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In situ Fourier transform infrared vibrational spectra of thiocyanate ions adsorbed on polycrystalline Ag electrodes as a function of electrode potential and electrolyte concentration are reported. Interpretation of the results are performed with the help of ab initio SCF calculations of the electronic structure and bonding of thiocyanate to small silver clusters. It was concluded that thiocyanate ion adsorbs with S-and N-end down in the double layer region for potentials greater than -0.3 V (versus Ag/AgCl). At potentials close to the potential of zero charge thiocyanate ion is adsorbed flat and cannot be detected by IR.

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