Charge Carrier Dynamics of CsPbBr<sub>3</sub>/g-C<sub>3</sub>N<sub>4</sub> Nanoheterostructures in Visible-Light-Driven CO<sub>2</sub>-to-CO Conversion
Yu‐Hung Chen, Kai‐An Tsai, Tzu-Wei Liu, Yao-Jen Chang, Yuchen Wei, Meng‐Wei Zheng, Shou‐Heng Liu, Mei‐Yi Liao, Pei-Yu Sie, Jarrn‐Horng Lin, Shih-Wen Tseng, Ying‐Chih Pu
Abstract
The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3 nanocrystals (NCs) and CsPbBr3/g-C3N4 nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3 NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4 NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4 NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3 to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4 NHS was extended two times more than that in the CsPbBr3 NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2 conversion.