Regulating the Tautomerization of β-Ketoenamine Covalent Organic Frameworks for Boosting the Photoenzyme Catalytic Hydrolyzation of Acetaminophen in Wastewater

The widespread use of acetaminophen (APAP), a common analgesic, has led to its increasing detection in wastewater, causing environmental pollution, particularly in aquatic ecosystems. This study introduces a novel photoenzyme catalytic system that combines β-ketoenamine covalent organic frameworks (COFs) with horseradish peroxidase (HRP) for efficient APAP degradation. By regulating the tautomerization of β-ketoenamine COFs, the synergistic effect of absorption, photocatalytic oxidation, and enzymatic degradation was optimized: β-ketoenamine COFs contribute to the absorption and photocatalytic oxidation of APAP and the generation of hydrogen peroxide (H₂O₂), and HRP further degrades APAP under the presence of H₂O₂. Within 1 h, the system achieves a 95.4% degradation rate of APAP. Additionally, it efficiently degrades nine other organic pollutants, with degradation rates ranging from 71 to 99%. This innovative approach shows great potential for treating pharmaceutical contaminants in wastewater, offering a promising path for the development of more sustainable and efficient wastewater treatment technologies.