Unraveling the Role of Interface in Photogenerated Charge Separation at the Anatase/Rutile Heterophase Junction

Heterophase junctions have emerged as an effective strategy for spatial charge separation in photocatalysis. However, the photogenerated charge separation pathway at the junction region remains in doubt, and how the interfacial structure affects charge separation is unclear. Herein, we fabricate well-defined TiO2 heterophase junctions between rutile and anatase and employ in situ photochemical probing reactions to track the interfacial charges distribution by means of spherical aberration correction transmission electron microscope (CS aberration TEM). The photoreduction deposition of platinum (Pt) nanoclusters and photo-oxidation deposition of metal oxide nanoparticles demonstrate that the photogenerated electrons smoothly migrate across the interfacial phase junction from rutile to anatase phases and the photogenerated holes move in an opposite direction, which provides direct evidence on the spatial charge separation at the heterophase junction. Moreover, the atomic interfacial structure of anatase/rutile TiO2 heterophase junction formed is conducive for photogenerated charges moving from one phase to the other. This study revises the photogenerated charge separation at the anatase/rutile heterophase junction and demonstrates the important role of the interfacial structure on spatial charge separation.