Abstract
Perovskite quantum dots(PQDs)hold immense potential as photocatalysts for CO2 reduction due to their remarkable quantum properties,which facilitates the generation of multiple excitons,providing the nec-essary high-energy electrons for CO2 photoreduction.However,harnessing multi-excitons in PQDs for superior photocatalysis remains challenging,as achieving the concurrent dissociation of excitons and interparticle energy transfer proves elusive.This study introduces a ligand density-controlled strategy to enhance both exciton dissociation and interparticle energy transfer in CsPbBr3 PQDs.Optimized CsPbBr3 PQDs with the regulated ligand density exhibit efficient photocatalytic conversion of CO2 to CO,achieving a 2.26-fold improvement over unoptimized counterparts while maintaining chemical integrity.Multiple analytical techniques,including Kelvin probe force microscopy,temperature-dependent photoluminescence,femtosecond transient absorption spectroscopy,and density functional theory calculations,collectively affirm that the proper ligand termination promotes the charge separation and the interparticle transfer through ligand-mediated interfacial electron coupling and electronic inter-actions.This work reveals ligand density-dependent variations in the gas-solid photocatalytic CO2 reduc-tion performance of CsPbBr3 PQDs,underscoring the importance of ligand engineering for enhancing quantum dot photocatalysis.
基金项目
National Natural Science Foundation of China(22225606)
National Natural Science Foundation of China(22261142663)
National Natural Science Foundation of China(22176029)
Sichuan Science and Technology Program(2022JDRC0084)
Sichuan Science and Technology Program(2021JDJQ0006)
CMA Key Open Laboratory of Transforming Climate Resources to Economy(2023005K)
NETL
NSTL
万方数据