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Evolution of Intermediates on Metal Oxide Photoanodes in a Full pH Range by Ji, Xing (author);Ou, Yinqing (author);Huang, Lu (author);Gan, Liyong (author);Zhang, Yunhuai (author);Xiao, Peng (author) is a Chemistry article available to read on EtoBox.

What is Evolution of Intermediates on Metal Oxide Photoanodes in a Full pH Range about?

Understanding the function of intermediates generated at the photoanode/ electrolyte interface is crucial for unraveling the reaction mechanisms and enhancing the efficiency of oxygen evolution reaction (OER). Previous studies have recognized one type of intermediate MO on Fe 2 O 3 in near-neutral electrolytes and verified it as the active species. Herein, we investigate the intermediates on metal oxides, including TiO 2 , Fe 2 O 3 , and WO 3 , using operando infrared spectroscopy and in situ light−dark electrochemical scans in a full pH range. We identified the low valence M−OH species at the metal oxide/electrolyte interface in pH = 11∼13, as well as the high valence MO species in pH = 1∼11. Density functional theory calculations point to a strong influence of the protonation or hydroxylation on the stability of the intermediates, resulting in the evolution of intermediates under different pH. We demonstrate the double role of M−OH intermediates which trigger recombination in near-neutral electrolytes and serve as an active center under high alkaline conditions, thus mediating the OER performance and making the reaction transition from single-site to multisite mechanisms as the

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Author

Ji, Xing (author);Ou, Yinqing (author);Huang, Lu (author);Gan, Liyong (author);Zhang, Yunhuai (author);Xiao, Peng (author)

Publisher

American Chemical Society (ACS)

Published

2023

Language

EN

Field

Chemistry (Physical Sciences)