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

Abstract

Abstract Ceria (CeO 2 ) 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/CeO 2 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 CeO 2 , 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 CeO 2 ‐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 CeO 2 , making Pt–Sn/CeO 2 a fully regenerable catalyst.

Authors:
ORCiD logo [1];  [2];  [3];  [3];  [4];  [5];  [1];  [3]; ORCiD logo [1]
  1. Department of Chemical &, Biological Engineering and Center for Microengineered Materials University of New Mexico Albuquerque NM 87131 USA
  2. Research Institute of Photocatalysis State Key Laboratory of Photocatalysis on Energy and Environment Fuzhou University Fuzhou 350002 China
  3. Inorganic Chemistry and Catalysis Debye Institute for Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands
  4. Department of Chemistry and Chemical Biology University of New Mexico Albuquerque NM 87131 USA
  5. Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99352 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1408256
Alternate Identifier(s):
OSTI ID: 1374922
Resource Type:
Published Article
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Name: Angewandte Chemie Journal Volume: 129 Journal Issue: 31; Journal ID: ISSN 0044-8249
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Xiong, Haifeng, Lin, Sen, Goetze, Joris, Pletcher, Paul, Guo, Hua, Kovarik, Libor, Artyushkova, Kateryna, Weckhuysen, Bert M., and Datye, Abhaya K. Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria. Germany: N. p., 2017. Web. doi:10.1002/ange.201701115.
Xiong, Haifeng, Lin, Sen, Goetze, Joris, Pletcher, Paul, Guo, Hua, Kovarik, Libor, Artyushkova, Kateryna, Weckhuysen, Bert M., & Datye, Abhaya K. Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria. Germany. https://doi.org/10.1002/ange.201701115
Xiong, Haifeng, Lin, Sen, Goetze, Joris, Pletcher, Paul, Guo, Hua, Kovarik, Libor, Artyushkova, Kateryna, Weckhuysen, Bert M., and Datye, Abhaya K. Wed . "Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria". Germany. https://doi.org/10.1002/ange.201701115.
@article{osti_1408256,
title = {Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria},
author = {Xiong, Haifeng and Lin, Sen and Goetze, Joris and Pletcher, Paul and Guo, Hua and Kovarik, Libor and Artyushkova, Kateryna and Weckhuysen, Bert M. and Datye, Abhaya K.},
abstractNote = {Abstract Ceria (CeO 2 ) 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/CeO 2 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 CeO 2 , 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 CeO 2 ‐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 CeO 2 , making Pt–Sn/CeO 2 a fully regenerable catalyst.},
doi = {10.1002/ange.201701115},
journal = {Angewandte Chemie},
number = 31,
volume = 129,
place = {Germany},
year = {Wed Jun 28 00:00:00 EDT 2017},
month = {Wed Jun 28 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/ange.201701115

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