Fabrication of PbS nanocrystal-sensitized ultrafine TiO2 nanotubes for efficient and unusual broadband-light-driven hydrogen production

It is highly desired to maximize the use of solar light by developing broadband-light-responsive H₂ production system in the field of photocatalysis. Herein, a novel PbS/(Pt–TiO₂) nanocomposite with efficient and unusual broadband-light-driven H₂ production feature is constructed by using infrared-bandgap PbS nanocrystals as sensitizer of Pt-loaded ultrafine anatase TiO₂ nanotubes (Pt–TiO₂). After optimizing the component ratio, the resultant PbS/(Pt–TiO₂) nanocomposite delivers a H₂ production activity of 813 and 186 μmol h^?1 under ultraviolet (UV)-visible (Vis)-near-infrared (NIR) and Vis-NIR light irradiation, respectively. Moreover, an apparent quantum yield of 38.6%, 26.2%, 2.43%, 3.21%, 2.17%, 0.36%, 0.11% and 0.01% can be attained from the PbS/(Pt–TiO₂) nanocomposite illuminated at 350, 420, 550, 700, 760, 850, 950 and 1064 nm monochromatic light, respectively. The intimate interfacial contacts in the PbS nanocrystals decorated ultrafine TiO₂ nanotubes, which serve as the support and electron acceptor of PbS nanocrystals, can effectively promote the photoexcited hot electrons transferring from PbS nanocrystals to TiO₂ nanotubes before the thermalization losses, and thus causing the efficient Vis-NIR-light-responsive H₂ production activity of the PbS/(Pt–TiO₂) nanocomposite. These results provide an intriguing application of infrared-bandgap materials to exploit the low-energy photons of the solar light for constructing efficient and unusual broadband-responsive H₂ production system.