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author:

Yao, Y. (Yao, Y..) [1] | Wang, J. (Wang, J..) [2] | Liu, Q. (Liu, Q..) [3] | Yu, C. (Yu, C..) [4] | Gao, Z. (Gao, Z..) [5] | Yuan, F. (Yuan, F..) [6] | Wang, X. (Wang, X..) [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:

Cobalt Dynamic trace CO2 co-feeding Heterogeneous catalysis Propane dehydrogenation Static Bi-doping

Community:

  • [ 1 ] [Yao Y.]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing, 100044, China
  • [ 2 ] [Yao Y.]Tangshan Research Institute of Beijing Jiaotong University, Beijing, Tangshan City, Hebei, 100044, China
  • [ 3 ] [Wang J.]Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 4 ] [Liu Q.]School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China
  • [ 5 ] [Yu C.]Institute of High Energy Physics, Chinese Academy of Sciences (CAS), Beijing, 100049, China
  • [ 6 ] [Gao Z.]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing, 100044, China
  • [ 7 ] [Yuan F.]State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
  • [ 8 ] [Wang X.]Department of Physics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing, 100044, China
  • [ 9 ] [Wang X.]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: 2024

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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