A Facile and Green Combined Strategy for Improving Photocatalytic Activity of Carbon Nitride

[Image: see text] We first report an efficient combined strategy that simultaneously integrates copolymerization, doping, and molecular self-assembly for the development of carbon-doping petal-like carbon nitride photocatalysts using melamine (MA), cyanuric acid (CA), and 2,4,6-triaminopyrimidine (TAP) as the starting precursors and water as the only green solvent. The morphology, textural, optical, and electronic properties of carbon nitride could be engineered by rationally manipulating the doping content of TAP. In the process of molecular self-assembly, TAP can insert the aggregate edge easily according to the results of density functional theory (DFT) calculations. The edge-termination effect of TAP made it easier for the modified carbon nitride materials to form petal-like nanosheets with porous structures and large BET surface areas. In addition, the incorporation of TAP also contributed to tuning the electronic band structures of carbon nitrides and enhancing the separation efficiency of photogenerated carriers. The as-prepared materials exhibited excellent photocatalytic activities in the degradation of tetracycline hydrochloride (TC-HCl) and rhodamine B (RhB). This work may not only offer universally powerful and stable photocatalysts for applications but also develop a new combined strategy to fabricate efficient photocatalysts in a facile and green way.