Structure-property relations for surface processes at the metal/solution interface

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Abstract
The recent development of special apparatus coupling electroanalytical cells directly to UHV surface analytical chambers has made possible definitive determination of structure-property relations for processes at metal electrode surfaces. Low-energy electron diffraction analyses of emersed platinum electrodes have provided direct evidence for place-exchange processes accompanying anodic oxidation, and combined with recent x-ray photoelectron spectroscopy and thermal desorption spectroscopy results these studies have refined our understanding of aqueous oxidation phenomena. The use of UHV annealed well-ordered single-crystal surfaces has produced some surprising results. The process of submonolayer metal ion deposition (so-called underpotential deposition) exhibits unexpected sensitivity to long-range order in the substrate, indicating that lateral bonding forces are of the same magnitude as the perpendicular bonding force. On a well-ordered Pt(111) surface, unexpected new surface processes have been observed that are unique to this surface, i.e., are not seen on either (100) or (110) surfaces, nor on polycrystalline surfaces. It appears that the new processes are associated with atomically flat regions of the (111) surface with a critical region size that is quite large, at least 2 nm. It is suggested that cooperative interactions in the double layer form a critical ensemble that react to form the new surface species. However, much further study utilizing in situ spectroscopy will be required to understand this new surface process in Pt(111).

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