First-principles design of a single-atom–alloy propane dehydrogenation catalyst

Hannagan, Ryan T.; Giannakakis, Georgios; Réocreux, Romain; Schumann, Julia; Finzel, Jordan; Wang, Yicheng; Michaelides, Angelos; Deshlahra, Prashant; Christopher, Phillip; Flytzani-Stephanopoulos, Maria; Stamatakis, Michail; Sykes, E. Charles H.

doi:10.1126/science.abg8389

DOE OSTI · 1798526

First-principles design of a single-atom–alloy propane dehydrogenation catalyst

Hannagan, Ryan T.·Giannakakis, Georgios·Réocreux, Romain·Schumann, Julia·Finzel, Jordan·Wang, Yicheng·Michaelides, Angelos·Deshlahra, Prashant·Christopher, Phillip·Flytzani-Stephanopoulos, Maria·Stamatakis, Michail·Sykes, E. Charles H.

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Abstract

The complexity of heterogeneous catalysts means that a priori design of new catalytic materials is difficult, but the well-defined nature of single-atom–alloy catalysts has made it feasible to perform unambiguous theoretical modeling and precise surface science experiments. Herein we report the theory-led discovery of a rhodium-copper (RhCu) single-atom–alloy catalyst for propane dehydrogenation to propene. Although Rh is not generally considered for alkane dehydrogenation, first-principles calculations revealed that Rh atoms disperse in Cu and exhibit low carbon-hydrogen bond activation barriers. Surface science experiments confirmed these predictions, and together these results informed the design of a highly active, selective, and coke-resistant RhCu nanoparticle catalyst that enables low-temperature nonoxidative propane dehydrogenation.

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Hannagan, Ryan T., Giannakakis, Georgios, Réocreux, Romain, Schumann, Julia, Finzel, Jordan, Wang, Yicheng, Michaelides, Angelos, Deshlahra, Prashant, Christopher, Phillip, Flytzani-Stephanopoulos, Maria, Stamatakis, Michail, Sykes, E. Charles H.. 2021-06-24. First-principles design of a single-atom–alloy propane dehydrogenation catalyst. https://doi.org/10.1126/science.abg8389

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