Interfacial Chemical-Bond-Modulated Charge Transfer of Heterostructures for Improving Photocatalytic Performance

Interface engineering of heterostructured photocatalysts plays a very important role in the transfer and separation process of interfacial charge carriers, but how to regulate the transfer and separation of photogenerated charge carriers still is a huge challenge at the nanometric interface of heterostructures (HCs). Herein, we demonstrate that interfacial chemical bonds can effectively modulate photogenerated charge transfer in nanoclay-based HCs constructed by natural Kaolinite (Kaol) nanosheets and P25-TiO2. Experimental results and density functional theory (DFT) calculations confirm that stable Al–O–Ti bonds form at the interfaces by interactions of the Al–OH groups of Kaol and (101) surfaces of anatase TiO2. The Al–O–Ti bond strengthens the energy band bending of the space charge region near the interfacial bond and thus provides a fast transfer channel for interfacial photogenerated charge, resulting in the boosted charge transfer and separation ability of Kaol/P25 HCs. The findings reported here provide a deeper insight into modulating interfacial charge transfer by chemical bonds and shed new light on interface engineering of efficient heterostructured photocatalysts for environmental applications.