Evidence of MarsVanKrevelen Mechanism in the Electrochemical Oxygen Evolution on Ni Based Catalysts
- Evidence of MarsVanKrevelen Mechanism in the Electrochemical Oxygen Evolution on Ni Based Catalysts
- 오형석; Jorge Ferreira de Araujo; Fabio Dionigi; Thomas Merzdorf; Peter Strasser
- Alkaline OER Catalyst; Differential Electrochemical Mass Spectrometry; Isotope 18O; Lattice Oxygen Evolution
- Issue Date
- Angewandte Chemie international edition
- VOL 게재예정, 게제예정
- Water oxidation is a crucial reaction for renewable energy conversion and storage. Among the alkaline oxygen evolution reaction (OER) catalysts, NiFe based oxyhydroxides show the highest catalytic activity. However, the details of their OER mechanism are still unclear, due to the elusive nature of the OER intermediates. Here by using a novel differential electrochemical mass spectrometry (DEMS) cell interface, we performed water isotope-labelled experiments in 18O-labelled alkaline electrolyte on Ni(OH)2 and NiFe layered double hydroxide nanocatalysts. Our experiments confirm the occurrence of Mars-van-Krevelen lattice oxygen evolution reaction mechanism in both catalysts to various degrees, which involves the coupling of oxygen atoms from the catalyst and the electrolyte. The quantitative charge analysis suggests that the participating lattice oxygen atoms belong exclusively to the catalyst surface, confirming DFT computational hypotheses. Also, DEMS data suggest a fundamental correlation between the magnitude of the lattice oxygen mechanism and the faradaic efficiency of oxygen controlled by pseudocapacitive oxidative metal redox charges.
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