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author:

Yao, Yongbin (Yao, Yongbin.) [1] | Wang, Jingnan (Wang, Jingnan.) [2] | Liu, Qiang (Liu, Qiang.) [3] | Yu, Can (Yu, Can.) [4] | Gao, Zhan (Gao, Zhan.) [5] | Yuan, Fangli (Yuan, Fangli.) [6] | Wang, Xi (Wang, Xi.) [7]

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Abstract:

Simultaneously enhancing selectivity and stability on supported propane dehydrogenation (PDH) catalysts remains a formidable challenge. Here, we report a combined static and dynamic strategy to address these issues synergistically. Firstly, we demonstrate a feasible sol-gel method for preparing atomically-dispersed Bi-decorated metal nanoparticle catalysts (MBi/Al2O3, M=Fe, Co, Ni, and Zn). In PDH testing, the total selectivity of by-products (CH4 and C2H6) significantly decreases to 4 % for CoBi catalysts due to the static Bi-doping, compared with 16 % for Co-supported catalysts. Secondly, to enhance catalytic stability, we introduce a dynamic trace CO2 co-feeding route. 10CoBi/Al2O3 catalysts exhibit superior durability against coke formation for 330 hours in PDH under a 40 % C3H8 atmosphere followed by pure C3H8 conditions at 600 °C while maintaining propylene selectivity at 96 %. Notably, introducing trace CO2 leads to a remarkable 6-fold decrease in the deactivation rate constant (kd). Multiple characterizations and density functional theory calculations reveal that charge transfer from atomically-distributed Bi to Co nanoparticles benefits lowering the energy of C3H6 adsorption thereby suppressing by-products. Furthermore, the dynamic co-feeding of trace CO2 facilitates coke removal, suppressing catalyst deactivation. The static Bi-doping and dynamic trace CO2 co-feeding strategy contributes simultaneously to increased selectivity and stability on supported PDH catalysts. © 2024 Wiley-VCH GmbH.

Keyword:

Catalysis Catalyst selectivity Cobalt Cobalt compounds Coke Dehydrogenation Rate constants Semiconductor doping Sol-gel process Sol-gels Zinc alloys

Community:

  • [ 1 ] [Yao, Yongbin]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing; 100044, China
  • [ 2 ] [Yao, Yongbin]Tangshan Research Institute of Beijing Jiaotong University, Beijing, Tangshan City, Hebei; 100044, China
  • [ 3 ] [Wang, Jingnan]Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
  • [ 4 ] [Liu, Qiang]School of Chemical Engineering and Technology, Tianjin University, Tianjin; 300072, China
  • [ 5 ] [Yu, Can]Institute of High Energy Physics, Chinese Academy of Sciences (CAS), Beijing; 100049, China
  • [ 6 ] [Gao, Zhan]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing; 100044, China
  • [ 7 ] [Yuan, Fangli]State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing; 100190, China
  • [ 8 ] [Wang, Xi]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing; 100044, China
  • [ 9 ] [Wang, Xi]Tangshan Research Institute of Beijing Jiaotong University, Beijing, Tangshan City, Hebei; 100044, China

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2025

Issue: 3

Volume: 64

1 6 . 1 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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