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author:

Shi, Y. (Shi, Y..) [1] | Li, P. (Li, P..) [2] | Chen, H. (Chen, H..) [3] | Wang, Z. (Wang, Z..) [4] | Song, Y. (Song, Y..) [5] | Tang, Y. (Tang, Y..) [6] | Lin, S. (Lin, S..) [7] | Yu, Z. (Yu, Z..) [8] | Wu, L. (Wu, L..) [9] | Yu, J.C. (Yu, J.C..) [10] | Fu, X. (Fu, X..) [11]

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Abstract:

Adsorption and activation of C–H bonds by photocatalysts are crucial for the efficient conversion of C–H bonds to produce high-value chemicals. Nevertheless, the delivery of surface-active oxygen species for C–H bond oxygenation inevitably needs to overcome obstacles due to the separated active centers, which suppresses the catalytic efficiency. Herein, Ni dopants are introduced into a monolayer Bi2WO6 to create cascaded active units consisting of unsaturated W atoms and Bi/O frustrated Lewis pairs. Experimental characterizations and density functional theory calculations reveal that these special sites can establish an efficient and controllable C–H bond oxidation process. The activated oxygen species on unsaturated W are readily transferred to the Bi/O sites for C–H bond oxygenation. The catalyst with a Ni mass fraction of 1.8% exhibits excellent toluene conversion rates and high selectivity towards benzaldehyde. This study presents a fascinating strategy for toluene oxidation through the design of efficient cascaded active units. © The Author(s) 2024.

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  • [ 1 ] [Shi Y.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 2 ] [Shi Y.]School of Chemistry and Chemical Engineering, Hainan University, Hainan, Haikou, 570228, China
  • [ 3 ] [Li P.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 4 ] [Chen H.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 5 ] [Wang Z.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 6 ] [Wang Z.]School of Chemistry and Chemical Engineering, Hainan University, Hainan, Haikou, 570228, China
  • [ 7 ] [Song Y.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 8 ] [Song Y.]School of Chemistry and Chemical Engineering, Hainan University, Hainan, Haikou, 570228, China
  • [ 9 ] [Tang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 10 ] [Lin S.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 11 ] [Yu Z.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 12 ] [Wu L.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 13 ] [Yu J.C.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China
  • [ 14 ] [Yu J.C.]Department of Chemistry, The Chinese University of Hong Kong, Hong Kong
  • [ 15 ] [Fu X.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fujian, Fuzhou, 350116, China

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Source :

Nature Communications

ISSN: 2041-1723

Year: 2024

Issue: 1

Volume: 15

1 4 . 7 0 0

JCR@2023

CAS Journal Grade:1

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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