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

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

doi:10.1038/s41467-018-06967-8

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

Journal Article · 25 October 2018 · Nature Communications

DOI: https://doi.org/10.1038/s41467-018-06967-8 · OSTI ID:1480621

Sun, Guodong ^[1];

^[1]; Mu, Rentao ^[1]; Zha, Shenjun ^[1]; Li, Lulu ^[1]; Chen, Sai ^[1]; Zang, Ketao ^[2]; Luo, Jun ^[2]; Li, Zhenglong ^[3]; Purdy, Stephen C. ^[4]; Kropf, A. Jeremy ^[5]; Miller, Jeffrey T. ^[4]; Zeng, Liang ^[1];

^[1]

Tianjin Univ., Tianjin (People's Republic of China); Collaborative Innovation Center for Chemical Science & Engineering (Tianjin), Tianjin (People's Republic of China)
Tianjin Univ. of Technology, Tianjin (People's Republic of China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); National Science Foundation of China; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1480621

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Size-Dependent Reaction Mechanism and Kinetics for Propane Dehydrogenation over Pt Catalysts Zhu, Jun; Yang, Ming-Lei; Yu, Yingda ACS Catalysis, Vol. 5, Issue 11 https://doi.org/10.1021/acscatal.5b01423	journal	September 2015
Platinum-Modified ZnO/Al ₂ O ₃ for Propane Dehydrogenation: Minimized Platinum Usage and Improved Catalytic Stability Liu, Gang; Zeng, Liang; Zhao, Zhi-Jian ACS Catalysis, Vol. 6, Issue 4 https://doi.org/10.1021/acscatal.5b02878	journal	February 2016
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Propylene Hydrogenation and Propane Dehydrogenation by a Single-Site Zn ²⁺ on Silica Catalyst Schweitzer, Neil M.; Hu, Bo; Das, Ujjal ACS Catalysis, Vol. 4, Issue 4 https://doi.org/10.1021/cs401116p	journal	March 2014
Supported Single Pt ₁ /Au ₁ Atoms for Methanol Steam Reforming Gu, Xiang-Kui; Qiao, Botao; Huang, Chuan-Qi ACS Catalysis, Vol. 4, Issue 11 https://doi.org/10.1021/cs500740u	journal	October 2014
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Single-Atom Pd ₁ /Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene Yan, Huan; Cheng, Hao; Yi, Hong Journal of the American Chemical Society, Vol. 137, Issue 33 https://doi.org/10.1021/jacs.5b06485	journal	August 2015
Tackling CO Poisoning with Single-Atom Alloy Catalysts Liu, Jilei; Lucci, Felicia R.; Yang, Ming Journal of the American Chemical Society, Vol. 138, Issue 20 https://doi.org/10.1021/jacs.6b03339	journal	May 2016
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Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation Marcinkowski, Matthew D.; Darby, Matthew T.; Liu, Jilei Nature Chemistry, Vol. 10, Issue 3 https://doi.org/10.1038/nchem.2915	journal	January 2018
Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts Strasser, Peter; Koh, Shirlaine; Anniyev, Toyli Nature Chemistry, Vol. 2, Issue 6 https://doi.org/10.1038/nchem.623	journal	April 2010
Platinum single-atom and cluster catalysis of the hydrogen evolution reaction Cheng, Niancai; Stambula, Samantha; Wang, Da Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13638	journal	November 2016
Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation Zhang, Zailei; Zhu, Yihan; Asakura, Hiroyuki Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms16100	journal	July 2017
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