High efficiency degradation of tetracycline by peroxymonosulfate activated with Fe/NC catalysts: Performance, intermediates, stability and mechanism

Abstract

Carbon-based catalysts have the advantages of biological cleaning, eco-friendly and cost-effective in water treatment. While, nitrogen doped biochar promotes the development of non-radical peroxymonosulfate (PMS) activation in environmental remediation. Thus, three-dimensional sponge-like porous Fe and N co-doped biochar (Fe/CN-30) with high catalytic activity for PMS activation was synthesized. In a wide pH range (1-11), the Fe/CN-30 catalyst can efficiently degrade tetracycline (TC) with a small amount of PMS. The non-radical pathways are prominent in the TC decomposition process according to the quenching experiments, electron paramagnetic resonance (EPR) and gas chromatograph-mass spectrometer (GC-MS) analysis, in which the contribution of high-valent iron-oxo species (Fe(IV) = O) was dominant. X-ray photoelectron spectroscopy and reaction kinetic experiments confirmed that the coordination sites of Fe and N in the Fe/CN-30 are the reactive centers for TC degradation. Moreover, the successive addition of low concentration PMS into the system was confirmed to favor the PMS utilization, and the high selectivity of the Fe/CN-30 was confirmed by the analysis of pollutant structure. Furthermore, by-products of TC degradation in the Fe/CN-30/PMS system and the possible TC degradation pathways were proposed via liquid chromatography-mass spectrometry (LC-MS). Therefore, this study dedicates to providing new insights into the non-radical pathway-catalyzed AOPs.

Keywords: High-valent iron-oxo species; Non-radical reaction; Peroxymonosulfate; Tetracycline.