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AgY吸附剂的制备及其吸附脱硫性能的研究

Study on Preparation of AgY Zeolites and Its Adsorptive Desulfurization Performance

【作者】 孙兴龙

【导师】 宋华;

【作者基本信息】 东北石油大学 , 化学工艺, 2011, 硕士

【摘要】 本文研究了AgY吸附剂吸附脱硫技术,考察了不同因素对脱硫效果的影响,找出了适宜的脱硫条件,并考察了含氮化合物和芳香族化合物的竞争吸附以及吸附脱硫过程的动力学模型进行了初步的探索。在液相离子交换法制备的AgYIE吸附剂吸附脱硫实验中,以噻吩/石油醚体系为模型化合物,考察了各因素对脱硫效果的影响,结果表明,⑴离子交换液浓度为0.25 mol/L、交换液用量为20 mL、离子交换时间为24 h、焙烧温度为500℃、吸附温度40℃、吸附时间30 min、吸附剂质量/原料油体积(g/mL)为1:40时,脱硫效果最好,脱硫率为93.81%;⑵40℃时,静态平衡吸附硫容为0.8523 mmol/g;利用固定床进行动态吸附,在环境温度压力下,流速为0.5 mL/min时,测得饱和吸附硫容为1.2188 mmol/g;⑶噻吩在AgYIE上的吸附动力学符合准二级速率方程,平衡吸附容量q2=181.83 mg/g,初始吸附速率k2=0.015 g/(mg·min);⑷含氮化合物或芳香族化合物竞争吸附对模拟油的脱硫率有很大的影响并且氮化物的影响比芳香烃化合物的影响更大。在微波辅助液相离子交换法制备的AgYMW吸附剂吸附脱硫实验中,以噻吩/石油醚体系为模型化合物,考察了各因素对脱硫效果的影响,结果表明,⑴离子交换液浓度为0.2 mol/L、微波功率为240 W、微波照射时间为20 min、焙烧温度为500℃、吸附温度40℃、吸附时间30 min、吸附剂质量/原料油体积(g/mL)为1:40时,脱硫效果最好,脱硫率为90.28%;⑵40℃时,静态平衡吸附硫容为0.7970 mmol/g;利用固定床进行动态吸附,在环境温度压力下流速为0.5 mL/min时测得饱和吸附硫容为1.0938 mmol/g;⑶噻吩在AgYMW上的吸附动力学符合准二级速率方程,吸附剂的平衡吸附容量q2=170.03 mg/g和初始吸附速率k2=0.018 g/(mg·min);⑷含氮化合物或芳香族化合物竞争吸附对模拟油的脱硫率有很大的影响并且氮化物的影响比芳香烃化合物的影响更大。

【Abstract】 The adsorptive desulfurization technology of AgY zeolite were researched in this article. The effects of different factors on the desulfurization were studied and proper desulfurization conditions were found out. At the same time the competition adsorptive of nitrogen compounds and aromatic compound were studied and the adsorptive desulfurization process kinetic model had a prelinibary exploration.The experiment of adsorptive desulfurization, AgYIE zeolite was prepared by ion exchange method. The effects of different factors on desulfurization with the thiophene/petroleumether model oil as feedstock were investigated. The result shows that the AgY zeolite with AgNO3 solution concentration of 0.25 mol/L and dosage of 20 mL, ion exchange time of 24 h and calcination temperature of 500℃exhibited the best desulfurization performance. Under the conditions of thiophene/petroleumether model oil 10 mL, adsorbents 0.2 g, adsorptive temperature 40℃, adsorptive time 30 min, the highest desulfurization rate is 93.81% and the static saturated equilibrium sulfur adsorption capacity was 0.8523 mmol/g. The dynamic saturated adsorption capacities of AgY zeolite was 1.2188 mmol/g at ambient temperature and pressure. Kinetics of adsorptive desulfurization over AgY zeolites meet the pesudo-second order model with the equilibrium adsorption capacity q2=181.83 mg/g and the initial adsorption rate k2=0.015 g/(mg·min). The competition absorptive of nitrogen compounds and aromatic compound have greet influence on absorptive desulfurization and nitrogen compounds has more influence than aromatic compound.The experiment of adsorptive desulfurization, AgYMW zeolite was prepared by microwave assist ion exchange method. The effects of different factors on desulfurization with the thiophene/petroleumether model oil as feedstock were investigated. The result shows that the AgY zeolite with AgNO3 solution concentration of 0.2 mol/L, microwave power of 240 W, microwave irradiation time of 20 min as well as calcined at 500℃was found to be optimal. Under the conditions of thiophene/petroleumether model oil 10 ml, adsorbents 0.2 g, adsorptive temperature 40℃, adsorptive time 30 min, the highest desulfurization rate is 90.28% and the static saturated equilibrium sulfur adsorption capacity was 0.7970 mmol/g. The dynamic saturated adsorption capacities of AgY zeolite was 1.0938 mmol/g at ambient temperature and pressure. Kinetics of adsorptive desulfurization over AgY zeolites meet the pesudo-second order model with the equilibrium adsorption capacity q2=170.03 mg/g and the initial adsorption rate k2=0.018 g/(mg·min). The competition absorptive of nitrogen compounds and aromatic compound have greet influence on absorptive desulfurization and nitrogen compounds has more influence than aromatic compound.

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