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Subtle surface modifications can have profound effects on catalytic and electrocatalytic chemistry. Reflection-AbsorptionInfrared Spectroscopy (RAIRS) using synchrotron radiation is potentially a very powerful probe of the surface interactionsinvolved provided that sufficiently high quality data can be obtained. The performance of the Daresbury RAIRS facility inits original configuration is illustrated with examples of complex adsorbate systems including trimethylamine adsorbed onNi{l 1 l}, CO coadsorbed with potassium on Cu{l 10) and formate on Cu{lOO} . The factors that limited performance arehighlighted, and the recent major reconstruction ofthe station to eliminate these is described.Keywords: Reflection-Absorption Infrared Spectroscopy, Synchrotron, trimethylamine, carbon monoxide, potassium,formate. 1. ThITRODUCTION The bonding of adsorbate molecules at metal surfaces plays a primary role in controlling the properties and performance ofmany interfacial catalytic phenomena, e.g., in electrocatalysis and heterogeneous catalysis. However, investigations of thesebonds has been limited, primarily by the lack of suitable instrumental methods which are capable of probing such bondingwith sufficient sensitivity in an interface created under realistic conditions. A powerful method of obtaining information onthe interaction of molecules to surfaces is to directly probe the vibrations of the metal-adsorbate bond, which occur below