Journal article
Reversible Atomization and Nano-Clustering of Pt as a Strategy for Designing Ultra-Low-Metal-Loading Catalysts
Surface Physics and Catalysis, Department of Physics, Technical University of Denmark1
National Centre for Nano Fabrication and Characterization, Technical University of Denmark2
Catalysis Theory Center, Department of Physics, Technical University of Denmark3
Department of Physics, Technical University of Denmark4
Catalysis and Operando Characterization, Nanocharacterization, National Centre for Nano Fabrication and Characterization, Technical University of Denmark5
University of Pennsylvania6
Haldor Topsoe AS7
Danish Technological Institute8
Lund University9
VISION – Center for Visualizing Catalytic Processes, Centers, Technical University of Denmark10
Nanocharacterization, National Centre for Nano Fabrication and Characterization, Technical University of Denmark11
...and 1 moreNoble metal-based catalysts have numerous industrial uses, and maximum utilization of the precious metals by lowering the metal loading is of significant interest in heterogeneous catalysis research. However, lowering the metal loading could lead to single-Atom metal species formation, which may not be active for important reactions like propylene oxidation.
We report a way to drastically reduce precious metal loading of catalysts by judiciously choosing an active metal/support pair and using the reversible atomization-nanoparticulate formation of transition metal on a high-surface area support. Here, Pt and MgAl2O4 are used as the transition metal and high-surface area support, respectively.
Through catalytic testing and characterization using scanning transmission electron microscopy and synchrotron X-ray absorption spectroscopy, a reversible change between atomization and nano-cluster formation under oxidizing and reducing conditions has been found. Via density functional theory, favorable sites for reversible Pt adsorption are identified, including ionic Pt4+ sites that can serve to nucleate nanoclusters.
Catalytic reaction modeling also rationalizes the catalytic inertness of atomic Pt sites. Finally, a re-Activation mechanism for the atomized Pt based on gases present during reaction has been formulated and demonstrated.
Language: | English |
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Publisher: | American Chemical Society |
Year: | 2022 |
Pages: | 16194-16203 |
ISSN: | 19327455 and 19327447 |
Types: | Journal article |
DOI: | 10.1021/acs.jpcc.2c05213 |
ORCIDs: | Chakraborty, Debasish , Smitshuysen, Thomas Erik Lyck , Krabbe, Alexander , Damsgaard, Christian Danvad , Helveg, Stig , Nørskov, Jens K. , Chorkendorff, Ib , 0000-0002-8553-7776 , 0000-0002-8067-1351 , 0000-0002-8586-9236 and 0000-0003-4620-6496 |