首页|Ligand-mediated exciton dissociation and interparticle energy transfer on CsPbBr3 perovskite quantum dots for efficient CO2-to-CO photoreduction

Ligand-mediated exciton dissociation and interparticle energy transfer on CsPbBr3 perovskite quantum dots for efficient CO2-to-CO photoreduction

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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.

Perovskite quantum dotsLigandsPhotocatalytic CO2 reductionExciton dissociationElectronic coupling

Fengyi Zhong、Jianping Sheng、Chenyu Du、Ye He、Yanjuan Sun、Fan Dong

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School of Resources and Environment,University of Electronic Science and Technology of China,Chengdu 611731,China

Research Center for Carbon-Neutral Environmental & Energy Technology,Institute of Fundamental and Frontier Sciences,University of Electronic Science and Technology of China,Chengdu 611731,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaSichuan Science and Technology ProgramSichuan Science and Technology ProgramCMA Key Open Laboratory of Transforming Climate Resources to Economy

2222560622261142663221760292022JDRC00842021JDJQ00062023005K

2024

10.1016/j.scib.2024.01.027

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(7)
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