Promoting effect of cyano groups attached on g-C3N4 nanosheets towards molecular oxygen activation for visible light-driven aerobic coupling of amines to imines

Di Zhang, Xinghua Han, Ting Dong, Xinwen Guo, Chunshan Song, Zhongkui Zhao

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Molecular oxygen activation shows a great potential for a wide range of applications in organic transformations, but remains a challenge owing to the high inertness from its high energy electrons. In this work, we firstly report the dramatically promoting effect of cyano groups on visible light-driven molecular oxygen activation over cyano-decorated g-C3N4 nanosheets (DCNNS) fabricated by a facile and green thermal post-treatment approach from g-C3N4 nanosheets (CNNS). Experimental studies and theoretical calculation reveal that the homojunction-like structure is constructed in DCNNS owing to the introduction of cyano-groups, which can facilitate the generation of hot carriers, and thus promotes the O2 [rad]− production. The optimized DCNNS exhibits 2.4 times higher activity than pristine CNNS for the visible light-driven oxidative coupling of benzylamine to imine, an industrially important transformation as a probe reaction. The discovered cyano groups-promoting visible light-driven molecular oxygen activation strategy has been extended to coupling of various amines to their corresponding imines. The present work could open a new horizon for designing highly efficient g-C3N4-based catalysts for diverse organic transformations via molecular oxygen activation.

Original languageEnglish (US)
Pages (from-to)237-244
Number of pages8
JournalJournal of Catalysis
Volume366
DOIs
StatePublished - Oct 1 2018

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Imines
Molecular oxygen
Nanosheets
imines
Amines
amines
Chemical activation
activation
oxygen
homojunctions
Hot carriers
high energy electrons
horizon
catalysts
probes
Catalysts
Electrons

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

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title = "Promoting effect of cyano groups attached on g-C3N4 nanosheets towards molecular oxygen activation for visible light-driven aerobic coupling of amines to imines",
abstract = "Molecular oxygen activation shows a great potential for a wide range of applications in organic transformations, but remains a challenge owing to the high inertness from its high energy electrons. In this work, we firstly report the dramatically promoting effect of cyano groups on visible light-driven molecular oxygen activation over cyano-decorated g-C3N4 nanosheets (DCNNS) fabricated by a facile and green thermal post-treatment approach from g-C3N4 nanosheets (CNNS). Experimental studies and theoretical calculation reveal that the homojunction-like structure is constructed in DCNNS owing to the introduction of cyano-groups, which can facilitate the generation of hot carriers, and thus promotes the O2 [rad]− production. The optimized DCNNS exhibits 2.4 times higher activity than pristine CNNS for the visible light-driven oxidative coupling of benzylamine to imine, an industrially important transformation as a probe reaction. The discovered cyano groups-promoting visible light-driven molecular oxygen activation strategy has been extended to coupling of various amines to their corresponding imines. The present work could open a new horizon for designing highly efficient g-C3N4-based catalysts for diverse organic transformations via molecular oxygen activation.",
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Promoting effect of cyano groups attached on g-C3N4 nanosheets towards molecular oxygen activation for visible light-driven aerobic coupling of amines to imines. / Zhang, Di; Han, Xinghua; Dong, Ting; Guo, Xinwen; Song, Chunshan; Zhao, Zhongkui.

In: Journal of Catalysis, Vol. 366, 01.10.2018, p. 237-244.

Research output: Contribution to journalArticle

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AU - Song, Chunshan

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