首页> 中文期刊> 《燃料化学学报》 >杂原子介孔 Ce-MCM-41分子筛的制备及其吸附脱除甲硫醚性能

杂原子介孔 Ce-MCM-41分子筛的制备及其吸附脱除甲硫醚性能

         

摘要

Heteroatomic mesoporous Ce-MCM-41 molecular sieve was synthesized by using hydrothermal synthesis method with cetyltrimethy ammoniumb romide (CTMABr) as template, cerium chloride as cerium source and sodium silicate as silica source.X-ray diffraction ( XRD) and infrared sp ectru m (FT-IR) re sults indicate that the well-orde red meso-porous structure was obtained when the Ce/Si mol ar ratioi s less than 0.04;Ce was incorporat ed intot he fra mework of MCM-41.Nitrogen physisorption measurements indicate that the average pore diameters of MCM-41 and Ce-MCM-41 are 2.82 and 2.46 nm, with pore vo lumes of 0.762 1 and 0.689 4 m3 /g and BE T surface areas of 986.42 and756 .8 m2 /g , respectively.Dimethy l sulfide with a moleculars ize of 0.464 8 nm can easily enter the meso-scale pores of MCM-41 and Ce-MCM-41.NH3-TPD results illustrate that the acidity of Ce-MCM-41 is stronger than that of MCM-41.As a result, for the adsorptive removal of dimethyl sulfide from nitrogen with a dimethyl sulfide content of58 μg/g, the desulfurization capacity of Ce-MCM-41 is 7.52 mg(S) /g, h igher than that of MCM-41 (4.57 mg(S) /g).Furthermore, both MCM-41 and Ce-MCM-41 molecular sieves could be easily regenerated after adsorption of dimethyl sulfide; the desulfurization capacity can be recovered up to 80% of the original capacity after regenerated for three times.%以十六烷基三甲基溴化铵为模板剂,正硅酸乙酯(TEOS)为硅源,硝酸铈为铈源,采用水热法合成了杂原子介孔分子筛 Ce-MCM-41。 XRD和 FT-IR 表征结果表明,当加入的 Ce/Si 物质的量比小于0.04时合成了规整有序的介孔结构,并将 Ce原子引入到 MCM-41骨架中。 N2吸附-脱附测试获得 MCM-41和 Ce-MCM-41(Ce/Si 物质的量比为0.04)的平均孔径分别为2.82和2.46 nm,孔容分别为0.762 1和 0.6894 m3/g,BET 比表面积分别为986.42和 756.8 m2/g。 NH3-TPD 表征结果表明, Ce-MCM-41的酸性要明显强于 MCM-41,但两种分子筛的酸性均较弱。利用合成的 MCM-41和 Ce-MCM-41吸附脱除甲硫醚浓度为58μg(甲硫醚)/g 的甲硫醚/氮气混合气中的甲硫醚。甲硫醚分子尺寸的模拟结果为0.4648 nm,可以很容易地进入分子筛的介孔孔道中。由于C e-MCM-41分子筛具有较多的酸量,其硫吸附容量7.52 mg(S)/g 明显高于 MCM-41的4.57 mg(S)/g。 MCM-41和 Ce-MCM-41都具有较好的再生性能,再生3次后硫吸附容量仍可恢复到初始容量的80%,分别为3.52和 5.86 mg(S)/g。

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