Graphitic carbon nitrides have appeared as a new type of photocatalyst for water splitting, but their broader and more practical applications are oftentimes hindered by the insolubility or difficult dispersion of the material in solvents. We herein prepared novel two-dimensional (2D) carbon nitride-type polymers doped by iron under a mild one-pot method through preorganizing formamide and citric acid precursors into supramolecular structures, which eventually polycondensed into a homogeneous organocatalyst for highly efficient visible light-driven hydrogen evolution with a rate of ∼16.2 mmol g(-1) h(-1) and a quantum efficiency of 0.8%. Laser photolysis and electrochemical impedance spectroscopic measurements suggested that iron-doping enabled strong electron coupling between the metal and the carbon nitride and formed unique electronic structures favoring electron mobilization along the 2D nanomaterial plane, which might facilitate the electron transfer process in the photocatalytic system and lead to efficient H2 evolution. In combination with electrochemical measurements, the electron transfer dynamics during water reduction were depicted, and the earth-abundant Fe-based catalyst may open a sustainable strategy for conversion of sunlight into hydrogen energy and cope with current challenging energy issues worldwide.

Direct solvent exfoliation of bulk MoS2 with the assistance of poly(3-hexylthiophene) (P3HT) produces a novel two-dimensional organic/inorganic semiconductor hetero-junction. The obtained P3HT-MoS2 nanohybrid exhibits unexpected optical limiting properties in contrast to the saturated absorption behavior of both P3HT and MoS2, showing potential in future photoelectric applications.

New all-inorganic perovskites like Cs4PbBr6 provide rich luminescent tools and particularly novel physical insights, including their zero-dimensional structure and controversial emitting mechanism. The ensuing debate over the origin of the luminescence of Cs4PbBr6 inspired us to tackle the issue through fabricating high-quality Cs4PbBr6 single crystals and employing ultrafast dynamics study. Upon photoexcitation, Cs4PbBr6 underwent dynamics steps distinct from that of CsPbBr3, including exciton migration to the defect level on a time scale of several hundred femtoseconds, exciton relaxation within the defect states on the picosecond time scale, and exciton recombination from the subnanosecond to nanosecond time scale. The observation disclosed that crystal defects of Cs4PbBr6 induced green emission while CsPbBr3 mainly relied on quantum confinement to emit at room temperature. The study provides an in-depth understanding of the photoinduced multistep dynamics steps of Cs4PbBr6 associated with display and photovoltaic applications, establishing Cs4PbBr6 as a new candidate for uses associated with the perovskite family of materials.

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