Efficient C(sp³)-H Bond Oxidation on Perovskite Quantum Dots Based on Ce-Oxygen Affinity

Area of Science:

• Materials Science
• Photocatalysis
• Quantum Dots

Background:

• Perovskite quantum dots (QDs) show promise in visible-light photocatalysis for synthesizing valuable chemicals.
• Catalyst stability under aerobic conditions is hindered by reactive oxygen species (ROS), particularly superoxide (O2⋅−).

Purpose of the Study:

• To develop a strategy using Ce3+ doping in perovskite QDs to control superoxide species for photocatalytic oxidation.
• To investigate the mechanism of Ce3+ doping in enhancing photocatalytic efficiency and stability.

Main Methods:

• Synthesis of Ce3+-doped perovskite quantum dots.
• Utilizing the doped QDs for C(sp3)-H bond oxidation reactions.
• Investigating reaction mechanisms through mechanistic studies.

Main Results:

• Ce3+ doping effectively guided superoxide species for photocatalytic oxidation reactions.
• Achieved stable operation of the catalytic system with high product conversion rates (15.3 mmol/g/h for benzaldehydes).
• Demonstrated that strong Ce-oxygen affinity accelerates exciton transfer to superoxide and inhibits radiative recombination.

Conclusions:

• Ce3+ doping offers a novel approach to utilize oxygen species on perovskite surfaces for photocatalysis.
• This strategy broadens the design principles for high-performance quantum dot photocatalysts.