Oxygen-doped nanoporous carbon nitride via water-based homogeneous supramolecular assembly for photocatalytic hydrogen evolution

• Published in: Applied catalysis. B, Environmental Vol. 221; pp. 9 - 16
• Main Authors: Zhang, Jing-Wen, Gong, Si, Mahmood, Nasir, Pan, Lun, Zhang, Xiangwen, Zou, Ji-Jun
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier B.V 01-02-2018; Elsevier BV
• Subjects: Assembly; Carbon nitride; Catalysts; Cyanuric acid; Electromagnetic absorption; Hydrogen; Hydrogen bonds; Hydrogen evolution; Hydrothermal treatment; Irradiation; Light irradiation; Mathematical morphology; Melamine; Oxygen; Oxygen-doping; Photocatalysis; Quantum efficiency; Radiation; Separation; Supramolecular assembly; Surface area; Surface charge; Wettability; Oxygen-doping; Supramolecular assembly; Photocatalysis; Hydrogen evolution; Carbon nitride
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2017.09.003

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•O-doped porous C3N4via water-based homogeneous supramolecular assembly.•g-C3N4 possess high surface area and well-defined 3D morphology.•Oxygen atom doping in the lattice of g-C3N4 enhance its electronic properties.•It Exhibits 11.3 times higher H2 evolution rate than bulk g-C3N4 under visible light.
Graphitic carbon nitride (g-C3N4) has emerged as a promising photocatalyst, but poor charge separation and low surface area limit its activity. Here, we report a hydrothermal method to generate hydrogen bonded supramolecular complex via water-based homogeneous supramolecular assembly, which is a promising precursor to fabricate porous and oxygen-doped g-C3N4. The hydrothermal treatment provides a homogeneous environment for hydrolysis of melamine to produce cyanuric acid and reaction of cyanuric acid with remained melamine to create the in-plane ordering and hydrogen bonded supramolecular complex. The complex can template uniform nanoporous structure and also provide an opportunity for O-doping in the g-C3N4 network upon calcination in air. The resulted g-C3N4(GCN-4) possesses high surface area, well-defined 3D morphology and oxygen-dopant in the lattice. Subsequently, the visible light absorption, charge separation, and wettability are considerably enhanced. This catalyst exhibits higher hydrogen evolution rate by 11.3 times than the bulk g-C3N4 under visible light irradiation, with apparent quantum efficiency of 10.3% at 420nm.