Enhanced activation of persulfate by sulfide-modified and biochar-supported nZVI for efficient tetracycline degradation: mechanisms and performance
摘要
Tetracycline (TC) is a common persistent pollutant in aquatic ecosystems. Building on the safe and efficient removal of organic pollutants by Peroxydisulfate (PDS)-based advanced oxidation processes (AOPs), this study prepared an environmentally friendly porous biochar from the simple pyrolysis of straw powder as a carrier matrix and loaded it with zero-valent iron. By introducing the environmentally benign element sulfur and employing a liquid-phase reduction method to sulfide-modify a carbon material loaded with zero-valent iron, a sulfide zero-valent iron catalyst (S-ZVI@BC) was prepared, thereby addressing the challenges of facile agglomeration and surface passivation of nano zero-valent iron particles. The sulfide-modified iron-based carbon material has a larger specific surface area, providing more catalytically active sites to activate PDS for the effective degradation of TC. Batch experiments were systematically conducted to investigate the effects of the S/Fe molar ratio, PDS concentration, S-ZVI@BC dosage, initial pH, coexisting anions, and humic acid on the degradation efficiency of TC. The results showed that the S-ZVI@BC/PDS system achieved a 99.05% degradation of 20 mg/L TC within 30 min and performed across a wide pH range (3–9). Electron paramagnetic resonance (EPR) studies and quenching experiments indicated that ·OH and SO4·− played important roles in the TC degradation process. The degradation intermediates detected by liquid chromatography-mass spectrometry (LC-MS) were used to propose a degradation pathway for tetracycline. This study highlights the high catalytic performance, recyclability, and broad pH tolerance of S-ZVI@BC, offering new catalyst design ideas for the degradation of antibiotic pollutants using high-catalytic nanomaterials.
Graphical Abstract