Air–Liquid–Solid Triphase Interfacial Microenvironment Regulation for Efficient Visible-Light-Driven Photooxidation Based on Ordered TiO2 Porous Films

The rational design and regulation of interfacial microenvironments represents an effective strategy for enhancing reaction performance. Previous studies have demonstrated that constructing air–liquid–solid triphase interfaces can substantially enhance catalytic reactions involving gaseous reactants. However, research on regulating the triphasic interfacial microenvironment remains limited and challenging. Herein, we fabricated a triphase photocatalytic system by depositing hydrophobic materials onto ordered TiO2porous (OTP), achieving significantly enhanced performance in visible-light-driven dye-sensitized photooxidation. Further, we regulated the triphasic microenvironment by systematically adjusting the chain length of hydrophobic molecules. It was found that the chain length greatly affects the interfacial properties, including O2concentration, the organic molecule adsorption and the interfacial electron transfer efficiency, thereby influencing photocatalytic reaction kinetics and pathways. We demonstrated a high-performance triphase photocatalytic system using 1H,1H,2H,2H-perfluorooctyl triethoxysilane as the hydrophobic material, which optimized multiple interfacial properties through synergistic effects, leading to optimal photocatalytic performance.