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

洪新; 唐克

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

洪新,
唐克

辽宁工业大学化学与环境工程学院, 辽宁锦州 121001

基金项目: 辽宁省自然科学基金(2014020113);辽宁省高等学校优秀人才支持计划(LJQ2012057);辽宁工业大学教师启动资金(X201311)。

详细信息

通讯作者:
唐克, Tel:86-416-4198019, Fax:86-416-4198019, E-mail:tangke0001@163.com。

中图分类号: X743
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出版历程
- 收稿日期: 2014-10-31
- 刊出日期: 2015-04-30

Preparation of heteroatomic mesoporous Ce-MCM-41 molecular sieve and its performance in the adsorptive removal of dimethyl sulfide

HONG Xin,
TANG Ke

School of Chemical and Environmental Engineering, Liaoning University of Technology, Jinzhou 121001, China

摘要

摘要: 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 0.689 4 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58 μg(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0.464 8 nm,可以很容易地进入分子筛的介孔孔道中。由于Ce-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。
- 甲硫醚 /
- 分子筛 /
- Ce-MCM-41 /
- 分子模拟 /
- 吸附 /
- 脱硫
Abstract: Heteroatomic mesoporous Ce-MCM-41 molecular sieve was synthesized by using hydrothermal synthesis method with cetyltrimethy ammonium bromide (CTMABr) as template, cerium chloride as cerium source and sodium silicate as silica source. X-ray diffraction (XRD) and infrared spectrum (FT-IR) results indicate that the well-ordered meso-porous structure was obtained when the Ce/Si molar ratio is less than 0.04; Ce was incorporated into the framework 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 volumes of 0.762 1 and 0.689 4 m³/g and BET surface areas of 986.42 and 756.8 m²/g, respectively. Dimethyl sulfide with a molecular size 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 of 58 μg/g, the desulfurization capacity of Ce-MCM-41 is 7.52 mg(S)/g, higher 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.
- dimethyl sulfide /
- mesoporous molecular sieves /
- heteroatom /
- Ce-MCM-41 /
- adsorption /
- desulfuration

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