Ensemble Effect Evidenced by CO Adsorption on the 3-Fold PdGa Surfaces

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• 作者：Jan Prinz ; Roberto Gaspari ; Quirin S. St枚ckl ; Peter Gille ; Marc Armbr眉ster ; Harald Brune ; Oliver Gr枚ning ; Carlo A. Pignedoli ; Daniele Passerone ; Roland Widmer
• 刊名：Journal of Physical Chemistry C
• 出版年：2014
• 出版时间：June 12, 2014
• 年：2014
• 卷：118
• 期：23
• 页码：12260-12265
• 全文大小：282K
• 年卷期：v.118,no.23(June 12, 2014)
• ISSN：1932-7455

文摘

The atomic structure and composition of a catalyst鈥檚 surface have a major influence on its performance regarding activity and selectivity. In this respect, intermetallic compounds are promising future catalyst materials, as their surfaces exhibit small and well-defined ensembles of active metal atoms. In this study, the active adsorption sites of the 3-fold-symmetric surfaces of the PdGa intermetallic compound were investigated in a combined experimental and computational approach using CO as a test molecule. The PdGa(111) and (鈭?鈥?鈥?) surfaces exhibit very similar electronic structures, but have Pd sites with very different, well-defined atomic coordination and separation. They thereby serve as prototypical model systems for studying ensemble effects on bimetallic catalytic surfaces. Scanning tunneling microscopy and Fourier transform infrared spectroscopy show that the CO adsorption on both surfaces is solely associated with the topmost Pd atoms and Ga acts only as an inactive spacer. The different local configurations of these Pd atoms dictate the CO adsorption sites as a function of coverage. The experimental results are corroborated by density functional theory and illustrate the site separation and ensemble effects for molecular adsorption on intermetallic single crystalline surfaces.