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author:

Zhou, Yanliang (Zhou, Yanliang.) [1] | Wei, Fenfei (Wei, Fenfei.) [2] | Qi, Haifeng (Qi, Haifeng.) [3] | Chai, Yicong (Chai, Yicong.) [4] | Cao, Liru (Cao, Liru.) [5] | Lin, Jian (Lin, Jian.) [6] | Wan, Qiang (Wan, Qiang.) [7] | Liu, Xiaoyan (Liu, Xiaoyan.) [8] | Xing, Yanan (Xing, Yanan.) [9] | Lin, Sen (Lin, Sen.) [10] | Wang, Aiqin (Wang, Aiqin.) [11] | Wang, Xiaodong (Wang, Xiaodong.) [12] | Zhang, Tao (Zhang, Tao.) [13]

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EI

Abstract:

Single-atom catalysts with uniform metal active sites show potential for selectivity control. However, their application to high-temperature propane dehydrogenation remains challenging. Here we develop a highly stable and efficient single-atom catalyst for propane dehydrogenation that is based on Ru single atoms on nitrogen-doped carbon (Ru1/NC). The turnover frequency of Ru1/NC is at least three times higher than that of nanoparticle counterparts, resulting in propylene selectivity of around 92% with a lower deactivation rate at 560 °C. Experimental and density functional theory studies reveal the important role of peripheral N species around the Ru1 centre. The inner-shell N stabilizes the atomically dispersed Ru to inhibit structure-sensitive propane cracking, while the outer-shell N promotes electron accumulation at the Ru1 centre, inducing a significant charge repulsion between Ru1 and propylene to facilitate its desorption. The combined functions of inner-shell and outer-shell N species at single-atom Ru sites contribute to the high efficiency of Ru1/NC. [Figure not available: see fulltext.] © 2022, The Author(s), under exclusive licence to Springer Nature Limited.

Keyword:

Atoms Catalyst activity Catalyst selectivity Dehydrogenation Density functional theory Doping (additives) Nitrogen Propane Propylene Shells (structures)

Community:

  • [ 1 ] [Zhou, Yanliang]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 2 ] [Wei, Fenfei]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 3 ] [Qi, Haifeng]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 4 ] [Chai, Yicong]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 5 ] [Chai, Yicong]University of Chinese Academy of Sciences, Beijing, China
  • [ 6 ] [Cao, Liru]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 7 ] [Cao, Liru]University of Chinese Academy of Sciences, Beijing, China
  • [ 8 ] [Lin, Jian]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 9 ] [Wan, Qiang]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 10 ] [Liu, Xiaoyan]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 11 ] [Xing, Yanan]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 12 ] [Xing, Yanan]University of Chinese Academy of Sciences, Beijing, China
  • [ 13 ] [Lin, Sen]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, China
  • [ 14 ] [Wang, Aiqin]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 15 ] [Wang, Xiaodong]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
  • [ 16 ] [Zhang, Tao]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China

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Source :

Nature Catalysis

Year: 2022

Issue: 12

Volume: 5

Page: 1145-1156

3 7 . 8

JCR@2022

4 2 . 9 0 0

JCR@2023

ESI HC Threshold:74

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 108

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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