Studies of the electrochemical adsorption and reactivity of small organic molecules at well- ordered Pt single-crystal surfaces in the region of underpotential deposition (UPD) of H have become a major activity in current electrochemical surface science. This work presents investigation of the processes of electrosorption of guanidonium (and structurally related) molecule-ions and the Faradaic reduction of two aliphatic oximes (formamidoxime and acetaldehyde oxime), at major Pt single-crystal planes. The results reveal remarkable specificities to Pt surface geometry upon adsorption and reactivity of these small molecules, observed in various electrolytic media. Application of two major electrochemical techniques and a complementary in situ FTIR spectroscopy method enables a thorough understanding of the mechanism of these unique surface electrochemical reactions. This work should be useful not only to professionals directly involved in electrochemistry of single-crystal electrodes, but also to all those working (and studying) in the field of applied electrochemistry, including fuel cell and battery-related processes.

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