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Noble Metal-Free Photocatalysts Consisting of Graphitic Carbon Nitride, Nickel Complex, and Nickel Oxide Nanoparticles for Efficient Hydrogen Generation.

A facile and simple synthetic route is developed to prepare earth-abundant and noble metal-free hybrid photocatalysts, which are composed of graphitic carbon nitride (CN), nickel complex, and NiO x nanoparticles. Bimolecular nucleophilic substitution reaction was employed to attach a nickel complex onto a graphitic CN framework through covalent bonds to support its high loading and dispersion. NiO x nanoparticles were further incorporated into the catalysts to serve as a hole-transporting medium to improve the separation of photogenerated carriers for higher photocatalytic activity. Both yNiL/CN and yNiL/NiO x/CN exhibit superb H2 evolution activity. The optimum H2 evolution rate of the binary photocatalysts yNiL/CN reaches 303.3 μmol·h-1·g-1, whereas that of the ternary photocatalysts yNiL/NiO x/CN reaches 524.1 μmol·h-1·g-1, and the apparent quantum efficiency reaches 1.46% at 450 nm. This finding reveals that coordination of a nickel complex is significant in promoting photocatalytic performance, and the incorporation of NiO x nanoparticles as a hole-transporting medium is beneficial for separation of the photogenerated charge carriers. The novel hybrid system offers a new horizon for designing transition-metal complex-modified graphitic CN as noble metal-free and highly active photocatalysts for efficient visible light-driven hydrogen generation.