Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria

Ceria (CeO2) supports are unique in their ability to trap ionic platinum (Pt), providing exceptional stability for isolated single atoms of Pt. The reactivity and stability of single‐atom Pt species was explored for the industrially important light alkane dehydrogenation reaction. The single‐atom Pt...

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Bibliographic Details
Published in:Angewandte Chemie (International ed.) Vol. 56; no. 31; pp. 8986 - 8991
Main Authors: Xiong, Haifeng, Lin, Sen, Goetze, Joris, Pletcher, Paul, Guo, Hua, Kovarik, Libor, Artyushkova, Kateryna, Weckhuysen, Bert M., Datye, Abhaya K.
Format: Journal Article
Language:English
Published: Germany Wiley Subscription Services, Inc 24.07.2017
Wiley
John Wiley and Sons Inc
Edition:International ed. in English
Subjects:
Adsorption
Alkanes
catalyst regeneration
Catalysts
ceria
Cerium oxides
Clusters
Coke
Communication
Communications
Dehydrogenation
Environmental Molecular Sciences Laboratory
light alkane dehydrogenation
Oxidation
Phase transitions
Platinum
Propane
Propylene
Selectivity
single atoms
subnanometer Pt–Sn catalysis
Thermal stability
Tin
Water vapor
subnanometer Pt-Sn catalysis
ceria
single atoms
catalyst regeneration
light alkane dehydrogenation
ISSN:1433-7851, 1521-3773, 1521-3773
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Summary:Ceria (CeO2) supports are unique in their ability to trap ionic platinum (Pt), providing exceptional stability for isolated single atoms of Pt. The reactivity and stability of single‐atom Pt species was explored for the industrially important light alkane dehydrogenation reaction. The single‐atom Pt/CeO2 catalysts are stable during propane dehydrogenation, but are not selective for propylene. DFT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions. In contrast, when tin (Sn) is added to CeO2, the single‐atom Pt catalyst undergoes an activation phase where it transforms into Pt–Sn clusters under reaction conditions. Formation of small Pt–Sn clusters allows the catalyst to achieve high selectivity towards propylene because of facile desorption of the product. The CeO2‐supported Pt–Sn clusters are very stable, even during extended reaction at 680 °C. Coke formation is almost completely suppressed by adding water vapor to the feed. Furthermore, upon oxidation the Pt–Sn clusters readily revert to the atomically dispersed species on CeO2, making Pt–Sn/CeO2 a fully regenerable catalyst. Isolated platinum single atoms are active but not selective for alkane dehydrogenation. Platinum single atoms self‐assemble into subnanometer platinum–tin clusters during reaction. The spent catalyst readily reverts to an atomically dispersed state after oxidation treatment without the need for added chlorine.
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USDOE
AC05-76RL01830
PNNL-SA-126830
ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.201701115