Regulation of Oxide Pathway Mechanism for Sustainable Acidic Water Oxidation

The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evol...

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Veröffentlicht in:Journal of the American Chemical Society 2024-11, Vol.146 (46), p.32049-32058
Hauptverfasser: Cao, Xuejie, Qin, Hongye, Zhang, Jinyang, Chen, Xiaojie, Jiao, Lifang
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Sprache:eng
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Zusammenfassung:The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evolution mechanism, while the lattice-oxygen-mediated mechanism undermines stability. Here, we propose a heterogeneous dual-site oxide pathway mechanism (OPM) that avoids these limitations through direct dioxygen radical coupling. A combination of Lewis acid (Cr) and Ru to form solid solution oxides (Cr x Ru1–x O2) promotes OH adsorption and shortens the dual-site distance, which facilitates the formation of *O radical and promotes the coupling of dioxygen radical, thereby altering the OER mechanism to a Cr–Ru dual-site OPM. The Cr0.6Ru0.4O2 catalyst demonstrates a lower overpotential than that of RuO2 and maintains stable operation for over 350 h in a PEM water electrolyzer at 300 mA cm–2. This mechanism regulation strategy paves the way for an optimal catalytic pathway, essential for large-scale green hydrogen production.
ISSN:0002-7863
1520-5126
1520-5126
DOI:10.1021/jacs.4c12942