期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 7, 期 3, 页码 480-485出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b02400
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资金
- Department of Energy [DOE FG02-10ER16170]
- European Research Council [616121]
- Royal Society through a Wolfson Research merit Award
- Engineering and Physical Sciences Research Council UK
- European Research Council (ERC) [616121] Funding Source: European Research Council (ERC)
- Engineering and Physical Sciences Research Council [1352369] Funding Source: researchfish
Key descriptors in hydrogenation catalysis are the nature of the active sites for H-2 activation and the adsorption strength of H atoms to the surface. Using atomically resolved model systems of dilute Pd-Au surface alloys and density functional theory calculations, we determine key aspects of H-2 activation, diffusion, and desorption. Pd monomers in a Au(111) surface catalyze the dissociative adsorption of H-2 at temperatures as low as 85 K, a process previously expected to require contiguous Pd sites. H atoms preside at the Pd sites and desorb at temperatures significantly lower than those from pure Pd (175 versus 310 K). This facile H-2 activation and weak adsorption of H atom intermediates are key requirements for active and selective hydrogenations. We also demonstrate weak adsorption of CO, a common catalyst poison, which is sufficient to force H atoms to spill over from Pd to Au sites, as evidenced by low-temperature H-2 desorption.
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