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利用锐钛矿 F、N 共掺杂 TiO/SiO2 纳米复合材料在可见光下光降解有机水污染物:半工业中试实验和密度泛函理论计算。

Photodegradation of organic water pollutants under visible light using anatase F, N co-doped TiO/SiO nanocomposite: Semi-pilot plant experiment and density functional theory calculations.

机构信息

Department of Natural Resources and Environment, Science and Research Branch, Islamic Azad University, Tehran, Iran.

Research and Development Department, Nanofy Technologies Pte. Ltd., Singapore 048580, Singapore.

出版信息

Chemosphere. 2021 Jul;275:129903. doi: 10.1016/j.chemosphere.2021.129903. Epub 2021 Feb 19.

Abstract

Visible-light driven photocatalysts are of great importance in wastewater treatment. In this work, fluorine and nitrogen co-doped titanium dioxide/silica nanocomposite (F-N-TiO/SiO) was synthetized using a sol-gel approach. The as-developed nanocomposite was well characterized using different techniques. In particular, an anatase structure with high surface area (345.69 m/g) and a band gap of 2.97 eV were observed for the as-synthesized nanocomposite, which makes it a potential candidate for photocatalytic applications under visible light. A systematic density functional theory calculation was performed to get more insight into the effect of dopant atoms on the band gap of TiO nanoparticles. To enhance the reusability of the photocatalyst in semi-pilot scale, the as-developed nanocomposite was immobilized onto the glass beads by coupling dip-coating and heat attachment methods. A semi-pilot scale custom-designed fixed-bed photoreactor was used to evaluate the photocatalytic performance of the as-developed nanocomposite under both visible and solar irradiations. A mixture of three azo dyes (i.e., basic red 29, basic blue 41 and basic yellow 51) was used as the model industrial wastewater. The analysis of the wastewater showed that the complete removal of the pollutants under visible light and sunlight can occurred at pH of 3 and flow rate of 280 mL/min. The durability results demonstrated the successful degradation of the pollutants for five cycles. The results of this study show how careful controlling the operational parameters as well as using a highly photocatalytic nanomaterial can lead to successful decontamination of organic water pollutants. This approach might open up new windows to the future applications of photocatalytic nanomaterials for wastewater treatment.

摘要

可见光驱动的光催化剂在废水处理中具有重要意义。在这项工作中,采用溶胶-凝胶法合成了氟氮共掺杂二氧化钛/二氧化硅纳米复合材料(F-N-TiO/SiO)。采用多种技术对所开发的纳米复合材料进行了充分的表征。特别是,所合成的纳米复合材料具有锐钛矿结构、高比表面积(345.69 m/g)和 2.97 eV 的带隙,使其成为可见光下光催化应用的潜在候选材料。进行了系统的密度泛函理论计算,以更深入地了解掺杂原子对 TiO 纳米粒子带隙的影响。为了提高光催化剂在半中试规模下的可重复使用性,通过偶联浸涂和热附着方法将所开发的纳米复合材料固定在玻璃珠上。使用半中试规模定制设计的固定床光反应器在可见光和太阳光下评估所开发的纳米复合材料的光催化性能。将三种偶氮染料(碱性红 29、碱性蓝 41 和碱性黄 51)的混合物用作模型工业废水。废水分析表明,在 pH 值为 3 和流速为 280 mL/min 的条件下,污染物在可见光和太阳光下可完全去除。耐久性结果表明,污染物在五个循环中成功降解。该研究结果表明,如何仔细控制操作参数以及使用高催化纳米材料可以成功净化有机水污染物。这种方法可能为光催化纳米材料在废水处理中的未来应用开辟新的途径。

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