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• W2058102484 abstract "• Superoxide and peroxide with upright orientation are ORR intermediates at alkaline pH. • Vibrational frequency of superoxide intermediate changes with electrolyte. • Relation between absorbance and current is discussed in a simple kinetic scheme. • A way is shown to obtain rate constants of individual steps in multistep reactions. • Reaction from superoxide to peroxide is faster in chloride than in perchlorate. For an understanding of the four electron transfer mechanism of the electrochemical oxygen reduction reaction (ORR), a direct detection of intermediates on well-defined working electrode surfaces is crucial, as it bridges the gap between electrochemistry and computation. Here, the ORR is studied on the crystalline semiconductor n-Ge(1 0 0) by electrochemical attenuated total reflection infrared (ATR-IR) spectroscopy in aqueous NaClO 4 and NaCl solutions at p H 10.5. Germanium-bound superoxide at a tilt angle of ∼45° with respect to the surface normal is found as an intermediate in both electrolytes. The frequency of the superoxide O O stretching mode differs by 25 cm −1 between the two electrolytes, hinting at a complex formation between at least one of the anions and the superoxo-intermediate. This complex formation may be related to the different surface terminations of germanium in the two electrolytes. The surface concentration of the superoxide intermediate is proportional to the ORR current. Analysis of the relation between absorbance and current shows that the rate constant of the second electron transfer step in the ORR, i.e. the step from superoxide to peroxide, in NaCl is three times as high as in NaClO 4 ." @default.
• W2058102484 created "2016-06-24" @default.
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• W2058102484 date "2013-09-01" @default.
• W2058102484 modified "2023-10-06" @default.
• W2058102484 title "In situ infrared spectroscopic investigation of intermediates in the electrochemical oxygen reduction on n-Ge(100) in alkaline perchlorate and chloride electrolyte" @default.
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• W2058102484 doi "https://doi.org/10.1016/j.electacta.2013.05.133" @default.
• W2058102484 hasPublicationYear "2013" @default.
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