Ag-Y/MIL-101吸附剂的制备及其吸附脱硫性能

通过银、钇双金属改性制备了Ag-Y/MIL-101吸附剂,并对Ag-Y/MIL-101进行了X射线衍射(XRD)、电镜(SEMEDS)、比表面积(BET)和热重(TG-DTG)表征。考察了Ag-Y/M IL-101金属负载顺序、金属负载浓度、金属溶液用量、负载时间对脱硫性能的影响,优化了吸附脱硫条件。结果表明,金属改性得到的Ag-Y/MIL-101保持了MIL-101的晶格结构。与M IL-101相比,Ag-Y/MIL-101的比表面积和孔容均有所下降。适宜Ag-Y/MIL-101的制备条件为:先负载银后负载钇,银离子和钇离子的负载浓度均为30 mmol/L,金属溶液用量均为1 mL,负载时间为8 h。适宜Ag-Y/MIL-101的吸附脱硫条件为:吸附剂用量0.05 g,模拟油为10 mL,吸附温度为60℃,吸附时间为8 h。在此条件下,Ag-Y/MIL-101对噻吩的吸附量达到21.7 mg/g。Ag能显著提高MIL-101的吸附硫容,Y能显著提高MIL-101的吸附选择性,因此,Ag-Y/MIL-101吸附剂中Ag和Y的协同作用使其拥有比MIL-101更高的硫容和噻吩脱硫选择性。

Preparation of Ag and Y loaded metal-organic framework Ag-Y/MIL-101 and its adsorption desulfurization performance

The Ag-Y/MIL-101 adsorbents were successfully prepared via loading Ag and Y onto MIL-101. The adsorbents were characterized by XRD, SEM-EDS, BET and TG-DTG methods. The effects of the loading order and concentrations of metals, the amount of AgNO₃ solution and Y(NO₃)₃ solution, and the loading residence time on adsorptive removal performance of thiophene were studied. The conditions of adsorptive desufurization were also optimized. The results show that the lattice structure of MIL-101 remains after the introduction of metals. Compared with MIL-101, the specific surface area and pore volume of Ag-Y/MIL-101 decrease. The optimal preparation conditions of Ag-Y/MIL-101 adsorbent are to load Ag first and then Y with 30 mmol/L of both the loading concentrations of Ag and Y ion, 1 mL of both the dosages of AgNO₃ solution and Y(NO₃)₃ solution, and 8 h of the loading residence time. The optimal desulfurization conditions are 10 mL of model oil, 0.05 g of Ag-Y/MIL-101 dosage, the adsorption temperature of 60℃, and the adsorption time of 8 h. At these conditions, the thiophene desulfurization capacity over Ag-Y/MIL-101 reaches 21.7 mg/g. The Ag can significantly improve the adsorption sulfur capacity of MIL-101, and Y can significantly improve the adsorption selectivity of MIL-101. Therefore, the synergistic effect of Ag and Y in Ag-Y/MIL-101 adsorbent makes it have higher sulfur capacity and thiophene desulfurization selectivity than MIL-101.