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    李红霞, 张涛, 唐盛伟. 负载离子液体调节MCM-36上异丁烷和1-丁烯的相对吸附量[J]. 华东理工大学学报(自然科学版), 2016, (6): 743-751. DOI: 10.14135/j.cnki.1006-3080.2016.06.001
    引用本文: 李红霞, 张涛, 唐盛伟. 负载离子液体调节MCM-36上异丁烷和1-丁烯的相对吸附量[J]. 华东理工大学学报(自然科学版), 2016, (6): 743-751. DOI: 10.14135/j.cnki.1006-3080.2016.06.001
    LI Hong-xia, ZHANG Tao, TANG Sheng-wei. Immobilizing Ionic Liquid on MCM-36 to Modulate the Relative Adsorption Capacities of Isobutane and 1-Butene[J]. Journal of East China University of Science and Technology, 2016, (6): 743-751. DOI: 10.14135/j.cnki.1006-3080.2016.06.001
    Citation: LI Hong-xia, ZHANG Tao, TANG Sheng-wei. Immobilizing Ionic Liquid on MCM-36 to Modulate the Relative Adsorption Capacities of Isobutane and 1-Butene[J]. Journal of East China University of Science and Technology, 2016, (6): 743-751. DOI: 10.14135/j.cnki.1006-3080.2016.06.001

    负载离子液体调节MCM-36上异丁烷和1-丁烯的相对吸附量

    Immobilizing Ionic Liquid on MCM-36 to Modulate the Relative Adsorption Capacities of Isobutane and 1-Butene

    • 摘要: 通过接枝将离子液体1-烷基-3-(三乙氧基硅丙基)咪唑硫酸氢盐(烷基:甲基、乙基、丁基)在MCM-36分子筛表面进行负载改性,通过1H-NMR、FT-IR、XPS、TGA、XRD、SEM、BET和正丁胺回滴法等对改性的MCM-36(MCM-36-ILs)进行表征。结果表明酸性离子液体通过化学作用在MCM-36表面进行负载;负载离子液体的催化剂可以在350℃以下稳定存在而不分解;负载离子液体能增加固体酸催化剂表面的酸量,但比表面积和平均孔容有一定程度的降低。Sip模型能很好描述异丁烷、1-丁烯在MCM-36负载离子液体前后固体酸催化剂上的平衡吸附量。异丁烷、1-丁烯在离子液体改性的MCM-36上的吸附性能与离子液体结构、离子液体负载量及催化剂表面特性等有关。负载酸性离子液体可以调节MCM-36上烷烯吸附比(nI/nO,相同压力下分子筛上吸附的异丁烷和1-丁烯的物质的量之比)。经1-乙基-3-(三乙氧基硅丙基)咪唑硫酸氢盐负载改性的MCM-36具有较好的烷烯吸附比调节性能,其表面的烷烯吸附比最高可以达到0.95,接近于烷基化反应所需的化学计量比。催化剂表面烷烯吸附比的改善有利于提高催化剂的性能和目标产物的选择性。

       

      Abstract: MCM-36 was modified by grafting ionic liquids (ILs) 1-alkyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfates (alkyl:methyl,ethyl,butyl).The modified MCM-36 catalysts (MCM-36-ILs) were characterized by 1H-NMR,FT-IR,XPS,TGA,XRD,SEM,BET and an n-butylamine titration method.The results show that the ILs were immobilized on MCM-36 by chemical bonds.MCM-36-ILs were stable below 350℃.The immobilizing of acidic ILs led to an increase of acid amount and a certain decrease of specific surface area and average pore volume of MCM-36.The equilibrium adsorption capacities of isobutane and 1-butene on MCM-36 and MCM-36-ILs could be described well by Sip model.The adsorption behaviors of isobutane and 1-butene on MCM-36-ILs were affected by the structure of IL,the loading amount of IL and the surficial properties of solid catalyst.The adsorption molar ratio of isoparaffin to olefin (nI/nO) on MCM-36 could be adjusted by supporting acidic ionic liquids.In this study,an adsorption nI/nO of 0.95 on MCM-36 loaded by 1-ethyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfate was achieved,which approximated to the stoichiometric coefficient of C4 alkylation process.The improvement of adsorption nI/nO on solid acid catalyst is beneficial to the improvement of catalyst properties and the selectivity of objective products.

       

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