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负载于玻璃载体上的FeO/TiO₂光催化活化过硫酸盐或羟基自由基去除阿莫西林:机理、转化产物及毒性评估

Visible-Light Activation of Persulfate or HO by FeO/TiO Immobilized on Glass Support for Photocatalytic Removal of Amoxicillin: Mechanism, Transformation Products, and Toxicity Assessment.

作者信息

Dela Rosa Francis M, Popović Marin, Papac Zjačić Josipa, Radić Gabrijela, Kraljić Roković Marijana, Kovačić Marin, Farré María José, Genorio Boštjan, Lavrenčič Štangar Urška, Kušić Hrvoje, Lončarić Božić Ana, Petrović Mira

机构信息

Faculty of Chemical Engineering and Technology, University of Zagreb, Marulićev trg 19, 10000 Zagreb, Croatia.

Catalan Institute for Water Research (ICRA), C/Emili Grahit, 101, 17003 Girona, Spain.

出版信息

Nanomaterials (Basel). 2022 Dec 5;12(23):4328. doi: 10.3390/nano12234328.

DOI:10.3390/nano12234328
PMID:36500951
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9738309/
Abstract

FeO/TiO nanocomposites were fabricated via a facile impregnation/calcination technique employing different amounts iron (III) nitrate onto commercial TiO (P25 Aeroxide). The as-prepared FeO/TiO nanocomposites were characterized by X-ray diffraction (XRD), Raman spectroscopy (RS), scanning electron microscopy/energy-dispersive spectroscopy (SEM/EDXS), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller analysis (BET), electron impedance spectroscopy (EIS), photoluminescence spectroscopy (PL), and diffuse reflectance spectroscopy (DRS). As a result, 5% () FeO/TiO achieved the highest photocatalytic activity in the slurry system and was successfully immobilized on glass support. Photocatalytic activity under visible-light irradiation was assessed by treating pharmaceutical amoxicillin (AMX) in the presence and absence of additional oxidants: hydrogen peroxide (HO) and persulfate salts (PS). The influence of pH and PS concentration on AMX conversion rate was established by means of statistical planning and response surface modeling. Results revealed optimum conditions of [SO] = 1.873 mM and pH = 4.808; these were also utilized in presence of HO instead of PS in long-term tests. The fastest AMX conversion possessing a zero-order rate constant of 1.51 × 10 M·min was achieved with the photocatalysis + PS system. The AMX conversion pathway was established, and the evolution/conversion of formed intermediates was correlated with the changes in toxicity toward . Reactive oxygen species (ROS) scavenging was also utilized to investigate the AMX conversion mechanism, revealing the major contribution of photogenerated in all processes.

摘要

通过一种简便的浸渍/煅烧技术,将不同量的硝酸铁(III)负载到商用二氧化钛(P25 型气相二氧化钛)上,制备了 FeO/TiO 纳米复合材料。采用 X 射线衍射(XRD)、拉曼光谱(RS)、扫描电子显微镜/能谱分析(SEM/EDXS)、X 射线光电子能谱(XPS)、布鲁诺尔-埃米特-泰勒分析(BET)、电子阻抗谱(EIS)、光致发光光谱(PL)和漫反射光谱(DRS)对所制备的 FeO/TiO 纳米复合材料进行了表征。结果表明,5%()的 FeO/TiO 在悬浮体系中具有最高的光催化活性,并成功地固定在玻璃载体上。通过在有和没有额外氧化剂(过氧化氢(HO)和过硫酸盐(PS))存在的情况下处理药物阿莫西林(AMX),评估了可见光照射下的光催化活性。通过统计规划和响应面建模确定了 pH 和 PS 浓度对 AMX 转化率的影响。结果显示最佳条件为[SO] = 1.873 mM 和 pH = 4.808;在长期试验中,在存在 HO 而非 PS 的情况下也采用了这些条件。光催化 + PS 体系实现了最快的 AMX 转化,零级速率常数为 1.51 × 10 M·min。确定了 AMX 的转化途径,并将形成的中间体的演变/转化与对的毒性变化相关联。还利用活性氧(ROS)清除来研究 AMX 的转化机制,揭示了光生在所有过程中的主要贡献。

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