Journal
NATURE CHEMISTRY
Volume 14, Issue 5, Pages 523-+Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41557-021-00855-3
Keywords
-
Categories
Funding
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Division [DE-SC0020147]
- US National Science Foundation [CBET-1748365]
- Computational Materials Education and Training (CoMET) National Science Foundation Research Traineeship [DGE-1449785]
- National Science Foundation [ACI-1548562]
- U.S. Department of Energy (DOE) [DE-SC0020147] Funding Source: U.S. Department of Energy (DOE)
Ask authors/readers for more resources
Intermetallic compounds provide unique opportunities for manipulating catalytic ensembles atom by atom through precise stoichiometric control, allowing the design of active sites with atomic-level precision.
Intermetallic compounds offer unique opportunities for atom-by-atom manipulation of catalytic ensembles through precise stoichiometric control. The (Pd, M, Zn) gamma-brass phase enables the controlled synthesis of Pd-M-Pd catalytic sites (M = Zn, Pd, Cu, Ag and Au) isolated in an inert Zn matrix. These multi-atom heteronuclear active sites are catalytically distinct from Pd single atoms and fully coordinated Pd. Here we quantify the unexpectedly large effect that active-site composition (that is, identity of the M atom in Pd-M-Pd sites) has on ethylene selectivity during acetylene semihydrogenation. Subtle stoichiometric control demonstrates that Pd-Pd-Pd sites are active for ethylene hydrogenation, whereas Pd-Zn-Pd sites show no measurable ethylene-to-ethane conversion. Agreement between experimental and density-functional-theory-predicted activities and selectivities demonstrates precise control of Pd-M-Pd active-site composition. This work demonstrates that the diversity and well-defined structure of intermetallics can be used to design active sites assembled with atomic-level precision.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available