The degradation of Pt-containing oxygen reduction catalysts for fuel cell applications is strongly linked to the electrochemical surface oxidation and reduction of Pt. Here, we study the surface restructuring and Pt dissolution mechanisms during oxidation/reduction for the case of Pt(100) in 0.1 M HClO by combining operando high-energy surface X-ray diffraction, online mass spectrometry, and density functional theory. Our atomic-scale structural studies reveal that anodic dissolution, detected during oxidation, and cathodic dissolution, observed during the subsequent reduction, are linked to two different oxide phases. Anodic dissolution occurs predominantly during nucleation and growth of the first, stripe-like oxide. Cathodic dissolution is linked to a second, amorphous Pt oxide phase that resembles bulk PtO and starts to grow when the coverage of the stripe-like oxide saturates. In addition, we find the amount of surface restructuring after an oxidation/reduction cycle to be potential-independent after the stripe-like oxide has reached its saturation coverage.
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| http://dx.doi.org/10.1002/anie.202304293 | DOI Listing |
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Article Synopsis
- Understanding hydrogen transfer on solid surfaces is crucial for improving reactions that involve hydrogen, but it's complicated by the structure of powder catalysts, especially oxides.
- The study constructs MnO monolayers on a Pt substrate and examines how hydrogen moves across these surfaces, finding that hydrogen diffuses differently depending on the structure (stripe vs. grid).
- Results show that hydrogen moves four times faster on MnO due to a unique surface effect, with theoretical insights highlighting the impact of oxygen atom distances on hydrogen diffusion efficiency.
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