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Introducing Brønsted acid sites to accelerate the bridging-oxygen-assisted deprotonation in acidic water oxidation
Oxygen evolution reaction (OER) consists of four sequential proton-coupled electron transfer steps, which suffer from sluggish kinetics even on state-of-the-art ruthenium dioxide (RuO(2)) catalysts. Understanding and controlling the proton transfer process could be an effective strategy to improve O...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9388623/ https://www.ncbi.nlm.nih.gov/pubmed/35982041 http://dx.doi.org/10.1038/s41467-022-32581-w |
Sumario: | Oxygen evolution reaction (OER) consists of four sequential proton-coupled electron transfer steps, which suffer from sluggish kinetics even on state-of-the-art ruthenium dioxide (RuO(2)) catalysts. Understanding and controlling the proton transfer process could be an effective strategy to improve OER performances. Herein, we present a strategy to accelerate the deprotonation of OER intermediates by introducing strong Brønsted acid sites (e.g. tungsten oxides, WO(x)) into the RuO(2). The Ru-W binary oxide is reported as a stable and active iridium-free acidic OER catalyst that exhibits a low overpotential (235 mV at 10 mA cm(−2)) and low degradation rate (0.014 mV h(−1)) over a 550-hour stability test. Electrochemical studies, in-situ near-ambient pressure X-ray photoelectron spectroscopy and density functional theory show that the W-O-Ru Brønsted acid sites are instrumental to facilitate proton transfer from the oxo-intermediate to the neighboring bridging oxygen sites, thus accelerating bridging-oxygen-assisted deprotonation OER steps in acidic electrolytes. The universality of the strategy is demonstrated for other Ru-M binary metal oxides (M = Cr, Mo, Nb, Ta, and Ti). |
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