Fluorination of Covalent Organic Framework Reinforcing the Confinement of Pd Nanoclusters Enhances Hydrogen Peroxide Photosynthesis

Metal-isolated clusters (MICs) physically confined onphotoactivematerials are of great interest in the field of photosynthesis ofhydrogen peroxide (H2O2). Despite recent importantendeavors, weak confinement of MICs in the reported photocatalyticsystems leads to their low catalytic activity and stability. Herein,we report a new strategy of fluorinated covalent organic frameworks(COFs) to strongly confine Pd ICs for greatly boosting the photocatalyticactivity and stability of H2O2 photosynthesis.Both experimental and theoretical results reveal that strong electronegativefluorine can increase the metal-support interaction and optimizethe d-band center of Pd ICs, thus significantly enhancing the stabilityand activity of photocatalytic H2O2. An optimalTAPT-TFPA COFs@Pd ICs photocatalyst delivers a stable H2O2 yield rate of 2143 & mu;mol h(-1) g(-1). Most importantly, the as-made TAPT-TFPA COFs@PdICs exhibit high catalytic stability over 100 h, which is the bestamong the reported materials.

Automated summary

Using fluorinated covalent organic frameworks (COFs) to strongly confine Pd ICs greatly enhances the photocatalytic activity and stability of H2O2 photosynthesis.