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author:

Wu, Shuhong (Wu, Shuhong.) [1] | Li, Chao (Li, Chao.) [2] | Wang, Ying (Wang, Ying.) [3] (Scholars:汪颖) | Zhuang, Yan (Zhuang, Yan.) [4] | Pan, Yi (Pan, Yi.) [5] | Wen, Na (Wen, Na.) [6] (Scholars:温娜) | Wang, Shuo (Wang, Shuo.) [7] | Zhang, Zizhong (Zhang, Zizhong.) [8] (Scholars:张子重) | Ding, Zhenxin (Ding, Zhenxin.) [9] | Yuan, Rusheng (Yuan, Rusheng.) [10] (Scholars:员汝胜) | Dai, Wenxin (Dai, Wenxin.) [11] (Scholars:戴文新) | Fu, Xianzhi (Fu, Xianzhi.) [12] (Scholars:付贤智) | Long, Jinlin (Long, Jinlin.) [13] (Scholars:龙金林)

Indexed by:

EI Scopus SCIE

Abstract:

The keto-switched photocatalysis of covalent organic frameworks (COFs) for efficient H-2 evolution was reported for the first time by engineering, at a molecular level, the local structure and component of the skeletal building blocks. A series of imine-linked BT-COFs were synthesized by the Schiff-base reaction of 1, 3, 5-benzenetrialdehyde with diamines to demonstrate the structural reconstruction of enol to keto configurations by alkaline catalysis. The keto groups of the skeletal building blocks served as active injectors, where hot & pi;-electrons were provided to Pt nanoparticles (NPs) across a polyvinylpyrrolidone (PVP) insulting layer. The characterization results, together with density functional theory calculations, indicated clearly that the formation of keto-injectors not only made the conduction band level more negative, but also led to an inhomogeneous charge distribution in the donor-acceptor molecular building blocks to form a strong intramolecular built-in electric field. As a result, visible-light photocatalysis of TP-COFs-1 with one keto group in the skeletal building blocks was successfully enabled and achieved an impressive H-2 evolution rate as high as 0.96 mmol g(-1) h(-1). Also, the photocatalytic H-2 evolution rates of the reconstructed BT-COFs-2 and -3 with two and three keto-injectors were significantly enhanced by alkaline post-treatment.

Keyword:

Electric Field Enol-Keto Tautomerism H-2 Production MIS Heterostructure Photocatalysis

Community:

  • [ 1 ] [Wu, Shuhong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 2 ] [Li, Chao]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 3 ] [Wang, Ying]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 4 ] [Zhuang, Yan]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 5 ] [Pan, Yi]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 6 ] [Wen, Na]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 7 ] [Wang, Shuo]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 8 ] [Zhang, Zizhong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 9 ] [Ding, Zhenxin]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 10 ] [Yuan, Rusheng]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 11 ] [Dai, Wenxin]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 12 ] [Fu, Xianzhi]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 13 ] [Long, Jinlin]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 14 ] [Wen, Na]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2023

Issue: 36

Volume: 62

1 6 . 1

JCR@2023

1 6 . 1 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: 50

SCOPUS Cited Count: 33

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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