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首页> 外文期刊>Environmental research >Controlled formation of magnetic yolk-shell structures with enhanced catalytic activity for removal of acetaminophen in a heterogeneous fenton-like system
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Controlled formation of magnetic yolk-shell structures with enhanced catalytic activity for removal of acetaminophen in a heterogeneous fenton-like system

机译：具有增强催化活性的磁性蛋黄壳结构的控制形成，用于在异质芬顿的系统中除去乙酰氨基酚

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Encapsulating magnetic nanoparticles in a silica shell is a promising approach in many research fields. We recently demonstrated that the magnetic yolk-shell structure of Fe3O4@SiO2, which consists of an inner magnetite core and outer silica shell separated by a hollow void space, and its modified counterparts can be used as an effective catalyst for removal of acetaminophen in a heterogeneous Fenton-like reaction. The present study develops this approach further in an effort to design an effective procedure for preparing an optimum yolk-shell structure capable of greater catalytic performance. We investigated the use of a controlled synthesis strategy to fabricate an Fe3O4@SiO2 yolk-shell structure under varying conditions. Our focus was a single-step process that examines the effects of Stober solution temperature, tetraethyl orthosilicate (TEOS) and hexadecyltrimethylammonium bromide (CTAB) concentrations, ethanol and water volume ratio, incubation time, and temperature on Fe3O4@SiO2 textural morphologies. The catalytic performance of the prepared materials was evaluated through oxidative degradation of acetaminophen in a heterogeneous Fenton-like reaction. Field emission transmission electron microscopy observation showed that magnetic yolk-shell structures with appropriate diameter, shell thickness, and hollow void space could be generated through tight control of synthesis conditions. Particle size and hollow void space increased when TEOS concentration increased from 22.10 to 88.50 mM. Hollow void space also increased as incubation time increased from 24 h to 72 h or incubation temperature increased from 50 to 90 degrees C. However, a yolk-shell structure did not form at a TEOS concentration of 11.10 mM, an incubation time of 3 h, or with an inappropriate ratio of ethyl alcohol and deionized water. Catalytic activity for degradation of acetaminophen increased with increasing hollow void space and thinning silica shell. In addition, the selected appropriate materials exhibited effective catalytic performance over five cycles of regeneration. This study demonstrates the significance of controlling the formation of yolk-shell structures, which enabled us to produce Fe3O4@SiO2 yolk-shell structures of desired and predictable size, hollow void space volume, and shell thickness for higher catalytic performance in degradation of pharmaceuticals in heterogeneous Fenton-like systems.
机译：在二氧化硅壳中封装磁性纳米颗粒是许多研究领域的有希望的方法。我们最近证明，由中空空隙空间分离的内磁铁矿芯和外二氧化硅壳组成的Fe3O4 @ SiO 2的磁性蛋黄壳结构，其改性对应物可用作除去乙酰氨基酚的有效催化剂异质的FENTON样反应。本研究进一步开发了这种方法，旨在设计一种用于制备能够更大的催化性能的最佳蛋黄壳结构的有效方法。我们调查了使用受控的合成策略在不同条件下制造Fe3O4 @ SiO2蛋黄结构。我们的重点是一种单步过程，检查STOB溶液温度，四乙基异硅酸盐（TEOS）和十六烷基三甲基溴化铵（CTAB）浓度，乙醇和水体积比，孵育时间和温度对Fe3O4造影形态的影响。通过在异质的Fenton样反应中的乙酰氨基酚的氧化降解来评价制备的材料的催化性能。场发射透射电子显微镜观察显示，通过对合成条件的紧密控制，可以产生具有适当直径，壳体厚度和中空空隙空间的磁性蛋黄壳结构。当TEOS浓度从22.10增加到88.50mm时，粒度和中空空隙空间增加。由于孵育时间从24小时增加到72小时或孵育温度从50至90℃增加，中空空隙空间也增加了，但是，蛋黄壳结构没有以11.10mm的TEOS浓度形成，孵育时间为3小时，或用乙醇和去离子水的不恰当的比例。随着中空空隙空间和稀释二氧化硅壳，乙酰乙酰氨基酚降解的催化活性增加。此外，所选择的适当材料表现出超过5个再生循环的有效催化性能。本研究证明了控制蛋黄壳结构的形成的重要性，这使我们能够生产所需和可预测尺寸，中空空隙空间体积和壳体厚度的Fe3O4 @ SiO2蛋白壳结构，以便在药物的降解中进行更高的催化性能。异质的Fenton样系统。

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