Interfacial Engineering of Semicoherent Interface at Purified CsPbBr3 Quantum Dots/2D-PbSe for Optimal CO2 Photoreduction Performance.

ABSTRACT

Heterogeneous photocatalysts are extensively used to achieve interfacial electric fields for acceleration of oriented charge carrier transport and further promotion of photocatalytic redox reactions. Unfortunately, the incoherent interfaces are almost present in the heterostructures owing to large lattice mismatch accompanied by the interfacial defects and high density of gap states, acting as high energy barriers for charge migration. In this work, we report the atomic engineering of CsPbBr3/PbSe heterogeneous interfaces and conversion from incoherent features to semicoherent characters via methyl acetate (MeOAc) purification of CsPbBr3 quantum dots (QDs) before composited with two-dimensional (2D)-PbSe, which is confirmed by high-resolution transmission electron microscopy. The photocatalytic performances and theoretical calculations indicate that semicoherent interfaces are favorable for improving the activity and reactivity of the heterostructure, triggering 3 times enhanced photocatalytic CO2 reduction rate with 91% selectivity and satisfactory stability. This study proposes a facile method for photocatalytic heterojunctions to transform incoherent interfaces to photocatalytically beneficial semicoherent boundaries, accompanying with a systematic analysis of the consequent chemical dynamics to demonstrate the mechanism of the semicoherent interface for supporting photocatalysis. The understandings gained from this work are valuable for rational interfacial lattice engineering of heterogeneous photocatalysts for efficient solar fuel production.