机构地区: 华南理工大学化学与化工学院
出 处: 《华南理工大学学报(自然科学版)》 2013年第12期24-28,42,共6页
摘 要: 采用重量法测定了298、303、308、313 K下CH4、CO2在MIL-101多孔材料上的吸附等温线,估算了MIL-101对CH4、CO2的等量吸附热,并利用DL-IAST模型计算出不同温度下CH4/CO2混合气中各组分的吸附分量,探讨了CO2的吸附选择性.结果表明:298 K、2500 kPa时,CO2在MIL-101上的吸附量为14.51 mmol/g,远高于同等条件下商业活性炭、沸石和分子筛对CO2的吸附容量;CH4、CO2在MIL-101上的吸附等温线与Double-Langmuir模型吻合很好,说明该吸附主要为双孔位吸附;CO2在MIL-101上的等量吸附热在19.3~25.5kJ/mol范围内;与CH4相比,CO2在MIL-101上的表面自由结合能更高;298K、250kPa时,MIL-101对CO2的吸附选择性指数为5.6;随着压力的增大,CO2的吸附选择性逐渐减小;随着混合气中CO2浓度的下降,CO2的吸附选择性上升. In this paper,the adsorption isotherms of CH4 and CO2 on MIL-101 were obtained by means of the gravi-metric method at 298,303,308 and 313 K,and the corresponding isosteric adsorption heat was estimated.Then, the pure gas adsorption was calculated by using the DL-IAST model,and the adsorption selectivity of CO2 on MIL-101 was discussed.The results show that (1)the adsorption capacity of pure CO2 on MIL-101 is up to 14.51 mmol/g at 298 K and 2500 kPa,which is much higher than that on activated carbon,zeolite and molecular sieve under similar conditions;(2)the isotherms of pure CO2 and CH4 well accord with the Double-Langmuir model,which shows the presence of two adsorption sites;(3)the isosteric adsorption heat of CO2 on MIL-101 ranges from 19.3 to 25.5 kJ/mol;(4)as compared with CH4,CO2 is of higher surface free energy for its interaction with the framework of MIL-101;(5)the adsorption selectivity index of CO2 over CH4 on MIL-101 is up to 5.6 at 298 K and 250 kPa;and (6)the adsorption selectivity of CO2 over CH4 gradually decreases with the increase of pressure and the concentration of CO2 in CH4/CO2 mixture.