Enhancing degradation of norfloxacin using chrysanthemum-shaped bimetallic NH2-MIL-53(Fe/Ti) photocatalysts under visible light irradiation

IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL
Wen Gao, Fangyuan Wang, Meilin Ou, Qianqian Wu, Lei Wang, Haonan Zhu, Yuanyuan Li, Ning Kong, Jianping Qiu, Shanshan Hu, Shuang Song
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Abstract

The presence of elevated levels of norfloxacin (NOR) in the aquatic environment presents a serious risk to both human health and environmental organisms due to its extremely toxic and persistent characteristics. Herein, a series of Fe/Ti bimetallic composites (NH2-MIL-53(Fe/Ti)) were prepared using a one-step hydrothermal method to assess their capability for NOR degradation and investigate degradation mechanisms. It was observed that the well-organized nanosheets interconnected to form chrysanthemum clusters contained a significant number of exposed edges and open pores, which facilitated the enrichment of NOR. Notably, the optimum NH2-MIL-53(Fe/Ti) (1.5:1) demonstrated excellent degradation performance for NOR under visible light, owing to an electronic interaction between Fe3+ and Ti4+ metal centers. Efficient NOR degradation by NH2-MIL-53(Fe/Ti) (1.5:1) was achieved at 84.6% after 120 min of irradiation. Furthermore, the NH2-MIL-53(Fe/Ti) (1.5:1) maintained excellent reusability and stability even after five cycles tests. Active species trapping experiments confirmed that the pivotal role of •O2− and h+ in photodegradation of NOR pollutants. A plausible photocatalytic mechanism was suggested according to various performance characterization and experimental results. Defluorination and ring opening were the main degradation pathways. This work advanced our understanding of photogenerated carriers transfer and energy conversion in bimetallic MOFs. Additionally, a novel strategy was presented for visible light catalytic degradation of NOR, which were highly relevant for the field of environmental treatment.
菊花形双金属NH2-MIL-53(Fe/Ti)光催化剂在可见光下对诺氟沙星的降解
由于诺氟沙星的剧毒和持久性,其在水生环境中含量升高对人类健康和环境生物构成严重风险。本文采用一步水热法制备了一系列Fe/Ti双金属复合材料(NH2-MIL-53(Fe/Ti)),考察了其对NOR的降解能力和降解机理。结果表明,结构良好的菊花簇纳米片含有大量的暴露边缘和开放的孔隙,有利于NOR的富集。值得注意的是,最优的NH2-MIL-53(Fe/Ti)(1.5:1)在可见光下表现出优异的NOR降解性能,这是由于Fe3+和Ti4+金属中心之间的电子相互作用。辐照120 min后,NH2-MIL-53(Fe/Ti)(1.5:1)对NOR的有效降解率为84.6%。此外,NH2-MIL-53(Fe/Ti)(1.5:1)即使经过5次循环试验也保持了良好的可重复使用性和稳定性。活性物种捕获实验证实了•O2−和h+在NOR污染物光降解中的关键作用。根据各种性能表征和实验结果,提出了一种合理的光催化机理。脱氟和开环是主要的降解途径。这项工作提高了我们对双金属mof中光生载流子转移和能量转换的理解。此外,还提出了一种可见光催化降解NOR的新策略,这在环境处理领域具有重要意义。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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