Self-assembled carbon nitride for photocatalytic hydrogen evolution and degradation of p-nitrophenol

•A multifunctional carbon nitride was synthesized via a “template-free” method.•In-situ heating measurements reveal the growth mechanism of carbon nitride.•The as-prepared catalyst shows superior activity than the bulk in H2 evolution.•Core-shell like carbon nitride is also efficient in the p-NP photo-degradation.

Carbon nitride has attracted significant interest as robust, low-cost alternative to metal-based materials in fields such as photo, electro and heterogeneous catalysis. However, the properties of the final material are hard to control by traditional synthetic methods Herein, we introduce a new strategy of material design that allows controlling the desired properties of the final material already from the molecular level by sequential solvent treatment of supramolecular aggregates that serve as the reactants. Due to in situ formation of a thermodynamic driven energy levels gradient, the as-prepared carbon nitride exhibits almost 10 times higher activity than the traditional carbon nitride (calcined from melamine) in the hydrogen evolution text. As a multifunctional catalyst, the core-shell like carbon nitride also shows a superior catalytic degradation activity for RhB and p-nitrophenol.

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