Proton-coupled electron transfer and lewis acid recognition at self-assembled monolayers of an oxo-bridged diruthenium(III) complex functionalized with two disulfide anchors

Hua Xin Zhang, Masaaki Abe, Yi Zhang, Guofang Li, Shen Ye, Masatoshi Osawa, Yoichi Sasaki

研究成果: Article査読

11 被引用数 (Scopus)

抄録

A new μ-oxo-bis(μ-acetato)diruthenium(III) complex bearing two pyridyl disulfide ligands {[Ru2(μ-O)(μ-OAc)2(bpy) 2(Lpy-SS)2](PF6)2 (OAc = CH3CO2-, bpy = 2,2′-bipyridine, L py-SS = (C5H4N)CH2NHC(O)(CH 2)4CH(CH2)2SS) (1)} has been synthesized to prepare self-assembled monolayers (SAMs) on the Au(111) electrode surface. The SAMs have been characterized by contact-angle measurements, reflection-absorption surface infrared spectroscopy, cyclic voltammetry, and reductive desorption experiments. The SAMs exhibited proton-coupled electron transfer (PCET) reactions when the electrochemistry was studied in aqueous electrolyte solution (0.1 M NaClO4 with Britton-Robinson buffer to adjust the solution pH). The potential-pH plot (Pourbaix diagram) in the pH range from 1 to 12 has established that the dinuclear ruthenium moiety was involved in the interfacial PCET processes with four distinct redox states: RuIIIRuIII(μ-O), RuIIRuIII(μ- OH), RuIIRuII(μ-OH), and RuIIRu II(μ-OH2). We also demonstrated that the interfacial redox processes were modulated by the addition of Lewis acids such as BF 3 or Al3+ to the electrolyte media, in which the externally added Lewis acids interacted with μ-O of the dinuclear moiety within the SAMs.

本文言語English
ページ(範囲)10110-10119
ページ数10
ジャーナルLangmuir
29
32
DOI
出版ステータスPublished - 2013 8 13
外部発表はい

ASJC Scopus subject areas

  • 材料科学(全般)
  • 凝縮系物理学
  • 表面および界面
  • 分光学
  • 電気化学

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