Electric potential stability and ionic permeability of SAMs on gold derived from bidentate and tridentate chelating alkanethiols

Wei Wang, Shishan Zhang, Pawilai Chinwangso, Rigoberto C. Advincula, T. Randall Lee

Research output: Contribution to journalArticle

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Abstract

The interfacial electrochemical properties of self-assembled monolayers (SAMs) on gold derived from a structurally tailored series of monodentate, bidentate, and tridentate chelating alkanethiols were investigated.Specific adsorbates included 1-hexadecanethiol (C16), 2-tetradecylpropane-1,3-dithiol (C16C2), 2-tetradecyl-2-methylpropane-1,3-dithiol (C16C3), 2,2- ditetradecylpropane-1,3-dithiol (C16C16), and 1,1,1-tris(mercaptomethyl) pentadecane (t-C16). Reductive desorption of the SAMs as a function of potential was probed by voltammetric measurements, which indicated the following relative order of electric potential stability: t-C16 > C16C2=C16C3=C16C16 > C16. The ionic permeability was investigated under various applied cathodic potentials by electrochemical impedance spectroscopy (EIS). An examination of SAMs prepared at room temperature and accessed by EIS at open-circuit potential showed that the ionic permeability increased in the order C16C2 > C16 > C16C3 > C16C16 > t-C16. The ionic permeability of films was further influenced by the electric potential of the metal substrate and the temperature at which the monolayers were assembled. The potential dependence of the ionic permeability was qualitatively rationalized by considering both the initial ionic permeability and the electric potential stability of the SAMs. Similarly, the ionic permeability of the SAMs prepared at elevated temperature showed contributions from both their thermal stability and their insulating properties at room temperature.

Original languageEnglish
Pages (from-to)3717-3725
Number of pages9
JournalJournal of Physical Chemistry C
Volume113
Issue number9
DOIs
Publication statusPublished - 2009 Mar 5
Externally publishedYes

Fingerprint

Self assembled monolayers
Chelation
Gold
permeability
gold
Electric potential
electric potential
thiols
Electrochemical impedance spectroscopy
Temperature
impedance
Adsorbates
Electrochemical properties
room temperature
Monolayers
Desorption
Thermodynamic stability
spectroscopy
Metals
thermal stability

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

Electric potential stability and ionic permeability of SAMs on gold derived from bidentate and tridentate chelating alkanethiols. / Wang, Wei; Zhang, Shishan; Chinwangso, Pawilai; Advincula, Rigoberto C.; Lee, T. Randall.

In: Journal of Physical Chemistry C, Vol. 113, No. 9, 05.03.2009, p. 3717-3725.

Research output: Contribution to journalArticle

Wang, Wei ; Zhang, Shishan ; Chinwangso, Pawilai ; Advincula, Rigoberto C. ; Lee, T. Randall. / Electric potential stability and ionic permeability of SAMs on gold derived from bidentate and tridentate chelating alkanethiols. In: Journal of Physical Chemistry C. 2009 ; Vol. 113, No. 9. pp. 3717-3725.
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AB - The interfacial electrochemical properties of self-assembled monolayers (SAMs) on gold derived from a structurally tailored series of monodentate, bidentate, and tridentate chelating alkanethiols were investigated.Specific adsorbates included 1-hexadecanethiol (C16), 2-tetradecylpropane-1,3-dithiol (C16C2), 2-tetradecyl-2-methylpropane-1,3-dithiol (C16C3), 2,2- ditetradecylpropane-1,3-dithiol (C16C16), and 1,1,1-tris(mercaptomethyl) pentadecane (t-C16). Reductive desorption of the SAMs as a function of potential was probed by voltammetric measurements, which indicated the following relative order of electric potential stability: t-C16 > C16C2=C16C3=C16C16 > C16. The ionic permeability was investigated under various applied cathodic potentials by electrochemical impedance spectroscopy (EIS). An examination of SAMs prepared at room temperature and accessed by EIS at open-circuit potential showed that the ionic permeability increased in the order C16C2 > C16 > C16C3 > C16C16 > t-C16. The ionic permeability of films was further influenced by the electric potential of the metal substrate and the temperature at which the monolayers were assembled. The potential dependence of the ionic permeability was qualitatively rationalized by considering both the initial ionic permeability and the electric potential stability of the SAMs. Similarly, the ionic permeability of the SAMs prepared at elevated temperature showed contributions from both their thermal stability and their insulating properties at room temperature.

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