Interfacial Reverse Charge Transfer Enabling Near 100% Selectivity of Glycerol Photooxidation into Formate over...

Area of Science:

• Catalysis
• Materials Science
• Photochemistry

Background:

• Photooxidation of organic feedstocks offers a route to valuable chemicals but suffers from poor product selectivity.
• Controlling oxidation pathways is crucial for efficient biomass upgrading.

Purpose of the Study:

• To enhance product uniformity and efficiency in glycerol photooxidation.
• To investigate the role of strong metal-support interaction (SMSI) in tuning catalyst interfaces.

Main Methods:

• Tuning the Schottky interface of gold/titanium dioxide (Au/TiO2) catalysts using SMSI.
• Inducing reverse charge transfer from TiO2 to Au, forming electron-rich Auδ- species and specific interfacial sites.
• Utilizing glycerol (GLY) photooxidation as a model reaction to assess catalyst performance.

Main Results:

• Achieved nearly 100% formate (FA) selectivity with a production rate of 2.15 mmol g⁻¹ h⁻¹, a 21.6-fold increase over conventional catalysts.
• Demonstrated selective activation of GLY via C-H bond adsorption and O2 activation at interfacial sites.
• Showcased spatially decoupled activation of reactants, favoring efficient C-C bond cleavage and oxygenation.

Conclusions:

• SMSI-induced reverse charge transfer strategy significantly enhances selectivity and efficiency in glycerol photooxidation.
• The developed catalyst design offers a promising approach for uniform product generation in biomass upgrading.
• This work provides insights into controlling catalytic pathways for value-added chemical production.