Reversible Atomization and Nano-Clustering of Pt as a Strategy for Designing Ultra-Low-Metal-Loading Catalysts
(2022) In Journal of Physical Chemistry C 126(38). p.16194-16203- Abstract
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... (More)
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.
(Less)
- author
- organization
- publishing date
- 2022-09
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Physical Chemistry C
- volume
- 126
- issue
- 38
- pages
- 10 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- scopus:85138768260
- ISSN
- 1932-7447
- DOI
- 10.1021/acs.jpcc.2c05213
- language
- English
- LU publication?
- yes
- id
- 33813fa2-3c31-47d2-a57f-54dbf32c980b
- date added to LUP
- 2022-12-19 15:01:05
- date last changed
- 2022-12-19 15:01:05
@article{33813fa2-3c31-47d2-a57f-54dbf32c980b,
abstract = {{<p>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.</p>}},
author = {{Chakraborty, Debasish and Smitshuysen, Thomas Erik Lyck and Kakekhani, Arvin and Jespersen, Sebastian Pirel Fredsgaard and Banerjee, Sayan and Krabbe, Alexander and Hagen, Nicolai and Silva, Hugo and Just, Justus and Damsgaard, Christian Danvad and Helveg, Stig and Rappe, Andrew M. and Nørskov, Jens K. and Chorkendorff, Ib}},
issn = {{1932-7447}},
language = {{eng}},
number = {{38}},
pages = {{16194--16203}},
publisher = {{The American Chemical Society (ACS)}},
series = {{Journal of Physical Chemistry C}},
title = {{Reversible Atomization and Nano-Clustering of Pt as a Strategy for Designing Ultra-Low-Metal-Loading Catalysts}},
url = {{http://dx.doi.org/10.1021/acs.jpcc.2c05213}},
doi = {{10.1021/acs.jpcc.2c05213}},
volume = {{126}},
year = {{2022}},
}