Enhanced degradation of norfloxacin by Ce-mediated Fe-MIL-101: catalytic mechanism, degradation pathways, and potential applications in wastewater treatment,Environmental Science: Nano

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Enhanced degradation of norfloxacin by Ce-mediated Fe-MIL-101: catalytic mechanism, degradation pathways, and potential applications in wastewater treatment
Environmental Science: Nano ( IF 5.8 ) Pub Date : 2021-06-18 , DOI: 10.1039/d1en00250c
Chaosheng Bao _{1,

2,

3,

4,

5} , Jian Zhao _{6,

7,

8,

9,

10} , Yuanyuan Sun _{1,

2,

3,

4,

5} , Xiaoliang Zhao _{1,

2,

3,

4,

5} , Xiaohui Zhang _{1,

2,

3,

4,

5} , Yukun Zhu _{1,

2,

3,

4,

5} , Xilin She _{1,

2,

3,

4,

5} , Dongjiang Yang _{1,

2,

3,

4,

5} , Baoshan Xing _{11,

12,

13,

14}

Affiliation

School of Environmental Science and Engineering
School of Materials Science and Engineering
State Key Laboratory of Bio-fibers and Eco-textiles
Shandong Collaborative Innovation Center of Marine Biobased Fibers and Ecological Textiles
Institute of Marine Biobased Materials
Laboratory for Marine Ecology and Environmental Science
Qingdao National Laboratory for Marine Science and Technology
Qingdao 266071
China
Institute of Coastal Environmental Pollution Control
Stockbridge School of Agriculture
University of Massachusetts
Amherst
USA

Novel Ce-mediated Fe-MIL-101 (Fe/Ce-MIL-101) Fenton catalysts were synthesized to efficiently remove norfloxacin (NOR). The substitution of Ce remarkably enhanced the catalytic performance of Fe-MIL-101, and the degradation efficiency of NOR (10 mg L⁻¹) increased from 50.1% to 94.8% within 60 min. NOR could be completely degraded by Fe/Ce-MIL-101 after 180 min. Moreover, Fe/Ce-MIL-101 showed excellent stability and reusability in simulated and actual wastewater samples. Density functional theory (DFT) calculations revealed that the introduction of Ce(III) and formation of hetero-coordinated Fe–O–Ce moieties in the secondary building units (SBUs) of Fe-MIL-101 could induce electronic distribution asymmetry, benefit the interaction between the metal sites and H₂O₂, accelerate electron transfer, and further facilitate H₂O₂ activation. The degradation pathways of NOR were identified based on liquid chromatography-mass spectrometry (LC-MS) analysis and Fukui function calculation. Nine benzene ring-containing intermediates were initially detected after 20 min of degradation, and only two byproducts (“harmless” category) were preserved after 180 min. The opening of the piperazine ring and transformation of the quinolone group were mainly caused by the formed hydroxyl free radicals (˙OH). This work demonstrates a new strategy to enhance the performance of Fe-based Fenton-like catalysts by mediating the asymmetrical electronic distribution of coordinated Fe sites.

中文翻译：

Ce介导的Fe-MIL-101对诺氟沙星的增强降解：催化机制、降解途径和在废水处理中的潜在应用

合成了新型 Ce 介导的 Fe-MIL-101 (Fe/Ce-MIL-101) 芬顿催化剂以有效去除诺氟沙星 (NOR)。Ce的取代显着增强了Fe-MIL-101的催化性能，NOR（10 mg L ^-1）的降解效率在60分钟内从50.1%提高到94.8%。180 分钟后 NOR 可以被 Fe/Ce-MIL-101 完全降解。此外，Fe/Ce-MIL-101 在模拟和实际废水样品中表现出优异的稳定性和可重复使用性。密度泛函理论 (DFT) 计算表明，在Fe-MIL-101 的二级构建单元 (SBU) 中引入 Ce( III ) 和形成异配位的 Fe-O-Ce 部分可以引起电子分布不对称，有利于金属位点与 H ₂之间的相互作用O ₂，加速电子转移，进一步促进H ₂ O ₂活化。基于液相色谱-质谱（LC-MS）分析和福井函数计算确定了NOR的降解途径。降解 20 分钟后最初检测到 9 种含苯环的中间体，180 分钟后仅保留了两种副产物（“无害”类别）。哌嗪环的打开和喹诺酮基团的转变主要是由形成的羟基自由基（·OH）引起的。这项工作展示了一种通过调节配位 Fe 位点的不对称电子分布来提高 Fe 基类芬顿催化剂性能的新策略。

更新日期：2021-07-09

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