Ce-modified NH2-MIL-88B enhances catalytic ozonation for effective antibiotic degradation

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Environmental Research Pub Date : 2025-06-15 Epub Date: 2025-03-18 DOI:10.1016/j.envres.2025.121388
Ying Yang, Shengwen Zhou, Yaoru Mao, Yuerong Zhou, Xiuwen Cheng
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Abstract

A Ce-doped NH2-MIL-88B(Fe) composite (Ce-NM8B) was synthesized via a hydrothermal method and used to catalyze ozone oxidation to degrade levofloxacin (LEF) in water. Moreover, comprehensive characterization of Ce-NM8B, including crystal structure, surface morphology, and electrochemical properties, was performed using XRD, SEM, BET, XPS, FT-IR, and ICP techniques. As a result, the Ce-NM8B/O3 system achieved an 84.2 % degradation of 10 mg/L LEF within 40 min under optimal conditions (0.20 g/L catalyst dosage, 0.20 L/min ozone flow, pH 7). Furthermore, EPR and radical quenching experiments confirmed the generation of ·OH, O2·-, and 1O2 species, in addition to direct ozone oxidation and catalytic adsorption. Additionally, HPLC-MS analysis identified key degradation pathways, including piperazine, quinolone, and morpholine ring cleavage, alongside decarboxylation, defluorination, and demethylation. In terms of toxicity, evaluation using T.E.S.T. revealed that intermediate products exhibited reduced toxicity. Moreover, Ce-NM8B demonstrated stable performance over three cycles. Finally, the system's applicability and practical potential were confirmed through the degradation of several antibiotics and testing in natural water substrates.
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Ce-修饰的 NH2-MIL-88B 可增强催化臭氧作用,从而有效降解抗生素。
通过水热法合成了掺杂铈的 NH2-MIL-88B(Fe)复合材料(Ce-NM8B),并将其用于催化臭氧氧化以降解水中的左氧氟沙星(LEF)。此外,还利用 XRD、SEM、BET、XPS、FT-IR 和 ICP 技术对 Ce-NM8B 进行了全面表征,包括晶体结构、表面形貌和电化学性能。结果表明,在最佳条件下(催化剂用量为 0.20 g/L,臭氧流量为 0.20 L/min,pH 值为 7),Ce-NM8B/O3 系统在 40 分钟内对 10 mg/L LEF 的降解率达到 84.2%。此外,EPR 和自由基淬灭实验证实,除了直接臭氧氧化和催化吸附外,还产生了 -OH、O2-- 和 1O2 物种。此外,HPLC-MS 分析确定了关键的降解途径,包括哌嗪、喹诺酮和吗啉环裂解,以及脱羧、脱氟和脱甲基。在毒性方面,使用 T.E.S.T. 进行的评估显示,中间产物的毒性有所降低。此外,Ce-NM8B 在三个周期内表现出稳定的性能。最后,通过降解几种抗生素和在天然水基质中进行测试,证实了该系统的适用性和实用潜力。
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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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