Abstract：
Tetracycline (TC) and Oxytetracycline (OTC) are common antibiotics increasingly detected in the environment, posing a potential risk to human and aquatic lives. Although conventional methods such as adsorption and photocatalysis are used for the degradation of TC and OTC, they are inefficient in removal efficiency, energy yield, and toxic byproduct generation. Herein, a falling-film dielectric barrier discharge (DBD) reactor coupled with environmentally friendly oxidants (hydrogen peroxide (HPO), sodium percarbonate (SPC), and HPO + SPC) was applied, and the treatment efficiency of TC and OTC was investigated. Experimental results showed that moderate addition of the HPO and SPC exhibited a synergistic effect (SF > 2), significantly improving the antibiotic removal ratio, total organic removal ratio (TOC), and energy yield by more than 50%, 52%, and 180%, respectively. After 10 min of DBD treatment, the introduction of 0.2 mM SPC led to a 100% antibiotic removal ratio and a TOC removal of 53.4% and 61.2% for 200 mg/L TC and 200 mg/L OTC, respectively. Also, 1 mM HPO dosage led to 100% antibiotic removal ratios after 10 min of DBD treatment and a TOC removal of 62.4% and 71.9% for 200 mg/L TC and 200 mg/L OTC, respectively. However, the DBD + HPO + SPC treatment method had a detrimental effect on the performance of the DBD reactor. After 10 min of DBD plasma discharge, the removal ratios for TC and OTC were 80.8% and 84.1%, respectively, when 0.5 mM HPO + 0.5 mM SPC was added. Moreover, principal component and hierarchical cluster analysis confirmed the differences between the treatment methods. Furthermore, the concentration of oxidant-induced in-situ generated ozone and hydrogen peroxide were quantitatively determined, and their indispensable roles during the degradation process were established via radical scavenger tests. Finally, the synergetic antibiotic degradation mechanisms and pathways were proposed, and the toxicities of the intermediate byproducts were evaluated.
摘要：
四环素(TC)和土霉素(OTC)是越来越多的常见抗生素,对人类和水生生物构成潜在风险。虽然传统的方法如吸附和光催化用于降解TC和OTC,它们的去除效率低下，能量产量，和有毒副产品的产生。在这里，降膜介质阻挡放电（DBD）反应器与环境友好的氧化剂（过氧化氢（HPO），过碳酸钠（SPC），并应用HPO+SPC)，并考察了TC和OTC的治疗效果。实验结果表明，适度添加HPO和SPC表现出协同作用（SF>2），显著提高抗生素去除率，总有机物去除率(TOC)，能源产量超过50%，52%,180%,分别。DBD处理10分钟后，对于200mg/LTC和200mg/LOTC，引入0.2mMSPC导致100％的抗生素去除率和53.4％和61.2％的TOC去除率，分别。此外，1mMHPO剂量在DBD处理10分钟后导致100％的抗生素去除率，对于200mg/LTC和200mg/LOTC，TOC去除率分别为62.4％和71.9％。分别。然而,DBD+HPO+SPC处理方法对DBD反应器的性能有不利影响。DBD等离子体放电10分钟后,TC和OTC的去除率分别为80.8%和84.1%，分别,当加入0.5mMHPO+0.5mMSPC时。此外，主成分和层次聚类分析证实了处理方法之间的差异。此外，定量测定了氧化剂诱导原位生成的臭氧和过氧化氢的浓度，通过自由基清除剂测试确定了它们在降解过程中不可或缺的作用。最后,提出了抗生素协同降解机制和途径，并对中间副产物的毒性进行了评价。
