Measurement of benzenethiol adsorption to nanostructured Pt, Pd, and PtPd films using Raman spectroelectrochemistry

Langmuir : the ACS Journal of Surfaces and Colloids
Michael B PomfretJeffrey C Owrutsky

Abstract

Raman spectroscopy and electrochemical methods were used to study the behavior of the model adsorbate benzenethiol (BT) on nanostructured Pt, Pd, and PtPd electrodes as a function of applied potential. Benzenethiol adsorbs out of ethanolic solutions as the corresponding thiolate, and voltammetric stripping data reveal that BT is oxidatively removed from all of the nanostructured metals upon repeated oxidative and reductive cycling. Oxidative stripping potentials for BT increase in the order Pt < PtPd < Pd, indicating that BT adsorbs most strongly to nanoscale Pd. Yet, BT Raman scattering intensities, measured in situ over time scales of minutes to hours, are most persistent on the film of nanostructured Pt. Raman spectra indicate that adsorbed BT desorbs from nanoscale Pt at oxidizing potentials via cleavage of the Pt-S bond. In contrast, on nanoscale Pd and PtPd, BT is irreversibly lost due to cleavage of BT C-S bonds at oxidizing potentials, which leaves adsorbed sulfur oxides on Pd and PtPd films and effects the desulfurization of BT. While Pd and PtPd films are less sulfur-resistant than Pt films, palladium oxides, which form at higher potentials than Pt oxides, oxidatively desulfurize BT. In situ spectroelectrochemical Ram...Continue Reading

References

May 1, 2004·Annual Review of Physical Chemistry·Zhong-Qun Tian, Bin Ren
Oct 7, 2005·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Roberto GómezAntonio Aldaz
Oct 20, 2005·Journal of the American Chemical Society·Christina RothDavid E Ramaker
Feb 14, 2007·Analytical Chemistry·Michael B PomfretRobert A Walker
Feb 24, 2007·Analytical and Bioanalytical Chemistry·Bin RenZhong-Qun Tian
May 18, 2007·Journal of the American Chemical Society·Mamdouh E AbdelsalamAndrea E Russell

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Citations

Aug 24, 2010·Langmuir : the ACS Journal of Surfaces and Colloids·Pilar CarroRoberto C Salvarezza
Dec 30, 2010·The Journal of Physical Chemistry. a·Manas Ranjan GartiaGang Logan Liu

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