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Título: | Structure matters: Asymmetric CO oxidation at Rh steps with different atomic packing |
Autor: | Garcia-Martinez, Fernando CSIC ORCID; Rämisch, Lisa; Ali, Khadiza CSIC ORCID; Waluyo, Iradwikanari; Castrillo-Bodero, Rodrigo CSIC ORCID; Pfaff, Sebastian; Villar-García, Ignacio J.; Walter, Andrew Leigh; Hunt, Adrian; Pérez-Dieste, Virginia; Zetterberg, Johan; Lundgren, Edvin; Schiller, Frederik CSIC ORCID; Ortega, J. Enrique CSIC ORCID | Fecha de publicación: | 2022 | Editor: | American Chemical Society | Citación: | Journal of the American Chemical Society 144(33): 15363-15371 (2022) | Resumen: | Curved crystals are a simple but powerful approach to bridge the gap between single crystal surfaces and nanoparticle catalysts, by allowing a rational assessment of the role of active step sites in gas-surface reactions. Using a curved Rh(111) crystal, here, we investigate the effect of A-type (square geometry) and B-type (triangular geometry) atomic packing of steps on the catalytic CO oxidation on Rh at millibar pressures. Imaging the crystal during reaction ignition with laser-induced CO2 fluorescence demonstrates a two-step process, where B-steps ignite at lower temperature than A-steps. Such fundamental dissimilarity is explained in ambient pressure X-ray photoemission (AP-XPS) experiments, which reveal partial CO desorption and oxygen buildup only at B-steps. AP-XPS also proves that A-B step asymmetries extend to the active stage: at A-steps, low-active O–Rh–O trilayers buildup immediately after ignition, while highly active chemisorbed O is the dominant species on B-type steps. We conclude that B-steps are more efficient than A-steps for the CO oxidation. | Versión del editor: | https://doi.org/10.1021/jacs.2c06733 | URI: | http://hdl.handle.net/10261/303450 | DOI: | 10.1021/jacs.2c06733 | E-ISSN: | 1520-5126 |
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strucpack.pdf | 5,02 MB | Adobe PDF | Visualizar/Abrir |
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