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在优化条件下超声合成用于降解和矿化双氯芬酸的太阳光响应型S-N-C-三掺杂TiO光催化剂。

Sono-synthesis of solar light responsive S-N-C-tri doped TiO photo-catalyst under optimized conditions for degradation and mineralization of Diclofenac.

作者信息

Ramandi Sara, Entezari Mohammad H, Ghows Narjes

机构信息

Sonochemical Research Center, Department of Chemistry, Ferdowsi University of Mashhad, 91779 Mashhad, Iran.

Sonochemical Research Center, Department of Chemistry, Ferdowsi University of Mashhad, 91779 Mashhad, Iran; Environmental Chemistry Research Center, Department of Chemistry, Ferdowsi University of Mashhad, 91779 Mashhad, Iran.

出版信息

Ultrason Sonochem. 2017 Sep;38:234-245. doi: 10.1016/j.ultsonch.2017.03.008. Epub 2017 Mar 7.

DOI:10.1016/j.ultsonch.2017.03.008
PMID:28633823
Abstract

C-N-S-tri doped TiO anatase phase was synthesized using a facile, effective and novel sonochemical method at low frequency (20kHz) and at room temperature. Titanium butoxide as the titanium precursor and thiourea as the dopant source were used in the synthesis of the photo-catalyst. The effects of important parameters such as thiourea/Ti molar ratio, ultrasound intensity, sonication time and temperature were studied on the synthesis of tri-doped TiO. The XPS results confirmed the presence of N, S, and C in the photo-catalyst. The photo-catalytic efficiency of the synthesized catalyst was studied toward the removal of Diclofenac as a model pharmaceutical organic pollutant. The results confirmed that the photo-catalyst synthesized with narrower band gap energy, shorter sonication time and higher ultrasound intensity leads to a rapid removal of Diclofenac. The effect of operational variables on the photo-catalytic activity of C-N-S tri doped TiO nanoparticles was studied and optimized using the Taguchi method as a statistical technique. Additionally, the degradation process followed the pseudo-first-order kinetics model and the highest apparent rate constant of 0.0632min achieved in 90min. Chemical oxygen demand (COD) analysis confirmed that the mineralization took place completely (100%) under the optimized conditions in 180min. Different scavengers were applied during the degradation process and active species such as OH and O had key roles in the photo-catalytic process.

摘要

采用简便、有效且新颖的低频(20kHz)室温声化学方法合成了C-N-S三掺杂二氧化钛锐钛矿相。以丁醇钛作为钛前驱体,硫脲作为掺杂剂源来合成光催化剂。研究了硫脲/钛摩尔比、超声强度、超声处理时间和温度等重要参数对三掺杂二氧化钛合成的影响。X射线光电子能谱(XPS)结果证实了光催化剂中存在氮、硫和碳。以双氯芬酸作为典型的医药有机污染物,研究了合成催化剂对其的光催化去除效率。结果证实,具有较窄带隙能量、较短超声处理时间和较高超声强度合成的光催化剂能快速去除双氯芬酸。采用田口方法作为一种统计技术,研究并优化了操作变量对C-N-S三掺杂二氧化钛纳米颗粒光催化活性的影响。此外,降解过程遵循准一级动力学模型,在90分钟内达到的最高表观速率常数为0.0632min⁻¹。化学需氧量(COD)分析证实,在优化条件下180分钟内完全发生了矿化(100%)。在降解过程中应用了不同的清除剂,羟基自由基(·OH)和超氧阴离子自由基(O₂⁻)等活性物种在光催化过程中起关键作用。

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