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author:

Chai, Yicong (Chai, Yicong.) [1] | Chen, Shunhua (Chen, Shunhua.) [2] | Chen, Yang (Chen, Yang.) [3] | Wei, Fenfei (Wei, Fenfei.) [4] | Cao, Liru (Cao, Liru.) [5] | Lin, Jian (Lin, Jian.) [6] | Li, Lin (Li, Lin.) [7] | Liu, Xiaoyan (Liu, Xiaoyan.) [8] | Lin, Sen (Lin, Sen.) [9] (Scholars:林森) | Wang, Xiaodong (Wang, Xiaodong.) [10] | Zhang, Tao (Zhang, Tao.) [11]

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SCIE

Abstract:

Dual-atom catalysts (DACs) with paired active sites can provide unique intrinsic properties for heterogeneous catalysis, but the synergy of the active centers remains to be elucidated. Here, we develop a high-performance DAC with Zn1Co1 species anchored on nitrogen-doped carbon (Zn1Co1/NC) as the dominant active site for the propane dehydrogenation (PDH) reaction. It exhibits several times higher turnover frequency (TOF) of C3H8 conversion and enhanced C3H6 selectivity compared to Zn-1/NC or Co-1/NC with only a single-atom site. Various experimental and theoretical studies suggest that the enhanced PDH performance stems from the promoted activation of the C-H bond of C3H8 triggered by the electronic interaction between Zn-1 and Co-1 colligated by N species. Moreover, the dynamic sinking of the Zn-1 site and rising of the Co-1 site, together with the steric effect of the dissociated H species at the bridged N during the PDH reaction, provides a feasible channel for C3H6 desorption through the more exposed Co-1 site, thereby boosting the selectivity. This work provides a promising strategy for designing robust hetero DACs to simultaneously increase activity and selectivity in the PDH reaction.

Keyword:

Community:

  • [ 1 ] [Chai, Yicong]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 2 ] [Chen, Yang]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 3 ] [Cao, Liru]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 4 ] [Lin, Jian]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 5 ] [Li, Lin]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 6 ] [Liu, Xiaoyan]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 7 ] [Wang, Xiaodong]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 8 ] [Zhang, Tao]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
  • [ 9 ] [Chai, Yicong]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 10 ] [Cao, Liru]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 11 ] [Chen, Shunhua]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 12 ] [Wei, Fenfei]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 13 ] [Lin, Sen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China

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Source :

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

ISSN: 0002-7863

Year: 2023

Issue: 1

Volume: 146

Page: 263-273

1 4 . 5

JCR@2023

1 4 . 5 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 67

SCOPUS Cited Count: 71

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

Online/Total:112/10275087
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