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Synthesis of Three-Dimensional Mesostructured Graphitic Carbon Nitride Materials and their Application as Heterogeneous Catalysts for Knoevenagel Condensation Reactions

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Abstract

Three-dimensional (3D) mesostructured graphitic carbon nitride materials with tunable surface areas (394–498 m2 g−1) and pore volumes (0.54–1.36 cm3 g−1) were synthesized through a nanocasting method. Mesocellular silica foam (MCF) was used as a template, and carbon tetrachloride (CTC) and ethylenediamine (EDA) were used as precursors. The effect of the ratio of the two precursors (EDA/CTC) on the textural properties and chemical compositions of the CN-MCF samples were investigated by several characterization techniques. The results revealed that the 3D mesostructures were maintained when the ratio of EDA/CTC was greater than 0.4. Among the different CN-MCF materials prepared, CN-MCF-0.4 demonstrated the highest catalytic performance for Knoevenagel condensation reactions, mainly because of its high amount of surface N, high surface area, and large pore volume. In addition, the CN-MCF-0.4 catalyst showed good stability as well as versatility for various substrates.

Graphical Abstract

Mesostructured graphitic carbon nitride materials have been synthesized using MCF as template and the effects of the ratios of the N & C precursors on their physicochemical properties have been comparatively investigated; the materials demonstrate effective and versatile catalytic performance for a series of Knoevenagel condensation reactions.

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Acknowledgments

This work was supported by National Natural Science Foundation of China (21203014), CNPC Innovation Foundation (2011D-5006-0508), Open Foundation of Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials attached to Fudan University (2011MCIMKF01), Open Foundation of Jiangsu Key Laboratory of Fine Petrochemical Engineering attached to Changzhou University (KF1201), and the project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions. Jie Xu also thanks Mrs. Li-Juan Zhang and Prof. Wei-Lin Dai, Fudan University for their kind help with SAXS and XPS characterization.

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Authors and Affiliations

  1. Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, College of Chemistry and Chemical Engineering, Changzhou University, Gehu Road 1, Changzhou, 213164, Jiangsu, People’s Republic of China

    Jie Xu, Kang Shen, Bing Xue & Yong-Xin Li

  2. Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200433, People’s Republic of China

    Yong Cao

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  1. Jie Xu
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  2. Kang Shen
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  3. Bing Xue
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  4. Yong-Xin Li
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Correspondence to Jie Xu or Yong-Xin Li.

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Xu, J., Shen, K., Xue, B. et al. Synthesis of Three-Dimensional Mesostructured Graphitic Carbon Nitride Materials and their Application as Heterogeneous Catalysts for Knoevenagel Condensation Reactions. Catal Lett 143, 600–609 (2013). https://doi.org/10.1007/s10562-013-0994-6

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  • DOI: https://doi.org/10.1007/s10562-013-0994-6

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