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Au nanoparticles at the TiO$_2$ surface can enhance the photocatalytic H$_2$generation performances owing to their electron transfer co-catalytic ability.Key to maximize the co-catalytic effect is a fine control over Au nanoparticlesize and placement on the photocatalyst, in relation to parameters such as theTiO$_2$ morphology, illumination wavelength and pathway, and light penetrationdepth in the photocatalyst. Here we present an approach for site-selectiveintrinsic-decoration of anodic TiO$_2$ nanotubes (TNs) with Au nanoparticles:we produce, by Ti and Au co-sputtering, Ti-Au alloy layers that featurecompositional gradients across their thickness; these layers, when anodizedunder self-ordering electrochemical conditions, can form Au-decorated TNs wherethe Au nanoparticle density and placement vary according to the Auconcentration profile in the metal alloy substrates. Our results suggest that,the Au co-catalyst placement strongly affects the photocatalytic H$_2$evolution performance of the TNs layers. We demonstrate that, when growingAu-decorated TNs, the use of Ti-Au substrates with a suitable Au compositionalgradient can lead to higher H$_2$ evolution rates compared to TNs classicallygrown with a homogenous co-catalyst decoration. As a side effect, a properplacement of the co-catalyst nanoparticles allows for reducing the amount ofnoble metal without dumping the H$_2$ evolution activity.

acs applied nano materials

Compositional gradients in sputtered Ti-Au alloys: Site-selective  Au-decoration of anodic TiO$_2$ nanotubes towards enhanced photocatalytic  H$_2$ evolution