Interfacial Microenvironment Engineering Based on Ordered <scp>TiO₂</scp> Porous Films for Enhanced Visible Light Driven Photocatalysis

Comprehensive Summary Visible‐light‐driven photocatalysis has great potential in environmental remediation and organic synthesis. Rational design and regulation of the reaction interfacial microenvironment is critical for photocatalytic performance, yet challenging. We report here a highly efficient photocatalytic system based on hydrophobic TiO 2 porous (H‐OTP) film for visible‐light‐driven dye‐sensitized photo‐oxidation. Such interface architecture design enhances the adsorption capability of organic dyes and enables the formation of air trapped triphase reaction interface microenvironment as confirmed via three‐dimensional (3D) laser scanning confocal microscopy. Based on this interface architecture, the concentrations of O 2 and organic molecule at the local reaction zone are both significantly increased, which promotes the generation of reactive oxygen species (•O 2 − and •OH), and enhances the photocatalytic performance in terms of both kinetics and organic mineralization efficiency. This study highlights the importance of interface microenvironment design and reveals an effective way to develop highly efficient photocatalytic systems.