Desulphurization of Simulated Oil Using SAPO-11 with CNT's as Adsorbent: A Kinetic Study

Gaith K. Jabaar, Hayder A. Al-Jendeel, Yasir Ali Alsheikh
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Abstract

In this study, sulfur was removed from imitation oil using oxidative desulfurization process. Silicoaluminophosphate (SAPO-11) was prepared using the hydrothermal method with a concentration of carbon nanotubes (CNT) of 0% and 7.5% at 190 °C crystallization temperature. The final molar composition of the as-prepared SAPO-11 was Al2O3: 0.93P2O5: 0.414SiO2. 4% MO/SAPO-11 was prepared using impregnation methods. The produced SAPO-11 was described using X-ray diffraction (XRD) and Brunauer-Emmet-Teller (N2 adsorption–desorption isotherms). It was found that the addition of CNT increased the crystallinity of SAPO-11. The results showed that the surface area of SAPO-11 containing 7.5% CNT was 179.54 m2/g, and the pore volume was 0.317 cm3/g. However, the surface area of SAPO-11 containing 0% CNT was 125.311 m2/g, and pore volume was 0.275 cm3/g, while nanoparticles with an average particle diameter of 24.8 nm were obtained. Then, the prepared SAPO-11 was used in the oxidative desulfurization process. The oxidative desulfurization was studied using several factors affecting desulfurization efficiency, such as time (40, 60, 80, 100, and 120) min, amount of MO/SAPO-11 (0.3, 0.4, 0.5, 0.6, and 0.7) g/100 ml of simulated oil (100 ppm of dibenzothiophene), the amount of hydrogen peroxide (4ml) oxidizer/100 ml of simulated oil, and the temperature ranges from (40, 50, 60, 70, and 80 °C). The results showed that an increase in MO/SAPO-11 led to an increase in desulfurization. The best removal percentage for sulfur content was 92.79%, obtained at 70 °C and 0.6 g of MO/SAPO-11 containing 7.5% CNT, and the removal was 82.34% at 0% CNT and the same other conditions. While the equilibrium was achieved after 100 min. The results revealed that Freundlich's model described the adsorption of sulfur compounds better than Langmuir's, where the R2 of the Freundlich model was 0.9979 and the R2 of the Langmuir model was 0.9554.
碳纳米管吸附剂SAPO-11对模拟油的脱硫动力学研究
本研究采用氧化脱硫法对模拟油中的硫进行脱除。采用水热法制备了磷酸硅铝(SAPO-11),碳纳米管(CNT)浓度分别为0%和7.5%,结晶温度为190℃。制备的SAPO-11的最终摩尔组成为Al2O3: 0.93P2O5: 0.414SiO2。采用浸渍法制备了4% MO/SAPO-11。利用x射线衍射(XRD)和Brunauer-Emmet-Teller (N2吸附-解吸等温线)对合成的SAPO-11进行了表征。结果表明,碳纳米管的加入提高了SAPO-11的结晶度。结果表明:含7.5%碳纳米管的SAPO-11的比表面积为179.54 m2/g,孔体积为0.317 cm3/g;而含0%碳纳米管的SAPO-11的比表面积为125.311 m2/g,孔体积为0.275 cm3/g,得到的纳米颗粒平均粒径为24.8 nm。然后将制备的SAPO-11用于氧化脱硫工艺。采用时间(40、60、80、100、120)min、MO/SAPO-11用量(0.3、0.4、0.5、0.6、0.7)g/100 ml模拟油(100 ppm二苯并噻吩)、过氧化氢用量(4ml)氧化剂/100 ml模拟油、温度范围(40、50、60、70、80℃)等因素对氧化脱硫效果进行了研究。结果表明,MO/SAPO-11含量的增加导致脱硫率的提高。在70°C和0.6 g含7.5%碳纳米管的MO/SAPO-11条件下,硫含量的去除率为92.79%,在0%碳纳米管和相同条件下,硫含量的去除率为82.34%。结果表明,Freundlich模型的R2为0.9979,Langmuir模型的R2为0.9554,Freundlich模型比Langmuir模型更好地描述了含硫化合物的吸附。
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