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Utilizing polymeric carbon nitride (CN) materials for photocatalysis is an evolving field, where variations in the synthesis process can continuously enhance activity by addressing the inherent limitations of these materials (light absorption, specific surface area, charge transfer, etc.). Among possible photocatalytic reactions, the most popular application of CNs is the hydrogen evolution reaction (HER).
Based on this, Menny Shalom (corresponding author) and colleagues from Ben-Gurion University of the Negev in Israel reported a precisely controlled carbon-doped porous CN rod with extended π-electron conjugation, composed of supramolecularly assembled melamine (melem) and co-monomers that partially replace carbon atoms on the melamine pyridine ring.
The dense hydrogen bonds and good thermal stability of the melamine-based supramolecular framework allow for the synthesis of more ordered structures to improve charge transfer; controlling the carbon substitution at nitrogen sites on a molecular level adjusts the band alignment and photogenerated charge separation. The optimal photocatalyst exhibits excellent HER rates (up to 10.16 mmol·h-1·g-1 under 100 W white LED illumination, with an apparent quantum efficiency of 20.0% at 405 nm, which is 23.2 times that of bulk CN reference).
The photocatalytic HER performance surpasses that of most CN materials synthesized through various methods with different morphologies. By simply adjusting the reaction atmosphere and time, selective control over the oxidation of aromatic alcohols to aromatic aldehyde or aromatic acid products can be achieved. The outstanding photocatalytic properties stem from:
(1) The unique porous structure, providing abundant active sites and facilitating light collection;
(2) The repetition of quinazoline units in the structure, allowing for rapid charge transfer;
(3) The substitution of some N for C in the quinazoline core (using co-monomers on the pyridine ring), increasing the carbon content of the resulting CN and leading to tail absorption and better charge separation efficiency.
This work exemplifies how the design of structural motifs in supramolecular assembly strategies can significantly enhance photocatalytic activity due to an understanding of the structure-function relationship.
Aromatic alcohols oxidation and hydrogen evolution over π-electron conjugated porous carbon nitride rods. Nano Research, 2022, DOI: 10.1007/s12274-022-4717-4.
https://doi.org/10.1007/s12274-022-4717-4.
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