Reversible Atomization and Nano-Clustering of Pt as a Strategy for Designing Ultra-Low-Metal-Loading Catalysts

Noble 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.

Smitshuysen, Thomas Erik LyckTechnical University of Denmark (författare)
Kakekhani, ArvinUniversity of Pennsylvania (författare)
Jespersen, Sebastian Pirel FredsgaardHaldor Topsøe A/S (författare)
Banerjee, SayanUniversity of Pennsylvania (författare)
Krabbe, AlexanderTechnical University of Denmark (författare)
Hagen, NicolaiTechnical University of Denmark (författare)
Silva, HugoDanish Technological Institute (DTI) (författare)
Just, JustusLund University,Lunds universitet,MAX IV-laboratoriet,MAX IV Laboratory(Swepub:lu)ju5031ju (författare)
Damsgaard, Christian DanvadTechnical University of Denmark (författare)
Helveg, StigTechnical University of Denmark (författare)
Rappe, Andrew M.University of Pennsylvania (författare)
Nørskov, Jens K.Technical University of Denmark (författare)
Chorkendorff, IbTechnical University of Denmark (författare)
Technical University of DenmarkUniversity of Pennsylvania (creator_code:org_t)

Ingår i:Journal of Physical Chemistry C: American Chemical Society (ACS)126:38, s. 16194-162031932-74471932-7455

Av författaren/redakt...: Chakraborty, Deb ...; Smitshuysen, Tho ...; Kakekhani, Arvin; Jespersen, Sebas ...; Banerjee, Sayan; Krabbe, Alexande ...; visa fler...; Hagen, Nicolai; Silva, Hugo; Just, Justus; Damsgaard, Chris ...; Helveg, Stig; Rappe, Andrew M.; Nørskov, Jens K.; Chorkendorff, Ib; visa färre...

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