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

Guodong Sun; Zhi Jian Zhao; Rentao Mu; Shenjun Zha; Lulu Li; Sai Chen; Ketao Zang; Jun Luo; Zhenglong Li; Stephen C. Purdy; A. Jeremy Kropf; Jeffrey T. Miller; Liang Zeng; Jinlong Gong

doi:10.1038/s41467-018-06967-8

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

Guodong Sun, Zhi Jian Zhao, Rentao Mu, Shenjun Zha, Lulu Li, Sai Chen, Ketao Zang, Jun Luo, Zhenglong Li, Stephen C. Purdy, A. Jeremy Kropf, Jeffrey T. Miller, Liang Zeng, Jinlong Gong

Research output: Contribution to journal › Article › peer-review

656 Scopus citations

Abstract

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.

Original language	English
Article number	4454
Journal	Nature Communications
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41467-018-06967-8
State	Published - Dec 1 2018
Externally published	Yes

Funding

The authors thank the National Science Foundation of China (21525626, 21506149, 91645106, U1663224) and the Program of Introducing Talents of Discipline to Universities (No. B06006) for financial support. S.C.P. and J.T.M. are supported in part by the National Science Foundation under Coopperative Agreement No. EEC-1647722. Use of the Advanced Photo Source is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DEAC02-06CH11357. MRCAT operations, beamline 10-BM, are supported by the Department of Energy and the MRCAT member institutions. Z.L is supported by the BioEnergy Technolgies Office, Office of Energy Efficiency and Renewable Energy, U.S. Department of Energy.

Access to Document

10.1038/s41467-018-06967-8

Cite this

@article{6eb4e224a1ff408f9892c511ebf51bfc,

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

abstract = "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 (\textasciitilde{}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.",

author = "Guodong Sun and Zhao, \{Zhi Jian\} and Rentao Mu and Shenjun Zha and Lulu Li and Sai Chen and Ketao Zang and Jun Luo and Zhenglong Li and Purdy, \{Stephen C.\} and Kropf, \{A. Jeremy\} and Miller, \{Jeffrey T.\} and Liang Zeng and Jinlong Gong",

note = "Publisher Copyright: {\textcopyright} 2018, The Author(s).",

year = "2018",

month = dec,

day = "1",

doi = "10.1038/s41467-018-06967-8",

language = "English",

volume = "9",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

TY - JOUR

T1 - Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation

AU - Sun, Guodong

AU - Zhao, Zhi Jian

AU - Mu, Rentao

AU - Zha, Shenjun

AU - Li, Lulu

AU - Chen, Sai

AU - Zang, Ketao

AU - Luo, Jun

AU - Li, Zhenglong

AU - Purdy, Stephen C.

AU - Kropf, A. Jeremy

AU - Miller, Jeffrey T.

AU - Zeng, Liang

AU - Gong, Jinlong

PY - 2018/12/1

Y1 - 2018/12/1

N2 - 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.

AB - 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.

UR - https://www.scopus.com/pages/publications/85055612123

U2 - 10.1038/s41467-018-06967-8

DO - 10.1038/s41467-018-06967-8

M3 - Article

C2 - 30367052

AN - SCOPUS:85055612123

SN - 2041-1723

VL - 9

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 4454

ER -

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

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this