl complex is in the oxidized form {RuIII-CO}RuIIIRuIII, the coordinated CO is replaced by an aqua ligand present in the bulk phase, which is followed by cyclic voltammetry at appropriate electrolysis time intervals. During 8000 s of electrolysis, ca. 67% of the initially assembled carbonyl complexes are converted to the triruthenium aqua complexes, while ca. 25% desorbed from the electrode surface.

Original languageEnglish
Pages (from-to)3420-3426
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume3
Issue number16
DOIs
Publication statusPublished - 2001
Externally publishedYes

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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