Direct Z-Scheme Heterojunction of Ligand-Free FAPbBr3/α-Fe2O3 for Boosting Photocatalysis of CO2 Reduction Coupled with Water Oxidation

ACS Appl Mater Interfaces. 2021 May 19;13(19):22314-22322. doi: 10.1021/acsami.1c01718. Epub 2021 May 7.

Abstract

Up to now, the majority of the developed photocatalytic CO2 reduction systems need to use expensive sacrificial reductants as electron source. It is still a huge challenge to drive the photocatalytic CO2 reduction using water as an electron source. Herein, we report a facile strategy for the construction of direct Z-scheme heterojunction of LF-FAPbBr3/α-Fe2O3, which is manufactured by the in situ and two-step controlled growth of ligand-free formamidinium lead bromide (LF-FAPbBr3) nanocrystals on the surface of α-Fe2O3 nanorods. The matchable energy levels and direct contact between LF-FAPbBr3 and α-Fe2O3 significantly accelerate the interfacial charge transfer, with a charge separation efficiency (ηseparation) of 93%, much higher than that of 11% shown by the ligand-capped FAPbBr3/α-Fe2O3 heterojunction. The resulting efficient separation and raised redox ability of photogenerated carriers endow the LF-FAPbBr3/α-Fe2O3 heterojunction with an outstanding photocatalytic performance for CO2 reduction (to CO and CH4) coupled with water oxidation (to O2), achieving a highest electron consumption rate of 175.0 μmol g-1 h-1 among the reported metal halide perovskite-based photocatalysts, which are 5 and 11 times higher in comparison with those of sole LF-FAPbBr3 and ligand-capped FAPbBr3/α-Fe2O3, respectively.

Keywords: CO2 reduction; Z-scheme; artificial photosynthesis; halide perovskite; heterojunction.