Targeted reactant activation and spatial charge separation for efficient photocatalytic C(sp³)-H bond oxidation.

Area of Science:

• Materials Science
• Photocatalysis
• Green Chemistry

Background:

• Semiconductor photocatalysis is key for sustainable organic synthesis.
• Efficient C(sp3)-H bond oxidation is hindered by poor charge separation and low surface reactivity.

Purpose of the Study:

• To develop a heterojunction photocatalyst for efficient C(sp3)-H bond oxidation.
• To enhance charge separation and surface activation for green synthesis.

Main Methods:

• Fabrication of a CsPCN-Cs3Bi2Br9 heterojunction.
• In situ experimental and theoretical studies to elucidate charge transfer mechanisms.
• Visible-light driven C(sp3)-H oxidation of ethylbenzene.

Main Results:

• The CsPCN-Cs3Bi2Br9 heterojunction demonstrated efficient charge separation and enhanced activation of oxygen and reactants.
• Achieved a high conversion rate of 8420 µmol g-1 h-1 for ethylbenzene to acetophenone, 4.3 times higher than Cs3Bi2Br9 alone.
• Showcased broad substrate applicability for C(sp3)-H functionalization.

Conclusions:

• The designed heterostructure effectively couples charge separation with surface reactant activation.
• This strategy enables efficient lead-free perovskite-based photocatalytic C(sp3)-H functionalization.
• The study provides a rational design for advanced photocatalysts in green organic synthesis.