Ultrasound enhanced destruction of tetracycline hydrochloride with peroxydisulfate oxidation over FeS/NBC catalyst: Governing factors, strengthening mechanism and degradation pathway

Abstract

In this study, FeS/N-doped biochar (NBC) derived from the co-pyrolysis of birch sawdust and Mohr's salt was applied to evaluate the efficiency of catalyzed peroxydisulfate (PDS) oxidation for tetracycline (TC) degradation. It is found that the combination of ultrasonic irradiation can distinctly enhance the removal of TC. This study investigated the effects of control factors such as PDS dose, solution pH, ultrasonic power, and frequency on TC degradation. Within the applied ultrasound intensity range, TC degradation increases with increasing frequency and power. However, excessive power can lead to a reduced efficiency. Under the optimized experimental conditions, the observed reaction kinetic constant of TC degradation increased from 0.0251 to 0.0474 min−1, with an increase of 89%. The removal ratio of TC also increased from ∼85% to ∼99% and the mineralization level from 45% to 64% within 90 min. Through the decomposition testing of PDS, reaction stoichiometric efficiency calculation, and electron paramagnetic resonance experiments, it is shown that the increase in TC degradation of the ultrasound-assisted FeS/NBC-PDS system was attributed to the increase in PDS decomposition and utilization, as well as the increase in SO4•− concentration. The radical quenching experiments showed that SO4•−, •OH, and O2•− radicals were the dominant active species in TC degradation. TC degradation pathways were speculated according to intermediates from HPLC-MS analysis. The test of simulated actual samples showed that dissolved organic matter, metal ions, and anions in waters can undercut the TC degradation in FeS/NBC-PDS system, but ultrasound can significantly reduce the negative impact of these factors.