Photoetching-Generated Redox Pairs in Confined Layered Structure Boost Single-Electron-Transfer-Mediated...

Area of Science:

• Materials Science
• Photocatalysis
• Sustainable Chemistry

Background:

• Single-electron-transfer (SET)-mediated photocatalysis is promising for sustainable synthesis but limited by electron quenching and low efficiency.
• Efficient utilization of photogenerated electrons is crucial for advancing photocatalytic processes.

Purpose of the Study:

• To propose a redox pair strategy for efficient photoelectron utilization and storage in photocatalysis.
• To develop a method for constructing redox pairs within a model photocatalyst framework.

Main Methods:

• Utilized a photoetching strategy on bismuth oxyiodate (BiOIO3) to create iodine redox pairs (Iδ+/IO3-).
• Employed theoretical calculations and spectral analyses to investigate the electronic structure modifications.
• Maintained the structural integrity of the [Bi2O2]2+ layers during the process.

Main Results:

• Successfully constructed iodine redox pairs within the [IO3]- layers of BiOIO3.
• Demonstrated that the iodine redox pairs significantly altered the electronic structure of BiOIO3.
• Observed prolonged charge carrier lifetimes and increased hot-electron density due to the modified electronic structure.

Conclusions:

• The designed iodine redox pairs enable efficient storage and release of photogenerated electrons.
• This approach offers a novel strategy to enhance electron utilization efficiency in photocatalysis.
• The findings pave the way for improved electron-mediated synthesis of high-value chemicals.