Graphitic carbon nitride (g-C3N4)-supported V2O5 catalysts were prepared by the impregnation pyrolysis method, and their physicochemical properties were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), Raman, X-ray photoelectron spectroscopy (XPS), UV–vis, TGA, N2 adsorption, and H2-TPR. These catalysts exhibit extremely high activity and selectivity in the aerobic oxidation of ethyl lactate to ethyl pyruvate. The excellent catalytic performance derives from the high surface-chemisorbed oxygen species. Low calcination temperature and interaction with g-C3N4 are conducive to increasing the surface-chemisorbed oxygen species of V2O5. The optimal catalyst 13V2O5/g-C3N4 gives 96.2% conversion of ethyl lactate with 85.6% selectivity toward ethyl pyruvate in 4 h at 130 °C and 1 atm oxygen, which is significantly superior to those of previously reported V-containing catalysts. This catalyst is also stable and reusable, and the ethyl pyruvate yield is reduced by less than 10% after four runs without any regeneration treatment.
A highly efficient bifunctional catalyst of an s-triazine-based carbon-nitride-supported cobalt oxide is developed for the aerobic oxidation–Knoevenagel condensation tandem reaction of benzyl alcohol and malononitrile, whereby 96.4% benzyl alcohol conversion with nearly 100% selectivity towards benzylmalononitrile can be obtained in 6 h at 80 °C. The excellent catalytic performance derives from the high basicity of carbon nitride and strong redox ability of Co species induced by carbon nitride. The catalyst is also quite stable and can be reused without any regeneration treatment, whose product yield is only an 11.5% reduction after four runs.
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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