Graphitic carbon nitride (g-C3N4), a polymeric semiconductor, has drawn great attention to solar energy conversion. Here we present our recent works in the electronic structure engineering and structural design of polymeric carbon nitride (PCN) and highly crystalline PCN for photo-involved applications. (1) A supramolecular preassembly method was used to synthesize hierarchical tubular carbon nitrides with oxygen doping and nitrogen defects, which can achieve a highly efficient photocatalytic hydrogen production of 5.29 mmol h-1 g-1 with a high apparent quantum yield of 32.4% at 420 nm. (2) Ru and Cu single atoms are simultaneously incorporated into polymeric carbon nitride (PCN) through a simple preassembly-coprecipitation-pyrolysis process. The Cu single atom acts as the active center for CO2 activation, and the Ru single atom serves as the active center for *CO adsorption and protonation. As a result, the dual-metal single-atom decorated photocatalyst shows a high selectivity of 95% for CH4 production under visible-light irradiation. (3) A highly-crystalline carbon nitride nanorod array was synthesized by molten salt-assisted pyrolysis of rod-like supramolecular precursors from the hydrolysis of melamine. The self-supporting array shows excellent properties of photocatalytic hydrogen evolution and oxidative organic synthesis. On the nanoscale, the highly crystalline PCN rod array has an omasum-like self-supporting architecture. At the molecular level, the triazine-heptazine heterojunction remarkably improves charge carrier transfer and separation. The nanorod array exhibits a high hydrogen production rate (11.72 mmol h-1 gcat-1) with a high apparent quantum yield (AQY) of 60% at 420 nm. In addition, the oxidation of aromatic hydrocarbons to aldehydes or ketones can be obtained under single wavelength (460 nm) irradiation with milligram yields, surpassing other photocatalysts so far.

Graphitic carbon nitride-based polymeric photocatalysts for solar energy conversion

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