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首页> 外文期刊>Fuel >Synthesis of two-dimensional TiO_2@multi-walled carbon nanotube nanocomposites as smart nanocatalyst for ultra-deep oxidative desulfurization of liquid fuel: Optimization via response surface methodology
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Synthesis of two-dimensional TiO_2@multi-walled carbon nanotube nanocomposites as smart nanocatalyst for ultra-deep oxidative desulfurization of liquid fuel: Optimization via response surface methodology

机译:二维TiO_2的合成二壁碳纳米管纳米复合材料作为液体燃料超深氧化脱硫的智能纳米催化剂:通过响应面方法优化

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The novel heterogeneous catalysts of 2D-TiO2@MWCNT nanocomposites are designed and synthesized via grafting TiO2 nanoparticles onto functionalized multi-walled carbon nanotubes and used for oxidative desulfurization of dibenzothiophene and real straight run light gas oil. The 2D-TiO2@MWCNT nanocomposite catalysts are completely characterized by FT-IR, Raman spectroscopy, XRD, TEM, NH3-TPD, ICP, and N-2 adsorption-desorption isotherms. At first, the effect of various loading Ti on the MWCNT for ODS efficiency was investigated. The results revealed that 2D-0.6TiO(2)@MWCNT had the highest sulfur removal for the model, and SRLGO fuel compared to the other catalyst. Then, the optimal design of experiments using Box-Behnken experimental design was used to evaluate the effects of individual process variables such as temperature, O/S molar ratio, time, catalyst dosage, and their optimum values were found to be 69 degrees C, 46 min(-1), O/S molar ratio: 9, and 0.03 g cat (25 ml DBT model fuel with 500 ppm S or 25 ml SRLGO with 12500 ppm S, 25 ml of acetonitrile), to achieve a high removal sulfur efficiency for DBT model oil (100%) and SRLGO (97.5 %), respectively. Based on optimal conditions, the 2D-0.6TiO(2)@MWCNT catalyst possesses superior catalytic activity and excellent reusability. The desulfurization reaction could be recycled for at least nine cycles without considerable reduction of catalytic performance, showing the good stability of the nanocomposite catalysts. An empirical kinetic model was applied to explain the rate data. Also, 2D-0.6TiO(2)@MWCNT nanocomposite catalyst had the lowest activation energy (27.65 Kj.mol(-1)) with the highest turnover frequency (16.15 h(-1), around 2-3 times of the best catalyst so far) in desulfurization reactions compared to any TiO2-based catalysts. Furthermore, the catalytic reaction mechanism is investigated.
机译:通过将TiO2纳米颗粒移植到官能化的多壁碳纳米管上,设计和合成了2D-TiO 2的新型异质催化剂,并用于官能化的多壁碳纳米管并用于二苯并噻吩和真正的直流轻质气体油的氧化脱硫。 2D-TiO 2 @ MWCNT纳米复合催化剂的特征在于FT-IR,拉曼光谱,XRD,TEM,NH 3-TPD,ICP和N-2吸附 - 解吸等温线。首先,研究了各种装载Ti对ODS效率MWCNT的影响。结果表明,与其他催化剂相比,2D-0.6TiO(2)〜0.6TiO(2)〜MWCNT最高的硫去除和SRLGO燃料。然后,使用Box-Behnken实验设计的实验的最佳设计来评估各个过程变量如温度,O / S摩尔比,时间,催化剂剂量,以及它们的最佳值,以及它们的最佳值为69℃, 46分钟(-1),O / S摩尔比率:9和0.03g Cat(25ml DBT模型燃料,500ppm S或25ml Srlgo,具有12500ppm s,25ml乙腈),以实现高脱硫硫DBT模型油(100%)和SRLGO(97.5%)的效率。基于最佳条件,2D-0.6TiO(2)〜MWCNT催化剂具有优异的催化活性和优异的可重用性。脱硫反应可以再循环至少9个循环,而无需大大降低催化性能,显示纳米复合催化剂的良好稳定性。应用经验动力学模型来解释速率数据。此外,2D-0.6TiO(2)【MWWNT纳米复合催化剂】具有最低的活化能量(27.65 kJ.mol(-1)),其周转频率最高(16.15小时(-1(-1),最佳催化剂的2-3次到目前为止)与基于TiO 2的催化剂相比,脱硫反应。此外,研究了催化反应机理。

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