Unraveling the Transformation from Type-II to Z-Scheme in Perovskite-Based Heterostructures for Enhanced Photocatalytic CO2 Reduction

• DOI: 10.1021/jacs.3c12073
• Publication Date: 2024-01-25T17:37:10Z
• Authors: Wentao Song; Kok Chan Chong; Guobin Qi; Yukun Xiao; Ganwen Chen; Bowen Li; Yufu Tang; Xinyue Zhang; Yingfang Yao; Zhiqun Lin; Zhigang Zou; Bin Liu

The ability to create perovskite-based heterostructures with desirable charge transfer characteristics represents an important endeavor render a set of perovskite materials and devices tunable optoelectronic properties. However, due similar material selection band alignment in type-II Z-scheme heterostructures, it remains challenging obtain favorable electron pathway for photocatalysis. Herein, we report robust tailoring effective via transformation highly efficient selective photocatalytic CO2 reduction. Specifically, CsPbBr3/TiO2 CsPbBr3/Au/TiO2 are synthesized then investigated by ultrafast spectroscopy. Moreover, taking as examples, operando experiments theoretical calculations confirm that the heterostructure could be readily transformed into through establishing low-resistance Ohmic contact, which indicates fast is crucial construction, further demonstrated CsPbBr3/Ag/TiO2 CsPbBr3/MoS2 heterostructures. In contrast pristine CsPbBr3 CsPbBr3/TiO2, exhibits 5.4- 3.0-fold enhancement consumption rate DFT situ diffuse reflectance infrared Fourier transform spectroscopy unveil superior CO selectivity attributed lower energy *CO desorption than hydrogenation *HCO. This meticulous design sheds light on modification multifunctional enlightens conscious optimization semiconductor-based catalysis applications.