Abstract
Visible light-driven water splitting (VLWS) into hydrogen and oxygen is attractive and depends on efficient photocatalysts. Herein, we demonstrate the first exploration of the capability to control the morphology of nanostructured TiO2 in conjunction with the choice of a suitable plasmonic metal (PM) to fabricate novel photocatalysts that are capable of harvesting visible light for more efficient VL-fuel conversion. This methodology affords us to successful access to the novel plasmonic Pt/TiO2-HA (large Pt nanoparticles (NPs) supported on TiO2 hierarchical nano-architecture (TiO2-HA)) photocatalysts that exhibit plasmon absorption in the visible range and consequent outstanding activity and durability for VLWS. Particularly, the Pt/TiO2-HA shows an excellent photocatalytic activity for overall water splitting rather than only for hydrogen evolution (HE), which is superior to those of the conventional plasmonic Au/TiO2 photocatalysts. The synergistic effects of the high Schottky barrier at the Pt–TiO2-HA interface, which induces the stronger reduction ability of hot electrons, and intrinsic Pt catalytic activity are responsible for the exceptional photocatalytic performance of Pt/TiO2-HA and simplify the composition of plasmonic photocatalysts.
Highlights
Design and fabrication of high-performance photocatalysts with suitable architectures for Visible light-driven water splitting (VLWS) into hydrogen and oxygen has been a topic of tremendous scientific interest in recent years because this process is promising for resolving today’s increased global environmental crisis and energy shortage[1,2,3,4]
The ultrathin TiO2 b-NWs provide a high specific surface area (SBET of 150.2 m2 g‒1, Fig. S3) for harvesting light, short distances for migration of charge carries, and a large contact area with electrolyte, while the large central trunks enhance light scattering. These features of TiO2-HA result in a significant extension of the light travelling distance within the ensemble of the TiO2-HAs and increase the probability of photons being absorbed by TiO2-HA
The plasmonic Pt NPs effectively activate the photocatalytic activity of pure TiO2 in the visible region and eliminate the use of additional chemical co-catalysts for hydrogen evolution (HE) and oxygen evolution (OE) reactions in the VLWS process
Summary
Design and fabrication of high-performance photocatalysts with suitable architectures for VLWS into hydrogen and oxygen has been a topic of tremendous scientific interest in recent years because this process is promising for resolving today’s increased global environmental crisis and energy shortage[1,2,3,4]. The exploration of highly efficient photocatalysts with a strong response to visible light, a high activity and stability, and low cost is critical to construct an artificial leaf for realizing solar energy conversion. The coverage of these PM-NPs could significantly diminish the catalytically active surface area[28] These drawbacks generally leads to the Au or Ag NPs-decorated semiconductor photocatalysts showing activity towards a half reaction of water splitting producing only H2 or O2 with the need of sacrificial regents (SR)[18,19,20,21,22,23,24,25] or additional driving bias[26,27,28,32,33]. Bigall et al have established some very effective methods to extend the localized surface plasmonic (LSP) absorption of Pt NPs to the visible and even near-IR regions of spectrum by enlarging their size[35,36,37]
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