Pt nanoparticles embedded spine-like g-C₃N₄ nanostructures with superior photocatalytic activity for H₂ generation...

Conventional two-dimensional (2D) graphitic carbon nitride, 2D g-C₃N₄ with its layered structures and flat and smooth 2D surface possesses certain disadvantages that is affecting their photocatalytic performances. In this paper, new nanostructured spine-like three-dimensional (3D) g-C₃N₄ nanostructures are created for the first time via a new three-step synthesis method. In this method, self-assembly of layered precursors and H⁺ intercalation introduced by acid treatment play an important role for the unique nanostructure formation of 3D g-C₃N₄ nanostructures. The spine-like 3D g-C₃N₄ nanostructures show a superior photocatalytic performance for H₂ generation, achieving 4500 μmol·g^-1·h^-1, 8.2 times higher than that on conventional 2D g-C₃N₄. Remarkably spine-like 3D g-C₃N₄ nanostructures demonstrate a clear photocatalytic activity toward CO₂ reduction to CH₄ (0.71 μmol·g^-1·h^-1) in contrast to the negligible photocatalytic performance of conventional 2D g-C₃N₄ for the reaction. Adding Pt clusters as co-catalysts substantially enhance the CH₄ generation rate of the 3D g-C₃N₄ nanostructures by 4 times (2.7 μmol·g^-1·h^-1). Spine-like 3D g-C₃N₄ caged nanostructure leads to the significantly increased active sites and negatively shifted conduction band position in comparison with conventional 2D g-C₃N₄, favorable for the photocatalytic reduction reaction. This study demonstrates a new platform for the development of efficient photocatalysts based on nanostructured 3D g-C₃N₄ for H₂ generation and conversion of CO₂ to useful fuels such as CH₄.