负载纳米零价铁的铁碳材料制备及其降解抗生素性能研究
Preparation of Iron-carbon Materials Loaded with nano Zero-Valent Iron and their Performance of Degrading Antibiotics
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摘要: 近年来,基于纳米零价铁(nano Zero-Valent Iron,nZVI)的非均相Fenton氧化技术成为了抗生素废水研究领域的热点,但是纳米零价铁易迁移和易团聚的缺点限制了其进一步应用。为了解决该问题,以乙二胺四乙酸(EDTA)和三聚氰胺(MA)为配体,以醋酸亚铁为铁源,采用机械球磨法-高温裂解相结合的方法制备了负载纳米零价铁的铁碳材料,并对其进行表征,以磺胺噻唑(Sulphaphenazole,STZ)为目标污染物,考察铁碳材料降解磺胺噻唑的影响因素,探究作用机制。表征结果表明,醋酸亚铁@乙二胺四乙酸(Fe@EDTA)材料中的纳米铁粒子的直径约为4 nm,在在碳层中均匀分布,这种结构使得材料具有较强的催化能力,而醋酸亚铁@三聚氰胺(Fe@MA)材料中的纳米零价铁则聚集成直径约为400 nm的大颗粒,被100 nm碳层包覆。Fe@EDTA材料的最佳铁碳比为2:1,材料的最佳铁碳比为3:1,最佳实验条件为初始pH为3,初始H2O2浓度为15 mM或25 mM,催化剂投加量为0.1 g/L或0.2 g/L,污染物浓度为10 mg/L或20 mg/L;磺胺噻唑的降解以及羟基自由基的产生均符合伪一级动力学模型;Fe@EDTA材料具有较好的重复利用性和稳定性,五次重复实验后,污染物的降解率仍高达82%。探讨了降解STZ的机理,铁碳材料与过氧化氢(Fe@C-H2O2)的非均相芬顿体系的机理是纳米零价铁诱导的类芬顿氧化,其中羟基自由基(∙OH)和超氧自由基(∙O2-)在氧化降解有机污染物过程中起到关键作用。Abstract:Abstract: In recent years, heterogeneous Fenton oxidation technology based on nano Zero-Valent Iron (nZVI) has become a hot topic in the field of antibiotic wastewater research. However, the disadvantages of nZVI's easy migration and agglomeration limit its further application. In order to solve this problem, iron-carbon nanoloaded zero-valent iron materials were prepared using ethylenediamine tetraacetic acid (EDTA) and melamine (MA) as ligands and ferrous acetate as iron source by a combination of mechanical ball milling and pyrolysis, and characterized by Sulphaphenazole (STZ) as the target contaminant. The influencing factors and mechanism of sulfathiazole degradation by iron carbon materials were investigated. Characterization results show that the acetic acid ferrous@ethylenediamine tetraacetic acid (Fe@EDTA) of the nano particle diameter of about 4 nm, the uniform distribution in the carbon layer, this structure makes material has stronger catalytic ability, and the nZVI in ferrous acetate@melamine (Fe@MA) aggregates into large particles with a diameter of about 400 nm and is coated with a carbon layer of 100 nm. The best Fe/C ratio of Fe@EDTA material is 2:1, the best Fe/C ratio of the material is 3:1, the best experimental conditions are the initial pH is 3, the initial H2O2 concentration is 15 mM or 25 mM, the catalyst dosage is 0.1 g/L or 0.2 g/L, the pollutant concentration is 10 mg/L or 20 mg/L; The degradation of sulfathiazole and the production of hydroxyl radical were in accordance with the pseudo-first-order kinetic model. Fe@EDTA material has good reusability and stability. After five repeated experiments, the degradation rate of pollutants is still up to 82%. The reusability and stability of Fe@MA materials are relatively general, and the degradation rates of pollutants in the fourth and fifth repeated experiments are about 52% and 48%. The mechanism of degradation of STZ was discussed. The mechanism of heterogeneous Fenton system between iron carbon materials and hydrogen peroxide (Fe@C-H2O2) was fenton-like oxidation induced by nanometer zero-valent iron, in which hydroxyl radical (∙OH) and superoxide radical (∙O2-) played a key role in the oxidative degradation of organic pollutants.
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Key words:
- Fenton-like /
- nano Zero-Valent Iron /
- sulfathiazole
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