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Electrochemical Insights Into Hydrogen Peroxide Generation on Carbon Electrodes in Alkaline Electrolytes: The Impact of Carbon Surface Structure and Alkali Metal Cations
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DOI：10.1002/cctc.70884.png)
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Abstract
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We examined oxygen reduction reaction (ORR) on basal- and edge-oriented pyrolytic graphite (PG) in alkaline media in the presence of different alkali cations. While in our previous work in acidic media PG electrodes exhibited an increase in faradaic efficiency (FE) upon the addition of alkali cations, and glassy carbon (GC) showed a pronounced decrease, in alkaline media the FE for H2O2 production did not exhibit clear trends. Nonetheless, the H2O2 production current densities clearly increased in the sequence Cs+>K+>Na+>Li+. The potentials of maximum entropy were similar and independent of the alkali cations present in the solution, in contrast to acidic media, implying that all electrodes underwent similar transitions from dominantly adsorbed anions to cations under these conditions. We explored the interfacial water structure using in situ FTIR to study the effect of the electrode structure and the nature of the alkali cation on the interfacial water layer and found that it is dominantly determined by the structure of the carbon electrode. In situ Raman spectroscopy provided additional evidence of cation–carbon interactions, as reflected by changes in the D′ band, particularly for PG-Edge. Our results demonstrate that the structure of the carbon surface plays a decisive role in governing cation–surface and cation–intermediate interactions.
Keywords:
basal/edge planes
carbon-based electrode
cation effect
hydrogen peroxide production
in situ Raman spectroelectrochemistry
oxygen reduction reaction
potential of maximal entropy
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