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

Abstract

CeO2 supports are unique in their ability to trap ionic Pt, providing exceptional stability for isolated single atoms of Pt. Here, we explore the reactivity and stability of single atom Pt species for the industrially important reaction of light alkane dehydrogenation. The single atom Pt/CeO2 catalysts are stable during propane dehydrogenation, but we observe no selectivity towards propene. DFT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions. In contrast, when Sn is added to ceria, 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 propene, due to facile desorption of the product. The CeO2-supported Pt-Sn clusters are very stable, even during extended reaction at 680 °C. By adding water vapor to the feed, coke formation can almost completely be suppressed. Furthermore, the Pt-Sn clusters can be readily transformed back to the atomically dispersed species on ceria via oxidation, making Pt-Sn/CeO2 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:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1374648
Report Number(s):
PNNL-SA-126830
Journal ID: ISSN 1433-7851; 48427; KP1704020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 31
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

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. United States: N. p., 2017. Web. doi:10.1002/anie.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. United States. doi:10.1002/anie.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". United States. doi:10.1002/anie.201701115.
@article{osti_1374648,
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 = {CeO2 supports are unique in their ability to trap ionic Pt, providing exceptional stability for isolated single atoms of Pt. Here, we explore the reactivity and stability of single atom Pt species for the industrially important reaction of light alkane dehydrogenation. The single atom Pt/CeO2 catalysts are stable during propane dehydrogenation, but we observe no selectivity towards propene. DFT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions. In contrast, when Sn is added to ceria, 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 propene, due to facile desorption of the product. The CeO2-supported Pt-Sn clusters are very stable, even during extended reaction at 680 °C. By adding water vapor to the feed, coke formation can almost completely be suppressed. Furthermore, the Pt-Sn clusters can be readily transformed back to the atomically dispersed species on ceria via oxidation, making Pt-Sn/CeO2 a fully regenerable catalyst.},
doi = {10.1002/anie.201701115},
journal = {Angewandte Chemie (International Edition)},
number = 31,
volume = 56,
place = {United States},
year = {Wed Jun 28 00:00:00 EDT 2017},
month = {Wed Jun 28 00:00:00 EDT 2017}
}