Inorganic-Organic Cs2SnBr6/COFs S-Scheme Heterojunction with Interfacial Electric Field for Promoted Peroxymonosulfate Activation and Tetracycline Degradation
摘要
Photocatalysis-driven peroxymonosulfate (PMS) activation has emerged as a highly promising strategy for eliminating refractory contaminants from wastewater. S-scheme heterojunctions are particularly appealing due to their ability to spontaneously generate a stable internal electric field (IEF), which simultaneously facilitates efficient charge separation and retains a high redox potential. Herein, an inorganic-organic S-scheme heterojunction integrating covalent organic frameworks (COFs) with Cs2SnBr6 (CSB) perovskite was rationally constructed, wherein CSB nanoparticles were homogeneously anchored within the COFs skeleton to ensure intimate interfacial contact. Comprehensive characterization confirmed the formation of a robust IEF at the heterojunction interface, which drives directional electron transfer from the COFs to CSB as the core mechanism for efficient charge separation. Benefiting from this well-defined charge migration pathway, the optimized CSB-COF75 composite achieved rapid and highly efficient photocatalytic degradation of tetracycline hydrochloride (TC) with an apparent rate constant of 0.30 min− 1, a 3.75-fold improvement over pristine COFs (0.08 min− 1). The dominant reactive oxygen species governing TC decomposition were identified via radical quenching experiments as superoxide radical anion (•O2−), sulfate radicals (•SO4−), singlet oxygen (1O2), and hydroxyl radicals (•OH). Liquid chromatography-mass spectrometry (LC-MS) analysis elucidated three plausible TC transformation pathways, with ecotoxicological evaluations indicating substantially reduced environmental risk of the intermediates. Collectively, these findings advance a rational and sustainable strategy for efficient antibiotic elimination from aquatic environments.