Russian Journal of Electrochemistry

, Volume 42, Issue 11, pp 1177–1192 | Cite as

Electrocatalytic properties of Au(111)-Pd quasi-single-crystal film electrodes as probed by ATR-SEIRAS

Article

Abstract

Electrochemical and electrocatalytic properties of thin films Au(111-25 nm), which are quasi-single-crystal electrodes 25 nm thick made of gold with the (111) preferential orientation, and same electrodes modified with a monolayer (ML) of palladium are studied in 0.1 M solutions of HClO4 and H2SO4 employing voltammetric techniques and surface enhanced infrared reflection absorption spectroscopy (ATR-SEIRAS). Spectroscopic experiments demonstrate strong adsorption of electrolyte species (H2O, OHads, anions) on the Pd surface. The weak and reversible adsorption of CO on Au(111-25 nm) does not change the interfacial-water structure. Adsorption of CO on the Pd-modified film results in an irreversibly adsorbed CO adlayer stabilized by co-adsorbed isolated water species. Various electrooxidation mechanisms are discussed. Electrochemical and spectroscopic investigations on the adsorption and electrooxidation of HCOOH on bare and 1 ML Pd-Au(111-25 nm) electrodes reveal that electrooxidation proceeds in both cases via a direct or dehydrogenation pathway. This mechanism involves the formation of formate as intermediate, which is detected by in situ ATR-SEIRAS. The reactivity on Pd-modified surfaces is higher than on bare gold. The specifically adsorbed anions (sulfate/bisulfate) and the oxide formation on the substrate surface lower the reactivity for CO and HCOOH on both surfaces.

Key words

SEIRAS quasi-single-crystal Au(111-25 nm) films palladium interfacial water carbon monoxide formic acid adsorption electrooxidation 

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Copyright information

© MAIK “Nauka/Interperiodica” 2006

Authors and Affiliations

  1. 1.Boreskov Institute of Catalysis, Siberian DivisionRussian Academy of SciencesNovosibirskRussia
  2. 2.Institute for Thin Films and Interfaces ISG 3Research Centre JuelichJuelichGermany

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