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Title: Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation

Abstract

Here, noble-metal alloys are widely used as heterogeneous catalysts. However, due to the existence of scaling properties of adsorption energies on transition metal surfaces, the enhancement of catalytic activity is frequently accompanied by side reactions leading to a reduction in selectivity for the target product. Herein, we describe an approach to breaking the scaling relationship for propane dehydrogenation, an industrially important reaction, by assembling single atom alloys (SAAs), to achieve simultaneous enhancement of propylene selectivity and propane conversion. We synthesize γ-alumina-supported platinum/copper SAA catalysts by incipient wetness co-impregnation method with a high copper to platinum ratio. Single platinum atoms dispersed on copper nanoparticles dramatically enhance the desorption of surface-bounded propylene and prohibit its further dehydrogenation, resulting in high propylene selectivity (~90%). Unlike previous reported SAA applications at low temperatures (<400 °C), Pt/Cu SAA shows excellent stability of more than 120 h of operation under atmospheric pressure at 520 °C.

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [2];  [3];  [4];  [5];  [4];  [1]; ORCiD logo [1]
  1. Tianjin Univ., Tianjin (People's Republic of China); Collaborative Innovation Center for Chemical Science & Engineering (Tianjin), Tianjin (People's Republic of China)
  2. Tianjin Univ. of Technology, Tianjin (People's Republic of China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Purdue Univ., West Lafayette, IN (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1480621
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sun, Guodong, Zhao, Zhi -Jian, Mu, Rentao, Zha, Shenjun, Li, Lulu, Chen, Sai, Zang, Ketao, Luo, Jun, Li, Zhenglong, Purdy, Stephen C., Kropf, A. Jeremy, Miller, Jeffrey T., Zeng, Liang, and Gong, Jinlong. Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation. United States: N. p., 2018. Web. doi:10.1038/s41467-018-06967-8.
Sun, Guodong, Zhao, Zhi -Jian, Mu, Rentao, Zha, Shenjun, Li, Lulu, Chen, Sai, Zang, Ketao, Luo, Jun, Li, Zhenglong, Purdy, Stephen C., Kropf, A. Jeremy, Miller, Jeffrey T., Zeng, Liang, & Gong, Jinlong. Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation. United States. doi:10.1038/s41467-018-06967-8.
Sun, Guodong, Zhao, Zhi -Jian, Mu, Rentao, Zha, Shenjun, Li, Lulu, Chen, Sai, Zang, Ketao, Luo, Jun, Li, Zhenglong, Purdy, Stephen C., Kropf, A. Jeremy, Miller, Jeffrey T., Zeng, Liang, and Gong, Jinlong. Fri . "Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation". United States. doi:10.1038/s41467-018-06967-8. https://www.osti.gov/servlets/purl/1480621.
@article{osti_1480621,
title = {Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation},
author = {Sun, Guodong and Zhao, Zhi -Jian and Mu, Rentao and Zha, Shenjun and Li, Lulu and Chen, Sai and Zang, Ketao and Luo, Jun and Li, Zhenglong and Purdy, Stephen C. and Kropf, A. Jeremy and Miller, Jeffrey T. and Zeng, Liang and Gong, Jinlong},
abstractNote = {Here, noble-metal alloys are widely used as heterogeneous catalysts. However, due to the existence of scaling properties of adsorption energies on transition metal surfaces, the enhancement of catalytic activity is frequently accompanied by side reactions leading to a reduction in selectivity for the target product. Herein, we describe an approach to breaking the scaling relationship for propane dehydrogenation, an industrially important reaction, by assembling single atom alloys (SAAs), to achieve simultaneous enhancement of propylene selectivity and propane conversion. We synthesize γ-alumina-supported platinum/copper SAA catalysts by incipient wetness co-impregnation method with a high copper to platinum ratio. Single platinum atoms dispersed on copper nanoparticles dramatically enhance the desorption of surface-bounded propylene and prohibit its further dehydrogenation, resulting in high propylene selectivity (~90%). Unlike previous reported SAA applications at low temperatures (<400 °C), Pt/Cu SAA shows excellent stability of more than 120 h of operation under atmospheric pressure at 520 °C.},
doi = {10.1038/s41467-018-06967-8},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Fri Oct 26 00:00:00 EDT 2018},
month = {Fri Oct 26 00:00:00 EDT 2018}
}

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