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author:

Liu, Qiang (Liu, Qiang.) [1] | Yao, Yongbin (Yao, Yongbin.) [2] | Li, Junmeng (Li, Junmeng.) [3] | Wang, Jingnan (Wang, Jingnan.) [4] | Chen, Lili (Chen, Lili.) [5] | Li, Wenlin (Li, Wenlin.) [6] | Guo, Yangyang (Guo, Yangyang.) [7] | Yao, Siyu (Yao, Siyu.) [8] | Yang, Yongan (Yang, Yongan.) [9] | Wang, Xi (Wang, Xi.) [10]

Indexed by:

EI Scopus

Abstract:

Cobalt-based catalysts have emerged as promising substitutes for Pt- and Cr-based propane dehydrogenation (PDH) catalysts. However, controlling the distribution of Co species and achieving stable active centers remains challenging. Here, we report that reaction-driven reconstruction of metallic cobalt (Co0) species within pure silica MFI zeolite (S-1) into CoOx clusters within silanol nests during PDH yields efficient and durable performance. Atomically dispersed CoOx clusters exhibit exceptional durability and high propylene space-time yield (STY), maintaining an ultrahigh propylene STY of 17.2 mmolC3H6 gcat−1 h−1 for over 260 h under industrially relevant conditions, surpassing previous cobalt-based PDH catalysts. Moreover, the catalyst operates stably at 520 °C for 170 h with near-equilibrium propane conversions. Comprehensive characterizations indicate the dynamic evolution process from the silanol nests effectively capturing and stabilizing Co0 species within S-1 zeolite, thereby promoting the dynamic formation of CoOx clusters during the PDH process. We also demonstrate that stable Co─O active centers formed by this unique anchoring strategy improve catalyst stability by suppressing coke formation and promoting efficient propane dehydrogenation. © 2025 Wiley-VCH GmbH.

Keyword:

Cobalt Dehydrogenation Propylene

Community:

  • [ 1 ] [Liu, Qiang]School of Chemical Engineering and Technology, Collaborative Innovation Center of Chemical Science and Engineering, Institute of Molecular Plus, Department of Chemistry, Tianjin University, Tianjin; 300072, China
  • [ 2 ] [Yao, Yongbin]Key Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing; 100044, China
  • [ 3 ] [Li, Junmeng]State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing; 102249, China
  • [ 4 ] [Wang, Jingnan]Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou University, Fuzhou; 350108, China
  • [ 5 ] [Chen, Lili]Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing; 100190, China
  • [ 6 ] [Li, Wenlin]College of Chemistry and Chemical Engineering, State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan; 030024, China
  • [ 7 ] [Guo, Yangyang]CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing; 100190, China
  • [ 8 ] [Yao, Siyu]College of Chemical and Biological Engineering, Zhejiang University, Hangzhou; 310027, China
  • [ 9 ] [Yang, Yongan]School of Chemical Engineering and Technology, Collaborative Innovation Center of Chemical Science and Engineering, Institute of Molecular Plus, Department of Chemistry, Tianjin University, Tianjin; 300072, China
  • [ 10 ] [Wang, Xi]State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing; 102249, China

Reprint 's Address:

  • [li, wenlin]college of chemistry and chemical engineering, state key laboratory of clean and efficient coal utilization, taiyuan university of technology, taiyuan; 030024, china

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2025

Issue: 21

Volume: 64

1 6 . 1 0 0

JCR@2023

CAS Journal Grade:1

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: 0

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