Wang, Yicheng;
Schumann, Julia;
Happel, Elizabeth E;
Çınar, Volkan;
Sykes, E Charles H;
Stamatakis, Michail;
Michaelides, Angelos;
(2022)
Observation and Characterization of Dicarbonyls on a RhCu Single-Atom Alloy.
Journal of Physical Chemistry Letters
, 13
(27)
pp. 6316-6322.
10.1021/acs.jpclett.2c01596.
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Abstract
Dicarbonyl species are ubiquitous on Rh/oxide catalysts and are known to form on Rh+ centers. However, dicarbonyl species have never been directly observed on single-atom alloys (SAAs) where the active site is metallic. Herein, using surface science and theoretical modeling, we provide evidence of dicarbonyl species at isolated Rh sites on a RhCu(100) SAA. This approach not only enables us to directly visualize dicarbonyl species at Rh sites but also demonstrates that the transition between the mono- and dicarbonyl configuration can be achieved by changing surface temperature and CO pressure. Density functional theory calculations further support the mono- and dicarbonyl assignments and provide evidence that these species should be stable on other SAA combinations. Together, these results provide a picture of the structure and energetics of both the mono- and dicarbonyl configurations on the RhCu(100) SAA surface and should aid with IR assignments on SAA nanoparticle catalysts.
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