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author:

Zhang, Jiangjie (Zhang, Jiangjie.) [1] | Shen, Jinni (Shen, Jinni.) [2] (Scholars:沈锦妮) | Li, Dongmiao (Li, Dongmiao.) [3] | Long, Jinlin (Long, Jinlin.) [4] (Scholars:龙金林) | Gao, Xiaochen (Gao, Xiaochen.) [5] | Feng, Wenhui (Feng, Wenhui.) [6] | Zhang, Shiying (Zhang, Shiying.) [7] | Zhang, Zizhong (Zhang, Zizhong.) [8] (Scholars:张子重) | Wang, Xuxu (Wang, Xuxu.) [9] (Scholars:王绪绪) | Yang, Weimin (Yang, Weimin.) [10]

Indexed by:

EI Scopus SCIE

Abstract:

Metal-decorated oxide semiconductors are overwhelming photocatalysts for nonoxidative coupling of methane (NOCM). However, the overall NOCM mechanism remains an unopened black box, which hinders the design of high-performance catalysts. Herein, we systematically studied a series of noble metal (Ag, Au, Pt, Pd, Cu, and Ni)-decorated oxides (NaTaO3, CaTiO3, LiNbO3, and TiO2) for NOCM. We proposed that the active sites for H abstraction and C-C coupling of CH4 are spatially separated. Specifically, NaTaO3 only completes the initial H abstraction of CH4 activation, while metal nanoparticles are responsible for the final C-C coupling. Noble metals dominate NOCM by significantly decreasing the energy barrier of CH4 dissociation and promoting C-C coupling. Among various metals, Ag is preferential for the weak adsorption of center dot CH3 intermediates and subsequent metal-induced CC coupling. This contributes to Ag/NaTaO3 the highest C2H(6) yield of 194 mu mol g-1 h(-1) and stoichiometric H-2 with 11.2% quantum efficiency. This work provides a molecular-level insight into the CH4 coupling mechanism on metal-decorated photocatalysts.

Keyword:

C C coupling H activation mechanism methane photocatalytic

Community:

  • [ 1 ] [Zhang, Jiangjie]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 2 ] [Shen, Jinni]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 3 ] [Li, Dongmiao]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 4 ] [Long, Jinlin]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 5 ] [Zhang, Zizhong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 6 ] [Wang, Xuxu]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China
  • [ 7 ] [Gao, Xiaochen]SINOPEC Shanghai Res Inst Petrochem Technol, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 201208, Peoples R China
  • [ 8 ] [Yang, Weimin]SINOPEC Shanghai Res Inst Petrochem Technol, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 201208, Peoples R China
  • [ 9 ] [Feng, Wenhui]Changsha Univ, Hunan Prov Key Lab Appl Environm Photocatalysis, Changsha 410022, Peoples R China
  • [ 10 ] [Zhang, Shiying]Changsha Univ, Hunan Prov Key Lab Appl Environm Photocatalysis, Changsha 410022, Peoples R China
  • [ 11 ] [Zhang, Zizhong]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China

Reprint 's Address:

  • [Zhang, Zizhong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350106, Peoples R China;;[Zhang, Zizhong]Qingyuan Innovat Lab, Quanzhou 362801, Peoples R China;;

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Source :

ACS CATALYSIS

ISSN: 2155-5435

Year: 2023

Issue: 3

Volume: 13

Page: 2094-2105

1 1 . 7

JCR@2023

1 1 . 7 0 0

JCR@2023

ESI Discipline: CHEMISTRY;

ESI HC Threshold:39

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 25

SCOPUS Cited Count: 16

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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