考察了Fe(Ⅲ)/过氧乙酸(PAA)体系对土霉素(OTC)的降解效能与机理,以及初始pH值、药剂投加量、水体基质对OTC降解的影响.结果表明:Fe(Ⅲ)/PAA体系降解OTC过程中,Fe(Ⅲ)与OTC发生络合形成Fe(Ⅲ)-OTC络合物,该络合物通过内部电子转移使Fe(Ⅲ)还原为Fe(Ⅱ),生成的Fe(Ⅱ)催化PAA产生活性物种,从而加快了OTC的降解.化学探针和自由基淬灭实验结果表明,有机自由基(CH3C(O)O•和CH3C(O)OO•)、HO•和Fe(Ⅳ)为该体系的主要活性物种.酸性条件有利于该体系对OTC的降解,在中性及弱碱性条件下,OTC在该体系中的去除主要是由于PAA氧化作用.随着PAA、Fe(Ⅲ)投加量的提高,OTC的去除效率逐渐增加,但是其过量则会抑制OTC降解.水中Cl-和天然有机物的存在会抑制OTC的降解,而NO3-、SO42-和HCO3-对OTC的降解几乎没有影响.Fe(Ⅲ)/PAA体系对其他四环素类污染物也有较好的处理效果.
Abstract
In this study, the degradation efficiency and mechanism of oxytetracycline (OTC) in the Fe(Ⅲ)/peracetic acid (PAA) system were investigated, and the effects of initial pH, reagents dosage and water components on OTC degradation were also explored. The results suggested that in the degradation of OTC by Fe(Ⅲ)/PAA system, Fe(Ⅲ) complexed with OTC to form Fe(Ⅲ)-OTC complex, which reduced Fe(Ⅲ) to Fe(II) through internal electron transfer. Subsequently, the generated Fe(II) catalyzed PAA to produce reactive species, thus accelerating the degradation of OTC. The results of chemical probe and radical quenching experiments showed that organic radicals (CH3C(O)O• and CH3C(O)OO•), HO• and Fe(IV) played major roles for the degradation of OTC in Fe(III)/PAA system. Acidic conditions were beneficial to the degradation of OTC in this system, while the removal of OTC under neutral and weakly alkaline conditions was mainly due to the PAA oxidation. The removal efficiency of OTC increased gradually with the increase of PAA or Fe(Ⅲ) dosage, but their excess concentration would inhibit OTC degradation. The presence of Cl- and natural organic matter in Fe(Ⅲ)/PAA system inhibited the degradation of OTC, while NO3-, SO42- and HCO3- had little effect on OTC removal. The Fe(Ⅲ)/PAA system also had a good treatment effect on the other tetracycline pollutants.
关键词
Fe(Ⅲ) /
高级氧化 /
过氧乙酸 /
土霉素
Key words
advanced oxidation /
Fe(Ⅲ) /
oxytetracycline /
peracetic acid
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基金
国家重点研发计划(2023YFB2390100);西南交通大学新型交叉学科培育基金项目(2682024QZ007)
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