Structures of Atoms and Molecules Adsorbed on the Surface of Single Crystal Electrodes and in situ Measurement of Kinetics of Electrode Reactions

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The aims of this project were to clarify the orientation and structure of atoms and molecules on well-defined single crystal electrodes by infrared reflection-absorption spectroscopy and other techniques, to measure heterogeneous rate constants of redox-electrode reactions on such electrodes and to elucidate the effect of the structure of electrode/solution interface on the rate constants. We obtained the following results. 1. We found that specific hydrogen wave observed in cyclic voltammograms on Pt (111) electrode is closely related to the anion adsorption. 2. We clarified the effects of anion and alkaline and alkaline-earth metal ions on the structure of water in the interfacial region. 3. We found that the rate of redox-electrode reaction of (II/III) at Pt single crystal electrodes decreases in the order : (111) > (100) > (110). FT-IR measurements also revealed that hexacyanoferrate decomposes to form adsorbed CN layr on platinum surface. Based on these findings, we proposed a reaction mechanism that gives reasonable explanation. 4. Response time of electrochemical thin-layr cells for in situ IR reflectance-absorption spectroscopy was theoretically treated. 5. The reaction mechanism of hydrogen peroxide oxidation at Ni complex modified electrodes was clarified from the infrared spectroscopic evidence.