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Author:

Xu, Liuxin (Xu, Liuxin.) | Tai, Xiaolin (Tai, Xiaolin.) | Feng, Lei (Feng, Lei.) | Zhang, Xu (Zhang, Xu.) | Pan, Ya (Pan, Ya.) | Tang, Bing (Tang, Bing.) | Xu, Ruichao (Xu, Ruichao.) | Shui, Yanna (Shui, Yanna.) | Yuan, Jinglin (Yuan, Jinglin.) | Lin, Yue (Lin, Yue.) | Zhang, Xiaolong (Zhang, Xiaolong.) | He, Shi (He, Shi.) | Sun, Zhihu (Sun, Zhihu.) | Wei, Shiqiang (Wei, Shiqiang.)

Indexed by:

Scopus SCIE

Abstract:

Propane dehydrogenation (PDH) using platinum-based intermetallic catalysts is an important approach for the industrial production of highly value-added propylene. Nevertheless, the high temperature needed for PDH inevitably causes deactivation of the intermetallic catalysts due to phase separation or particle aggregation. Herein, we showcase that a Pt shell offers a promising solution to protect intermetallics under harsh PDH environments. Through selective removal of the surface Zn atoms, a core/shell architecture with 1-2 atomic layers of Pt coating PtZn intermetallic nanoclusters is constructed. No deactivation was observed within an 80 h long-term stability test at 580 degrees C on the optimal PtZn/Pt catalyst, affording an extremely low deactivation rate constant of 0.0007 h-1. Furthermore, the construction of the PtZn/Pt core/shell promotes the catalytic efficiency, with a high propylene formation rate of 124.8 mol of C3H6 gPt -1 h-1 that surpasses that of most of the Pt-based PDH catalysts reported. Density functional theory calculations reveal that the Pt shell plays dual roles in stabilizing the intermetallic core and modifying the electronic structure of the ensemble by inducing a compressive strain. This lattice strain downshifts the d-band center to a lower value of -3.02 eV and decreases propylene desorption energy to a level lower than the barrier energy of C-H breaking by 0.66 eV, resulting in enhanced coking resistance and reactivity.

Keyword:

nanocluster propane dehydrogenation in situcharacterization strain intermetalliccatalysts core/shell

Author Community:

  • [ 1 ] [Xu, Liuxin]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 2 ] [Pan, Ya]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 3 ] [Tang, Bing]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 4 ] [Xu, Ruichao]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 5 ] [Shui, Yanna]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 6 ] [Yuan, Jinglin]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 7 ] [Sun, Zhihu]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 8 ] [Wei, Shiqiang]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
  • [ 9 ] [Tai, Xiaolin]Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem, Hefei 230026, Peoples R China
  • [ 10 ] [Lin, Yue]Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem, Hefei 230026, Peoples R China
  • [ 11 ] [Feng, Lei]Univ Sci & Technol China, Dept Chem Phys, Hefei 230029, Peoples R China
  • [ 12 ] [Zhang, Xu]Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstruct & Properties Solids, Beijing, Peoples R China
  • [ 13 ] [Zhang, Xiaolong]Univ Sci & Technol China, Div Nanomat & Chem, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
  • [ 14 ] [He, Shi]Duke Univ, Dept Chem, Durham, NC 27708 USA

Reprint Author's Address:

  • [Sun, Zhihu]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China;;[Zhang, Xiaolong]Univ Sci & Technol China, Div Nanomat & Chem, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China;;[He, Shi]Duke Univ, Dept Chem, Durham, NC 27708 USA

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Source :

ACS CATALYSIS

ISSN: 2155-5435

Year: 2025

Issue: 5

Volume: 15

Page: 4172-4184

1 2 . 9 0 0

JCR@2022

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 7

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