期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 9, 期 14, 页码 3753-3762出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy00927b
关键词
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资金
- National Natural Science Foundation of China (NSFC) [21878162, 21603107]
- Natural Science Foundation of Tianjin of China (NSFT) [16YFZCGX00020]
- Foundation from the Ministry of Education of China (MOE) [IRT-13R30, 113016A]
- Research Fund for the 111 Project [B12015]
- Fundamental Research Funds for the Central Universities
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.
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