Controlling Selectivity in Unsaturated Aldehyde HydrogenationUsing Single-Site Alloy Catalysts
2019
Selectivity in catalysis is key to many industrial processes, yet it is often difficult to control. One promising approach is to use so-called single-atom catalysts, whereby one catalytic component is isolated within a second phase to add a key but otherwise unavailable functionality. Here, we report the use of metal alloys consisting of Pt single atoms diluted within Cu nanoparticles to selectively promote the hydrogenation of C═O bonds in unsaturated aldehydes, a reaction of interest in fine chemical manufacturing. Our rationale, that Cu surfaces may favor C═O over C═C hydrogenation steps with atomic hydrogen but may require Pt sites to promote the initial activation of molecular hydrogen, was corroborated by kinetic catalytic experiments. However, fundamental surface science studies and quantum mechanics calculations showed that the explanation for the observed catalytic performance is more nuanced. For one, titration experiments using carbon monoxide failed to identify Pt atoms accessible on the surf...
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