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Issue 14, 2019
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Constructing a fragmentary g-C3N4 framework with rich nitrogen defects as a highly efficient metal-free catalyst for acetylene hydrochlorination

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Abstract

Graphitic carbon nitride (denoted as “g-C3N4”), as a graphite-like CN material, is widely used in catalysis. In this paper, a fragmentary g-C3N4 framework with a porous structure and rich nitrogen defects was synthesized for acetylene hydrochlorination, using melamine formaldehyde (MF) resin as an oxygen-containing precursor. The fragmentary g-C3N4 shows a highly efficient activity with acetylene conversion reaching 94.5%, which is 30 times higher than that of pure g-C3N4 prepared by direct pyrolysis of melamine. Both experimental and characterization studies by XRD, XPS and TG-MS reveal that the high activity of the catalyst is mainly derived from the porous structure and rich nitrogen defects, which are attributed to the etching of the g-C3N4 framework by oxygen species in the MF resin. Moreover, density functional theory (DFT) calculations demonstrated that the nitrogen defects in the g-C3N4 framework greatly improved the adsorption of HCl and acetylene, and at the same time significantly reduced the energy barrier from 62.0 to 38.1 kcal mol−1 at the rate-determining step.

Graphical abstract: Constructing a fragmentary g-C3N4 framework with rich nitrogen defects as a highly efficient metal-free catalyst for acetylene hydrochlorination

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Publication details

The article was received on 14 May 2019, accepted on 16 Jun 2019 and first published on 17 Jun 2019


Article type: Paper
DOI: 10.1039/C9CY00927B
Catal. Sci. Technol., 2019,9, 3753-3762

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    Constructing a fragmentary g-C3N4 framework with rich nitrogen defects as a highly efficient metal-free catalyst for acetylene hydrochlorination

    X. Qiao, Z. Zhou, X. Liu, C. Zhao, Q. Guan and W. Li, Catal. Sci. Technol., 2019, 9, 3753
    DOI: 10.1039/C9CY00927B

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