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author:

Xiao, Z. (Xiao, Z..) [1] | Wan, Z. (Wan, Z..) [2] | Zhang, J. (Zhang, J..) [3] | Jiang, J. (Jiang, J..) [4] | Li, D. (Li, D..) [5] | Shen, J. (Shen, J..) [6] | Dai, W. (Dai, W..) [7] | Li, Y. (Li, Y..) [8] | Wang, X. (Wang, X..) [9] | Zhang, Z. (Zhang, Z..) [10]

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Scopus

Abstract:

Photocatalytic methane conversion into liquid oxygenates using O2 oxidants provides a promising approach for high-value chemicals. The generation of reactive oxygen species and their reaction pathway are key to determine the oxygenate selectivity. Here, an interstitial Zni defect ZnO (ZnO(Zni)) is developed through thermal decomposition of the ZnO2 precursor. Zni favors the O2 adsorption at a terminal adsorption configuration and induces effectively the conversion O2 into the desired •OOH instead of •OH for improving the yield and selectivity of oxygenates. For comparison, O2 adsorbed in a lateral configuration tends to be converted into excessive •OH on the typical Au/ZnO. As a result, ZnO(Zni) shows the liquid oxygenates yield of 6080 μmol g-1 with 98.6% selectivity, which leads to 10 times lower than Au/ZnO for CO2 release of overoxidation. This work provides a pathway for O2 adsorption and activation to regulate the photocatalytic CH4 oxidation conversion into liquid oxygenates. © 2024 American Chemical Society.

Keyword:

defects interstitial zinc methane conversion oxygen activation selectivity

Community:

  • [ 1 ] [Xiao Z.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 2 ] [Xiao Z.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 3 ] [Wan Z.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 4 ] [Wan Z.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 5 ] [Zhang J.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 6 ] [Zhang J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 7 ] [Jiang J.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 8 ] [Jiang J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 9 ] [Li D.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 10 ] [Li D.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 11 ] [Shen J.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 12 ] [Shen J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 13 ] [Dai W.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 14 ] [Dai W.]Qingyuan Innovation Laboratory, Quanzhou, 362801, China
  • [ 15 ] [Dai W.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 16 ] [Li Y.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 17 ] [Wang X.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 18 ] [Wang X.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 19 ] [Zhang Z.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 20 ] [Zhang Z.]Qingyuan Innovation Laboratory, Quanzhou, 362801, China
  • [ 21 ] [Zhang Z.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Source :

ACS Catalysis

ISSN: 2155-5435

Year: 2024

Issue: 12

Volume: 14

Page: 9104-9114

1 1 . 7 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: 1

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