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Citation: Wu Jiequn, Hua Weiming, Yue Yinghong, Gao Zi. Swelling Characteristics of g-C3N4 as Base Catalyst in Liquid-Phase Reaction[J]. Acta Physico-Chimica Sinica, ;2020, 36(1): 190406. doi: 10.3866/PKU.WHXB201904066 shu

Swelling Characteristics of g-C3N4 as Base Catalyst in Liquid-Phase Reaction

  • Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, P. R. China

  • Corresponding author: Yue Yinghong, yhyue@fudan.edu.cn
  • Received Date: 17 April 2019
    Revised Date: 5 May 2019
    Accepted Date: 22 May 2019
    Available Online: 24 January 2019

    Fund Project: the National Natural Science Foundation of China 21273043the Science & Technology Commission of Shanghai Municipality, China 13DZ2275200the National Natural Science Foundation of China 91645201the National Key R&D Program of China 2017YFB0602204The project was supported by the National Natural Science Foundation of China (91645201, 21273043), the National Key R&D Program of China (2017YFB0602204), and the Science & Technology Commission of Shanghai Municipality, China (13DZ2275200)

  • Graphitic carbon nitrides (g-C3N4) with different surface areas were prepared by pyrolysis using different precursors including melamine, dicyandiamide, thiourea and urea, and subsequently characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectra (FTIR), X-ray photoelectron spectroscopy (XPS), thermal gravimetric analysis (TGA) and N2 adsorption. Their basicities were measured by temperature-programmed desorption of CO2 (CO2-TPD) and acid-base titration. The catalytic properties for the Knoevenagel condensation of benzaldehyde and malononitrile were investigated in various solvents. In non-polar toluene solution, the benzaldehyde conversions of the g-C3N4 catalysts were low and changed according to their respective surface areas and basicities. However, in polar ethanol solution, the benzaldehyde conversions of all catalysts were similar, and much higher than those in toluene. This could not be explained by the results obtained from either of the two conventional basicity measurements. Further experimental results proved that g-C3N4 catalysts swelled in polar solutions, and more basic sites were exposed on the surface of the swollen catalysts, leading to the imminent increase in catalytic activity. This was proved by the catalyst poisoning data, which showed that the g-C3N4 catalyst lost its activity completely in toluene by adding 40.9 mmol·g-1 benzoic acid, while the same catalyst was still active in ethanol until the added amount exceeded 143.3 m·g-1. Additionally, the reaction tests in various solutions showed that the swelling effect was enhanced according to the polarity of the solvent used. A similar conclusion could be reached for the Knoevenagel condensation of furfural and malononitrile in various solvents. The reusability of g-C3N4 catalyst in Knoevenagel condensation was also studied, which showed that g-C3N4 was stable in liquid-phase reactions, whose activity dropped from 74.2% to 63.8% after three regeneration processes.
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