Single Atoms in Photocatalysis: Low Loading Is Good Enough!

We disperse Pt single atoms (SAs) with different loading densities on anatase TiO2 thin films and evaluate the photocatalytic H-2 generation as a function of the incident light intensity. We show that under common illumination intensities (such as terrestrial solar illumination), a minuscule Pt SA loading of similar to 10(5) atoms mu m(-2) (surface Pt content similar to 0.1 at.%) is sufficient to achieve a maximized H-2 production rate. This results in a maximum turnover frequency at a single Pt atom site of similar to 300 H-2 molecules s(-1). For a vast majority of illumination conditions and a suitable surface configuration, it is not the density of co-catalytic sites that is rate-determining (a high loading is not needed!), but the charge carrier generation (and flux of photoelectrons to the co-catalytic centers) determines the overall reaction rate. This is in stark contrast to SA catalysis of classic chemical reactions where generally a maximum loading of reactive SA delivers a maximum activity.

Automated summary

We disperse Pt single atoms on TiO2 thin films and evaluate the photocatalytic H-2 generation. We find that a minuscule loading of Pt single atoms is sufficient to achieve maximized H-2 production rate under common illumination intensities. The overall reaction rate is determined by charge carrier generation, rather than the density of co-catalytic sites.