Highly-ordered mesoporous carbon nitride with ultrahigh surface area and pore volume as a superior dehydrogenation catalyst

  • Zhao Z
  • Dai Y
  • Lin J
 et al. 
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Abstract

In this work, a highly ordered mesoporous carbon nitride nanorods with 971?1124 m2 g?1 of superhigh specific surface area, 1.31?1.79 cm3 g?1 of ultralarge pore volume, bimodal mesostructure, and 9.3?23 wt % of high N content was prepared via a facile nanocasting approach using SBA-15 as template and hexamethylenetetramine as carbon nitride precursor, and the specific surface area and pore volume as well as N content are strongly dependent on the chosen precursor and pyrolysis temperature. The as-prepared materials were well characterized by HRTEM, FESEM, XRD, BET, Raman, FT-IR, XPS, and the textural structure and morphology were confirmed. The finding breaks through the bottleneck problems for fabricating mesoporous carbon nitride with both ultrahigh surface area and super large pore volume by employing an unexplored hexamethylenetetramine as carbon nitride precursor. The current synthetic strategy can be extended to the preparation of various mesoporous carbon nitride with different textural characteristics by using diverse templates under changeable preparation conditions. The developed mesoporous carbon nitride material with 750 °C of pyrolysis temperature exhibits high superior catalytic performance, ascribed to the promoting effect of nitrogen within the carbon matrix, the rich C═O group and defect/edge feature on the surface, small size of graphitic crystallite, as well as the ultrahigh surface area and pore volume. It can also be concluded that the microstructures including bulk and surface structure features and surface chemical properties of the carbon-based materials have a decisive influence on their catalytic performance. The developed material can be employed in various organic transformations such as the base-catalyzed reactions, selective oxidation, dehydrogenation, photocatalysis, and electrocatalysis as well as acting as a novel and efficient candidate for CO2 capture, supercapacitor, purification of contaminated water, and future drug-delivery systems.
In this work, a highly ordered mesoporous carbon nitride nanorods with 971?1124 m2 g?1 of superhigh specific surface area, 1.31?1.79 cm3 g?1 of ultralarge pore volume, bimodal mesostructure, and 9.3?23 wt % of high N content was prepared via a facile nanocasting approach using SBA-15 as template and hexamethylenetetramine as carbon nitride precursor, and the specific surface area and pore volume as well as N content are strongly dependent on the chosen precursor and pyrolysis temperature. The as-prepared materials were well characterized by HRTEM, FESEM, XRD, BET, Raman, FT-IR, XPS, and the textural structure and morphology were confirmed. The finding breaks through the bottleneck problems for fabricating mesoporous carbon nitride with both ultrahigh surface area and super large pore volume by employing an unexplored hexamethylenetetramine as carbon nitride precursor. The current synthetic strategy can be extended to the preparation of various mesoporous carbon nitride with different textural characteristics by using diverse templates under changeable preparation conditions. The developed mesoporous carbon nitride material with 750 °C of pyrolysis temperature exhibits high superior catalytic performance, ascribed to the promoting effect of nitrogen within the carbon matrix, the rich C═O group and defect/edge feature on the surface, small size of graphitic crystallite, as well as the ultrahigh surface area and pore volume. It can also be concluded that the microstructures including bulk and surface structure features and surface chemical properties of the carbon-based materials have a decisive influence on their catalytic performance. The developed material can be employed in various organic transformations such as the base-catalyzed reactions, selective oxidation, dehydrogenation, photocatalysis, and electrocatalysis as well as acting as a novel and efficient candidate for CO2 capture, supercapacitor, purification of contaminated water, and future drug-delivery systems.

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Authors

  • Zhongkui Zhao

  • Yitao Dai

  • Jinhan Lin

  • Guiru Wang

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